Biomaterials

in Food Packaging
Biomaterials

in Food Packaging

edited by
Mohd Yusuf

Shafat Ahmad Khan

Published by

Jenny Stanford Publishing Pte. Ltd.

101 Thomson Road
#06-01, United Square
Singapore 307591

Email: [email protected]
Web: www.jennystanford.com

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Biomaterials in Food Packaging

Copyright © 2022 Jenny Stanford Publishing Pte. Ltd.

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ISBN 978-981-4877-98-5 (Hardcover)

ISBN 978-1-003-25678-6 (eBook)
 Contents

Preface xiii

1. Biomaterials for Food Packaging:

An Overview 1

Fazilah Ariffin, Hanisah Kamilah, Kaiser Mahmood,

and Alias A. Karim
1.1 Introduction 2

1.2 Categories of Biomaterials 3

1.3 Advantages and Disadvantages of Biomaterials 8

1.4 Degradation of Biomaterials 9

1.5 Biomaterials vs. Synthetic Plastics for

Food Packaging 12

1.6 Methods of Forming

Biomaterial-Based Packaging 17

1.6.1 Film Preparation Methods 17

1.6.2 Advancements in Packaging Material

Development 21

1.7 Safety Concerns of

Biomaterial-Based Packaging 29

1.8 Global Trends toward Biodegradable

Polymers Packaging 33

1.9 Conclusion 35

2. Active Ingredients Enabled Edible Coatings and

Films Improve Shelf Life of Food: An Overview 49

Tanvir Arfin
2.1 Introduction 50

2.2 Background 51

2.3 Functions and Advantages 52

2.4 Importance of EC and EF 53

2.5 Structural Matrix 53

2.6 Synthesis of EF 55

vi Contents

2.7
Barrier Feature 55
2.8
Active Biopackaging 55
2.9
Chemistry of EF and EC 57
2.9.1 Polysaccharide 58

2.9.2 Protein 65

2.9.3 Composite 68

2.10
Economic and Nutritional Influences 69
2.11 Protection of Food Product:

Mechanism Phenomena 70

2.12
Healthy Foods: Public Demands 70

2.13
Conclusion 70

3. Surface Chemistry for Intelligent Food Packaging 83

Sivapriya Veeraiyan, Abdul Azeez Nazeer,

Saravanan Dhandapani, and

Sudarshana Deepa Vijaykumar

3.1 Introduction 84

3.2 Simple Food Package and Intelligent Devices 85

3.3 Intelligent Packaging Technique 86

3.4 Devices Used in IPT 86

3.5 Indicators of IPT 87

3.5.1
Temperature Indicators 87
3.5.2
Gas Indicators 89
3.5.3
Freshness Indicators 90
3.5.4
Sensors 92
3.5.5
Data Carriers 97
3.6 Other IPT Systems 99

3.7 Summary and Future Prospects of IPT 99

4. Brief Overview of Aspiring Properties of Functional

Biopolymers for Food Packaging Applications 105

Pooja Agarwal, Anjali Gupta, and Divya Tripathy

4.1 Introduction 106

4.2 Biopolymer 107

4.2.1 Polysaccharide-Based Biopolymer 108

4.2.2 Synthetic Biopolymer 109

 Contents vii

4.3 Desirable Properties of Biopolymers for

Food Packaging Application 111

4.3.1 Gas Barrier 111

4.3.2 Thermal and Mechanical 112

4.3.3 Moisture Barrier 113

4.3.4 Biodegradability 114

4.4 Functional/Active Packaging 114

4.5 Conclusion 116

5. Recent Research and Development in

Food Packaging Technologies: A Review 121

Syed Dilshad Alam, Rupak Raja, Vikas Shirsath,

Arvind Kumar Jain, Shafat Ahmad Khan, and

Imran Ali

5.1 Introduction 122

5.2 Key Functions and Requirements of

Food Packaging 122

5.3 Packaging Technologies Prospects 123

5.3.1 Conventional Technology 124

5.3.2 Modern Technology 124

5.4 Conclusion and Future Dimension 131

6. Edible Coatings: Recent Advancements on

Protein- and Polysaccharide-Based Films 137

Anjali Gupta, Divya Tripathy,

Meenu Aggarwal, and Pooja Agarwal

6.1 Introduction 138

6.2 Protein-Based Edible Films and Coatings 139

6.2.1 Globular Proteins 140

6.2.2 Fibrillar Proteins 143

6.3 Polysaccharide-Based Edible

Films and Coatings 144

6.3.1 Starch-Based Coatings and Films 145

6.3.2 Cellulose-Based Coatings and Films 147

6.3.3 Chitosan-Based Coatings and Films 147

6.3.4 Pectin-Based Coatings and Films 148

6.3.5 Alginate-Based Coatings and Films 149

6.4 Conclusion 150

viii Contents

7. Characterization of Cassava Starch-Zinc

Nanocomposite Film for Food Packaging 159

Adeshina Fadeyibi
7.1 Introduction 160

7.2 Materials and Methods 162

7.2.1 Synthesis and Particle Size Analysis of

Nanoparticles 162

7.2.2 Development of Nanocomposite Film 162

7.2.3 Determination of Structural and

Barrier Properties 163

7.2.4 Determination of Thermal and

Rheological Properties 165

7.3 Results and Discussion 166

7.3.1 Permeability of Nanocomposite Film 166

7.3.2 Thermal Stability of

Nanocomposite Film 169

7.3.3 Mechanical Properties of

Nanocomposite Film 170

7.3.4 Structural Stability of

Nanocomposite Film 173

7.4 Conclusion 176

8. Review on Advanced Food Packaging Materials

Based on Functional Biopolymer Matrix 181

Md. Aftab Alam, Rizwana Khatoon, Shamsul Huda,

and Pramod Kumar Sharma

8.1 Introduction 182

8.2 Origin and Description of Bio-Based Polymers 184

8.3 Polysaccharides 184

8.3.1 Plant-Based Polysaccharides 185

8.3.2 Animal-Based Polysaccharides 187

8.4 Proteins 191

8.4.1 Plant-Based Proteins 191

8.4.2 Animal-Based Proteins 193

8.4.3 Microbial-Based Proteins 195

 Contents ix

8.5 Edible Films and Coatings 196

8.6 Properties of Edible Films 197

8.6.1 Antimicrobial Activity 197

8.6.2 Antioxidant Activity 197

8.7 Alginate-Based Edible Films 198

8.8 Protein-Based Edible Films 198

8.9 Fossil-Based Biopolymeric Blends 199

8.10 Future Perspective 199

8.11 Conclusion 200

9. Prospects of Nanomaterials in Active Finishing

of Food and Food Packaging: A Review 219

Divya Bajpai Tripathy, Anjali Gupta,

and Pooja Agarwal

9.1 Introduction 220

9.2 Food Packaging Applications of Nanomaterials 221

9.2.1
Protective Finishing of Food 222
9.2.2
Enhancement of Barrier Properties 222
9.2.3
Active Packaging 222
9.2.4
Intelligent or Smart Packaging 223
9.2.5
Surface Biocides 224
9.2.6
Antioxidant Properties 224
9.2.7 Detection of Spoilage and Pathogenic
Microorganisms 225
9.2.8
Humidity Indicators 226
9.2.9
Bio-Based Food Packaging 227
9.3 Nanotechnology: Environmental and

Human Safety Prospects 227

9.4 Conclusion 227

10. Applications of Nano-Biocomposite Materials

as Antimicrobial and Antioxidant Finishing

Agents for Packaged Food Products 233

Md. Aftab Alam, Rizwana Khatoon, Shamsul Huda,

Niyaz Ahmad, and Pramod Kumar Sharma

x Contents

10.1 Introduction to Nanotechnology in

Food Packaging Systems 234

10.2 Packaging Technologies Based on

Nanotechnology 236

10.2.1 Nanotechnological Systems for

Active Packaging 236

10.2.2 Nanotechnological Systems for

Smart/Intelligent Packaging 238

10.2.3 Nanotechnological Systems for

Improved Packaging 241

10.3 Biodegradable Nanocomposites 242

10.4 Other Polymer Matrix-Based

Nanocrystal Systems 243

10.5 Conclusions and Future Perspective 246

11. Antioxidant Finishing Enabled Packaging

for Improved Shelf Life of Food 257

Meenu Aggarwal, Anjali Gupta, Vanita Sapra,

Meenakshi Singhal, and Nisha Saini

11.1 Introduction 258

11.2 Current Challenges in

Food Packaging Industry 258

11.3
Smart Packaging Systems 259

11.4 Biopolymer Packaging:

Edible Films and Coverings 261

11.4.1 Bioactive Packaging 261

11.4.2 Antioxidant Properties in

Biopolymer Packages 262

11.5
Nanotechnology in Food Packaging Industry 267
11.6
Conclusion and Future Remarks 268

12. Active Finishing Agents for Food

Bio-Preservation Based on Natural Origin
to Prevent Microbial Risks 275
Smrita Singh, Lalit Prasad, Ashutosh Singh Chauhan,
and Shafat Ahmad Khan
 Contents xi

12.1 Introduction 276

12.2 Active Finishing Agents from

Bacterial World in Food Preservation 277

12.2.1 Major Derived Components 277

12.2.2 Minor-Derived Components 280

12.3 Toxicological and Safety Aspect 285

12.4 Conclusion and Future Outlook 286

13. Upsurgence of Bio-Based Packaging Materials:

Emphasis on Biodegradable Plastics

as a Greener Alternative 293

Divya Bajpai Tripathy, Pinki Chakraborty,

Munesh Sharma, and Mohd Yusuf
13.1 Introduction 294

13.2 Types of Biodegradable Plastics 295

13.2.1 Polyhydroxyalkanoates 299

13.2.2 Polylactic Acid 299

13.2.3 Starch-Based Plastics 299

13.2.4 Cellulose-Based Plastics 300

13.2.5 Lignin-Based Polymer Composites 300

13.3 Bioplastics vs. Compostable Plastics 300

13.4 Mechanism of Biodegradation 300

13.5 Factors Influencing Biodegradation 302

13.5.1 External Factors 302

13.5.2 Internal Factors 304

13.6 Economic Aspects 305

13.7 Industrial Aspects 306

13.8 Conclusion and Future Outlook 307

Index 313

 Preface

This book presents fundamental to advanced knowledge and

practical applications of the food packaging materials derived
from natural resources. It not only encompasses a comprehensive
overview of environment-compatible and biodegradable
biomaterials but also highlights the recent trends in their
applications in food packaging. The book successfully provides a
cool answer to develop biodegradable materials as a promising
alternative to their harmful synthetic counterparts. With 13
chapters prepared by prominent contributors from reputed
institutes, it provides the reference material that includes current
developments and the future outlook on the theme and discusses
the advances made in bioactive, biodegradable, and edible films
and nano-based smart materials for food packaging applications
that can substitute their synthetic counterparts to enhance food’s
shelf life significantly.
Our sincere thanks go to the eminent authors for their valued and
priceless contributions with informative coverage. The readers are
welcome to provide us their valuable comments and suggestions,
which will help to improve future volumes.
We are highly grateful to our research guide, Dr. F. Mohammad, ex-
professor, Department of Chemistry, Faculty of Natural Sciences,
Jamia Millia Islamia, India. We would also like to thank Jenny
Stanford Publishing, especially Ms. Jenny Rompas and Mr. Stanford
Chong, for inviting us to compile this volume.

March 2022
Mohd Yusuf, Editor
Associate Professor
Department of Natural and Applied Sciences
School of Technology, The Glocal University
Mirzapur Pole, Saharanpur, Uttar Pradesh 247121, India

Shafat Ahmad Khan, Coeditor

Assistant Professor
Department of Chemistry, Galgotias University
Greater Noida, Uttar Pradesh 203201, India
Chapter 1

Biomaterials for Food Packaging:

An Overview

Fazilah Ariffin,a Hanisah Kamilah,b Kaiser Mahmood,a and

Alias A. Karima
a Food Technology Division, School of Industrial Technology,

Universiti Sains Malaysia, Penang, Malaysia

b Faculty of Agriculture, Science and Technology, Universiti Putra Malaysia,

Bintulu Sarawak Campus, Bintulu, Sarawak, Malaysia

[email protected]

The food industry is growing tremendously, where food packaging

materials are being widely used. Currently, most of the food packaging
materials are made of fossil-fuel sources, known as synthetic plastics.
The passive degradation products of synthetic packaging materials
are piling up pollution to the environment, typically to marine life.
It is estimated that the synthetic plastics will occupy more than half
of the sea by 2050, overriding the marine population. Indirectly, the
food supply will be declined, which needs to be ameliorated. Hence,
utilizing biomaterials is preferable for food packaging, since these
are eco-friendly and biodegradable. In this chapter, a few major
groups of biomaterials, which are potential alternatives to synthetic
packaging materials, such as (i) directly extracted from biomass:
polysaccharides, lipids, and proteins; (ii) produced by microbes:

Biomaterials in Food Packaging

Edited by Mohd Yusuf and Shafat Ahmad Khan
Copyright © 2022 Jenny Stanford Publishing Pte. Ltd.
ISBN 978-981-4877-98-5 (Hardcover), 978-1-003-25678-6 (eBook)
www.jennystanford.com
2 Biomaterials for Food Packaging

polyhydroxyalkanoate (PHA), bacterial cellulose, and xanthan;

and (iii) obtained by polymerization route: polylactic acid, will be
discussed. The methods (solution casting, blending, extrusion, and
others) and current trends (electrospinning and 3D printing) in
developing bio-based active materials will also be summarized.
The technical advancements in the field of food packaging will ensure
sustainable food supply, conserve the ecosystem, and ultimately
assist in accomplishing the goals of Industry 4.0.

1.1 Introduction

The synthetic plastics industry has been growing widely since World
War II. The polymer industry has been developing since then to
replace and fulfil the shortage of silk. In 2015, about 320 million tons
of synthetic plastics were produced, globally, and the production is
continuously increasing up to 5% annually. The sources of synthetic
plastics are mainly petroleum and natural gases. Approximately
7% of the sources are being used to produce plastics, and 40% of
the total production is oriented for packaging. Currently, plastic
is synthesized to be resistant against water, air, sunrays, or any
substance that a plastic may encounter in the environment. Synthetic
plastics, such as polyethylene terephthalate (PET), polyvinylchloride
(PVC), polyethylene (PE), polypropylene (PP), polystyrene (PS), and
polyamide (PA), are in high demand, due to their high-resistance
property. These synthetic plastics are preferable in packaging, as
they provide convenience and containment to ensure the quality of
packaged food products. The low price of the synthetic plastics with
excellent mechanical properties, better tensile strength, good barrier
to oxygen and carbon dioxide, heat sealability, and durability of the
plastics are preferable for daily usage of food packaging [1, 2].
However, resistance and accumulation of synthetic plastics
have caused tremendous pollution to the environment, including
the marine habitat, as they require longer period to degrade. The
swallowed plastic particles by fish may transfer to human by the
food cycle and risk to cause various diseases. It is predicted that
by 2050, the accumulation of synthetic plastics will override the
marine population. Hence, the food supply will be reduced, and it
is unfortunate that the human population is expected to increase
  Categories of Biomaterials 3

thrice, reaching up to ~9 million by 2050 [3]. Currently, there is no

efficient method to recycle used synthetic plastics. The presence of
food waste and biological substances mixed with the used synthetic
plastics make them difficult to be recycled and reused.
Thus, it is important to develop biomaterial-based packaging
that has comparable properties as synthetic plastics, yet degradable
and environmental-friendly [4]. Hence, this chapter will discuss
the current findings on biomaterials as food packaging. It will also
include technological advancements in biomaterials, as bio-based
active materials to overcome packaging issues in the supply chain.
This information will be crucial to prepare biomaterial-based food
packaging, especially in pursuance of Industry 4.0.

1.2 Categories of Biomaterials

Biomaterials are vastly available in nature and few exist in the form
of dry materials. Most of them are fully degraded in the environment
and produce natural by-products, such as gases (nitrogen and carbon
dioxide), water, biomass, and inorganic salts [5−8]. Based on the
European standard EN 16575, a biomaterial is derived from biomass,
which has biological origin and not a material that is embedded in
geological formations (EN 16575, 2014) [9].
Nowadays, biomaterials have become the main focus in replacing
synthetic plastics, especially for food packaging. This is due to
the degradable characteristic and relatively short functional life
(disposable) of the biomaterials. The lower carbon footprint or
renewable resources are the key factors that lead to the development
of biomaterials. Since 2013, biomaterials have replaced 5−10%
of synthetic plastics in the market [8]. The biomaterials can be
formed naturally or synthetically, and most of their composition are
consisted of ester, amide, and ether functional groups that determine
their properties [10].
Basically, biomaterials can be divided into two large groups: agro­
polymers and biopolyesters. The agro-polymers are polymers that are
derived from biomass, including polysaccharides and proteins. The
structure of polysaccharides is formed by the presence of glycosidic
bond, where the hemiacetal or saccharide is bonded to alcohol via
loss of water. Cellulose, hemicellulose, and lignin are the foremost
4 Biomaterials for Food Packaging

natural polymers [11, 12]. Modified natural polymers that consist

of starch and cellulose derivatives are also the examples of agro­
polymers. These polymers are available under the trade names as
Mater-Bi®, Solanyl®, BIOpar®, Cellgreen® Cornpol®, and Cellgreen®.
Amino acids are the main components that form proteins. The amino
acids link to each other by the reaction of condensation and form
peptide bonds that consist of amide functional groups. Table 1.1
shows the properties and applications of common agro-polymers in
food packaging.
Whilst, the biopolyesters are polymers that are synthetically made
by polymerization or extracted from microorganisms. Synthetically
made biomaterials produced by chemical polymerization of

Biomaterials

Biopolyesters Agro- polymers

Microorganisms
Synthetic Polysaccharides Proteins
(viaextraction)

Collagen
Polylactic acid Polyglycolide Alginate

Polyhydroxy- Gelatin
alkanoate Carrageenan
Poly(lactic-co­
glycolicacid)

Wheyprotein
Cellulose

Gellan Soy protein

Pectin Zein

Pullulan

Starch

Xanthan

Figure 1.1 Classification of biomaterials [6, 7].

Table 1.1 Properties and applications of common agro-polymers in food packaging

Agro­ Thermal property Tensile Degradation Structure Application Reference

polymer strength period
(MPa) (days)
Tm Tg
(°C) (°C)
Starch 60−80 77−90 3−20 15−21 Amylose (α-1,4 glycosidic linkage) Paper [13−16]
making, food
packaging,
thickener,
food
ingredients,
Amylopectin (α-1,6 glycosidic linkage)
etc.

 Categories of Biomaterials
(Continued)

5
Table 1.1 (Continued)

6
Biomaterials for Food Packaging
Agro­ Thermal property Tensile Degradation Structure Application Reference
polymer strength period
(MPa) (days)
Tm Tg
(°C) (°C)
Cellulose 260−270 180−230 200−4600 18−20 Food [17−19]
coating, food
packaging,
food additives

Gelatin 30−40 217−230 123−126 10−15 Food coating, [20−23]

paper
making, food
adhesives, etc.

Chitosan 290 140−150 50−80 ~30 Food [24, 25]

packaging,

nanofilm,

antioxidant

film,

antimicrobial

film

Table 1.2 Properties and applications of common biopolyesters in food packaging

Biopolyester Thermal Tensile Degradation Structure H2O O2 Application Reference

property strength period permeability permeability
(MPa) (months)

Tm (°C) Tg
(°C)
PLA 150−178 45−65 21−60 12−16 1.42−1.8 0.175−0.219 Food [26, 27]
×1013 ×1013 packaging,
O
(25 °C) (25 °C) antimicrobial
packaging,
O n
cold drink
cups,
cutleries, etc.
PGA 225−230 35−40 60−99.7 6−12 O
11 0.9−1.1 Food [26, 28]
HO
O
O
H
(g/m2•day) (cc/ packaging,

 Categories of Biomaterials
CH3
n
O
m
m2•day•atm) barrier
material
PHA 50−180 4−8 17−43 ~2 R O 0.168×1013 ≈0.09 ×1013 Food [29, 30]
(25 °C) (25 °C) packaging,
CH
O C paper coating
H2 m
n

7
8 Biomaterials for Food Packaging

monomers are derived from biological processes, for example,

poly(lactic acid) (PLA), poly(glycolic acid) (PGA), poly(lactic acid­
co-glycolic acid) (PLGA), or poly(ɛ-caprolactone) (PCL) [6]. Table
1.2 shows the common applications of biopolyesters complemented
with their properties. Biopolyesters are sold under the trade names
of NatureWorks®, Hycail HM, Hycail LM, Lacea®, U’z, GS Pla, and
Bionolla. PHA is an example of biopolyesters obtained via the
extraction from microorganisms. It is sold under the trade names
of Biomer®, MirelTM, Biogreen®, Biocycle®, and Biopol®. Figure 1.1
shows the overall biomaterials classification.

1.3 Advantages and Disadvantages of Biomaterials

The conventional plastics lack in degradability and caused environmental

pollution. Biomaterials require around 65% less energy to produce 1
kg mass, as compared to synthetic plastics and reduce the emission of
greenhouse gases (GHGs) about 30−80% [31, 32]. Biomaterials are also
suitable for production of compost to deliver nutrients and organic matters
to plants. Typically, biomaterials from starch degrades 10−20 times
faster than that of the synthetic plastics [33]. Incineration of synthetic
plastics generates toxic smoke and fumes, as compared to biomaterials,
which decomposes into natural gases in the environment. The possibility
of addition of various nanoparticles in the biomaterials results in
improved material stability against heat, controlled permeability, tensile
strength, and antimicrobial properties. Moreover, increasing demand
for biomaterials may reduce the emission of GHGs. More land will be
utilized to produce biomaterial feedstock, such as maize, oil palm, and
seaweed. Thus, it will reduce the GHG emission with direct or indirect
use of land [34, 35]. However, disadvantages of biomaterials still hinder
their preferred use as an alternative for food packaging. The abundant
usage of biomaterials may affect the agriculture sector by causing
eutrophication and acidification of soils or water. The faster degradation
of biomaterials may provide excessive nutrients to the plants that could
lead to their unfavorable growth and loss of crops.
  Degradation of Biomaterials 9

1.4 Degradation of Biomaterials

Biomaterials are preferable to be stable and durable; however, the

degradation property is the most crucial criterion to be used in
any application. The degradation of biomaterials normally begins
from end groups, as most of these biomaterials have strong carbon
backbone that is difficult to break. Thus, an area that has higher
surface tends to degrade first, due to the easy access of chemicals,
light, or microorganisms [6]. Commonly, biomaterials formed by
chain branching as crosslinking decreases the number of end groups
per unit weight.
The degradation of biomaterials forms gases, salts, and biomass.
Complete degradation is occurred when there is no oligomers and
monomers left [6, 7]. The major factors that influence the degradation
rate of biomaterials are: bond type, solubility, copolymerization, pH,
temperature, microorganisms, and humidity. The biodegradation
process is divided into two mechanisms: physical decomposition
and biological process. The physical decomposition occurs when
the reactions of hydrolysis and photo degradation occurred. This
may lead to partial or complete degradation. Whereas, the biological
process is divided into two conditions: aerobic and anaerobic. The
degradation that comes from aerobic condition (Eq. 1.1) produces
carbon dioxide (CO2) and water (H2O). However, methane (CH4)
together with CO2 and H2O is produced when the degradation is
exposed in an anaerobic circumstance (Eq. 1.2). Yet, within any
degradation condition, carbon (C) residues and biomass are always
obtained [7]. The general equations below show the summary of the
explanation:
Cpolymer + O2 → Cresidue + Cbiomass + CO2 + H2O (1.1)

Cpolymer + O2 → Cresidue + Cbiomass + CO2 + CH4 + H2O (1.2)

Numerous microorganisms could degrade natural polymers. The
microorganisms will digest the polymer’s fragments (oligomers or
monomers) to produce energy, adenosine triphosphate (ATP), and
biomaterials by-products (Eqs. 1.1 and 1.2). Oxidation and hydrolysis
reactions take place for the conversion and assisted by the enzymes,
which mainly are proteases, esterases, or glycosidases [7]. Few of
biomaterials can be hydrolyzed in water, but they are not totally
10 Biomaterials for Food Packaging

biodegradable, while the modified natural polymers can only be

enzymatically degraded. Contrary to biopolyesters, PHA undergoes
both the hydrolysis and enzymatic reactions [36].
It was reported that PGA degrades rapidly in aqueous solution.
Deterioration of mechanical integrity was observed within two to
four weeks. Addition of methyl group in the repeating unit of PLA
may result it to be more hydrophobic, reducing the molecular affinity
to water and leads to improve resistant against degradation. Thus,
the compound inside the structure has major influence toward
the potential degradation. Different biopolyesters have different
degradation rates. PCL is known as the slowest to degrade, as
compared to other biopolyesters. Thus, PCL is preferable to be
used in long-term implant and controlled release applications. Yet,
Woolnough and co-workers reported that PHA has the shortest period
of degradation (40−50 days) as compared to other biopolyesters
[37]. Having such unique properties, PHA are among the materials
of interest that could be chosen to replace petrochemical synthetic
polymers [29, 38, 39]. The degradation rates reduce in the following
manner [40]:
PHA > PGA > PLA > PCL
Unfortunately, the petroleum-based synthetic plastics require
hundreds of years to degrade. This is due to the long chain and unusual
bonds, including different organic and inorganic materials such as
carbon, hydrogen, chloride, oxygen, nitrogen, coal, and natural gases
[41]. Yet, recently, a small number of microorganisms have been
identified for their capability to degrade synthetic plastics (Table
1.3). The potential to degrade the synthetic plastics is suspected to
come from the enzymes of microbes, itself. However, the study is still
at the preliminary stage, thus, biomaterials are current alternatives
to mitigate the issues. Table 1.3 shows the microorganisms that
are capable to degrade biomaterials, including synthetic plastics.
Biodegradable Product Institute, an organization that encourages
recycling of biodegradable materials, has collaborated with American
Society for Testing and Materials (ASTM) to provide ASTM standards
(ASTM D6400, D6866). Thus, these standards are the principal
database for the degradation practices at industrial scale [42].
  Degradation of Biomaterials 11

Table 1.3 Microorganisms degrading polymers

Polymer Microorganism Reference

Synthetic polymer
PE Brevibacillusborstelensis, [43−47]
Comamonasacidovorans TB-35,
Pseudomonas
chlororaphis, P.
aeruginosa, P. fluorescens,
Rhodococcuserythropolis, R.
rubber, R. rhodochrous,
Staphylococcus cohnii, S.
epidermidis, S. xylosus,
Streptomyces badius, S. setonii,
S. viridosporus, Bacillus

amyloliquefaciens, B.

brevis, B. cereus, B. circulans, B.

circulans, B. halodenitrificans, B.

mycoides, B.

pumilus, B. sphaericus, B.

thuringiensis, Arthrobacter

paraffineus, A. viscosus,

Acinetobacter baumannii,

Microbacteriumparaoxydans,

Nocardia asteroides,

Micrococcus luteus, M. lylae,

Lysinibacillusxylanilyticus,

Aspergillus

niger, A. versicolor, A. flavus,

Cladosporium cladosporioides,

Fusarium redolens,

Fusarium spp. AF4, Penicillium

simplicissimum YK, P.

simplicissimum,

P. pinophilum, P. frequentans,

Phanerochaetechrysosporium,

Verticillium

lecanii, Glioclodiumvirens, Mucor

circinelloides, Acremonium

Kiliense,

Phanerochaetechrysosporium

12 Biomaterials for Food Packaging

Polyvinyl chloride Pseudomonas fluorescens B-22, [43, 47]

(PVC) P. putida AJ, P. chlororaphis,
Ochrobactrum
TD, Aspergillus niger
Polyurethane (PU) Comamonasacidovorans TB­ [43, 44, 47]
35, Curvularia senegalensis,
Fusarium solani,
Aureobasidium pullulans,
Cladosporium sp., Trichoderma
DIA-T spp.,
Trichoderma sp.,
Pestalotiopsismicrospora
Biopolyester
Poly(3­ Pseudomonas lemoignei, [43, 44, 47]
hydroxybutyrate) Alcaligenes faecalis,
(PHB) Schlegelellathermodepolymerans,
Aspergillus fumigatus, Penicillium
spp., Penicillium funiculosum
Poly(3­ Clostridium botulinum, C. [43, 44, 47]
hydroxybutyrate­ acetobutylicum, Streptomyces sp.
co­ SNG9
3-hydroxyvalerate)
(PHBV)
PCL Bacillus brevis, Clostridium [43, 44, 47]
botulinum, C. acetobutylicum,
Amycolatopsissp,
Fusarium solani, Aspergillus
flavus
PLA Penicillium roqueforti, Bacillus [43]
brevis, Rhizopus delemar
Source: Reproduced from Pathak and Navneet [42].

1.5  Biomaterials vs. Synthetic Plastics for Food

Packaging

Several efforts have been made to substitute synthetic plastics

with biomaterials for food packaging. However, few obstacles and
challenges need to be overcome and evaluated prior to the full or
Table 1.4 The comparison of synthetic polymers and biomaterials based on their properties (mechanical and barrier) and applications

Synthetic polymer
Polymer Melting Tensile Elongation at Young’s H 2O O2 permeability Application Reference
temperature, strength break (%) modulus permeability
Tm (°C) (MPa) (GPa)w
Low-density 110 13.65 533.49 0.3 93×1013 5.18×1013 (25 °C) Trays, juice [50, 51]

polyethylene (25 °C) cartons, plastic

(LDPE) wraps, etc.

-Polyolefin

 Biomaterials vs. Synthetic Plastics for Food Packaging

High-density 120−135 18 >70 1.095−1.25 137 0.31×1013 (25 °C) Oxygen barrier [52−54]

polyethylene (37.8 °C) materials,

(HDPE) (gm.cm/cm2.s) 3D printing

-Polyolefin plastics, etc.

PP 162−175 24.5 493 0.855 38.3×1013 (25 0.77×1013 (25 °C) Microporous [55−57]
-Polyolefin °C) membranes,
glame-
retardant films
PVC 100 3.8 240 7.19 1–2×1013 (23 °C) 0.02–0.09×1013 Electrical [58, 59]
-Vinyl (23 °C) carriers
PS 100 48.9 5.6 1.3 0.78–3.9 1.34–1.79×1013 Filtration films [60, 61]
-Styrenic (g.mm/ and beads, etc.
m2.day)

(Continued)

13
Table 1.4 (Continued)
Synthetic polymer

14
Polymer Melting Tensile Elongation at Young’s H 2O O2 permeability Application Reference

Biomaterials for Food Packaging

temperature, strength break (%) modulus permeability
Tm (°C) (MPa) (GPa)w
PET 270 55–75 50–150 2.8–3.1 0.5–2×1013 0.01–0.06 ×1013 Plastic bottles [62]

-Polyester (23 °C) (23 °C)

Polybutylene 223−250 54−143 25 2.8−10 2.27 537 Insulators, [63, 64]

Terephthalate (g 100 μm m−2 (cm3 (STP) 100 thermoplastics,

(PBAT) d−1 mbar−1) mm m−2 d−1 bar−1) etc.

-Polyester
Polycarbonate 190 55−75 80−150 2−2.4 1400×1010 1.4×1010 Electronic [65]

(PC) (25 °C) (25 °C) components,

-Polyester construction

materials, etc.

Biomaterial
Alginate 150 25.8 2.5−5 13 25.745×10−6, 8.94×10−6(mL.mm/ Food coatings [66]
(g.m/Pa.h.m2) m2.day.pa)
Carrageenan 70 45.7−70.16 8.3−10.76 0.04 1.16 45 Coatings, [66]
(×10−9 g m/m2 (cm3/mm2/24h) encapsulation
Pa s) aromatic
compounds
Cellulose 260–270 118−120 14 0.07 142.78×10−13 0.0015×10−13 Cellophane [67, 68]
(25 °C) (25 °C) packaging films

(Continued)
Table 1.4 (Continued)

Synthetic polymer
Polymer Melting Tensile Elongation at Young’s H2O O2 permeability Application Reference
temperature, strength break (%) modulus permeability
Tm (°C) (MPa) (GPa)w
Chitin >300 13−80 0.6−10 0.3−2 ­ 0.003 Packaging films, [69−71]
paper making,
etc.
Chitosan 220−290 8.25−14.6 16.8−45.9 0.07 12×10−13 0.00122×10−13 Edible [70, 71]
(25 °C) (25 °C) membranes
and coatings,
packaging films
Galacto­ 100−110 1−7 35−70 0.2 6.78−10.69 1.64−2.94 × 10−15 Edible coatings [72−74]

 Biomaterials vs. Synthetic Plastics for Food Packaging

mannan ×10−11 g m (Pa s m2)−1 and films
(g m−1 Pa−1 s−1)
Konjac 103−107 12 7.5−10 2.7−3 1.37 ×1014 8−10 Edible films [75, 76]
Glucomannan (kg Pa−1 s−1 m−1)
cm3·µm/(m2·d·kPa)
Starch 60−70 2.85−9.9 13−21.4 2.7 9.25×10−13 0.0140×10−13 Flexible [77, 78]
(25 °C) (25 °C) packaging, rigid
packaging as
thermoformed
trays
Gellan gum 70−80 2.14−3.70 12.2−14.98 0.039−0.058 352−489 - Edible coatings [79, 80]
(g m−2d−1) and flavor
encapsulation
materials
Pullulan 95 32−41 3.2 1.8 7.053×10−6(g.m/ 0.48×10−6(mL.mm/ Coating, [81]
Pa.h.m2) m2 .day.Pa) seasoning bags

15
16 Biomaterials for Food Packaging

partial replacement of synthetic plastics. An ideal biopolyester as

food packaging material should be resistant to environmental factors
of food deterioration, such as temperature, oxygen or carbon dioxide,
humidity, and light or external forces. The preferable food packaging
is mostly relying on the type of food products intended to be packaged.
Food products, such as beer or soft drinks, require an opaque and
air impermeable packaging. However, fruits and vegetables require a
permeable packaging for the transfer of oxygen and carbon dioxide,
and moisture exchange [48]. Hence, the barrier, mechanical, and
thermal properties are crucial in the selection of a food packaging.
Generally, an ideal packaging material is with a lower rate of oxygen
permeability and water vapor permeability. The characteristics of
limited light transmission and resistance to mechanical or thermal
risks are also preferable in food packaging [49]. Table 1.4 shows
the comparison of biomaterials and synthetic plastics in term of
properties and applications.
On the other hand, the costs of biomaterials and synthetic
plastics have a substantial difference when the weight basis is
considered. Biomaterials have higher density as compared to the
synthetic plastics. PLA is preferable than PS, as the film thickness
can be altered to less thickness of up to 0.66 mm [82]. It is expected
that the price of synthetic plastics will rise, due to the fluctuation in
petroleum prices. Thus, the biomaterials price will reduce with the
circumstances of economic production and conversion into products.
Table 1.5 shows the difference of price between the synthetic plastics
and biomaterials.

Table 1.5 Price level of synthetic plastics and biomaterials in 2016 [9]

Biomaterial Price level (€/kg) Density (kg/m3)

Plastic
Cellulose acetate 5 1200−1300
Bio-polyamide +10−20% 1040−1190
Bio-polyethylene +20−40% 910−970
Bio-polyethylene terephthalate - 1370−1390
Bio-polypropylene +80−100% 900−920
Polypropylene (Certified bio) +40−50% 900−920
Polybutylene adipate terephthalate 3.5 1250
(Continued)
  Methods of Forming Biomaterial-Based Packaging 17
Table 1.5 (Continued)

Biomaterial Price level (€/kg) Density (kg/m3)

Plastic
Bio-polybutylene succinate 4 1260
Polyhydroxyalkanoate 5 1200−1250
Polylactic acid 2 1250
Polytrimethylene terephthalate 4 1320
Starch blend 2−4 1250−1350
Synthetic plastic
Low-density polyethylene 1.250−1.450 910−940
High-density polyethylene 1.200−1.500 930−970
High-impact polystyrene 1.350−1.525 1080
Polyethylene 0.850−1.050 1370−1390
Polypropylene 1.000−1.200 900−920
Polystyrene 1.250−1.430 1040
Polyvinyl chloride 0.800−0.930 1100−1450

1.6  Methods of Forming Biomaterial-Based

Packaging

1.6.1 Film Preparation Methods

Biomaterial film is known as a dried and extensively interacting
polymer network with three-dimensional gel structure. The film is
formed by a spatially rearranged polymer matrix, which has been
incorporated with plasticizer, solvent, and other additives. The
formation processes of biomaterial films can be divided into two
groups: wet and dry processes [83].

1.6.1.1 Wet process

It is also known as solvent casting technique that is based on the

controlled drying of the film forming polymer solution (Figure 1.2).
This method consists of three steps: (i) polymer solubilization, (ii)
pouring or casting, and (iii) drying under controlled temperature
and humidity [84]. In the solubilization of biomaterials, the choice of
18 Biomaterials for Food Packaging

solvent is water, alcohol, or their mixture and some organic solvents.

The solvent for food grade packaging development is water and
alcohol or a combination of both. The polymer solution is casted
through an applicator at a uniform thickness on a smooth surface of
glass or Teflon. To obtain the cohesive matrix of the film, the formation
of three-dimensional continuous network of polymer chains is very
crucial. This depends on the biomaterial and solvent types, pH of
the solution, drying temperature, rate of drying, and final moisture
content. During the drying process, solvent evaporation enhances
the polymer chain entanglement and results in a gelling state that
shifts to a solid matrix after further drying [85]. Various additives
are admixed to improve the processability and enhance mechanical
or barrier properties of the casting films. Common additives include
plasticizers, emulsifiers, antimicrobials, antioxidants, micro or
nanoparticles, and cross-linkers. Generally, the solvent casting is
conducted either in a continuous manner or isolated molds in batch
process. Solvent casting is carried out with the solution of polymers,
but not with the polymer melts, hence, the severe anisotropic effect
is not observed in the films. Moreover, this technique does not
exert any thermal stress on the polymer. Currently, various types
of blended, layered and composite films are designed through
casting, with different kinds of biomaterials and natural nanofibers
or nanocrystals, or inorganic metals or organoclays are mixed to
tailor the functional properties of the resulting films for packaging
applications [86].

Figure 1.2 Casting method of biomaterial film.

  Methods of Forming Biomaterial-Based Packaging 19

1.6.1.2 Dry process

Dry process is based on the thermoplastic properties of biomaterials.

Usually, the thermoplastic biomaterials are heated above the glass
transition temperature (Tg) and in low moisture contents. Heat
changes the amorphous polymers into soft and rubbery state, which
assists the formation of films after cooling. The dry method requires
more equipment as compared to wet process, yet the dry method
provides the platforms of industrial implementation and reduces the
solubility of a biomaterial film. This is resulting from highly cross­
linked film network that is developed from the film forming process.
Examples of dry process of biomaterial film formation methods are
extrusion, thermoforming and coating [84, 87, 88].

1.6.1.2.1 Extrusion

The required time and space for preparation and drying of casting
films make the process limited to be adopted in industries. Extrusion
is an alternative technique that facilitates the commercial production
process [88] (Figure 1.3). In this technique, the granular polymer
material is processed after melting it. An extruder is used, which is a
screw conveyer, and has heated barrel where feed material is melted
and squeezed under pressure and temperature and forced through
a die to get a sheet. There are several types of extrusions, such as
hot extrusion, cold extrusion, warm extrusion, friction extrusion, and
micro extrusion [84]. In the extrusion process, the molecular structure
of biomaterials is modified by aligning due the flow. Additionally, the
screw speed, feed rate, heat and mechanical energy, and die shape
determine the extent of aggregation, denaturation, or crosslinking
of the polymeric chains [89]. Similar to the process of casting, some
additives or plasticizers are added in the extrusion process to improve
the processability of polymers [88]. The extrusion and compression
moldings have been applied for thermoplastic biomaterials, such as
gelatin, soy protein, myofibrillar protein, whey protein, wheat gluten,
zein, different starches, and banana flour [84, 87].
20 Biomaterials for Food Packaging

Figure 1.3 The extrusion process of a biomaterial.

1.6.1.2.2 Thermoforming
Thermoforming is one of the methods to fabricate packaging films,
where a thermoplastic and viscoelastic polymer is heated under
pressure and cooled to form a sheet. The films are stabilized by
hydrogen bondings, covalent links, ionic interactions, or hydrophobic
interactions [89]. The thermoforming or thermo-pressing unit
consists of two thermostated plates that are used for pressing
polymers into sheets. The parameters of thermo-pressing, such as
working temperature, applied pressure, duration, moisture, and type
and percentage of additives, regulate the final product properties.
However, an adequately high temperature is mandatory to obtain
a desired degree of aggregation or denaturation of homogeneous
polymer films [90]. The denaturation sometimes favors the process
by exposing the functional groups and establishing new interactions,
leading to desired properties of the packaging materials [89].
In the case of sulfhydryl bonds in proteins, during the extrusion
processing, the crosslinking reaction is favorable and it results in
enhancement of physico-chemical properties of the packaging films
[91]. Thermoforming could be used alone or in combination with the
extrusion technique. This method makes possible to design single or
multilayered sheets, trays, or pots, which could be of great interest
in food packaging application. Biomaterials including proteins
and starches from various sources have been processed through
thermoforming method [84].
  Methods of Forming Biomaterial-Based Packaging 21

1.6.1.2.3 Coating
Coating is generally a thin layer of matrix forming biomaterial melts
(carbohydrates, lipids, proteins, or their mixture) applied on food
packaging films to improve the barrier or functional properties of the
packaging [92]. Polymer melts or emulsions are directly applied on
packaging for coating purpose. Coatings are sticky on the packaging
materials that sometimes used to fabricate layer-by-layer type of
packaging films with desired functionalities. However, adhesion of
coatings to food packaging materials remains challenging in case of
difference in the hydrophilicity of the both materials, hence addition
of surfactants in coating dispersions helps in improving the adhesion
and overall process of coatings [93]. Biomaterial-based coatings
could be applied by spraying, spinning, dipping, and rubbing [92].
The coatings are applied externally to the packaging material or
sandwiched between two layers of polymer films based on required
functionalities. Overall, the matrix of coatings is formed by two basic
mechanisms such as gelation/thermal coagulation and coacervation.
In the thermal coagulation or gelation process, heat denatures the
proteins or melts the starches followed by the precipitation and
gelation, respectively. However, cooling of dispersion of proteins
(gelatin) and polysaccharides (agar) induces gelation and results
in matrix formation. While, in case of coacervation, a charged
hydrocolloid is dispersed in water and later precipitated by adding
a non-electrolyte anti-solvent, such as ethanol. The phase change
is caused by the addition of an electrolyte either by crosslinking or
salting out. When two solutions of oppositely charged hydrocolloids
are mixed, the interaction results in precipitation of the resulting
complex and is termed as coacervation [94].

1.6.2 Advancements in Packaging Material

Development

1.6.2.1 Nanocomposites
Nanocomposites are the combination of polymers with non-
polymeric substances (fillers) of smaller than 100 nm in at least one
22 Biomaterials for Food Packaging

dimension to form a mixture with improved properties [95]. The

resultant nanocomposite material displays improved mechanical,
barrier, thermal, optical, electrical, and biodegradability properties,
as compared to conventional composites [96]. Nanofillers could be
classified as natural fibers from biomaterials or inorganic materials,
such as metals and organoclays. Polymer-clay nanocomposites
are usually obtained by using montmorillonite, kaolinite, saponite,
hectorite [97], carbon nanotubes, graphene nanosheets, and others
[98]. The greater surface area and higher aspect ratio (50–1000)
of montmorillonite with minimum platelet thickness (1 nm) make
it suitable for reinforcement of the nanocomposites [99]. Once the
polymers are mixed with clays, three types of nanocomposites are
obtained: intercalated, exfoliated, and tactoids. In intercalated
nanocomposites, single-polymer chains are sandwiched between
the clay layers, however, the system retains ordered stack type of
arrangements. In the case of exfoliated nanocomposites, the layers
of clays are delaminated and well dispersed between the polymer
chains. The formation of intercalated and exfoliated composites
depends on the type of the clays and the processing conditions [100].
In case of tactoids, the clay particles are dispersed in the polymer
matrix without separating the layers. Among these three types, the
exfoliated is suggested to present the most desirable properties of
nanocomposites.
Nanocomposites with submicron size of natural fibers as fillers
(microfibrils or nanocrystals) have been studied, where cellulosic
fibers from cotton, rice husk, bagasse, flax, hemp, wheat straw, kenaf,
bamboo, coir, date palm, oil palm, sisal, jute, curaua, and jowar have
been tested [101]. The relative advantages of the natural fibers
include low cost, biodegradability, and lightweight.
Cellulose microfibrils and nano-whiskers are two types of fillers
that have been used in developing nanocomposites. Microfibrils
have length in micrometers, while the diameter is in the range of
nanometers [102]. Nano-whiskers are crystalline cellulose obtained
after acid digestion of the amorphous components, and include
cellulose nanocrystals and nanorods [103]. Nanocomposites are
developed by three main pathways: (i) solution intercalation,
(ii) melt intercalation, and (iii) in situ polymerization. In the solution
  Methods of Forming Biomaterial-Based Packaging 23

intercalation method, firstly, the clay is thoroughly swelled in the

solvent and then the polymer is solubilized in the solvent. Later
both the components are combined, and the polymer chains
intercalate the layers of clay by displacing the solvent [104]. In
the melt intercalation, the polymer is heated above the melting
temperature and the clay is added, and the temperature is kept
higher under shear to accelerate the intercalation and exfoliation
of the clay. In in situ polymerization, organoclays and monomers
are combined, and the polymerization of the monomers is carried
out, which precisely locks the exfoliated particles of the clays
in the nanocomposites. Among these three methods, the melt
intercalation is the most desirable approach, as it is compatible
with the extrusion and other techniques of similar kinds. Moreover,
it is benign as no solvent is used in the process [104]. On the other
hand, the solution intercalation is just a type of solution casting that
is considered suitable for preparation of nanocomposites of many
biomaterials that degrade under high-processing temperature
[105].

1.6.2.2 Electrospinning
Electrospinning is a nanotechnological method through which
nanofibers are produced under the influence of electrostatic forces
(Figure 1.4). It is a simple and versatile technology and it has
enabled the development of encapsulated active components as food
ingredients or for packaging. The nanofibers provide high-surface
area for effective release and mass transfer, lower degradation and
faster release, and control on the release by controlling the ratio of
the polymer to active component [106, 107]. Various approaches in
electrospinning have been adopted to obtain the desired encapsulation
and release of active ingredient, including blend electrospinning,
core-shell electrospinning, emulsion electrospinning, and surface
loading of nanofibers. These approaches dictate the pattern of
loading of active ingredient to get a desired release performance of
the nanostructure for food packaging [108].
24 Biomaterials for Food Packaging

Figure 1.4 Basic electrospinning setup for fabricating nanofilms.

1.6.2.2.1 Blend electrospinning
In this method, a direct dissolution of the active ingredient in the
polymeric solution is done and electrospinning is conducted (Figure
1.5). The uniformity of the electrospun nanofilm depends on the
compatibility of both the polymer carrier and the active component,
which later determines the release performance [109]. For instance,
in case of higher affinity of active component to the polymer carrier
than the solvent, it will migrate into the inner of the fiber than the
surface. This technique is considered suitable for encapsulation of
active components that are not sensitive to the solvents, however, it
is not suitable for enzymes [110].

Figure 1.5 Blend electrospinning of active agent in polymeric nanofilms.

  Methods of Forming Biomaterial-Based Packaging 25

1.6.2.2.2 Core-shell electrospinning
The core-shell electrospinning provides nanofibers where the core
is concentrated with the active ingredient and the shell that provides
protection and modulates the release of active ingredient. The polymer
and the active ingredient are kept separate by simultaneous spinning
of two coaxial spinnerets to get a core-shell nanofiber structure [111]
(Figure 1.6). This method provides more flexibility in designing the
nanofibers because the core could be any active agent, which may
be spinnable or non-spinnable [112, 113]. Additionally, it provides
effective protection to the light sensitive active ingredient [114].

Figure 1.6 Core-shell electrospinning method.

1.6.2.2.3 Emulsion electrospinning
In this electrospinning method, the active ingredient, which is
surrounded by the surfactants or emulsifiers, is loaded to the
polymeric carrier (Figure 1.7). This helps to design a control or
sustained release packaging system [115]. Contrary to the core-shell
two feeding spinnerets, emulsion electrospinning provides a core-
shell type of fibers with a single spinneret [108]. This technique serves
as an alternative to core shell, as it can assist to incorporate a lipophilic
active component in a hydrophilic polymeric carrier to avoid burst
release [116]. It is suggested that the electrostatic forces influence
the stretching of polymeric emulsions, induce de-emulsification,
and creates core-shell fiber structures. The fabricated emulsion
26 Biomaterials for Food Packaging

electrospun nanofibers could be tuned based on the choice of solvent,

polymer, emulsifier, and surfactant, and by the electrospinning
condition, such as applied electrostatic potential [115].

Figure 1.7 Emulsion electrospinning and de-emulsification of active agent

in polymeric nanofibers.

1.6.2.2.4 Surface loading of nanofibers

This technique allows the post-spinning loading of active ingredient,
where nanofibers act as supporting structures because of their
higher specific surface area and porosity. Surface loading could be
realized either by physical adsorption or chemical immobilization
or by multilayer assembly. The physical adsorption is a straight­
forward dipping of nanofibers within the solution or suspension of
active ingredient. The adsorption is occurred by specific affinity or
electrostatic forces on the surface of the nanofibers. However, this
method is not suitable for controlled release of the active agent. In
the chemical immobilization method, active ingredient is attached
on the nanofiber surface by chemical bonding. The functional groups
of primary significance are the hydroxyl, carboxyl, and amine groups
that provide platform for chemical immobilization [117]. In the layer­
by-layer assembly, the poly-electrolytes are adsorbed on the surface
of the nanofibers to design a multilayer coating. Besides, hydrogen
boding, covalent bonding, hydrophobic interaction, and molecular
recognition are also used in developing multilayer coatings. Persano
et al. published a comprehensive review on industrial up-scaling and
commercialization of electrospinning, suggesting the electrospinning
for the food industry [118].
  Methods of Forming Biomaterial-Based Packaging 27

Figure 1.8 Surface loading of nanofibers: (a) physical adsorption, (b)

chemical immobilization, and (c) layer-by-layer deposition.

1.6.2.3 3D printing
It is a process of fabricating 3D objects from the digital models
by deposition of multilayer of biomaterials [119]. Use of natural
biomaterials for 3D printing involves cellulose, starch, lignin,
alginate, and chitosan, which are good in meeting demand and
sustainable in terms of producing non-toxic by-products upon
degradation [120]. Based on various materials, 3D printing technique
involves extrusion, solidification of powder, direct-energy deposition,
photopolymerization, and sheet lamination. The 3D printing
technology for food applications would mainly involve extrusion-
based printing, inkjet printing, binder jetting, and selective­
sintering printing (with hot air or laser) [121]. However, different
3D techniques and applications need different types of biomaterials.
The most common used thermoplastic material is PLA. Based on the
desired applications, the biomaterials could be converted to products
by blending, compounding, or copolymerization. In compounding,
various additives like plasticizer, color pigment, nucleating agent,
chain extender, and UV-stabilizer could be added.
Development of biopolymeric 3D-printed-smart materials is
ongoing. Smart biomaterials have one or more character that changed
with external stimuli such as temperature, pH, pressure, or light.
Other materials change in size and shape with the heat or self-healing
properties. This smart technology will help to fabricate whole lot of
products for novel applications. A comprehensive review has recently
28 Biomaterials for Food Packaging

published on biomaterials use in 3D printing [122]. 3D printing has

been adopted more successfully to design food packaging of different
textures and develop active or smart packaging materials. Technical
advancement in fabricating biomaterial-based feedstock for 3D
printing technology has presented success at lab scale, however, to
relish the full potential of biomaterials in 3D printing, it is needed
to thoroughly evaluate their processability, mechanical, bio-chemical,
and degradation behaviors. Therefore, it could be speculated
that future 3D printing materials will be biomaterial-based green
feedstock.

1.6.2.4 Smart interactive active packaging

On the other side, research studies have been expanded to produce
biomaterial-based smart-food packaging. Moving toward Industry
4.0, food packaging has become a crucial issue in the supply chain of
the food industry. The consumers tend to purchase food packaging
products in bulk and it is important to maintain the quality of the
products during the storage. Human workforce is limited to fulfilling
the complicated tasks of recording data and protecting the printed
documents. At the same time, the increased pollution by synthetic
plastics has become an obstacle to further utilize these materials.
Hence, biomaterial-based smart-food packaging is expected to be the
alternative. This packaging is in demand and is expected to increase
due to Industry 4.0.
There are two different types of smart-food packaging. One is
intelligent packaging, in which the packaging is done with the help
of sensors, with or without the complementation of electronics. It
provides relative humidity, temperature, and light data to identify
the shelf-life of chilled food, including fruits, vegetables, or meat.
Normally, intelligent packaging is presented as tag and QR code, and
complemented with apps in smartphones. The intelligent packaging
is not the focus of this literature. Another smart-food packaging is
interactive packaging, in which it is interacting with food products.
Normally, the active packaging is made up of biomaterials and
complemented with functional additives, such as plant extracts,
antioxidants, or antimicrobials. As the food comes in contact with
biomaterials, the biomaterials indicate the change in color, odor, or
graphic symbol. This interactive packaging is used to wrap vegetables
and fruits [123].
  Safety Concerns of Biomaterial-Based Packaging 29

Smart-food packaging can be alternatively produced from

biomaterials such as gelatin, starch, chitosan, PHA, or PLA. This
packaging is efficient in maintaining the freshness and the safety
of the food. A smart-food packaging can be a moisture absorber,
antimicrobial, antioxidant packaging, carbon dioxide emitter,
and oxygen scavenging, which enhances product attributes (e.g.
appearance, taste, flavor, aroma, and others) [123, 124]. This
packaging is also cost effective and has potential to reduce food
waste, especially when it is applied in large-scale production. Hence,
the smart-food packaging is a potential alternative toward the
development of Industry 4.0.

1.7  Safety Concerns of Biomaterial-Based

Packaging

In recent packaging technology, the use of various polymers with

functional additives or fillers of nanosize is very common. However,
almost every innovative technology brings some unknowns to the
consumers and society. Nanotechnology though has played a pivotal
role in revolutionizing the packaging industry; however, thorough
understanding of possible interaction between nanoparticles in
packaging films with food or food environment is crucial. Poor
packaging may result in issues regarding food deterioration and
contamination, and may alter the appeal and organoleptic properties
of the food product and render it inappropriate for consumer safety
and acceptability [125, 126]. The most challenging part of the current
advancement in packaging technology is the lack of comprehensive
understanding of toxicity and possible fate of the nanoparticles and
their impact on the human and environment [127].
On the other hand, the interaction of nanomaterials with the
biological systems is not yet elucidated well. Nanoparticles get
into the body via ingestion of food and interaction with biological
macromolecules and stay in the body fluids, including blood. It
is reported that the nanomaterials have the ability to penetrate
biological systems and present incomplete clearance from the body
based on their shape and size [127, 128]. Smaller nanoparticles
with their high-surface area have found to be more toxic than the
larger counterparts [129]. Besides the size, surface functionalization
30 Biomaterials for Food Packaging

and charge on the nanoparticles worsen the situation. Cationic

nanoparticles exceed in toxicity than anionic or neutral particles,
resulting by their higher affinity toward the negative charge on the
plasma membranes [130, 131].
In order to ensure there is no contamination of food that may harm
the consumers, migration tests are performed on various packaging
materials. The study of migration should include following aspects,
in order to minimze the consumers’ exposure to risk factors: The
physico-chemical properties of biomaterials need to be evaluated and
compared with synthetic plastics, as these may affect the migration
rate of the compounds. Theoretical models should be applied in
the aspect to estimate the migration of stabilizers and additives
from food packaging to the food. Migration limits are defined in two
possible ways: specific migration and overall migration limits. The
specific migration limit of an individual substance is set based on the
acceptable daily intake (ADI) established by food authorities. In the
case of overall migration limit, a 60 mg of all the possible migrating
substances in 1 kg of the food matrix is set by the European Food
Safety Authority (EFSA) [132].
Many studies on the migration of nanoparticles in biopolymeric­
and synthetic plastic-based nanocomposite packaging have been
done for food or food simulants [133]. Usually, the nanomaterials in
food matrix are in low concentration and to investigate them, very
sensitive techniques are needed. Among the techniques currently
being used in detection and analysis are: (i) Imaging technique:
Scanning or transmission and atomic force microscopy,
(ii) Spectroscopic technique: X-ray diffraction and scattering, and
dynamic light scattering, and (iii) Quantitative technique: Atomic
absorption, and inductively coupled plasma with mass spectrometry.
Few other methods are used in combination based on the
particles complexity [134−137].
However, the selection of correct set of experimental conditions
and simulants or food matrices is very crucial in defining the
migration issues more clearly. Studies on nanocomposites with most
common fillers, i.e. nanoclays indicate the intercalated composites
that provide less migration of clays than exfoliated structures.
Migration of few compounds, such as lactic acid and dimer from PLA,
was evaluated, however, no significant toxicological data was seen,
and it was categorized as a Generally Recognized as Safe (GRAS)
  Safety Concerns of Biomaterial-Based Packaging 31

substance. Similarly, the migration of polyhydroxybutyrate (P3HB)

was not in concern, as it is not harmful to the consumers. Other than
that, a study has evaluated the migration of natural antimicrobials
from thermoplastic starch. The antimicrobial concentration was
very low, but still considerable. However, the toxicological profile
of other monomers, such as bisphenol A (BPA), bisphenol S (BPS),
vinyl chloride, acrylamide, nanoclay, pro-degradant, benzophenone,
and dithiocarbamate, should be taken into consideration during
the production or after migration. Only a standard concentration of
additives can be used for specific application. Though the migration
studies are providing better idea about possible transfer of additives
or monomers, however, the suitability and compatibility of the
simulant or food matrix, and the studied experimental conditions are
very crucial to avoid under or overestimation of migration behavior
of any substance of concern [132].
Other than that, with rapid increase in use of nanotechnologies
in food packaging, it is direly needed to lay down legislation and
regulation for the safety of the contained food products. Currently,
partial regulations on safety assessment of nanomaterials are
existing. Mostly the nanomaterials are regulated horizontally based
on the food laws existing in different countries [138, 139]. Due to
the lack of sufficient and inconclusive scientific evidences, mostly
precautionary approaches are implemented in the regulations of
nanotechnologies in food packaging [140]. The institute of Food
Science and Technology (IFST) has mentioned the deficiency of
regulations related to the impact of nanomaterials in food packaging.
The Scientific Committee of the European Food Safety Authority
(EFSA) has highlighted the hurdles in authenticating the possible
risks of nanomaterials, including the difficulty in detecting and
characterizing and lacking toxicology data [141]. Consumers must
have adequate information about the presence of nanoparticles
in the food packaging, processing methods of packaging, and
the related safety concerns. Very few agencies have established
regulations and standards to regulate the use of nanotechnology.
Some cases of existing regulations on nanotechnology have been
reviewed by Farhoodi (2015). Regulation (EC) No.1272/2008 deals
with the classification, labeling, and packaging of various materials
and their mixtures. The U.S. Food and Drug Administration (USFDA)
has awarded “Generally Recognized As Safe” (GRAS) status to a few
32 Biomaterials for Food Packaging

nanomaterials as food contact materials, including nanoclays, carbon

blacks, zinc oxides, and alumina. While according to the European
Regulations only silica, titanium nitride, and carbon blacks can be
casted-off in food packaging. Other nanomaterials such as aluminum
nanomaterials, zinc oxides, nanoclays, and silver materials are not
authorized for food packaging [127].
The Codex Alimentarius Commission, a joint agency of the
U.S. Food and Agriculture Organization (FAO) and the World
Health Organization (WHO), is endorsing the food safety
regulations and standards designed by governmental and non­
governmental organizations, worldwide. The Commission should
take into consideration the deliberate use of nanomaterials and
nanotechnologies in food and food packaging to minimize the
regulatory gaps. Hazardous materials presence should be informed
to the consumers by new labeling systems, including new safety
symbols where possible. Moreover, materials safety data sheets
must be provided to the users and with changing the size to nano
level, the substance could be classified differently. Unfortunately,
there are very few international regulations on nanomaterials and
nanoproducts. Additionally, most of the studies regarding the safety
of nanomaterials are rarely focusing on food nanomaterials and
similar aspects. Though the use of nanotechnology is rising massively
in the food industry, yet the lack of clear definitions, food safety
evaluations, and appropriate regulations and standards jeopardize
its core potential.
As far biomaterials are concerned, a few prospects of regulations
and standards are taken into consideration. In Europe, the application
of biomaterials is under the regulation of Commission Regulation
(EU) 10/2011. A biomaterial needs to fulfill the standards of
compostability and biodegradability to be defined as biodegradable.
There are three international standards of compostability: EN
13432:2000, ISO 17088:2012, and ASTM D6400-12. These standards
are applying similar set of characteristics such as (i) material
characterization, (ii) disintegrating ability of the material, (iii)
biodegradation of the material into carbon dioxide, biomass, and
water, within 6 months, and (iv) ecotoxicity tests of the material
compost. As per the standards of biodegradability, the characteristics
are directly related to compostability. The test of biodegradability
  Global Trends toward Biodegradable Polymers Packaging 33

is conducted in different environments, such as aquatic, marine,

compost, soil, landfill, or under aerobic/anaerobic conditions.
It is crucial to measure the presence of carbon content in any
biomaterial products. Thus, the standards for the quantification of
carbon-14 (14C) contents are ASTM D6866-12, ASTM D7026-04, and
CEN/TS 16137:2011. Only 14C can be found in biomaterials instead of
fossil fuel. Lastly, the biomaterial producers are required to proceed
with certifications and labeling. Certifications are based on the
voluntary of the producers and verified by few organizers such as DIN
CERTCO, Vinçotte (both EU), Biodegradable Products Institute (US),
or Japan BioPlastics Association. Successful certified biomaterial
products are given a verified ‘seedling’ logo that is provided by
EN13432, DIN CERTCO, and Vinçotte. Usually, “OK compost” logo is
issued by Vinçotte. The Japanese BiomassPla logo is only issued to
the material that consists of more than 25% of bio-based resources.

1.8  Global Trends toward Biodegradable

Polymers Packaging

The legislative banning of synthetic plastics in various countries

resulted in initiatives to develop biodegradable plastics. Typical to
the food packaging products, the factor of biodegradability is driving
the demand for biodegradable biomaterials. However, the packaging
foams and bags, in terms of volume, are on the top of the list. It is
reported that a 67-fold rise in demand for biodegradable polymers
is expected by 2050 [142]. Hence, in terms of demand, the annual
growth for biodegradable plastics will be around 15%. The term
sustainable development was introduced by the World Commission
on Environment and Development in 1987 in a report entitled “Our
Common Future”. The World Packaging Organization (WPO) raise
a slogan “Better quality of life, through better packaging, for more
people,” aiming to retain the nutritional quality and minimize the
food spoilage by educating on packaging. Food packaging is sharing
almost 50% of the market of the packaging industry. Thus, the USFDA
is focusing on the ability of food packaging to preserve the quality
of food and control the migration of unwanted chemicals to the food
during the service life of the packaging [143].
34 Biomaterials for Food Packaging

The FDA is administering the packaging industry to follow the

recyclability regulations regarding the threshold for food contact
materials and packaging materials [144]. A few initiatives have been
taken to promote sustainable packaging instead of focusing on the
waste management [145]. Amongst in the first few attempts, the
Sustainable Packaging Alliance of Australia defined the sustainable
packaging [146, 147]. The European Parliament and Council
Directive 94/62/EC’ was made on 20th December 1994 to minimize
the packaging waste (Council for the European Union, 1994). Later,
the amended directives on packaging and its waste were: Directive
2004/12/EC, 2005/20/EC, and Directive 2013/2/EC, and the
latest was Directive (EU) 2015/720 regarding the preferred use
of lightweight plastic bags [145]. The expansions in sustainable
packaging resulted in the startup of “The Global Packaging Project”
in France, in collaboration with “The Consumer Goods Forum”. In
November 2008, more than 650 global retailers, producers, and
stakeholders across 70 types of businesses were the part of this
association. Across the globe, Latin America alone is producing
33% of the overall biodegradable materials for packaging. Similarly,
the abundant feedstock in Brazil is paving way for the commercial
production of bio-based and biodegradable materials for food
packaging [146].
Commercial availability of cellulose derivatives was started, but
interestingly in 1993, it was considered that these derivatives were
non-biodegradable, however, fully biodegradable cellulose acetate
was developed by Eastman Chemical Company, USA [148−150].
Polylactides, poly-hydroxyalkanoates, and polycaprolactones are
biopolyesters whose good mechanical and barrier properties with the
ease of processability render those suitable candidates in fabricating
biodegradable packaging. The polylatcides alone shares almost half
of the total demand for biodegradable polymers followed by starch
(~41%). Cargill Dow and Mitsui are the two major companies
producing PLA; Cargill is currently using genetically engineered
yeast in conversion of raw sugars to the lactic acid [151]. PLA has
its applications in developing food packaging films, short shelf-life
bottles, thermoformed bowls and cups, and others. Polybutylene
succinate is also one of the biodegradable polymers, which could
be processed into various suitable shapes for food packaging
applications. SUCCIPACK® is a European company developing
several articles from the bio-based polybutylene succinate, including
  Conclusion 35

packaging films, trays, and pouches. Thermoformed PBS articles,

such as cups, trays, and containers, were firstly patented by Li and
Co-workers in 2013 [152].
Other than that, the emergent use of biomaterials as feedstock
for food packaging may limit their supply for food production and
result in an undesirable competition. In 2008, food prices were
increased, as the edible feedstock supply was limited due to the usage
of the feedstock in synthesis of biofuels. However, for biomaterials
production, it is expected to utilize lower grade of edible feedstock.
Thus, it is suggested that the production of biomaterials as food
packaging may not affect the price of food. The consumption of
biomaterial sources as feedstock is relatively small. The European
Bioplastics data shows that approximately 0.02% of land was needed
in 2018 to grow the feedstock of biomaterial-based plastics. Besides,
it is expected that there will be alternative feedstock following the
development of biomaterials [153]. Food waste such as spent cooking
oil, organic fraction from municipal food waste, or interesting
molecules from side streams of the agro industry (such as beet pulp)
can be the alternative feedstock for biomaterials production [154,
155]. The side streams are favorable for biopolyesters production.
With time, the applications of the biomaterials in food packaging
are increasing because of the lack of the land and space to manage
synthetic plastic waste. The current existing biodegradable polymers
with myriad properties can combat this challenge; however, more
scientific studies are mandatory to integrate the further developments
in the properties of these bio-based plastics.

1.9 Conclusion

In overall, biomaterials for food packaging are gaining importance

especially in the current time of Industrial Revolution 4.0. However,
it is challenging to find the most appropriate alternatives to synthetic
plastics that have similar properties. Hence, blending of biomaterials
is actively tested and it showed that biomaterials have potential in
the future of packaging. Yet the production methods are also a major
challenge, the method that is efficient in production and economically
feasible, especially in large-scale production, is preferred. Thus, this
literature is able to provide various methods for the formation of
biomaterials as future of food packaging.
36 Biomaterials for Food Packaging

Acknowledgement

The authors would like to acknowledge the Fundamental

Research Grant Scheme; Malaysia Rising Star Award (Grant no:
203PTEKIND6711530) to support this research studies. Mahmood
K. acknowledges the USM-Global Fellowship Scheme for supporting
the study.

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Chapter 2

Active Ingredients Enabled Edible

Coatings and Films Improve Shelf Life of
Food: An Overview

Tanvir Arfin
Environmental Materials Division,

CSIR-NEERI (National Environmental Engineering Research Institute),

Nagpur, Maharashtra, India

[email protected]

The coatings and films embedded in the edible form to the processed
vegetables and fruits enhance their life span, and these even maintain
the microbiological, sensory, as well as nutritional qualities of the
fruits and vegetables. The different formulations are done and
clinically tested for inhibiting the polyphenol oxidase activity and for
retarding the movement of browning in fruits and vegetables. The
edible coatings and films are responsible for transporting essential
materials, and they even provide benefits to the consumer in the form
of encapsulating bioactive compounds by offering new innovative
products posing functional and nutraceutical effects. These
products have various properties, such as solubility and adhesion
transparency. After evaluation of such properties, the behavior and
composition can be predicted and then the optimization can be

Biomaterials in Food Packaging

Edited by Mohd Yusuf and Shafat Ahmad Khan
Copyright © 2022 Jenny Stanford Publishing Pte. Ltd.
ISBN 978-981-4877-98-5 (Hardcover), 978-1-003-25678-6 (eBook)
www.jennystanford.com
50 Active Ingredients Enabled Edible Coatings and Films Improve Shelf Life of Food

done. The coating of the edible products involves different events,

namely consumption of oil to be minimized in the deep fried fat
products, transportation of bioactive compounds, and life expansion
of perishable substances. Hence, the primary emphasis in the study
is undertaken on the characterization of newly hydro colloidal
films, which are produced by non-conventional sources. Another
focus is related to the determination of capability of compounds in
discharging the molecules along with features like antioxidants and
aromatics. Lastly, the interacting activity is enabling them to show an
encapsulating matrix in the particles.

2.1 Introduction

In the current scenario of the research field in the development

of society is a significant concern with sustainable development.
The ideas of such studies have attracted the interest basically for
influence and regeneration aspect, as these are referred to maintain
justice on using resources that interact with a human being as well
as the ecosystem [1−5]. In the present scientific study, it has been
found that integration of a new material in influencive form is
regarded as a better option [6−10]. The new materials are employed
in various branches of analytical chemistry for the identification of
quantitatively and qualitatively with minimum sample available in
the very complex form [11−15]. The content is said to be favorable
for carrying out research activity in techno-economic processing on
large extent [16−20].
Most of the materials applied to the packaging industry are made
up of fossil fuels, which are non-degradable. Therefore, these lead
to hazardous environmental problems, globally [21]. Significant
effects are put into practice to enhance the shelf life and develop
the quality of food at the time of packaging by the innovation of
new materials like edible and biodegradable films from renewable
sources [22]. It is observed that because of the biodegradable nature,
the environmental problems could be solved to some extent. The
biodegradable packaging material is made up of polymer that is
degraded by microorganisms by the process of composting, which on
the other hand, liberates the compounds, namely CO2, H2O, CH4, and
biomass. Biodegradable polymers are of two types: edible and non-
edible [23]. The biodegradable film is produced by the derived food
 Background 51

components, employing the wet and dry manufacturing processes.

The edible film (EF) resulting from the processes is a free-standing
sheet kept in between the elements of food. EF is a layer of material
employed for wrapping and covering food products to extend their
life. The EF can be consumed with the food also. The edible coating
(EC) is a thin layer of material that can be eaten and is applied to
the outer surface of the food by the processes of panning, dipping,
and spraying. The edible packaging material can be fed with the
meal or as a part of the product. It even accomplishes the function
such as acting like a carrier for additives, namely antioxidants and
antimicrobial agents. The EF and EC can be used even for various
other functions such as inhibiting moisture, CO2 or O2 migration, and
enhancing mechanical integrity of food products [24]. There are some
differences between EC and EF, such as EC is applied in the form of
liquid to the food products, which can be possible by immersing the
products in a solution obtained from the structural matrix, namely
carbohydrate and lipid. Whereas, EF is firstly molded into solid sheets
and then wrapped over the food products. It is preliminary essential
that EF needs to be safe, according to GRAS (generally recognized
as safe), and should fulfill the limits according to the Food and Drug
Administration (FDA). The material applied for food contact will have
to go through regulatory scrutiny, where biopolymers act as additives
that migrate toward the food products.
The EC and EF applied to food, such as horticultural products, are
affected by features, such as optical and mechanical characteristics.
Such features are affected by various factors like pH, solvent,
temperature, etc. [25].

2.2 Background

EC or EF has been used for many years for food products to safeguard
the materials. Cellulose coatings are most popular in the meat
industry and waxing in the vegetable and fruit industry. During
the mid-20th century, a layer is used for preventing loss of water
and providing shining texture to vegetables and fruits. The EF and
EC are shaping the barrier for the changes in term of chemical,
biological, and bodily means. During the purchase of vegetables
and fruits, buyers mainly think about healthy food items, depending
on freshness and appearance. The main issue regarding this is to
52 Active Ingredients Enabled Edible Coatings and Films Improve Shelf Life of Food

manage pathogenic microorganisms and spoilage growth in the fruit

market and godowns. The first approach to get rid of this problem is
to make use of EC [26]. The EC provides an extra protecting coating
to get sparkle and influence the storage atmosphere to modify inner
gasoline composition. Nowadays, the EC is employed intensively to
preserve vegetables and fruits, including capsicum, cucumber, apple,
and others. Application of EC is a successful process and does not
depend on the manipulation of the inner composition of gasoline.

2.3 Functions and Advantages

The functions and advantages of EF and EF are exhibited in Figure 2.1.

The main benefits of such food packaging are its eco-friendly nature.
The fresh product involves enhanced shelf life. The EC or EF is the
transporter of antimicrobial substances, and it is finally considered
for food products. It is an active component that is united in the
matrix of polymer and can be eaten along with the food, improving
the essential requirements, such as safety, nutritional, and sensory
needs. It also fulfills some other functions, such as protecting the
products from physical, microbial, and chemical actions.

Figure 2.1 Functions and advantages of EC and EF.

 Importance of EC and EF 53

The biodegradable films are produced by making the use of two

basic techniques. Firstly, using wet solvent processing called solution
casting. This was developed 100 years ago. The solution was spread
on the plates such as acrylic, Teflon, or silicon plates, which were later
following with the process of drying under controlled conditions,
such microwave energy and hot air, at the ambient situation. The
extrusion was used in manufacturing of thermoplastic polymers
after 1950, and it was regarded as the central production process
applied for the manufacture of plastics. The method of extrusion
employs the elevated temperature, and it gets soften by trimming,
and finally, the polymer is melted as a result of which cohesive film
matrix is formed.

2.4 Importance of EC and EF

The film is employed for improving the organoleptic features of

packaged foods. The film/coating behaves as a carrier of various
substances, such as antimicrobials and coloration [27]. The film is
implemented in the form of an interior heterogeneous component at
interfaces on a specific sheet of food products. It is suitable for saving
the deteriorative component moisture as well as the movement of
solute in food products, such as pizzas and candies [28]. The EF or EC
is also applied as a multilayer food packaging material. The functional
activity and permeability of the EC and EF are minor in comparison
to the artificial film, which is causing pollution [29]. Along with the
function as a selective barrier for moisture, gas, and solute migration,
the EC helps in minimizing the growth of microorganisms in solid
and semi-solid food. It can be possible by reducing the diffusion rate
of antimicrobial agents to coat substances instead of food [30].

2.5 Structural Matrix

The EC and EF are categorized based on the structural material. The

primary sources of molecular groups are lipids, polysaccharides, and
proteins. The origins of EF and EC are shown in Figure 2.2.
54 Active Ingredients Enabled Edible Coatings and Films Improve Shelf Life of Food

Figure 2.2 Various types of biopolymer origin.

The edible and biodegradable films are manufactured with

the combination of different polysaccharides, lipids, and proteins
that have useful features of a specific compound. The barrier and
mechanical features of the films depend on the compound employed
during the matrix of polymer and the compatibility [31]. The main
compounds used in the EF and EC structural matrices are summarized
in Table 2.1.

Table 2.1 Summary of various materials applied in EC and EF

S. No. Material Reference

1. Chitosan [32]
2. Alginate [33]
3. Lipid [34]
4. Cellulose [35]
5. Starch [36]
 Synthesis of EF 55

2.6 Synthesis of EF

EF is prepared by the dispersion of film-material using alcohol and

water as solvents. For producing EF, colors, plasticizers, and flavors
are added by adjusting pH. Some of the polymeric film solutions need
to be heated for facilitating the dispersion. Later, the solution is cast
and then dried at ambient temperature for attaining standalone films.
Food application can be accessible by adopting various methods,
such as spraying, brushing, and dipping.

2.7 Barrier Feature

The barrier features of EF are volatile permeability, gas permeability,

and so on, which are the significant factors in food application. The
effectiveness of the film is decided through the investigation of
permeability of water vapor and permeability of oxygen (O2). For
determining the rate of oxidation and respiration of food products,
the O2 and CO2 permeability is regarded as an essential parameter.
The EF is composed of polar polymer that forms cracks because of
the high sensitivity of changing humidity. The lipid material exhibits
least water vapor, and it also performs as a distinguished moisture
barrier. The demerit of the lipid material is that it is considered as a
less effective gas barrier and cannot form a film without any help of
agents, namely proteins and lipids.

2.8 Active Biopackaging

The active biopackaging is considered as the creative prospect, as it

possesses the inherent ability to control the transmission of active
agents from packaging substances. It is observed that the active
agents on directly combining with the packaging substances can be
recognized as favorable and reliable, but their quantity should be
limited as per the use, which is reflected in Figure 2.3.
56 Active Ingredients Enabled Edible Coatings and Films Improve Shelf Life of Food

Figure 2.3 Different adaptation processes of additives.

For attaining active packaging and coating functions, the

emulsifiers, antioxidants, and antimicrobial agents are assimilated
within the film-forming solution. There are various antimicrobials,
which are integrated into the EF and EC, which involve polypeptides,
organic acids, and so on. The primary function of EF and EC is to
protect food products from oxidation and spoilage that results in
improving the quality and safeguard the products [37].
The most significant approach for food production is the
optimization of EF composition because it needs to be framed as per
the features of vegetables and fruits, on which it has to be applied [38].
Therefore, it is necessary to characterize and test different coating
solutions on the food for maintaining and enhancing its quality [39].
The multicomponent and composite EF is optimized due to the
mechanical features, transparency of food, and handling of food
products. Hence, to fulfill such target, suitable designing of the surface
methodology is to be done for determining the optimal mixture of
components that could be beneficial [40]. As such, on adding lipid
to enhance the features of the moisture barrier, the transparency
features get affected.
The coating, which is dependent on polysaccharides, has enhanced
application, and it has even improved the shelf life of vegetables and
fruits because of its ability to be selective permeability of polymers
 Chemistry of EF and EC 57

toward O2 and CO2. Summary of some compounds with their effects

is shown in Table 2.2. The polysaccharide-based coating is applied
for modifying the internal environment of fruits, which delays
senescence [38]. The EC develops passive modified atmosphere,
influencing the changes in fresh and least processed food products,
such as color and volatile compound [39].

Table 2.2 Summary of various biomaterials behavior

S. No. Component Behavior Reference

1. Chitosan Antimicrobial [41]

2. Chitosan Tissue conservation [42]

3. Chitosan Antifungal [43]

4. Chitosan Shelf life [44]

5. Chitosan Mammalian cell [45]

The demand of the consumers in accumulating in term of

preservation of food naturally is leading to improve the alternative
approach. The biopolymer is used widely, as it is generated from
renewable sources or their by-products. The EF or EC is the main
topic of interest because of its feature to increase the shelf life of food
products. The shelf life of the food component can be enlarged by a
decrease in respiration. The EC is a biodegradable material and eco-
friendly substance, which is employed for reducing the application
of plastic packaging. The enrichment of shelf life is significant, as it
increases the economic benefits for food processing companies.

2.9 Chemistry of EF and EC

The quantity of material applied in the food industry is confined so, it

should be capable of forming a film. The material should be capable of
dispersing in a favorable food safe solvent and should be in harmony
58 Active Ingredients Enabled Edible Coatings and Films Improve Shelf Life of Food

to plasticizers, antimicrobial agents, etc. The material is classified as

composite, lipid, and hydrocolloid [46−48].

2.9.1 Polysaccharide
Polysaccharide is a natural polymer employed for the preparation
of EF or EC, involving the cellulose and pullulan [49]. It is an
essential coating considered as an effective blocker for O2 because
of its organized H-bond network. Since it exhibits hydrophilic
nature, it is not capable of acting as a moisture barrier [50]. The
coating comprising polysaccharide polymer shows fragile water
vapor barrier feature, so it enables in the delay of moisture loss
from meals [51]. Its coating has different characteristics, such
as it is colorless, oil-free coating, and has minor caloric content.
Such layer is employed to extend the shelf life of vegetables, fruits,
and meat by the reduction of dehydration, surface darkening, and
so on.

2.9.1.1 Cellulose

Cellulose is a renewable polymer resource found in large amount in

the world. It is predicted that through the photosynthesis process,
1011−1012 tons of cellulose are synthesized every year in the
pure form, but sometimes it is combined with lignin or different
polysaccharides of woody plants [52−55]. It is the polymeric raw
material employed for the two specific functions. For instance, it
has been used in the form of construction material as textile fibers,
and intact wood. The stable cellulose derivatives are applied in
the various technical aspect and domestic life [56−58]. Multiple
features of cellulose were obtained, which could be noticed from
the information based on dyeing the cellulose fibers. It holds a
unique position in the anecdote of the polymer. It also possesses
hydrophilic as well as hydrophobic feature that accomplishes
self-association of the respective polymer in water [59−61]. The
structure of cellulose is shown in Figure 2.4.
 Chemistry of EF and EC 59

Figure 2.4 Structure of cellulose.

The cellulose, as well as its derivatives, has been used for

manufacturing the processed food from many decades. The cellulose
that is physically modified provides a useful strategy for many
products in bulking features such as minimized or low-calorie diet,
and flow of the products posing an ability of natural sweeteners
and favor packets, as well as imbiber the oil flavor. The wide use of
cellulose is mainly due to its rheology and textural characteristics,
controlled water interaction, and chemical features. Microcrystalline
cellulose (MCC) and the soft cellulose play a significant role to
provide bulking low-calorie food products. The chemically modified
cellulose derivatives perform five vital functions such as organizing
flow features, stability of foam, emulsification, strength as well as
development for water binding, and ice crystal production. The
physical and chemical characteristics can devise the use of cellulose
in food application [62, 63].
The cellulose derivatives are chosen as the best option for
developing baked products because of their beneficial properties.
Bread requires a specific size value for the development of the fine
texture and cell structure. The selection of various qualities as well
as the quantity of diverse wheat flour decides the qualification of
the food product. Therefore, additives are used for correcting such
circumstances. There is a requirement of a particular readjusting
for supplying nut structure and also the baked quality that could
be compared with products comprised wheat flour. The high-fiber
bread applies different derivatives of cellulose. The MCC or cellulose
derivatives can be substituted with the wheat flour, even the
modified cellulose performs with least ability in the baked products.
60 Active Ingredients Enabled Edible Coatings and Films Improve Shelf Life of Food

However, the specific component needs to be changed for attaining

the appropriately qualified products.

2.9.1.2 Chitin
Chitin, abundantly found in nature, derives the poly-cationic
polysaccharide called chitosan. The chitosan has more than 5000
units of glucosamine, which can be collected from shrimps shell;
crab comprised chitin and N-acetyl glucosamine unit. It is obtained
through the process of partial chemical de-acetylation of chitin that is
extracted from the crustacean group, including animals such as crab,
shrimp through deproteination, decolorization, and decalcification,
and also from fungi through the process of enzymatic extraction [64,
65]. The structure of chitosan is shown in Figure 2.5. It has features,
such as biodegradable, antimicrobial, and biocompatible, which
enable it to be used for different applications. Till date, very restricted
consideration is given to the use of chitosan in the food industry. It is a
cost-effective polymer because it can be easily obtained from nature.
The main aim of the current review is the transition of marine, as
well as terrestrial processing, which dumps into the profitable by-
products making the material adequate for research in term of food
and its development. The extensive application involves the recovery
of waste substance by various approaches, such as processing
castoffs, protection, development, amplification, cleansing, and
deacidification. In this support, multiple researchers have suggested
by carrying out antifungal and antimicrobial performance [66, 67].

Figure 2.5 Structure of chitosan.

The introduction of green extraction approach based on the

green chemistry theory includes addition of higher concentration,
supporting the application of microorganism enzymes for extraction
of chitin. The result of the approach clarified that the use of
microorganisms in comparison to that of enzyme is much more
 Chemistry of EF and EC 61

superior, as it conserves the structure of chitin. The biological method

of extracting chitin is high reproducible, even in a short period by
pure exploitation, and it uses a small solvent with consuming low
energy [68]. But yet, the biological approach faces some limitation in
the laboratory-scale production, as shown in Figure 2.6.

Figure 2.6 Development of chitosan from materials.

The physiochemical and biological features of chitosan oligomer

(CO) attained by the marine diversity depend on the molecular
weight, where order length is bounded. The naturally obtained CO
offers more significant advantages in comparison to the synthesized
chitosan. The antioxidant potential of CO and its derivatives can be
improved by converting the chitosan nanobiofilm (CN) to reinforce
the application of CN in the food industry. The chitosan nanoparticles
released tend to raise free radical scavenging behavior of biofilm for
the extended time of food storage in the industry. Therefore, the brief
physiological and sensory estimation are required for determining the
molecular mechanism of antifungal and antimicrobial characteristics.
This can provide little knowledge of the influence of chitosan for the
exertion of high-quality food products.
62 Active Ingredients Enabled Edible Coatings and Films Improve Shelf Life of Food

2.9.1.3 Starch
Starch is made up of two glucose polymers, such as amylose and
amylopectin, as exhibited in Figure 2.7. It is a polymer of glucose
residue connected by the glycoside bonds. Such a relationship is
delicate where the hydrolysis process is attained at a low pH value
[69]. It is the carbohydrate stored in very high amount in plants and
also regulated as a critical factor to determine the quality of food
products. It is the only polymer that can be applied daily in large
amount for food and well as non-food application [70]. The starch
has various features such as naturally occurring polymer, present in
large quantity, cost effective, and consumed and eaten by all living
creatures. The main biopolymer used in large amount is the starch, as
it can be available very quickly and easily, because it is produced from
various sources, namely corn and rice [71].

Figure 2.7 Structure of protein.

 Chemistry of EF and EC 63

Corn starch is the most valuable starch in comparison to other

starches for industrial application. The starch segregated from the
corn is intermixed in the baked products, namely cake and cookies,
as it possesses the ability for preserving the moisture content of the
products, preventing the development of crystal from sugar, and
finally improving the juiciness of the goods [72]. The corn starch
helps in providing consistency and offering efficient gelling features
at the time of heating corn-banana [73].
Wheat with the botanical name “Triticumaestivum” is the highly
consumed crop and it is used in a different ways like bread, as it
provides energy and different exclusive nutrients [74]. The baked
products obtained from wheat, such as cake and bread, depend
on molecular structure and characteristics of the wheat [75]. Corn
is even considered as an excellent source to provide thickening in
formula milk of infants [76].

2.9.1.4 Pectin

Pectin, the structural hetero-polysaccharide, is available in terrestrial

plants. It bears rhamnose and methyl-esterified galacturonic acid
units. Its structure is shown in Figure 2.8. The proportion of the
rhamnose units and the availability of other essential units are mainly
dependent on the plants, from which pectin gets detached. Since
pectin can be produced from various plants, but yet the industrial
pectin gets extracted from citrus peel as well as apple pomace, at
the mild acidic circumstance. In such condition, pectin leads to form
gels, and such feature has enabled pectin to be used as an additive in
products, such as jam and confectionaries. It is even the significant
food component that is present in high amount in the agricultural
waste as well. It holds nutritional advantages for health-related issues
of human beings and also has pharmaceutical behavior, which makes
it clear that it can be applied in various food components. Its coatings
are further studied to specify its capability in retarding the migration
of lipid and loss of moisture and also to enhance the appearance as
well as better handling of food products.
64 Active Ingredients Enabled Edible Coatings and Films Improve Shelf Life of Food

Figure 2.8 Structure of pectin.

Maftoonazad and Ramaswamy [77] employed pectin-based composite

coating on the fruit avocado to test the limits of change in quality at
different temperature of storage and kinetic parameters, and to determine
the loss of quality of the avocado that was stored. The results signified
that such coating is responsible for reducing the rate of various parameter
changes in the avocado at the time of storage, and it even prolonges the
shelf life of the product at 10 °C for one month.

2.9.1.5 Pullulan
Pullulan, a neutral linear polysaccharide, is made up of α-1, 6-linked
maltotriose residue as well water soluble products. It is a fungal
exopolysaccharide obtained from the starch through the fungus
Aureobasidium pullulans. Bauer, in 1938, had given his observation
about this exopolymer by the name pullulan. The structure of pullulan is
shown in Figure 2.9.

Figure 2.9 Structure of pullulan.

It is used on a large scale in the food processing industry. The

pullulan slowly digested macromolecule posing the ability of tasteless
and odorless, so it is considered to be applied on low-calorie food
that provides bulk as well as texture to the products. It is an oxygen
 Chemistry of EF and EC 65

barrier polysaccharide, posing excellent moisture retention ability

and also inhibiting fungal growth. All such properties enable pullulan
to be an excellent material used in the preservation of food and thus
it is employed in large scale in the food industry [78].

2.9.1.6 Alginate
Alginate is a polymer posing features such as biocompatible,
hydrophilic, biodegradable, and economical. It is found within
Phaeophyceae brown algae in the marine as a structural component,
and also obtained from some bacteria in the form of capsular
polysaccharides. The structure of alginate is shown in Figure 2.10.

Figure 2.10 Structure of alginate.

The alginate is a versatile biopolymer with specific chemical

and physical features. It possesses the selective binding ability of
multivalent cations, which are the basis of gel formation. Also, it
has hydroxyl and carboxylic acid features that can be able to accept
and release a proton with the change in pH, due to which alginate is
considered as pH-sensitive [79].

2.9.2 Protein
The material-based protein is obtained from silk and wool of animals
[80−83]. The polypeptide chains are linked with each other to frame
a fibrous structure. The fibrous protein is featured by both primary
and secondary structures, in which the basic material is made up
of amino acid sequencing, and secondary structure is comprised
H-bond in between the polypeptides chain, as shown in Figure 2.11.
The features of the protein are exhibited in Figure 2.12.
66 Active Ingredients Enabled Edible Coatings and Films Improve Shelf Life of Food

Figure 2.11 Structure of protein.

Figure 2.12 Various properties of protein.

Bacteriocin is an excellent antimicrobial agent for obtaining an active

biopolymer film to be used in the food packaging industry. But it is
found that the use of such bacteriocin is limited in food preservation
because of the decrease in activity of antimicrobial peptides as well
as protein [84]. As such bacteriocins are manufactured from various
microorganisms, the direct assimilation of strain in the film can be
considered as the promising substitutes.
The production of protein film comes with various problems
based on costing and performance. The cost of the film can be
 Chemistry of EF and EC 67

decreased by suitable exploitation of by-products of the food industry

for the extraction of protein, and the performance problem can be
overcame by reinforcement or through modification method of the
protein matrix. Therefore, more elaborate and precise studies are
required to be carried out for putting the features of films in large-
scale processing and application in the food industry.

2.9.2.1 Gelatin
The skin of pig has been applied in the form of raw material for
manufacturing gelatin since 1930, and it even considered as
the essential material in large-scale production of food, but for
pharmaceutical work. Protein is also obtained from fish and mammal.
It is also produced by the bones of cattle, which is very complicated,
and the extraction process is costly. The structure of gelation is shown
in Figure 2.13.

Figure 2.13 Structure of gelatin.

It is a biocompatible and biodegradable polymer obtained

by chemical, physical, and thermal degradation of collagen [85].
Depending on the origin and varieties of tissue, the various processes
for the extraction of gelatin can be used, as exhibited in Figure
2.14. Collagen is a fiber that is biopolymeric in nature, and it is also
available in high abundant. It is the protein found in connective tissue
serving as the vital component for stress bearing in connective tissue
and it is also rich in residues such as proline and hydroxyproline.
68 Active Ingredients Enabled Edible Coatings and Films Improve Shelf Life of Food

Figure 2.14 Gelatin production process.

The melting temperature of gelatin gel is less in comparison

with other starches, which makes it favorable to be used in the food
industry in term of flavor release [86].
In upcoming years, the agro-industrial by-products have gathered
interest for the production of gelatin, and even it is at the pace of
development. Therefore, the revalorization is increasing, as it is a
capable material of exploration. The application of gelatin residue
liberated from capsules produced by nutraceutical area is increasing
day by day, for the disposal and treatment processes of waste that are
expensive and have different environmental problems.

2.9.3 Composite
Research activities on edible components have mainly intensive on the
composite, multi-component films for developing significant benefits
 Economic and Nutritional Influences 69

of every element and also for minimizing demerits [87]. The films are
incorporated in various forms such as suspension, dispersion, and
so on. The successive layer film or coating has a significant demerit,
such as the method of preparation includes four stages including
two casting stages and two drying stages. The laminated film is least
employed in the food industry, in spite of exhibiting sound barrier
feature, as compared to water vapor [88]. The research activities
carried out in such field show that successive layer films delaminate
after some time, and it establishes cracks or pinholes showing the
non-uniform surface [89]. The functional characteristics of such
components are dependent on the process of preparation, amount,
and type of the components [90].

2.10 Economic and Nutritional Influences

The vegetables and fruits are the essential ingredients of diet for
every human being, and these are in demand in each part of the world.
Both vegetables and fruits are the origins of vitamins, antioxidants,
minerals, fibers, and etc. It is also responsible for providing flavor
to the compounds that are affected by biotic and abiotic adversities.
The use of vegetables and fruits in the diet leads to decrease danger
caused by various chronic diseases, namely dementia, stroke, and
cancer [91]. The healthy diet advantages on the consumption of the
stored vegetables and fruits get reduced because of the decrease
in Vitamin C and polyphenols, which is mainly due to physiological
changes taking place at the time of storage [92]. Protein is recognized
as an essential component required for better survival of human
beings and animals. Its main characteristic is to provide the proper
amount of amino acids. The first class protein that is subscribed to
add dietary as well as nutritive value to the food is dependent on
the amount of amino acid and its use after the process of digestion
and absorption. The demand for plant-based protein, in spite of the
animal protein, has increased due to economic issues, health anxiety,
and emerging drift toward vegetarianism [93]. Therefore, it is evident
that the film formed from plant protein enables it to be an excellent
substance for healthy EF and plastic opportunity biodegradable
packaging materials [94].
70 Active Ingredients Enabled Edible Coatings and Films Improve Shelf Life of Food

2.11 Protection of Food Product: Mechanism

Phenomena

The primary role of the fruit industry is to reduce the browning of fresh
fruits that occurs due to polyphenol oxidase mechanism taking place
after cutting and peeling [95].The browning activity can be treated
by inhibitors, which impart the growth of brown discoloration [96].
The film forming substance can be either hydrophobic or hydrophilic,
but to maintain useful feature only H2O or C2H5OH can be employed
as a solvent at the time of processing. Various other materials can
be further added to the matrix for improving the functional features.
The main benefit of the dry process as the eco-friendly method
is that it does not make any use of solvents. There are different
approaches that are utilized to prolong the life of fruits [97].

2.12 Healthy Foods: Public Demands

The demand for vegetables and fruits are increasing continuously

in the market, as these are functional food components, and these
contain nutrients, antioxidant, and other important ingredients,
which prevent various types of cancers and degenerative diseases.
The vegetables and fruits have a short shelf life, as they are
decomposable. The main challenge for the whole world is the
preservation of vegetables and fruits. Such trouble can be solved by
EC and EF, which help in preserving the products in a safe and healthy
way and are beneficial to the consumer as well as the environment.
Nowadays, herbal EC is used in the fitness and nutraceutical field. It
possesses an extraordinary barrier residence for CO2, O2, and others,
and it is recognized as an outstanding transporter of nutrients. These
are the main factors that contribute to its market value.

2.13 Conclusion

In the developing world of science, the edible coatings and films

are considered as an essential part of output forward for various
 Acknowledgement 71

applications [98−102]. The different functions of the materials said

to be commercially applied, showing protuberant results and positive
aspects [103−107]. The independent studies carried out have made
it clear that EF and EC are excellent healthy agents for the protection
of food products from different means, since they occur naturally,
and are cheap and renewable as well. The EF is a superb transporter
of nutrients that the human beings take through food. The research
activities performed till date have offered outstanding results, with
least drawbacks, and also provided the very particular concept of
essential oils as well as herbal coatings. More explosive researchers
are needed to increase the beneficial outcomes of EC and EF for
human beings involving production and applications. Today, there is
a trend of employing active envelopes, which involves reducing the oil
consumption of deep-fried products. The application of EC and EF in
the form of appropriate packaging for the food industry has gathered
attraction, due to the promising attempt to prolong the shelf life of
the food products. Such film and coating show different functional
aspects when used in lipids to reduce moisture and other issues. The
EC and EF perform the same function as synthetic packaging film,
but yet these are chosen as the best option for packaging based on a
specific application. The EF is capable enough for minimizing a few
traditional polymeric packaging substances for correct use. Therefore,
to carry out such activities, the bio-based packaging should work as a
standard packaging by providing the critical function of preservation
and cost-effective features. In the current chapter, the extensive study
related to chemistry, merits, and requirements of healthful EF and EC
are explained, keeping in minds the nutritional as well as economic
aspects, followed by the increasing demand for food products from
the human beings.

Acknowledgement

Authors would like to acknowledge the Knowledge Resource Centre,

CSIR-NEERI, (CSIR-NEERI/KRC/2019/MAY/EMD/1), for their
support.
72 Active Ingredients Enabled Edible Coatings and Films Improve Shelf Life of Food

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Chapter 3

Surface Chemistry for Intelligent Food

Packaging

Sivapriya Veeraiyan,a Abdul Azeez Nazeer,a Saravanan

Dhandapani,b and Sudarshana Deepa Vijaykumarc
a Nano-Bio Translational Research Laboratory, Department of Biotechnology,

Bannari Amman Institute of Technology, Sathyamangalam, India

b Department of Textile Technology, Kumaraguru College of Technology,

Coimbatore, India

c Department of Biotechnology, National Institute of Technology,

Tadepalligudem, Andhra Pradesh, India

[email protected]

Food packaging is the major factor that determines the quality of

finished food products, which have to undergo transportation,
storage, and end application. The four thumb rules of food
packaging are protection of the content, communicate the
details about the product, convenient to transport and open, and
containment. In recent years, food packaging has witnessed a new
era of development with two major concepts: (i) active packaging to
extend the shelf life and perpetuate the quality of the food, and (ii)
intelligent packaging to monitor the condition of the food products
and their surroundings (indicators). The intelligent packaging
system has three central technologies: (i) indicators to communicate
the food quality to users, (ii) data carriers to track the storage and

Biomaterials in Food Packaging

Edited by Mohd Yusuf and Shafat Ahmad Khan
Copyright © 2022 Jenny Stanford Publishing Pte. Ltd.
ISBN 978-981-4877-98-5 (Hardcover), 978-1-003-25678-6 (eBook)
www.jennystanford.com
84 Surface Chemistry for Intelligent Food Packaging

distribution, and (iii) sensors for quick and precise quantification of

analytes in the food. Understanding the surface chemistry of these
sensors and indicators can conduce to bestow the biomaterials
in these applications. The use of biomaterials in intelligent food
packaging is advantageous over conventional materials, in the
aspect of environment friendliness. Hence, in this chapter, the
surface chemistry of the intelligent packaging to monitor or indicate
the food quality that performs the convenience and communicative
functions of packaging is discussed.

3.1 Introduction

Food packaging technology is repetitively fluctuating to encounter the

mounting challenges of the contemporary civilization. Packaging is a
solitary process to retain the quality of the food products throughout
the distribution, stocking, and application. It decelerates the rate of
decay, enabling the supply and promotion more competent. Package
guard products from peripheral milieu interconnect with the patron
over extolled scripts, brand emblem, and graphics; billet the existence
of the patron or assemble the management of packaged food easier
for the patron; and turn as ampoules for differently molded products
with the aim of enhancing the logistic proficiency. Preservation and
protected delivery of packaged food products are the foremost goals
all over the food industry [1]. Nevertheless, the loss of food traits, due
to physical, chemical, and biological ruins, arises during the storage
and distribution of the food products. Safeguarding the food quality is
an imperative research goal since it is closely associated with the aim
all over the world to improve the effective and healthy food supply
chain. Food quality control is essential, as it aids to shield patrons
against food-borne disease and to exploit the productivity of the food
commerce. Different dynamic constituents can be merged into the
packaging material to develop the functionality of food packages.
Novel ideas have significantly subsidized to accomplish an advanced
perception for effective food packaging, i.e. the active packaging and
intelligent packaging ideas.
The active packaging materials (APMs) are the substances
envisioned to prolong the shelf life or to extend the pristineness
 Simple Food Package and Intelligent Devices 85

of the packaged food. The purpose of APMs is to integrate with the

constituents that would absorb or release the elements from the
packaged food or into the atmosphere around the food. Numerous
APMs, such as oxygen (O2) and ethylene scavengers, moisture
curbers, carbon dioxide (CO2) scavengers and emitters, controlled
release of antioxidant and antimicrobial agents, and sensory devices,
to regulate the liberation or adsorption of flavors and odors, have
been merged to progress the quality of food packages.
The intelligent packaging materials (IPMs) are the substances
that surveil the changes and communicate the condition in the
environment around the packaged food. Intelligent packaging intends
to carry the information associated with the food quality to investors
of the food supply chain. For instance, an intelligent packaging system
can display the freshness and shelf life of the food products; it can
display temperature of the food product using thermochromic inks;
and it can even show the temperature history via time−temperature
indicators. This chapter summarizes the intelligent devices integrated
with food packages, as there is a growing interest in intelligent
developments in the food sector.

3.2 Simple Food Package and Intelligent Devices

The conventional/simple food packaging techniques, such as

wrapper and cold storage, have helped to preserve food materials
for an extended duration by guarding the products. But they do
not provide the information dealing with the quality regarding gas
concentration, temperature change, and growth of microorganisms
within the packaged environment. Hence, there is a need for an
intelligent device system that continuously supervises and conveys
the information concerning the food quality whenever necessary,
since simple packaging is not sufficient for keeping up the quality
of the food products. Therefore, various intelligent components
should be combined with the simple packaging system to convey the
customers concerning the condition of the food package.
86 Surface Chemistry for Intelligent Food Packaging

3.3 Intelligent Packaging Technique

Unlike the conventional packaging techniques, the intelligent

packaging techniques (IPTs) are used to record the variations in both
the internal and external environments and to convey the status of the
packaged food products to users [2]. In general, they sense and record
the quality of the products and their environments, and indicate the
information about the packaged food quality. This approach is highly
beneficial, as it provides timely indication to the users concerning the
food quality inside the packaging system. The IPT further displays
the detailed information on ingredients, expiry date, manufacturing
place, batch and process, and storage stipulations [3]. Study has
been conducted on developing the improvised transparent labels or
seals that remain unchanged until the package is damaged. Once the
package is damaged, the chemically reactive sensors change its color
indicating the damage [4]. This can be accomplished by integrating
sensors or indicators that potentially sense the changes in the
packing system. Therefore, IPT is a prodigious accomplishment for
the continuous monitoring and maintenance of the packaged food
items for the prolonged period to the consumers [5].

3.4 Devices Used in IPT

There are various approaches including the microbial and chemical

techniques to regularly supervise the quality of the food materials
throughout processing. Nevertheless, there are certain parameters
that need continuous assessment during the entire supply chain.
Unfortunately, the quality parameters vary recurrently, which could
affect the quality of the food items, making it difficult for the patrons
to appraise the quality inside the package. The IPT sorts out this
limitation and enables to know the condition of the food inside the
package. There are devices fabricated for this purpose that are either
placed inside or outside the package to screen the quality of the food
products or to convey the consumers regarding the safety issues
associated with the products.
 Indicators of IPT 87

There are three main technologies of intelligent packaging

systems that are broadly acknowledged: (i) indicators, which aim to
deliver the information on food quality to the users, (ii) data carriers,
which are precisely envisioned for recording the information about
packaging, storage time and place, distribution method, and delivery
data, and (iii) sensors, which precisely quantify analytes in the
packaged food [6].

3.5 Indicators of IPT

The indicators are used to convey information related to the status

or any characteristic changes in the food materials contained
within the package or the environment surrounding the package by
perceiving visual changes. The information regarding changes can
be immediately displayed visually, e.g. different color concentrations
[7]. The unique feature of the indicators is that they provide various
direct visual signals depending on the food environment. They do
not have any specific receptors to provide information to the users
regarding food quality. The indicators that synced with the food
packaging materials include time-associated temperature indicators,
freshness indicators, and gas indicators [8].
The time-allied temperature indicator is used to measure
variations in specific temperature of the food package. It will also
provide information regarding the presence of any microbial
contamination and the structural anomaly if any happened while
processing and packing the food [9]. The freshness indicator tells
about the deterioration of food products due to chemical changes
or microbial growth. Gas indicators are usually produced as labels
or badges to indicate the emission of various gases from the food
products within the packaging system [10, 11].

3.5.1 Temperature Indicators
Temperature is an important parameter that determines the
storage period of a particular food product. Immediate rise or fall
in temperature is responsible for maintaining the quality of the
88 Surface Chemistry for Intelligent Food Packaging

processed food products. It is mandatory to check the temperature

at every phase of the delivery from packing to consumption of the
food products for the purpose of quality. There are intelligent tools
used for evaluating the temperature of the food materials at different
times during the delivery of the package. The temperature indicators
are classified in two different types: simple temperature indicator
(STI) and time temperature indicator (TTI).
The STI shows the fluctuations in temperature and warns the
consumers about the rise and fall of temperature with respect to
the critical point. It signals the users about the protein denaturation
and possible existence of microorganisms in the processed food
package [12].
The TTI is the first-generation temperature indicator, which
is an integrated pointer of time and temperature. It conveys the
information about the history of both time and temperature of the
packaged food. It also displays any unfavorable condition such as
temperature change over time [13]. TTIs are used in the form of small
self-adhesive labels attached to the food packages or containers.
Chemistry involved: The simple principle behind TTI depends on
mechanical, enzymatic, microbiological, chemical, and electrochemical
reactions, which describe the result in the form of mechanical
distortion or color change [14]. Kim et al. (2016) [15] developed
a sample isopropyl palmitate (IPP), which is a diffusion-based TTI
used for examining the microbial quality of unpasteurized juice. The
different temperature ranges have been calculated by the diffusion
of IPP, which is placed inside the indicator. The diffusion of IPP up to
7 mm from the indicator is proved to be the accurate indicator level
that represents the evaluation of spoilage by microorganisms in the
packed unpasteurized juice. However, the technologically advanced
TTI could be used for the successful indication of microbial spoilage
at 13 °C or even higher. A precise and cost-effective TTI fabricated
from the natural components to use as IPT device was developed
by Pereira et al. [13]. The TTI used as labeling film was developed
using isolated anthocyanin pigment from red cabbage combined with
chitosan and polyvinyl alcohol. Anthocyanin can be used as a natural
indicator, as it undergoes chemical changes during pH variations.
Hence, this pigment can be used for analyzing quality of the food
products by assessing the pH variations in the packed food. The
developed system can able to detect the variations in temperature
 Indicators of IPT 89

circuitously by assisting the pH change of the food products. In last

few years, there has been an increasing development and application
of several categories of TTIs, such as photochrome-driven, polymer-
based, microbe-based, diffusion-based, and enzyme-based TTIs for
the assessment of time and temperature of different unpreserved
food items.
TTIs have received growing attention for their advantage
in providing the data on the time vs temperature history of the
packed food, which is very instrumental in instigating the physical
and chemical worsening kinetics. These are readily operational
devices and user friendly. The digital signals obtained by the
indicators are easily understandable by the users, as they display
direct information related to the quality of the packed content at a
particular temperature [13].

3.5.2 Gas Indicators
To preserve the fresh, unprocessed, and organic food products, such
as fruits and vegetables, are challenging to pack and store for a long
time, due to various reasons including their respiration, leakage of
gas from and to the package, and variation in gas concentration due
to the microbial growth and metabolism inside the packaged system
[16]. The gas indicators are used as a solution for such problems.
These indicators provide information on the concentration of O2 and
CO2 inside the packaging system by varying the color of the package,
due to the particular enzymatic or chemical reaction. These indicators
provide information regarding the presence or absence of gases, as
these are directly attached to the packaged food materials [1]. As the
gas indicators are placed within the systems, some parameters such
as their toxicity, reactivity, and hydrophobic nature of the substances
are needed to be taken serious care of while designing the devices.
The components integrated while designing should have food
contact approval. There is an increasing interest in the development
of O2 and CO2 indicators among researchers, as there is a remarkable
importance of these gases in food packaging applications [17, 18].
An IPT system to surveil the intermediate moisture level through the
assessment of CO2 gas concentration inside the food package was
developed by Nopwinyuwong et al [19]. The microorganism growth
is detected by the respective color indication, as an outcome that
represents the emission of CO2 gas from the spoiled food.
90 Surface Chemistry for Intelligent Food Packaging

Chemistry involved: The gas indicator devices have three major

components, namely the Redox dyes such as methylene blue or
2,6-dichloroindophenol, an alkaline compound, and a reducing
agent such as proton donor. These indicators suffer a drawback of
dye leakage, as they are in contact with the environmental moisture
around the package. The gas indicators are commercially presented
in the form of labels, printed layers, and tablets attached to the
package or as monolayer coatings over the polymer sheets.
Vu and Won [18] developed O2 gas indicator, which detects
the emission of O2 and inhibits the leaching out of dyes printed on
the packaging medium. The recent advancement in this indicator,
which uses UV-stimulated colorimeter to sense the O2 leakage, has
addressed this issue and reduced the dye leaching by encapsulating
the device. The UV-activated O2 indicators have a redox dye Zein,
photosensitive Thionine, P25 TiO2, dispersive medium glycerol, and
polymer to encapsulate these components. The dye leakage was
stretched virtually to 80% when the Zein coated film was placed in an
aqueous environment for 24 h. The use of alginates to encapsulate the
indicator system can decrease the leakage of dye to approximately 6%,
since the ion binding ability can inhibit the cation dye from leakage
into water. This indicator system is highly sensitive and changes color
drastically upon contact with the gas present inside the package.
Hong and Park [20] developed an IPT device, which detects
the presence of CO2 gas without engendering any damage to the
packaging material. Bromocresol purple or methyl red is a basic dye,
unified to the polymeric surface (polypropylene resin and calcium
hydroxide) of the food package. This consequently helps detect the
changes in the quality of the food during transportation and storage.
This IPT system is based on calorimetric change with respect to pH
regardless of temperature variation. The change in concentration of
CO2 inside the food package gives rise to alteration in the pH that is
detected by the indicator and changes the color.

3.5.3 Freshness Indicators
Freshness indicators are developed to detect the microbial
contamination and notify the consumers regarding the freshness
of food materials in the packaging system [21]. Due to the growing
demand for fresh and healthy foods in the last two decades, the
 Indicators of IPT 91

research and development of freshness indicators have increased

massively. This indicator has to be proposed as smart device that
could monitor the grade of the packaged food products during
transportation and storage.
Chemistry involved: Freshness deterioration may be due to the
revelation of food products to unfavorable state and increased
shelf life. The organic substances emit nitrogen, amine, and other
chemicals, when they start decaying due to various factors, including
microbes. Hence, the freshness indicators are generally fabricated
with the ingredients that are associated to the microbial growth, such
as starch source, ethanol, nitrogen compounds (trimethyl amines),
different organic acids (lactic acid or acetic acid), CO2, sulfuric
compounds, and biogenic amines, to evaluate the freshness of
packaged food products [22]. They provide unswerving information
to the users regarding the integrity of the products concerning the
chemical changes or microbial growth within the package.
The quality of meat products is determined by hydrogen sulfide
(H2S) indicators. The H2S is a gas released during aging of meat matrix
and is associated with the color of the protein myoglobin, which
acts as the quality indicator for fresh meat products. Smolander et
al. introduced a freshness indicator with the principle similar to the
pre-existed modified-atmosphere technique to monitor the packed
poultry meat [23]. Other freshness indicators are developed based
on the microbial sensitivity using chemicals such as ethanol, diacetyl,
and CO2.
Rukchon et al. [24] came up with an indicator to monitor the
freshness of the packed chicken breast meat. The system is developed
based on the pH variation of the meat and the pH sensitive dye used
for the detection. This system works by determining the resulting
color produced at different levels of CO2 emitted from the packaged
chicken breast meat, which would vary the pH.
Rokka et al. [25] built a freshness indicator to surveil the
packed whole broiler chicken quality. It was developed based on
the thermo-sensitive biogenic amines, such as putrescine, tyramine,
and cadaverine. The levels of different amines vary with respect to
the varying temperatures in the broiler chicken package, thereby
representing the freshness of the meat at different times.
Zhai et al. [26] developed a freshness indicator to monitor the
freshness of packed fish using colorimetric principle. They mended
92 Surface Chemistry for Intelligent Food Packaging

the starch/polyvinyl alcohol with roselle (Hibiscus sabdariffa L.)

anthocyanins that would change the color in the presence of total
volatile nitrogen amines leaked from the spoiled seafood. These
indicators work even at the freezing temperatures. The colorimetric
film assesses the visible color changes. Hence, this film is used to
detect the freshness of fish inside the packaging device.
Ripe Sense is an aroma testing IPT device developed by a New
Zealand-based group of labs, Jenkins Group. This indicator is used to
alert the ripening of fruits at various stages, deliberating their phase
of ripening. Initially, the indicator displays red color that turns into
orange, and further into yellow, with the passage of time of maturity
levels of fruits. This device can be used for monitoring the freshness
of aromatic fruits, such as pears, kiwi, melon, mango, and stone fruits
including peach, apricot, and plum, and others [27].

3.5.4 Sensors
Sensors are the utmost integral, pioneering, and propitious
technologies for the upcoming intellectual packaging systems [3]. A
sensor is a system that has a processing and control unit made up of
electronic components, software, and an interconnection network. A
sensor is used to detect a signal for monitoring the physicochemical
properties to which the system responds.
Generally, the sensors are designed with four major functional
units: (i) Receptor, which is a signal/analyte receiving part of the
sensor that is made of a sampling unit, where the reaction between
the analyte and the sensor surface molecules take place. The analytes
are adsorbed on the surface. Upon the adsorption, the reaction
between the analyte and the surface chemicals alter the energy,
which is closely related to detect the analyte transforms or disorients,
and the physicochemical characteristics of the receptor such as redox
potential, pH, and temperature. (ii) Transduction element, which
is a measuring part of the sensor such as an electrode. This unit is
able to transform the variations in energy and carry the data into an
analytical signal, which is optical, electrical, chemical, or thermal. (iii)
Signal processing electronics, which translate the processed data of
the transducer into the readable output language. (iv) A signal display
unit, which shows the result of the analysis [28].
 Indicators of IPT 93

The ideal sensor should possess the ensuing features: (i) specificity
for the target species (i.e. selectivity); (ii) sensitivity to changes in
target species concentrations; (iii) fast response time; (iv) extended
lifetime of at least several months; and (v) small size (miniaturization),
with the possibility of low-cost manufacture. There are various types
of sensors that have been developed for food applications, such as
electrochemical sensors and luminescence sensors.
Electrochemical sensor is a significant section of the sensors,
where an electrode is used as the transducer [29]. The electrochemical
sensor is driven by the redox reaction at the periphery of the
electrode with the analyte medium; thereby stimulates the voltage of
a potentiostat. The electrons transferred between the electroactive
species in the analyte solution and the electrodes generate a
current, which is directly proportional to the analyte concentration.
The emission of fluorescence or chemiluminescence signals in
luminescence sensor is measured only after the subsequent analyte
adsorbed on an appropriate solid support, which gives origin to
the expression solid-phase luminescence. The luminescent signals
produced by the sensors are associated with the concentration of
the analytes in the food packages under certain conditions [30]. Most
of the developments are concerned on the sensing and monitoring
the food package for pollutants or contaminants that could spoil or
intoxicate the food. Even though the most advanced flexible printed
chemical sensors are amalgamated into the food packaging system,
the IPT still has a wide scope to witness more advancement, in terms
of most progressive sensor technologies that can integrate with the
intelligent devices into the packaging systems. The future scope of
IPT would be on developing the biosensors and gas sensors.

3.5.4.1 Biosensors
The major difference between the chemical receptor and biological
sensor is the receptor molecules that are made up of synthetic chemical
compounds in chemical sensors, while the biocomponents, such as
antigens, antibodies, enzymes, nucleic acids, and phages, constitute
the receptor surface of the latter [31]. Currently, the biosensors are
employed only in few food packaging applications. For instance, Food
Sentinel System was developed by SIRA Technologies (USA); it is a
packaging barcode technology that provides complete details on the
94 Surface Chemistry for Intelligent Food Packaging

history of the product that went through adverse conditions. This

device is provided with a membrane of antibody corresponding to
the certain pathogen, and the membrane is attached to the barcode.
An ink is attached to the biosensor will turn red in the presence of
contaminated bacteria and the data transmission through the barcode
will be rendered when scanned [32]. Similarly, a visual diagnostic
tool, Toxin Guard (Toxin Alert Inc., USA) is used to detect pathogens
that may deteriorate food. This type of sensor basically works on
the immunoassay of pathogenic antigen presents in analyte with
the antibody attached on the polymer packaging film. In this system,
the toxic metabolite from the pathogen reacts with the antibodies
decorated on a thin film of flexible polymer layer exhibiting a clear
color change in the device that indicates the presence of pathogens in
the food package [33]. A system that interpolates biochemistry and
electronics, Bioett, is used to track the changes in the temperature
of the packed food materials during the course of refrigerated
transportation. This system includes a biosensor incorporated into
the food package, a detector system made up of radio frequency (RF)
chip to read the data sent by the biosensor, and a database to store
the processed information about the products. In this IPT device, the
data can be read using a handheld scanner at any point in the food
supply chain [8]. A commercially available biosensor, which is flexible
to detect the toxins in food, was developed by Flex Alert; it specifically
detects the pathogens, including Escherichia coli O157, Listeria spp.,
and Salmonella spp., and aflatoxins [4].

3.5.4.2 Gas sensors
Studies have been carried out recently for the advancement of
sensors that can analyze quantitatively the gaseous analytes with
satisfactory results. Recognized systems for gas analysis include
piezo electric crystal sensors, metal oxide semiconductor field-effect
transistors (MOSFETs), organic conducting polymers, potentiometric
CO2 sensors, and amperometric O2 sensors. Though these systems
possess several limitations, these IPTs encompass various critical
analyses of packages in most of the cases. The current developments
mainly engrossed in O2 and CO2 sensors, which help overcome the
limitations. The progress of smart sensors to detect O2 concentration
that can pervade in and around the packaging system has attracted
 Indicators of IPT 95

significant attention over the past few decades. The general O2

sensors are based on sensing the luminescence and the progressive
advancements when associated with the systems based on absorption
or reflectance. These signify an alternative method to evaluate the
O2 concentration and visually indicate the results with increased
sensitivity and quantitative accuracy measurements [34]. Diverse
structures of these IPTs provide the opportunity to quantify the
analytes in three-dimensional (3-D) samples with non-destructive
analysis. Additionally, they provide faster response without the need
to produce any electrical connection or consume analyte.
Huber et al. developed a novel non-destructive, non-invasive
fiber-optic O2 meter that is used to detect O2 permeability of plastic
bottles and containers [35]. The basic principle of this is the reduction
of luminescence produced by the collision between molecular O2 and
luminescent dye molecules, when they are in the excited state in both
gaseous and liquid phases. The disadvantage of cross-sensitivity
among H2S, CO2, ammonia (NH3), pH, or any ionic species such as
sulfide (S2–), sulfate (SO42–), or chloride (Cl–), is eliminated in this IPT
and the salinity factor does not impact the measurement. Even the
turbidity of the medium and the variations in the stirring rates during
the food processing do not influence the measurement. These IPTs can
be used with the alcohol and the combination of alcohols. Fitzgerald
et al. invented a competent and more sensitive phosphorescence-
based O2 sensor using the complexes of fluorescent ruthenium(II) and
platinum(II)-octaethylporphiryne-ketone (PtOEPK) dye [36]. They
have also tested the real sample, such as smoked fish, raw and cooked
meat, and packaged sliced ham, using this sensor. This indicates that
the sensor provides accurate and dependable outcomes on real-time
applications in the market.
Baleizao et al. [37] developed a rapid and sensitive optical dual
sensor based on the luminescence measurements for the gaseous O2
and temperature monitoring. It consists of polymer films prepared
using two different luminescent compounds, one sensitive to
temperature, while other to O2. Ruthenium tris-1,10-phenanthroline,
due to its effective temperature-dependent luminescence, is used as a
temperature-sensitive dye and is conjugated with poly(acrylonitrile)
to evade cross-sensitivity with O2. For detecting the O2, Fullerene
C70 probe is used, due to its stability, thermally activated, sustained
fluorescence at elevated temperature, and exceptional O2 sensitivity.
96 Surface Chemistry for Intelligent Food Packaging

The dual sensor exhibits an operational temperature range 0−120 °C,

and detects O2 limits in the range up to 50 ppm O2 concentrations.
The progress of CO2 sensors is only the second preference with
respect to O2 sensors for food packaging applications, as O2 plays
an important role in degradation of several food products. The
application of modified atmosphere packaging (MAP) system has
been recognized, as it controls the volume of CO2 in food packages
[38]. Conservative methods for a qualitative and quantitative analysis
of CO2 consist of infrared (IR) spectroscopy, mass spectroscopy (MS),
and gas chromatography (GC). However, these techniques proposed
brilliant results, but are expensive due to sophisticated equipment
utilization [39].
There has been a great effort from the past two decades to
manufacture sensitive, rapid, economic, tuneable, and easily
contracted sensors to analyze CO2 in the food package. Von
Bultzingslowen et al. [40] fabricated an optical sensor based on the
pH-driven fluorescent indicator to monitor CO2 in MAP practices
using 1-hydroxypyrene-3,6,8-trisulfonate (HPTS), immobilized in
a hydrophobic, organically modified silica (ormosil) matrix. The
reference luminophore is encapsulated in polymer nanobeads to
inhibit the cross-sensitivity of O2, Cl–, and varying pH.
Borisov et al. [41] settled a silicone matrix-based optical CO2
sensor emulsion at room temperature using the ionic liquids and
(RTILs)–1-butyl-3-methylimidazolium salts. This fluorimetric
sensor employs 8-hydroxypyrene-1,3,6-trisulfonate (HPTS) for
the quantitative analysis of CO2, which is applicable in various
fields. Borchert et al. developed yet another opto-chemical CO2
sensor with an indicator dye, such as a phosphorescent, a reporter
dye (pentafluorophenyl)porphyrin (PtTFPP), and a colorimetric
pH indicator α-naphtholphthalein, combined with the plastic
matrix organized with a phase transfer agent tetraoctyl- or
cetyltrimethylammonium hydroxide [42]. Experiments carried
out to test the efficiency of these sensors revealed that at 4 °C, the
sensor acquired its high sensitivity to CO2 for 21 days in the food and
peripheral atmosphere environments. This efficiency is adequate for
several packaged food products.
 Indicators of IPT 97

3.5.5 Data Carriers
The notification on the quality control methods and information
about the time-dependent parameters of the packed food at every
particular time through the data carrier devices during the food
supply chain is more competent for the benefits of food safety and
quality. The data carrier device does not afford any data related
to the status of food quality, instead it is proposed for traceability,
automation, counterfeit protection, and prevention from theft [43].
The data carriers are usually used on large containers, such as multi-
box containers that contain a number of small packed units, and
shipping crates that are used to transport a large number of packed
containers, pallets, and large paperboard packages. Barcodes and
radio frequency identification (RFID) tags are the most significant
data carrier devices in the food packaging industry. These data
carrier devices belong to the chief category of convenience-enhancing
intelligent systems [44].

3.5.5.1 Barcodes
The first ever Universal Product Code (UPC) barcodes originated
in the market application in the 1970s. These barcodes are majorly
applied in the high-scale retail trade and in stores to enable inventory
control, since these are economical [45]. A barcode is a sequential
pattern of parallel lines organized to denote 12 digits of the data. An
optical barcode data scanner reads the encoded data and transmits
the information to an operating system, such as a computer, where
it is translated, displayed, and stored [1]. Initially, the barcodes
developed were one dimensional (1-D), and the primary operating
principle was closely similar to that of laser beam from the vertical
code bars cutting a horizontal slice. The first-generation barcode
had very limited storage capacity such as to store the item number
and manufacturer’s number [46]. Hence, the file size of the data
was reduced and the reduced space symbology (RSS) barcode was
developed to encode huge amount of data in a limited space. The
RSS-14 stacked omni-directional barcode and the RSS-expanded
barcode are the most commonly used RSS [47]. The two-dimensional
(2-D) barcode can able to encode more information to be stored, as
compared to 1-D barcode, which can be linked by spaces and dots
98 Surface Chemistry for Intelligent Food Packaging

organized in a matrix. This allows storing an increased density of

data within a reduced space. The quick response (QR) barcode is
the most recently used technology that can encode myriad volume
of data and then store using various encoding approaches, such as
numeric (numbers alone), alphanumeric (number and letters), byte/
binary, and kanji (logographic Chinese characters). Reading the 2-D
barcode symbologies require a scanning device that is potential to
scan the data in both vertical and horizontal matrix simultaneously.

3.5.5.2 RFID systems
The RFID tags are one of the most sophisticated technologies for the
data carrier applications. The three basic functional units of the RFID
system are a tiny antenna made up of a microchip connected to a tag
to store the data, a reader to send and receive radio signals, and a
middleware [48]. The long-distance communication up to 100 m with
the help of RF technology and the space of 1 MB to store enormous
data are the two significant advantages of the RFID system. These help
in improvising automatic identification of products and traceability
operations [49]. There are two types of tags used in the RFID, namely
the active tags that work on the power from a battery source, and the
passive tags that do not need any such power from external source.
Despite the RFID technology being very popular, it took long time
to find its spot in the food packaging market, as it is not economical
[50]. However, it should not be considered as an alternative for
barcodes for their advantages on distant communication and storage
space. Currently, the RFID tags are used only to control the road traffic,
identification of marked pallets, security alarms, parking guidance for
automobiles, and even the tracing and identification of wild animals
in forest for the census studies. Their application in the food industry
is limited to a few purposes such as product identification and tracing
the supply path, cold chain monitoring, livestock management, and
shelf life prediction [51].

3.6 Other IPT Systems

Some of the useful intelligent devices, such as doneness indicators

that are used to inform the proper completion of processed food and
 Summary and Future Prospects of 99

thermochromatic inks, are found to have fewer applications when

compared to other systems [44]. The thermosensitive thermochromatic
inks that change color with the change in temperature are printed
on the food packages. There will be an indication of color change, as
the temperature within the food packages deviates from the optimal
consumption temperature. Sometimes, the color change is convoyed
by a synchronized display of a brief message, such as “ready to serve”.
Majorly these thermochromatic inks are synthesized in companies
based in the U.S. (LCR Hallcrest, CTI Inks, QCR Solutions Corporations,
and others) and the U.K. (Siltech Limited, B&H Colour Change, and
others). The difficulty in spotting the color change is one of the
main limitations of this indicator [44]. The IPT device tackling theft,
counterfeiting, and tampering are trapping huge interest, although
it is not common in the food industry. Electronic article surveillance
(EAS) is an example of the system that is in contradiction with theft
control equipment, which is in the form of electronic-tagging system,
while anti-counterfeiting and anti-tampering devices are in the form
of holograms, thermochromatic inks, micro-tags, tear labels, and
tapes [1, 52].

3.7 Summary and Future Prospects of IPT

The IPT has modernized the food packaging sector. This technology
has enabled the producers and distributors to provide food products
to the consumers with the best possible quality and safety. The
consumers are majorly benefitted from the technology, as they are
provided with the fresh and better-quality food products, with the
help of TTIs, freshness indicators, gas concentration indicators,
and others. The distributors and retailers, on the other hand,
are benefitted by the IPT devices, including barcodes, RFID tags,
thermochromatic inks, holograms, and tear taps, to protect the
food products from counterfeiting and misplacements. The future
of IPT is very optimistic with the progression of the technology.
Electronic labeling through embedding electronic chips on the
packages with the ink technology is one of the most sophisticated
100 Surface Chemistry for Intelligent Food Packaging

technologies that may substitute the existing IPT systems. With the
advancing technologies, such as artificial intelligence (AI), there are
several developments in interactive IPT devices for food packages.
These systems could guide the consumers to improve the storage
parameters, thereby increasing the shelf life of the food products.
Simple IPT systems, such as thermochromatic inks, are used to
prevent the food package from the sunlight by varying the color
in response to the temperature without any need of electronic
assistance. There are various single-purpose-IPT devices, such as
gas concentration indicators, freshness indicators, and TTIs, used in
the current food packaging industry. A technology to unify all these
sensors together to fabricate an integrated multi-purpose device
would be more prevailing and useful for providing data concerning the
quality feature of the food products. This demands the collaboration
of various fields of research, such as the food nutrition, mechanical
engineering, and electronics and instrumentation engineering,
into the intelligent food packaging domain. Though the intelligent
packaging plays a vital role in improving the safety and quality of
delicate food products, progress has to be made in this technology
to minimize the cost of production and processing. According to an
educated approximate calculation, the cost of an intelligently packed
food is at least double the cost of the original food product. Further,
food administrative agencies have raised concerns and legal issues
related to the safety of the reactive labels coming in proximity to the
eatables. Hence, besides working on research for cost reduction of
IPTs, there is a stringent need to work on safe implementation of the
intelligent packaging system.

References

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“Intelligent packaging for food products”, Han, J.H. (ed.), Academic
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2. Yam, K.L. (2012). Emerging food packaging technologies: Principles
and practice, Chapter 8 “Intelligent packaging to enhance food
safety and quality”, Yam, K.L., Lee, D.S. (eds.), Woodhead Publishing,
Philadelphia, pp.139−155.
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3. Bagchi, A. (2012). Intelligent sensing and packaging of foods for

enhancement of shelf life: Concepts and applications, Int. J. Scientific
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Chapter 4

Brief Overview of Aspiring Properties

of Functional Biopolymers for Food
Packaging Applications

Pooja Agarwal, Anjali Gupta, and Divya Tripathy

Division of Chemistry, Galgotias University, Greater Noida, Uttar Pradesh, India
[email protected]

Increased use of plastics has created serious environmental issues

because of their resistance to biodegradation. In last few years,
interest has been developed for biodegradable polymeric materials
in packaging because of their biodegradable nature and also having
desirable properties like conventional polymers. Biopolymers have
been categorized into three classes based on their origins. Biopolymers
can be produced from biomass, can be synthesized from monomers
that are obtained from biological sources, and can be produced from
microorganisms. Functions of biopolymers depend upon different
features like physical, mechanical, thermal, and barrier properties.
Besides, the recent trend of lifestyle also poses challenges toward
innovative modes of food packaging. Functionality in packaging
material can be involved through active packaging concept. Modern

Biomaterials in Food Packaging

Edited by Mohd Yusuf and Shafat Ahmad Khan
Copyright © 2022 Jenny Stanford Publishing Pte. Ltd.
ISBN 978-981-4877-98-5 (Hardcover), 978-1-003-25678-6 (eBook)
www.jennystanford.com
106 Properties of Functional Biopolymers for Food Packaging Applications

food-packaging techniques involve hygienic processing and as a

result extend the shelf-life of food without causing any bad effect on
the health of the consumer. This chapter highlights different kinds
of biopolymers; their preferable characteristics for food packaging
application, with special emphasis on biopolymeric materials,
which appear as a promising solution for food packaging; and new
advancement in terms of functionalities, with the replacement of
conventional plastic packaging materials.

4.1 Introduction

Packaging term refers to the protection, safety, secure handling,

and improved usability of products. The commonly used packaging
materials are wood, plastic, paper, metal, and glass. Presently, plastic
is the most frequently used packaging material because of its unique
features like lightweight, non-permeable, flexible, stable (inactive to
environment), durable, and inexpensive. Due to these properties,
it persists for the long time in the environment and accumulated as
solid waste [1, 2]. Plastic also contains additives, plasticizers, and
colorants, which are responsible for serious environmental problems
during its disposal [1, 3]. Therefore, environmental concerns and
petroleum resource limitations have increased the attention for
products that are safer, environmentally friendly, non-toxic, and cost
effective. Over the past two decades, it has been the major concern
of researchers to develop polymers from renewable resources in
the area of plastic productions. Use of biodegradable polymers as
bioplastic is a promising approach to decrease the amount of plastic
waste. In addition to biodegradability, biopolymers have other
features like air penetrability, sealability at low temperature, ease
availability, and economically favorable. Starch, cellulose, protein,
polylactic acid (PLA), and polyhydroxybutyrate (PHB) are the latest
developments designed for packaging purposes. These have been
conversed in this chapter, along with the development in functionality
for active packaging.
The concept of active packaging has good effect on marketing of
food, due to its performance and fitness for food packaging. In the
last decade, many developments in packaging technology have been
  Biopolymer 107

done, such as active packaging, which can behave as an antimicrobial

agent, an oxygen scavenger, a respiration regulator, and an odor
absorber [4]. The packaging industry will stimulate due to these
evolving developments for better quality and safety products that
help in decreasing losses of food [5], along with the environmental
sustainability.

4.2 Biopolymer

It is an organic polymer that can degrade into simpler molecules

like carbon dioxide, methane, and water. It is a good alternative to
petroleum-based polymers (traditional plastics). The most familiar
biopolymers are starch, protein, peptide, DNA, and RNA. The
biopolymers are derived from renewable natural resources, which
are eco-friendly and mostly non-toxic. These are of biological origin
such as animals, plants, and microorganisms, or can be synthesized
chemically from materials that are of biological origin such as sugar,
starch, oil, and natural fat [6−12].
Origin and description of bio-based polymers: Biologically origin
polymers can be classified into three groups based on their source
and synthesis:
Group 1: The biopolymers in this category are obtained by biomass
directly. Several polysaccharides like starch, cellulose, and proteins
(casein and gluten) are some example of biopolymers in this group.
All the polymers of this category are hydrophilic in nature rather
crystalline. These polymers have excellent barrier property, still
poor in performance particularly in context of packaging of moist
food products.
Group 2: The biopolymers in this category are manufactured by a
conventional polymerization method from monomers of biological
origin. One of the excellent examples of biopolyester is PLA, which
can be produced by polymerization of bio-based monomer lactic
acid.
Group 3: The biopolymers in this group are obtained from
microorganisms. The most common example of this class is
polyhydroxyalkanoate (PHA).
108 Properties of Functional Biopolymers for Food Packaging Applications

4.2.1 Polysaccharide-Based Biopolymer

4.2.1.1 Starch
Starch is the most abundant polysaccharide, and it is inexpensive
and widely available. Due to these factors, starch-based biomaterial
has received great attention. Starch is a hydrocolloid biopolymer
belongs to the class of carbohydrate. It consists of linear chain
amylose and branched amylopectin, made up of glucose molecule
joined together by glycosidic linkage. The variation of contents of
amylase and amylopectin affects the end properties of the starch.
Elongation strength of the starch rises with the increase of amylose
content, when there is no plasticizer. High amylopectin is favorable
when plasticizer is used. For the preparation of biopolymers, several
varieties of starches like potato, corn, rice, cassava, and tapioca are
used [13]. Starch is generally used due to its thermoplastic property.
Its plasticization occurs by the process of destructuration at high
temperature in presence of water or plasticizer. However, poor
moisture barrier and mechanical properties limit its uses. These
shortcomings are improved by preparation of its bio-composites
with several other biopolymers and additives.

4.2.1.2 Cellulose

Cellulose is biological origin polymer, which is available in abundance

on the planet. It is a major component of plant cell walls. Cellulose-rich
materials are wood, cotton, and paper. The cellulose is found in plants
in abundance and works as a strengthening material [7]. It is a linear
homopolymer of glucose, which is linked by β-glycosidic linkage. It is
a tougher fiber because hydrogen bonding occurs between glucose
units, within a chain, and even between the neighboring chains.
Building and arrangement of hydroxyl group in cellulose are likely
to create strong hydrogen-bonded crystal structure. This allows the
crystallization of chains in linear conformation. Micro-fibrils in the
range of sub-micron diameter are associated along the cellulose fibers
and are called single fiber. Commonly produced cellulose derivatives
are methyl cellulose, carboxymethyl cellulose (CMC), ethyl cellulose,
hydroxyl ethyl/propyl cellulose, and cellulose acetate [14].
  Biopolymer 109

4.2.1.3 Protein
Proteins are polymeric structures made by repeating units of amino
acids with peptide linkages. There are total 22 amino acids that are
usually found in protein [15]. The proteins can be synthesized by
the chemical route or fermentation process [16]. These are used for
coating and film preparation, which can be attained from animals
e.g. casein, whey from milk protein, as well as from plants e.g. corn
zein protein, soy protein, etc. These have different physicochemical
characters according to sources from which they are obtained. The
proteins in wheat gluten and corn zein are occurred in globular form,
while casein and gelatin are example of fibrous protein [17−19].
Protein-based films are superior to polysaccharide-based films, in
respect to mechanical strength and barrier properties, along with
the better nutritional value [20]. Although, there are restrictions
in packaging with protein films and coatings because of their weak
mechanical strength related to synthetic polymeric material and
their low-moisture barrier property due to hydrophilicity [21].

4.2.2 Synthetic Biopolymer

4.2.2.1 PLA
Application of PLA has increased in recent years because of its
economical property and commercial feasibility. It is a biopolyester of
2-hydroxypropanoic acid commonly known as lactic acid. Microbial
fermentation of carbohydrate is major source of lactic acid, and it
also synthesizes chemically from petrochemicals. The lactic acid
can exists in two stereo-isomeric forms: L(+) and D(-) lactic acids.
Suitable microbe is used for the synthesis of required isomer L-lactic
acid or D-lactic acid. There are three common methods to synthesize
PLA viz: direct condensation of D- or L-lactic acid, dehydration
polymerization method, and the most prominent method is ring
opening polymerization of lactide dimer. The PLA obtained can be
classified as poly(D-lactide) (PDLA), poly(L-lactide) (PLLA), and
poly(D, L-lactide) (PDLLA), according to the isomer of lactide dimer
selected, and all these isomeric forms of polymer have different
properties [22−24].
110 Properties of Functional Biopolymers for Food Packaging Applications

The properties of PLA, like high-molecular weight, good process

ability, water-solubility resistance, and biodegradability, make it
a suitable food packaging material. These are the key reasons that
PLA has become a key substitute as a green packaging material [24,
25]. It has superior properties related to several polymers like better
mechanical strength, flavor perseverance, and odor barrier properties
than non-degradable polymers like polyethylene and poly vinyl
chloride. Also, the PLA has better thermal resistance and processing
capability than polystyrene. It also has more grease resistance and
printability to polyethylene. Thus, it is the future biodegradable
polymer that can be employed in packaging of different food items.
Although it has some restrictions in unchanged form, it degrades
easily at extensive temperature and also brittle in nature.

4.2.2.2 PHA
PHA belongs to polyester family produced by various microorganisms.
Bacterial fermentation of sugar and lipid under unbalanced growth
condition is the major production method of this polymer. The PHA
has macromolecular structure made up of 3-hydroxy fatty acid
monomer units. It is a biodegradable and biocompatible polymer
that can be acquired from renewable resources. Thermo-mechanical
property of PHA is similar to synthetic polymers like polypropylene
[25, 26]. Due to the biodegradable and biocompatible nature of this
biopolyester, it is used in several applications as degradable packaging
materials like bottles, films, sheets, laminates, coatings, and fibers.
The characteristics of the PHA depend on monomer arrangement.
Poly (3-hydroxybutyrate) is naturally occurring β-hydroxy acid
thermoplastic linear polyester and biomimetic analog of PHA
[27−29]. More than 100 monomers and copolymers can be derived
from PHAs. Recent researches have also showed that, with PHB,
many varieties of PHAs can be produced by microbial fermentation.
Nature of the carbon source and microorganism involved decides
the monomer composition of PHAs. The PHAs with middle chain
lengths show elastomeric property with low-melting point and
have comparatively lower crystallinity; whereas, PHB is crystalline
thermoplastic substance. Water vapor permeability of PHA is very
low and closer to that of LDPE, which is a very substantial property
for food packaging application [30].
  Desirable Properties of Biopolymers for Food Packaging Application 111

The homopolymer chain of PHB makes it brittle and shows glass

thermal degradation in the region of melting point [31]. It is similar
to isotactic polypropylene (iPP) in the aspect of melting temperature
(175−180 °C) and mechanical transition temperature (55 °C). It is also
similar in mechanical property as of synthetic degradable polyesters.
The PHB can be decomposed by several microorganisms in numerous
environmental conditions [32]. Its hydrolytic degradation produces
3-hydroxy butyric acid. Properties of PHA like good mechanical
strength, flavoring agent, printability, heat locking, temperature
stability, resistance to lubricants, and high dye efficacy, increase its
food packaging application [15, 33]. “Metabolix PHA” is a blend of PHB
and poly (3-hydroxyoctanoate), produced by a U.S.-based company
Metabolix. It has been approved by the FDA for making packaging
material that preserves all the desired features of non-degradable
plastics [34]. Further, the PHB and associated materials can be
applied in various areas like covering, agricultural, hygiene-related,
and biomedical products. Some other recently end-use applications
are paints, pressure-sensitive adhesives, biodegradable rubbers, and
cheese coverings. Therefore, the future prospects of PHAs are very
promising.

4.3  Desirable Properties of Biopolymers for Food

Packaging Application

4.3.1 Gas Barrier
Specific gas pressure and atmospheric conditions are required in
the food packaging industry to sustain the freshness and shelf life
of food products and to retain quality during their storage. There is
increasing requirements of food that is packed in presence of shielding
atmosphere with a particular combination of gases, including
oxygen, nitrogen, and carbon dioxide, or combination of these [33].
Packaging material requires certain gas barrier properties to hold
up specific gas composition in the packaging. The gas barrier feature
of bioplastics is very much associated to their penetration capability
[14]. The gas penetration behavior of biopolymeric materials can
be enhanced with humidity, due to hydrophilic behavior of the
materials. Multilayer structure employs better barrier property for
112 Properties of Functional Biopolymers for Food Packaging Applications

food packaging materials. Multilayers can be produced by various

methods such as electron beam evaporation, atomic deposition
technique, magnetron sputtering, and sol/gel process [14]. One of
the major requirements in the food packaging industry is to maintain
water and oxygen penetrability throughout the shelf life of thermally
treated food items.
Researches showed that gas barrier characteristics of PLA and
PLA-based substances are strongly related with the humidity [33]. As
reported by many researches, crystallinity also influences mechanical
and gas barrier characteristics of PLA sheets for food packaging. The
gas barrier property is also enhanced with the crystallinity of the
materials. According to a study, the barrier property of plasticized
edible film is related to the mechanical strength of the materials with
the decrease in tensile strength and increase in percentage elongation
(25–45%) [12, 33]. Percentage of solubility in water increases with
plasticization effect; however, elastic modulus and glass transition
temperature decrease.

4.3.2 Thermal and Mechanical

Thermal and mechanical performances are significant since they
determine fitness of biopolymers. Therefore, next to the barrier
property, the thermal and mechanical behaviors of packaging
substances are significant for processing. Good mechanical and
thermal properties are also important for the safety of products
against thermal or mechanical damage during storage period. Most
of the biopolymer materials show similar properties to conventional
polymers, such as polystyrene, which is comparatively rigid material;
polyethylene, which is relatively flexible polymer; and PET, which is
comparatively stiff material. The mechanical properties in aspect to
modulus and stiffness are very much similar as compared to traditional
polymers. The modulus range of bio-based materials can vary from
2500−3000 MPa and it is low for stiff polymers like thermoplastic
starches, i.e. up to 50 MPa, and also lower for rubbery materials like
medium chain PHAs. Various techniques like plasticization, blending
with polymeror fillers, cross-linking method, or addition of fibers, can
be applied for the processing of biopolymers to achieve the required
  Desirable Properties of Biopolymers for Food Packaging Application 113

mechanical properties [35]. Thermal and mechanical properties

of bioplastics can be varied through plasticization process, by
increasing thermal degradation temperature [33, 36]. Like bacterial
cellulose can be used to provide particular mechanical properties
in the materials. Speculation says that the materials from biological
origin can be synthesized having comparable strength as compared
to the materials that are in use currently [36].

4.3.3 Moisture Barrier
The water resistance capability of bioplastic to prevent the entry
of undesired vapors is termed as moisture barrier property. This
property can be defined as the diffusivity, permeability, and solubility
across the packaging film, and also the attraction of the packaging
substance toward moisture, which is calculated by water vapor
transmission rate. Hydrophobic nature of bio-based materials
reduces moisture barrier property of natural polymers [14, 30].
Water absorbance of packaging materials can create unwanted
effects like moisture recovery of dry food or surface drying of frozen
food. These concerns can be overcome with materials having good
moisture barrier property.
There are several methods to prepare moisture-resistant
films, e.g. polyester, wax, and fatty acid, which can be used as
hydrophobic materials for external coating. The cross-linking
of bio-materials can be done with inorganic fillers, blending
with moisture-resistant substances of polymers. This is also a
promising method, strengthening natural fibers such as jute, coir,
and sisal [37]. Morphological properties like crystallinity and chain
conformation also characterize the barrier property. This property
increases with the crystallinity of the materials [35]. Improved
moisture barrier property of packaging material is a significant
factor in the food packaging industry because it enhances shelf life
of the food. Relative study on degree of water vapor transmission of
biopolymeric substance with petroleum-based synthetic polymers
showed that bio-based materials have equivalent properties over
the conventional petroleum-based materials.
114 Properties of Functional Biopolymers for Food Packaging Applications

4.3.4 Biodegradability
Biodegradability of a polymer can be defined as the ability of
constituent, product, or waste of material to be broken down
into simpler constituents by the action of naturally occurring
microorganisms like bacteria, fungi, or algae in a biodegrading
environment. The process of biodegradation is a subjective to
environmental factors like temperature, moisture, existing nutrients,
and pH, in which the materials and microbes are exposed [14]. The
fragmentation takes place in the first step of biodegradation, which
is initiated by moisture, heat, and microbial enzymes. It is followed
by the second step in which transformation of longer molecular
material into smaller molecules takes place, which is started by
enzymes and naturally occurring acids. When the molecules are
broken into appropriate size, these are absorbed by the cell walls
of the microorganisms and metabolized for energy [38]. In this
whole procedure, carbon dioxide and methane are produced. The
polymer degradation can take place either due to photo degradation,
microbial action, or by chemical action. Degradability of a polymer
can be accelerated by the use of oxidation and additive technology in
oxo-degradation. Degradation is generally introduced by light, heat,
or microorganisms in the control degradation process.

4.4 Functional/Active Packaging

As discussed, bio-based functional packaging materials are

obtained from renewable resources and can be degraded by natural
compositing method with least environmental impact. Other than
this, recent development is made for active packaging. The active
packaging enhances storage time and preserves food quality (Figure
4.1). This can be used as an alternate to traditional food processing
procedures like high-thermal treatment and preservation by
additives, which can bring acidification and dehydration to the food
[39]. Functionality can be created by the incorporation of particular
components in biopolymers to produce active packaging materials.
Incorporation of the polymer substances with additives having anti­
microbial properties is a new development in the field of active
packaging [40]. The benefits of using such polymeric materials
  Functional/Active Packaging 115

are that these can release functional agents like antioxidants and
antimicrobials, and also maintain undesirable food components like
ethylene, oxygen, and water [41]. Direct incorporation of additives
into the food creates undesirable odor and taste, while controlled
release of functional materials into the food by packaging cover for
prolonged duration of storage and supply, and controls the growth of
undesirable properties in the food [42]. Synthetic additives produce
toxicity due to their movement into the food products. In place of
these additives, essential oils have been used nowadays. The essential
oils as natural extracts can be obtained from species of herbs and
spices, tocopherol, and extracts from plants, which are considered
safe and facilitate the chemical stability of oxygen-sensitive food
[43]. Selection of an antioxidant for functional packaging system is an
important step, which needs suitable considerations. Type of food and
its quality efficiency are the base for the selection of an antioxidant.
The antioxidant selected should be capable to make homogenous
spreading to the food and also compatible with the packaging
material. To reduce or slow down the growth of microorganisms in the
packaged food is the main purpose of using antimicrobial substances
in food packaging [44]. Antimicrobial agents can be either directly
added in packaging materials for slow dispersion through food
surface or can be filled in vapor form. Oxygen scavengers also can
be introduced in food packaging to prevent oxidation by eradicating
the oxygen. Most commonly used oxygen scavengers are ferrous
oxide, which reacts with oxygen to reduce its extent [15−18]. Carbon
dioxide scavengers and mediators can be used inside packaging
system to reduce the frequency of respiration of food and these can
also minimize difference in pressure, thus these avoid collapsing of
package due to oxygen absorption [41]. Absorbent pads or moisture-
mediated bicarbonate chemicals can be used to add carbon dioxide in
packets. Moisture controlling substances like natural clays, calcium
oxide, and silica gel can also be employed for active packaging [43].
These act as desiccants for dry food while as internal humidity
regulators for the food with large moisture extent. These substances
can be applied as porous sachets kept inside or can be applied as
permeable water vapor barrier plastic holders with desiccants [38,
39]. Humidity controllers can decrease the moisture loss, preserve
necessary relative moisture, and reduce additional moisture content
within package [40]. Treatment of packaging surfaces or films
116 Properties of Functional Biopolymers for Food Packaging Applications

through micro pores or perforations can behave as gas adsorbents

[44]. Bicarbonate of soda and activated charcoal as flavor binding
agents and food-derived colorants and pigments as color providing
agents are also used in packaging [42, 45]. Anti-foaming, light-
absorbing, and temperature-regulating agents are required in some
particular packaging systems [46−48].

Figure 4.1 Active/functional packaging system.

4.5 Conclusion

Non-biodegradable petroleum-based polymers can be replaced by

the bio-based renewable polymeric materials in food packaging,
which will help create sustainable and green environment, and will
also reduce the waste disposal cost. Biopolymers for packaging
application obtained from renewable resources show comparable
properties with the conventional plastics. These biopolymer
materials can be obtained from natural feedstock, microorganisms,
or chemical synthetic procedures. Moreover, research and
development (R&D) in this field offers advancement in innovative
functional food packaging techniques. These advanced packaging
approaches deliver enhanced food quality, protection, feasibility, and
bioactivity of functional components. Usefulness of biopolymers and
innovative packaging techniques is increasing extensively because of
their agreeable health and environmental impact and also they help
in reducing the waste.
 References 117

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Chapter 5

Recent Research and Development in

Food Packaging Technologies: A Review

Syed Dilshad Alam,a Rupak Raja,a,b Vikas Shirsath,a

Arvind Kumar Jain,b Shafat Ahmad Khan,b and Imran Alic,d
a Jubilant Biosys Limited, Noida, Uttar Pradesh, India
b Division of Chemistry, School of Basic and Applied Sciences,
Galgotias University, Greater Noida, Uttar Pradesh, India
c Department of Chemistry, Jamia Millia Islamia, New Delhi, India
d Department of Chemistry, College of Sciences, Taibah University,

Al-Madinah Al-Munawarah, Kingdom of Saudi Arabia

[email protected]

In the current scenario, packaging for food items is a great concern.

The main focus of the food industry is to provide safe, hygienic, and
testy packed food products. There is a lot of packed food items exist
in the market for consumption. The main objective of packaging
is to envisage the quality of food items packed inside it for a long
period. Novel packaging ideas in practice ensure that the products
are properly packaged with date and code, and entertain food quality
through the food labeling and auto coding. This chapter reviews
the latest advancement, research and development (R&D) in food
packaging and technologies, and their applications. Various methods
for incorporating food packaging technologies, issues related to
packaging designs and different materials, and solutions employed
are also reviewed in the chapter.

Biomaterials in Food Packaging

Edited by Mohd Yusuf and Shafat Ahmad Khan
Copyright © 2022 Jenny Stanford Publishing Pte. Ltd.
ISBN 978-981-4877-98-5 (Hardcover), 978-1-003-25678-6 (eBook)
www.jennystanford.com
122 Recent Research and Development in Food Packaging Technologies

5.1  Introduction

In the present era, uses of packed food products are very common
among families from villages to cities. In large cities, packed food
is the first choice of people to eat. Commonly, packed food attracts
the young generation. Due to the short time, the packed food
products are very easy to cook. It has also been noticed that most
of the families prefer to take lunch and dinner, outside in different
types of restaurant. Some packed food items are ready to eat and
easily available in stores. The packing materials that are being used
should be tested and certified by certain regulatory bodies. Due to
degradation nature of the packing materials, it is necessary.
Innovations in food packaging improve, combine, or extending
the four key modalities [1] such as:
(i) Protection: To prevent food products from external damage
(leak or break-up) and internal fouling;
(ii) Communication: Communication through proper way with
regulated information showing the ingredients and nutritional
contents and best use time;
(iii) Convenience: Food packaging devoted to consumers for their
best convenience; and
(iv) Containment: Fundamental information about the packaged
items with easy handling, uses, and transportation [2].
The literature dictates that most of the industries are opting
smart indicators and their demand is continuously increasing. At
present, various types of indicators available and are being used with
different benefits for producers, retailers, and consumers [3].

5.2  KeyFunctionsandRequirementsofFood
Packaging

In general, shelf-life of food has increased through the packaging

process, so that packaged food products could be stored for a certain
timespan and consumed whenever needed. However, it is an integral
way to choose appropriate packaging materials with the balance
in food protection with other issues, including material and energy
consumption, environmental concern, and strict regulations to
  Packaging Technologies Prospects 123

minimize pollution. There are many key functions for radiant food
packaging to be undersigned, including preservation, convenience,
communication, protection, temper indication, containment, and
food waste reduction [1, 2]. Advances are made on the latest trends
concerning the goal of food packaging to continue food safety with
minimization of adverse impacts on the environment.

5.3 PackagingTechnologiesProspects

Packaging of food products is a key factor to prevent them from

deterioration and extend their shelf-life. Simultaneously, the
packaging also protects the products against external as well as
internal damage, which can be caused by biological, chemical, or
physical interaction. Importantly, the packaging is also functioning
as a physical barrier to moisture, O2, volatile entities, and microbes.
It is well documented that the package is an integral part of the
preserving system that provides a shield between the food items and
the external environment [4]. It is the fundamental requirement of
food packaging as a preservation system, which is directly related to
the safety of customers. The performance of packaging is based on
various factors, such as distribution method, processing operation,
initial food quality, and size and shape of the package [5]. The
benefits of food processing include marketing and distribution tasks,
preservation, toxin removal, and improvement of overall quality of
food. By using food processing technology, the manufacturers and
suppliers of processed food products are getting more benefits.
In general, widely used tools for food preservation are modified
atmosphere packaging (MAP) and vacuum packaging (VP) [6]. By
adopting the above mentioned strategies of packaging, the food can
be protected against deteriorative effects, such as discoloration,
flavor change, odor, texture change, nutrient loss, pathogenicity, and
other measurable factors. It is also noticed that MAP and VP, which
seem to be the ideal preservative methods applicable for many food
types, are cheap and easy to handle. Their continuous demand for
preserving fresh and natural products without adding any hazardous
chemical is a big choice of interest. Nowadays, bio-plastic materials
(polymer-based) are used widely in food packaging, without much
effect on the food quality [7]. A pathway of food packaging technology
124 Recent Research and Development in Food Packaging Technologies

is shown in Figure 5.1. Besides, the different classes of food packaging

technologies are given below.

5.3.1 ConventionalTechnology
The conventional packaging technology has been used since the
past six decades. Conventional systems of food packaging have been
utilized to provide physical support from external damage and other
kinds of stimuli during the distribution, storage, and transportation
[7, 8]. To the latest regulations and designing of food packaging, four
key functionalities should be met in order to maintain shelf-life of the
item that satisfies human environment properly. The conventional
technology is known due to its availability in the open market. It
means that the presence of an infrastructure supports it uses [8].

5.3.2 ModernTechnology
The developments of advanced technologies are increasing day by
day. Nowadays, consumers are being in practice to use processed
food more than staples. Interestingly, the current advances in food
processing and technology are fulfilling the demand by opting
monitoring methods and techniques with control as well as refined
automation. The packed food that the consumers are using is an
example of hard work in food research, and thorough investigation
of a variety of food properties and actual compositions. Food can
be defined in many ways, in food events and food conferences. For
instance, it is defined as: food is a fuel that provides energy to perform
daily functions and maintain the metabolic processes in the body [9].
Therefore, the ideas of modern packaging systems for food packing
support the following:

5.3.2.1 Activepackaging
The very first Labuza [10] had used the term active packing. The
active packaging refers to the packaging that maintains the quality
of products in terms of external environment, self-life, safety,
and sensory properties. The term “active packaging” is entirely
different from “intelligent packaging”, which gives information to
the consumer regarding current properties of the food, records, or
  Packaging Technologies Prospects 125

its history. Rooney [11] enhanced the R&D of active packaging with
its scope followed by Gontard and Brody et al. [12, 13]. It contains
the interaction of environment to the packaging and product. On the
other hand, it is a system in which physical, chemical, and biological
activities are responsible for the condition of the packaged food,
which cause an extension of its shelf-life, sustainability, and sensory
properties, and microbial safety as well, while maintaining its quality
[14, 15]. The packaging production industry is a big area, globally,
characterized by its internal diversity. Its each sector affects the
overall packaging system’s demand in the market and is systematically
growing. Contrarily, it is a big challenge for manufacturers and R&D
units associated with food packaging materials to improve active
packaging [16, 17]. In this context, the manufacturers are looking
for the best solutions and being compelled to develop improved
packaging materials, which are capable of protecting food, extending
its storage period, and improving transportation, gas barrier, and
environmental performances [18], during the bio-chemical reactions
with the internal atmosphere and the product [19−22]. High-impact
processes are emerged using active packaging, including physiological
processes, chemical processes, physical processes, microbiological
changes, and infections [23−25].
It is a well-known fact that inside packaging, atmosphere can be
curbed using scavengers or emitters for gases/moisture to remove
the harsh elements from the inside environment and enhance shelf-
life of food materials [26]. Another group of packaging is based on
emitters, which releases friendly substances to the packaging system
to impart improved shelf-life [27]. Emitters can be preservatives
(sodium benzoate, benzalchonium chloride, mehylparaben,
propylparaben, etc.), humidity regulators, fragrant substances, food
additives, and biologically active compounds that inhibit the growth
of spoilage microbes. Mostly, ethanol, sulfur dioxide, and carbon
dioxide are being used as antimicrobials to avoid the growth of
microorganisms [26].
The selection of choosing packaging substitutes to impart active
properties for any food or beverages is a scientific art, based on the
nature of the item. Besides, other things considered for this include
process engineering limitations, convenience, economic advantage,
usefulness, environmental impacts, and secondary effects resulting
from some other changes in the processing or packaging. By using a
126 Recent Research and Development in Food Packaging Technologies

new technology, a new product introduced and can remove others,

due to the lifestyle changes and the limitation of old experience
[28]. Figure 5.1 depicts the pictorial representation of processing of
packaging to end user supply.

Figure5.1 Schematic pathway of food packaging technology. Reproduced

with minor modification from ref. [29], under the Creative Commons
Attribution 4.0 International (CC BY 4.0) License, 2019.

5.3.2.2 Intelligentpackaging

As per the European Union, an intelligent packaging referred as

the packing system that gives the exact condition of packaged food
during transportation and storage [30]. It is an advanced form of
traditional food packaging, and for the consumers, it is a medium of
information about the product, in terms of its properties, records of
changes, and quality. It may also useful to improve Hazard Analysis
and Critical Control Points (HACCP) and Quality Analysis and
Critical Control Points (QACCP) systems [31]. The given two control
checkpoints examine the following considerations [32]:
(i) to sense unsafe food within time;
(ii) to recognize possible hazards to health and make strategies for
preventing, reduction, and elimination thereof; and
(iii) to identify most effective methodologies that could improve the
food quality.
  Packaging Technologies Prospects 127

5.3.2.2.1  Intelligent packaging technology:

Future perspective

The advanced intelligent packaging has been reached the new phases
of technologies. The emerging organic or inorganic-based photonics
and electronics, which are being studied about optical and electrical
circuits, can be integrated with organic or inorganic materials like
polymers instead of silicon. Researches currently based on the
generation of new advanced materials with suitable functionalities
are to be a part of intelligent packaging [31, 32]. The researchers are
continuously working in this area for the development of advanced
intelligent packaging, which is in the early stage and will take time to
be commercialized in future.

5.3.2.2.2  Carbon photonics

Of late, a carbon nanomaterial (CN) proves that it has superior
electrical and mechanical properties. At the same time, it also
demonstrates a unique optical property, which might be used for the
futuristic fabrication of optical sensors, as an alternate or balance to
silicon photonics; for example, optical biosensors based on CN were
produced successfully with considerable functionality [33]. Similarly,
carbon dots and emission-color-tuning CNs have been developed
with great analytical and bioanalytical potentials, as a class of strongly
fluorescent photonics [34−36].

5.3.2.3 Smartpackaging
Earlier it was a big challenge to develop smart packaging; for instance,
to combine and integrate the active and intelligent packaging
conceptual technologies. Such type of packaging system offers several
angles to monitor changes in the products and their surrounding
environment by getting feedbacks [37]. Natural preservatives and
antioxidants inside the food items give high potential of protection
and improved shelf-life. Also, the active packaging having antioxidant
properties maintains the quality of food and it is one of the best-
gifted substitutes to traditional packaging. The antioxidants possess
the potential to reduce oxidation of the food, which is responsible for
food spoilage [38].
128 Recent Research and Development in Food Packaging Technologies

5.3.2.4 Time−temperatureindicator(TTI)
The TTIs play critical responsibility in optimizing temperature in the
food product, which is a specific quality parameter. Generally, they
composed of small, self-adhesive labels attached to single package or
larger configuration, for Fresh-Check from Lifeline technologies. The
TTIs display the temperature used during distribution with different
colors concerning mechanical, chemical, electrochemical, enzymatic,
or microbial changes. They are considered as user-friendly,
specialized to provide regularity of food safety and quality, and also
applied to monitor the temperature changes in the distribution and
storage processes [39].

5.3.2.5 Freshnessindicator
It is the direct and quick source of product quality information
after the microbial growth in the food product and gives indication
even at just starting phase. The quality standard is identified by the
chemical reaction between integrated indicators within the package
and growth metabolites of spoilage microbes [40]. The main role of
freshness detector is to determine amine, ammonia, carbohydrate
diacetyl, and ethanol; all of these are in the packaging. This can also
be applied to provide a rough estimation of the remaining shelf-life of
consumable products.

5.3.2.6 Nanotechnologyinfoodpackaging
At present, nanotechnology enhances and is capable to transform
food packaging materials continuously. It is applied to monitor the
matter of very small size of 1−100 nanometers [41]. Due to nanoscale
innovation, much interesting and amazing food packaging with
maintaining quality and food safety is achieved. Aluminum-based
nanolayer coated inside many snacks food packages is a simple
innovation and an example of nanotechnology that is already using in
food packaging [42]. Nanomaterials are being developed due to their
value-addition nature. They can be prepared top to down from huge
structures through many methodologies, including self-assembly,
layer-by-layer deposition, lasers, chemical reduction, vaporization,
and biomass. The alternate common bottom-up method for the
synthesis of complex nanoparticles is being in practice [43].
  Packaging Technologies Prospects 129

Nanosensor is a very small device that binds and responsible for

detection and displaying a signal. Contrarily, these sensors have the
strength to detect and respond to physicochemical signal (sensors)
and biological signal (biosensors), resulting to transfer that response
into a signal that can be used by humans. In the last few years, many
nanosensors have been developed for the detection of internal and
external conditions in food packaging [44]. It can also be applied to
determine microbes, contaminants, pollutants, and finally the quality
of the food [45]. By this technique, the amount of nanoparticles can
be reduced for improving the quality of packaging. However, the
quality of food depends on the composition of the nanomaterials
used. Nanomaterials and nanoparticles could be of such nanoforms:
nanotubes, fullerenes, nanofibres, nanoparticles, nanowhiskers, and
nanosheets [46]. Although, nanoparticles in the food industry show
various benefit, toxicity in the environment is a great concern by
using nanoparticles in the industry, [47]. It needs time for regulations
of nanomaterial before its implementation into food processing,
packaging, and food contact [48]. In the beginning, the manufacturers
should monitor any new product with the nanotechnology in the food
system and its risk on living kingdom before commercialization [49].

5.3.2.7 Antimicrobialpackaging
A suitable antimicrobial substance is necessarily be added for a better
packaging system to prevent microbial growth [50]. Antimicrobial
food packaging system has been achieved a remarkable milestone, as
it controls the growth of pathogenic and spoilage microbes on food
surfaces [51]. A multidisciplinary approach is required in the fields
of food and material sciences for the development of antimicrobial
packaging. So far, a thorough search dictates that various types of
studies have been done on different nano-based materials [52].
The studies revealed that nanoparticles alone (i.e. nano Ag, Au, Fe,
etc.) as well as their composites impart the antimicrobial properties
to packaging materials and therefore improve the food’s shelf-life
[48−53]. The strong interconnection between the food products
and the packaging materials results in potential applications of food
packing for a number of perishable eatables [54].
130 Recent Research and Development in Food Packaging Technologies

5.3.2.8 Ediblecoatingandfilm
It is composed of a thin layer of material that inhibits and functions as
a barrier to moisture and O2, followed by the easy movement for the
food. The integral part of the food product contains edible films and
coatings that unable to interfere with sensory characteristics [51].
Edible coatings and films function as a carrier for antimicrobial and
antioxidant compounds to provide preservatives on the food surfaces.
Due to the presence of edible coatings and films, the moisture
remains unaffected during the storage of food. These also maintain
lipid oxidation and brown coloration due to rancidity, reduce a load
of spoilage and pathogen microorganisms on the surface of food, and
useful in volatile flavor loss [55]. These are eco-friendly in nature, as
biopolymers do not affect the food’s surrounding environment [56].
By opting edible films and coatings, the recyclability of packaged food
materials is enhanced, as compared to other traditional packaging
materials, and in this way, these replace the synthetic polymer films
[57]. Food graded antimicrobial packaging films show the potential
of food packaging materials, due to biodegradability nature that gives
sustainable improvement for the modern society [58].

5.3.2.9 Sustainablepackaging
It is a well-known fact that sustainable and green protocols urge
to use biodegradable and environmentally safe alternates for food
packaging applications to reduce waste, which is being generated from
other packaging materials. For example, an improved aim is created
on sustainable packaging using materials based on polylactide acid
(PLA), starch-based films, fiber composite sugar cane pulp, and many
more [59]. Sustainable, biodegradable, and environmentally safe
materials with significant biodegradability are being achieved from
renewable sources such as biological products and microorganisms,
obtained from naturally occurring biological probes such as starch,
sugar, and natural fat or oil [60].

5.3.2.10 MAP
Advanced food packaging technologies, including MAP, maintain the
quality and freshness of the food products and also enhance their
  Conclusion and Future Dimension 131

shelf-life. Furthermore, the MAP is more appropriate packaging

technology through which the shelf-life of the packed products
increases, which are found fit for human consumption while
maintaining their essential nutrients and bioactive compounds. The
demand for MAP technology is increasing continuously to extend
shelf-life, improve product image, and avoid wastage of a large range
of fresh fruits and vegetables. The technology is found very suitable
for products because it uses permeable films and at a specific
temperature, the rate of respiration changes the concentration of
carbon dioxide and oxygen around the products. By applying this
technology, the respiration of fresh vegetables and fruits can be
minimized. The gases most frequently used in MAP are N2, CO2, and
O2. The accepted limit of O2 in MAP for fruits and vegetables is 1−5%,
concerning the safety and quality [61−63].

5.4  ConclusionandFutureDimension

In the recent era, the first choice of the customers depends on

new packaging technologies with upgraded innovations and
developments. Continuous R&D activities are being running toward
active and intelligent packaging materials to achieve dynamically and
environment-friendly packaging pieces of stuff. Nevertheless, both
the active and intelligent packaging technologies are very demanding
and widely used for food products. Additionally, the resurgence in
R&D will also improve the quality of the food packaging materials.

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Chapter 6

Edible Coatings: Recent Advancements

on Protein- and Polysaccharide-Based
Films

Anjali Gupta,a Divya Tripathy,a Meenu Aggarwal,b

and Pooja Agarwala
a Division of Chemistry, School of Basic & Applied Sciences,

Galgotias University, Greater Noida, Uttar Pradesh, India

b Department of Chemistry, Aggarwal College,

Ballabgarh, Faridabad, Haryana, India

[email protected]

Nowadays, the food industry has gained considerable attention by

consumers and improved food quality has become priority for the
ones involved in manufacturing, packaging, selling, and purchasing
of food items. In this regard, edible films and coatings have drawn
interest to improve the quality and safety of food products. The
edible materials processed into thin layers and coated on the food
products, in the form of coatings and films, which play a significant
role in their storage, marketing, and selling. These coatings and films
protect the eatables from physical or mechanical damage and also
possess chemical and microbiological activities thereby increasing
the shelf life of the food products.

Biomaterials in Food Packaging

Edited by Mohd Yusuf and Shafat Ahmad Khan
Copyright © 2022 Jenny Stanford Publishing Pte. Ltd.
ISBN 978-981-4877-98-5 (Hardcover), 978-1-003-25678-6 (eBook)
www.jennystanford.com
138 Edible Coatings

6.1 Introduction

Edible coating is a thin layer used for the packaging of food items and
can be safely consumed along with it. In recent years, biodegradable
edible films or coatings have considerably grabbed attention to
extend the shelf life of fresh fruits and minimally processed products.
Polymer materials, which are obtained as by-products and products
of agriculture, may be used as an alternative in the form of edible
coatings to reduce postharvest loss. The major advantages with these
biodegradable films and coatings are reduction of plastic packaging,
retention of aroma and moisture, and restriction of lipid migration
between food components. These properties differentiate them from
other conventional packaging materials. It has been observed that
most of the synthetic commercial packages hold average lifetime
of around 200 years in marine environment; whereas, edible films
decompose readily providing an environment-friendly solution.
Why do we require edible films? The food that directly comes
from the nature is stored, transported, and then distributed to
supermarkets and warehouses or to processing facilities. Hence, it
takes appreciable time for products to finally reach the consumers,
due to which the deterioration of their flavor, nutritional value,
and other physiological reactions take place. This gives rise to the
discovery of edible films and coatings, which cover the natural skin of
fruits and remain as one of the most cost-effective ways to maintain the
fresh food quality and safety. The demand for quality and processed
food products, storage techniques, and increased awareness toward
environmental protection has led researchers to focus on edible and
biodegradable coatings [1]. Microbial attack on the upper layer of
food is a major concern in fresh as well as processed items. In this
regard, packaging with antimicrobial coatings minimizes or inhibits
the growth of microbes on the food surface [2−4]. Edible coating is a
semi-permeable layer over food surface that acts as a barrier to air,
moisture, and microbes, increases the shelf life of the products [5−7],
retains their nutrients and aroma, and caters to the needs of the food
industry and consumer demand for fresh fruits and vegetables [8].
These days, varied edible coatings have been applied successfully
for the preservation of strawberries, tomatoes, apples, oranges,
grapefruit, capsicum, and many more. Hence, edible coatings could
  Protein-Based Edible Films and Coatings 139

be one of the alternatives to control fresh quality, spoilage, and

pathogenic bacteria. The different constituents and properties of
coatings have been reviewed by varied researchers [9−12]. This
article emphasizes the progress and development of protein- and
polysaccharide-based coatings to preserve fresh vegetables and
fruits, with an update of current research findings (Figure 6.1).

Figure 6.1 Types of edible coatings.

6.2 Protein-Based Edible Films and Coatings

Proteins function as promoters of varied biochemical processes and

tissue building. They majorly exist in the form of fibrous or globular
proteins as main classes having different physical and chemical
behaviors. Due to their nutritional value, abundance availability, and
other desirable mechanical and transparency properties, protein-
based films have been widely explored [13].
In a research article, the effect of edible films from defatted sesame
protein was discussed, and the consequences of variation in pH,
concentration, plasticizer, and temperature were studied. It was found
that all these variables drastically affected the properties of films like
tensile strength, solubility, and water vapor permeability. Maximum
tensile strength and low solubility was observed at pH 12, protein
concentration 9%, and plasticizer 10% at temperature 90 oC; while at
50 oC, thermogravimetric analysis (TGA) scan showed good thermal
stability for optimized film [14]. Potato proteins are considered to be
of great nutritional quality as compared to other proteins due to their
composition of balanced amino acids, and especially, high amount of
lysine (around 8%). Moreover, they also possess superior functional
140 Edible Coatings

properties like high foaming and emulsifying capacities. Recently,

mechanical and barrier performance of potato protein isolate has
been investigated to prove its appropriateness as a potential and new
source for bio-based edible films. Potato protein isolate plasticized
with glycerol possesses less cross-linking and less solubility in water
as compared to whey protein at pH 7. The mechanical and barrier
performance is also found to be 80%, as compared to whey protein [15].
Another source of edible films that is cheaper and has high nutritional
value, but still unexplored, is legume protein. Montalvo-Paquini et
al. developed a film from concentrated bean protein obtained from
seven Mexican varieties (Phaseolus vulgaris L.) with glycerol used as a
plasticizer. After evaluating various physical, mechanical, and chemical
properties, it was concluded that this legume family can be considered
as a potential alternative for biodegradable edible films [16].

6.2.1 Globular Proteins

6.2.1.1 Whey-based coatings and films

Whey protein constitutes around 20% soluble component of
cow milk and its by-products obtained during manufacturing of
casein and cheese. But, due to the high cost for its processing and
transportation and large water content, whey is still underused.
Although, researchers have started taking interest in whey protein,
due to its highly nutritious constituents like α-lactalbumin and
β-lactoglobulin and their integration with antipathogenic oils make
whey-based coatings perfect for various food applications.
Sharma et al. found that edible films made up of whey protein and
pectin integrated with cinnamon essential oil showed appreciable
antibacterial activity with better physical parameters. The antibacterial
activity for the two films were against Listeria monocytogenes (zones
of inhibition 14.56 mm and 26.88 mm, respectively), Escherichia
coli (zones of inhibition 11.66 mm and 15.55 mm, respectively),
and Staphylococcus aureus (zones of inhibition 13.78 mm and 26.39
mm, respectively), which are food associated pathogens. Hence, as
an alternative to sustainable packaging material, the whey-based
film can be exclusively used in processing of food items like meat,
  Protein-Based Edible Films and Coatings 141

vegetables, and bakery products [17]. In another research article,

films made up of whey protein isolate were integrated with walnut oil
and almond oil (with concentrations 1% and 0.5 %, respectively) to
improve properties of the films. The combination increased the films’
opacity, carbon dioxide and oxygen permeability, as well as improved
their hydrophobic character. The addition of oil also decreased the
water vapor permeability, swelling, and surface hydrophilicity of
the films developed from whey protein [18]. Another whey-based
coating used by researchers for the preservation of fresh cut apples,
potatoes, and carrots was blend of whey and pectin protein film that
was prepared with transglutaminase. A significant reduction in the
weight loss was observed in the coated samples even after 10 days.
The cross-linked blended coating also inhibited microbial growth
in all the analyzed samples as well as preserving their phenolic
components [19].
Nanocomposites were formed from gelatin and whey protein
obtained from orange peel with different concentrations and Cloisite
30B (dry whey protein 5% w/w). The prepared edible films were
biodegradable, as well as at 21% v/v concentration, they were highly
antibacterial in nature with higher tensile strength and aqueous
solubility, but with low transparency and moisture content. However,
addition of Cloisite 30B and tripolyphosphate cross-linkers improved
their transparency and other properties [20]. In another article,
researchers prepared biodegradable films with whey protein isolate
and glycerol, and the effects of variables, pH, whey protein isolate
(WPI) to glycerol ratio, and sonication amplitude were analyzed. It
was concluded that the packaging film was produced by WPI/glycerol
in the ratio of 1.5 at pH 7.08 with sonication amplitude of 100 to
obtain 0.275698 mm film thickness, with density 1.85064 gm/cm3,
transparency 2.32937, and moisture content 27.7102% [21].

6.2.1.2 Wheat gluten-based coatings and films

Wheat gluten, a by-product of the cereal processing industry, is
another edible biopolymer that can be explored in the polymer
market. But, its applications are limited due to its susceptibility to
water and moisture that makes the polymer dimensionally unstable,
prone to microbial attack with substandard mechanical properties.
To increase its water and moisture resistance properties, chemical
142 Edible Coatings

modification of wheat gluten by using cross-linkers was carried out,

but still the majority of layers applied to wheat gluten lacked the
appropriate adhesion.
Taking these problems into consideration, Das et al. tested a
cross-linker Jeffamine diamine on wheat gluten for adhesion of
polyethylene terephthalate film to make it more water resistant. The
resultant layer also resolved the issue of dimensional instability to
great extent [22]. It was also observed that gluten quality affects the
properties of the film. Sharma et al. prepared gluten-based films from
two Indian wheat cultivars like RAJ-3765 and C-306 with glycerol
having different concentrations and their properties were compared.
Water and acid solubility and water vapor transmission rate were
found to be lower in case of C-306 [23].
In another research article, lipid phase was incorporated in wheat
gluten-based edible films and its effect on their functional properties
was studied [24]. It was very well established with the studies that
the resultant films showed decreased hydrophilicity, water sorption
and water transfer, decreased rigidity, and increased extensibility.

6.2.1.3 Soy protein-based coatings and films

Another potential isolate that can be explored as a renewable and
biodegradable packaging material is soy protein isolate. But, its
applications are limited due to high sensitivity to moisture and inferior
mechanical properties. These properties are found to be enhanced by
the incorporation of poly-vinyl alcohol, 1,2,3-propanetriol-diglycidyl­
ether, and halloysite nanotubes by casting method without disturbing
its transparency [25].
Carpine et al. developed and studied edible films based on
emulsions whereby soy lecithin and virgin coconut oil were added to
soy protein isolate and was plasticized with glycerol. Consequently,
the moisture content decreased and elongation increased for the
films containing these components. The peroxide value was also
increased rapidly for olive oil that was stored in these film sachets,
but did not attain the maximum value as recommended by Codex
Alimentarius [26].
During slaughter process, meat can be contaminated with
pathogenic bacteria that can cause serious illness and even death. In
an article, antimicrobial films were studied using soy protein isolate,
  Protein-Based Edible Films and Coatings 143

sodium lactate, Nisin, and Ethylenediamine tetraacetic acid (EDTA).

These films showed bacteriostatic effect on meat against Salmonella,
E. coli, and Bacillus cereus having zones of inhibition 33.33 mm, 32
mm, and 32.33 mm, respectively. The films extended the shelf life of
meat by 3−6 days as compared to ordinary wraps [27].
In another article, inhibitory activities of soy-based edible coatings
incorporated with thyme and oregano essential oils at different
concentrations were evaluated. The studies were carried out on fresh
beef against E. coli O157:H7, S. aureus, and L. monocytogenes during
refrigeration. Maximum antibacterial activity was found against S.
aureus with addition of 3% essential oils to soy protein isolate films.
These films did not only control the pathogenic bacteria, but also
found to enhance color stability along with satisfactory sensory
characteristics [28].
Nowadays, attention has been drawn by bio-nanocomposite
for coating eggshells, due to deterioration in egg quality. Yu et al.
developed and studied the effect of integration of pine needle extracts
and cellulose nanocrystals with soy protein on various properties of
the coatings. The study clearly indicated that these coatings showed
decreased moisture content and increased tensile strength with
potential antioxidant activities [29]. Another edible coating that was
found to enhance the apricots’ shelf life is soybean protein isolate
chitosan stored at 2 °C. This coating not only significantly prevented
weight loss and decreased firmness in apricots, but also improved
textural properties by inhibiting pectin degradation [30].

6.2.2 Fibrillar Proteins

6.2.2.1 Gelatin- and collagen-based coatings and films

Skin of goat is one of the by-products of slaughtering house that could
be explored as a raw material for edible films. Said et al. combined
collagen extracted from goatskin with glycerol and found improved
properties of edible films like thickness and elongation at break and
tensile strength [31].
Gelatin is also an important resource of protein obtained from
collagen hydrolysis that can be explored to be used as edible films.
Yang et al. studied the extraction of gelatin coating from duck feet,
144 Edible Coatings

combined with cinnamon bark oil, and evaluated its physical

properties and enhancement of microbial safety during packaging
of cherry tomatoes. This coating was found to reduce the growth
of Salmonella typhimurium on cherry tomatoes while storage, as
well as inhibit the color change [32]. Aitboulahsen et al. integrated
an essential oil Mentha pulegium (1%) with gelatin-based coating
and studied its effect on different physicochemical parameters of
strawberries in cold storage. The edible coating was found to inhibit
various properties responsible for the deterioration of postharvest
strawberries, such as weight loss, color, firmness, total phenolic
content, total soluble solids, pH, and microbial activity [33]. In
another article, citric acid was incorporated in gelatin-based coating
and found that it inhibited the growth of E. coli [34]. It was concluded
that films based on gelatin may emerge as potential biopolymers as
compared to other protein-based films.
Wang et al. studied various properties of collagen-based films
mixed with sodium alginate. It was concluded that the thermal
stability and viscosity of the films were significantly improved
with better tensile strength (26.49 MPa), water vapor permeability
(1.79 × 10−10 g·cm−1·s−1·Pa−1), and oxygen permeability (3.77 ×
10−5 cm3·m−2·d−1·Pa−1) [35].

6.3  Polysaccharide-Based Edible Films and

Coatings

Other commonly discussed natural polymers are polysaccharides

that are extensively used for the preparation of edible coatings. They
include starch, cellulose, pectin, chitosan, and alginate, and their
chemical structures are given in Figure 6.2. They are considered to
be potential oxygen blocker, but on the contrary being hydrophilic
in nature, they possess reduced water vapor barrier properties.
These coatings increase the shelf life of vegetables, fruits, and
meat products by drastically inhibiting darkening of the surface,
dehydration, and oxidative rancidity.
  Polysaccharide-Based Edible Films and Coatings 145

6.3.1 Starch-Based Coatings and Films

The most abundant natural carbohydrate polymer is starch that
comprises amylose and amylopectin. The coatings made up of starch
are found to be tasteless, odorless, transparent, and good O2 and CO2
barrier [36, 37]. However, they show poor water vapor barrier, due
to their hydrophilicity, non-thermoplasticity, and poor mechanical
properties [38−40].
Zuo et al. developed corn wheat starch based bilayer films
incorporated with zein protein, and their physical and mechanical
properties, antioxidant activity, and water vapor permeability were
evaluated. It was found that the bilayer film exhibited excellent
antioxidant activity, highly compact and smoother surface, with
better cross-section that made it an excellent packaging material for
seasoning, oil sauces, and dry vegetables [41]. In another research
article, thermoplastic starch films were produced from different
sources with plasticizer as glycerol and their physical and chemical
properties were compared. It was found that films with high amylose
content showed improved mechanical properties that might be
attributed to highly crystalline domains [42]. Similar results were
obtained when rice starch and corn starch were added; i.e. amylose
content was increased to produce bioplastics. They were also found
to possess better biodegradability and improved tensile properties
[43]. Addition of nanoemulsion of nutmeg oil and glycerol further
enhanced the functional and mechanical properties of the films. They
were also found to show bactericidal activities against E. coli and S.
aureus [44].

CH2OH H OH
O H
H
O OH O OH H O
OH H OH
H
H O
H OH CH2OH
Cellulose
146 Edible Coatings

CH2OH H NH2
O H
H
O OH O OH H O
OH H H
H
H O
H NH2 CH2OH

Chitosan

COONa H H
O H
H
O H O OH OH O
OH HO H
H
H O
H H COONa
Sodium Alginate

H OH COOH
O H
H
O OH H O H O
H OH H
H
O H

COOCH3 H OH

Pectin
CH2OH 1,4-linkage CH2OH
O O
H
O H O H
OH H OH H
H
H
H OH H OH O
1,6-linkage

CH2OH H2C
O O
H
O H O H O
OH H OH H
H
H
H OH H OH
Starch
Figure 6.2 Chemical structures of some polysaccharides.
  Polysaccharide-Based Edible Films and Coatings 147

6.3.2 Cellulose-Based Coatings and Films

Da Silva et al. prepared different types of coatings incorporated with
nanocrystals of cellulose, lemongrass essential oils, and glycerol.
The coatings were applied on strawberries during refrigeration and
their effects on acidity, weight loss, pH, total soluble content, and
anthocyanin content were studied after different durations. It was
found that as compared to uncoated fruits, the coatings not only
minimized the weight loss and titratable acidity related to storage time,
but at the same time controlled the increase of anthocyanin content
and total soluble solids content, which were otherwise remarkably
higher in uncoated fruits [45]. Similar results were obtained for
the coatings based on cellulose nanofibers, hydroxypropyl methyl
cellulose, glycerol, and k-carrageenan applied on Vitis vinifera L.
grape surface for 41 days. It showed around 30−34% less water
vapor permeability and weight loss, as compared to uncoated grapes,
suggested an extension of shelf life of the product [46].
Moreover, hydroxypropyl methylcellulose and methylcellulose
have been broadly used to decrease absorption of oil during deep
frying foodstuffs. Methylcellulose has been applied on confectionery
food items to block lipid passage [10].

6.3.3 Chitosan-Based Coatings and Films

Chitosan, derived from chitin, comprises exoskeleton of mollusks and
crustaceans, and is produced by deacetylation of chitin in alkaline
solution. It is a natural, safe, allergen-free, and sustainable polymer
with improved medicinal properties [47]. Chitosan coatings have
been successfully applied in the food industry, due to its properties
[10] of forming continuous coating layer on food items. Kumar et al.
recently reviewed its physicochemical properties and applications in
the food industry [48].
Xinyu tangerine, a citrus fruit found in China with plentiful
nutrients is prone to fungal infection by Penicillium italicum that
reduces its commercial value. Recently, Chen et al. studied the effect
of chitosan (CS)-based edible coating mixed with antimicrobial agent,
i.e. fruit Ficus hirta Vahl. extract (FFE) on Xinyu tangerines at 5 °C.
Antifungal activities were observed against P. italicum, with EC50
148 Edible Coatings

value 12.543 mg/mL in vivo. It was also found that FFE–CS edible
coating exhibited great reduction of titrable acid, total soluble solid,
and ascorbic acid content, due to the reduction in weight loss, fruit
decay rate, malondialdehyde content, and respiration rate at 5 °C.
Furthermore, the activities of defensive enzymes like peroxidase,
superoxide dismutase, and phenylalanine ammonia lyase were
higher in the fruits coated with FFE–CS [49].
In another research article, the effect of chitosan-polyvinyl
pyrrolidine coating incorporated with salicylic acid was studied on
the shelf life of guava fruits at different color maturity stages. The
edible coating was found to improve the antioxidant activities as well
as browning parameters like total phenolic content, phenylalanine
ammonia lyase, and polyphenol oxidase [50]. Similar effect was
observed when CS/carboxymethyl/Moringa leaf extract coating was
applied on avocado fruit. This coating was efficiently found to reduce
the moisture loss, respiration rate, and firmness that significantly
improved the shelf life and quality of the fruit [51]. Treviño-Garza
et al. studied the extended shelf life and retained quality of cut fruit
when CS/linseed or CS/Aloe mucilage edible coatings were applied
on freshly cut pine apple [52]. Similar results were obtained when
mango fruit was coated with CS/beeswax coating that improved its
shelf life and maintained firmness up to three weeks, as compared to
the uncoated fruit [53].
Another edible coating investigated for the increasing shelf life of
blueberries was the blend of chitosan, quinoa protein, and sunflower
oil at 4 oC. It was observed that this coating significantly controlled
the growth of yeast and molds during the storage period of 32 days.
Its elongation and tensile strength at break were also found to be
117.2% ± 7% and 0.45 ± 0.29 MPa, respectively, with water vapor
permeability of 3.3 × 10−12 ± 4.0 × 10−13 g s−1 m−1 Pa−1 [54].

6.3.4 Pectin-Based Coatings and Films

Pectin is a soluble component of plant fiber derived from cell walls
of plants. It is also referred to as a detoxifying agent and prebiotics,
as it exerts beneficial effects in the gastrointestinal system. Several
researchers used pectin for layer-by-layer coating to increase the
shelf life of freshly cut cantaloupe, pear, mango, peach, avocado,
and cucumber [55−57]. Maftoonazad et al. studied the effect of
  Polysaccharide-Based Edible Films and Coatings 149

pectin-based coating on the physical, chemical, and physiological

properties of lime fruits. The moisture loss in the coated fruits was
found to be lower as compared with the uncoated fruits along with
better firmness, color retention, and other quality parameters [58].
In a research article, pectin-based coating was proved to improve
the nutritional quality of dried red guava, as it acted as a barrier to
carotenoid oxidation and also retained the total phenolic content of
the fruit [59]. In another article, pectin gels were used as coatings to
increase the lifetime of strawberries. Better results were obtained
in terms of quality, color parameters, and humidity loss in coated
strawberries [60]. In order to preserve black raspberry, pectin
coating, enriched with thyme and lemon essential oils at 5 oC, was
applied and its effect was studied for a period of 12 days. Due to
its highly sensitive nature to fungal attack, high water content, and
metabolic activity, the postharvest life of black raspberry is very
short. The shelf life of the coated fruit was increased, due to delayed
degradation of vitamin C, anthocyanin, and controlled loss of fruit
moisture and weight, thereby preserved the quality and appearance
of the fruit [61]. Other studied coatings that were designed to
increase the shelf life of tomatoes were pectin, and beetroot- and
corn flour-based coatings. After the application of these coatings,
significant increase in the shelf life of tomatoes along with retention
of quality was observed. This was attributed to the controlled loss
of weight and other phenolic acids, respiration rate, ripening index,
firmness, and antioxidant activity (2,2-diphenyl-1-picryl-hydrazyl­
hydrate [DPPH]) [62].

6.3.5 Alginate-Based Coatings and Films

Alginate is a polysaccharide of great concern as an effective
biopolymer film or coating constituent, due of its distinctive colloidal
characteristics such as thickening, gel forming, film forming, and
emulsion stabilizing agent. Vieira et al. observed the antipathogenic
effect of alginate-based edible coating combined with essential oils
against Salmonella enterica and Listeria monocytogenes on apples.
It was shown that alginate coating enriched with citral and eugenol
was found to be antipathogenic, thereby ensured the food safety and
enhanced the shelf life in case of apples [63]. It was also observed
that coatings made up of alginate (3%) and chitosan mixed with
150 Edible Coatings

extract of olive leaves retarded the ripening process when applied

over sweet cherries. This increased the shelf life of the fruit and
retained the phytochemicals with better antioxidative property even
after 20 days [64].
Similar results were obtained when strawberries and fresh cut
cantaloupe were covered with sodium alginate-based layer. The
coating significantly reduced the loss of water in cantaloupe pieces
and, on the contrary, promoted water loss in case of strawberries
[65]. Yin et al. also proved the significance of multilayer alginate­
based coatings for the preservation of mangoes [66]. It was found
that mangoes coated with five layers showed delayed decay,
extended shelf life, nutrition preservation, and improved physical
and chemical parameters. Alginate- and chitosan-based coatings
incorporated with cinnamon oil microcapsules when applied over
mangoes layer-by-layer helped in maintaining their commercial and
nutritional value.

6.4 Conclusion

Since vegetables and fruits preservation is becoming a challenging

task for the entire world, researchers have acknowledged edible
films and coatings as a solution. This may be attributed to their
characteristics, i.e. they are biodegradable, naturally occurring,
renewable, and cheap, and also contain essential nutrients and
natural antimicrobials. The researchers have also mixed various
essential oils in coatings to minimize its shortcomings and maximize
their health benefits (Table 6.1). These coatings and films not only
possess varied nutraceutical features, but also retain the physical
and chemical aspects of the fruits and vegetables to prevent
postharvest losses. The coatings act as perfect barriers to moisture
content, CO2, O2, and water vapor; thereby maintaining the aroma,
flavor, texture, color, look, and nutritional value of the products,
and protecting them from microbes. Keeping these benefits in
mind, this article emphasizes on different polysaccharides and
protein-based edible coatings to preserve various food items by
increasing their shelf life.
Table 6.1 Effect of essential oils incorporation in various edible coatings

S. Basic component Essential oil used Food product Activity Reference

No. of edible coating
1 Whey protein Cinnamon Meat, bakery Antibacterial activity against [17]
essential oil products, Listeria monocytogenes, Escherichia
vegetables coli, and Staphylococcus aureus
2 Pectin Cinnamon Meat, bakery Antibacterial activity against L. [17]
essential oil products, monocytogenes, E. coli, and S.
vegetables aureus
3 Soy protein Thyme and Fresh beef Antibacterial activity against E. [28]
oregano essential coli O157:H7, S. aureus, and L.
oils monocytogenes
4 Gelatin Mentha pulegium Strawberries Antimicrobial activity [33]
(1%)
5 Chitosan Ficus hirta Vahl. Xinyu Antifungal activity against [49]
extract tangerine Penicillium italicum (EC50 = 12.543
(Chinese mg/mL)
citrus fruit)
6 Pectin Thyme and lemon Black Antifungal [61]
essential oils raspberry
7 Alginate Citral and eugenol Apples Antibacterial activity against [63]

Conclusion
essential oils Salmonella enterica and L.
monocytogenes

151

152 Edible Coatings

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Chapter 7

Characterization of Cassava Starch-Zinc

Nanocomposite Film for Food Packaging

Adeshina Fadeyibi
Department of Food and Agricultural Engineering,

Faculty of Engineering and Technology,

Kwara State University Malete,

P.M.B. 1530, Ilorin, Kwara State 234/North Central, Nigeria

[email protected]

Performance of a pure thermoplastic film can be enhanced by

adding nanoparticles of the size ranging 1–100 nm for application
in food packaging. This research was carried out to develop
a nanocomposite by mechanically homogenizing different
proportions of cassava starch (1000 g), glycerol (45–55%, w/w),
and zinc nanocomposites (0–2%, w/w). A dispersed mixture of 24 g
of these products was then mixed with distilled water (600 ml) and
heated for 30 min at boiling temperature to form a thermoplastic
solution. The film was formed in different sizes (15, 16, and 17 µm
thickness) by casting the solution on a 350 mm ×180 mm plastic
mold of different depths (8, 10, and 12 mm). The performance
of the film, including barrier, thermal, and structural properties,

Biomaterials in Food Packaging

Edited by Mohd Yusuf and Shafat Ahmad Khan
Copyright © 2022 Jenny Stanford Publishing Pte. Ltd.
ISBN 978-981-4877-98-5 (Hardcover), 978-1-003-25678-6 (eBook)
www.jennystanford.com
160 Characterization of Cassava Starch-Zinc Nanocomposite Film for Food Packaging

was determined using standard methods. The results showed that

the oxygen and water vapor decreased with the thickness and
increased with the concentration of the glycerol. Plastic d-spacing
increased with an increase in thickness, and this might indicate
the ability of the material to intercalate and exfoliate at some
points during a prolonged packaging application. It might also
indicate the short-range order of the material constituents in the
film for a better service performance. A small degradation of the
film was observed between 30 °C and 60 °C. This indicated that
the film was thermally stable and might be suitable for packaging
applications, especially in the tropical climes. The information of
the characterized attributes and optimization of the cassava starch
zinc-nanocomposite films justified their alternative application to
pure thermoplastic and conventional films for food packaging.

7.1 Introduction

Nanocomposite films are prepared from the homogeneous mixture

of renewable raw materials, such as starch, proteins, or any
polysaccharide, with a nontoxic plasticizer like glycerol in boiling
water at 95 °C [1–4]. Normally, the constituent materials are chosen
based on their cost and availability, in order not to interfere with
the primary need of the products for food packaging. All kinds of
the nanocomposite films, regardless of their source, should have
enhanced service performance, and those made from the starch are
preferred for economic reason. Due to this, starch is often used in
the production of nanocomposite film [3, 4– 6]. However, despite
the huge potentials of the starch-based biodegradable materials,
the poor service performance in terms of their physical, mechanical,
thermal, and structural attributes have greatly limited their
applications [7]. Hence, the nanoparticles are often added during
the formulation process of the film to provide the attributes required
for the packaging applications. The nanoparticles are organic or
inorganic materials whose particle size does not exceed 100 nm [8,
9]. These materials can interact with the other material constituents
in the biodegradable film because of their large reactive surface area
  Introduction 161

to volume ratio [5–7]. The resulting blend will thus influence the
structural build-up of the molecules, thereby inducing the desired
improvement of the film’s properties [7].
Many different formulations of nanocomposite films have been
reported for application in food packaging [1−7, 9, 10]. For instance,
Dang and Yoksan [1] developed a thermoplastic starch from a blend of
a plasticized starch and chitosan nanoparticles. Fadeyibi et al. [2, 5, 6]
developed a biodegradable film from a blend of the cassava starch
and zinc nanoparticles. Chung at al. [3] prepared a biodegradable
film from a blend of starch and clay nanocomposites. Dai et al. [7]
developed a biodegradable film from a blend of corn starch and taro
starch nanoparticles. Tall et al. [9] prepared a biodegradable film
from a blend of starch and Ni–Ti nanoparticles. However, the issue
with the above-mentioned films is how to solve the possibility of
material migration into the packaged food. For this reason, many
other types of nanocomposite films are being developed to address
this challenge. One way out research has suggested to use a health-
friendly nanocomposite material for inclusion in the film formulation.
Typically, zinc nanoparticles have been reported to possess this quality
and can be used in the formulation of the nanocomposite film, but the
quantity added must not exceed 2% (w/w) [2, 5, 6, 10, 11]. Therefore,
the study on the characterization of the nanocomposite film prepared
from the blend of starch, plasticizer, and zinc nanoparticles cannot be
over emphasized.
Application of this class of material in the food packaging has been
widely reported. For instance, Fadeyibi et al. [5, 11] used the cassava
starch-zinc nanocomposite film to preserve the nutrition qualities,
hinder microbial growth, and extend the shelf-lives of tomatoes,
cucumber, and garden eggs. Also, Zhang et al. [10] proposed the use of
zinc oxide nanoparticles as an effective antimicrobial agent for the use
in the preservation of fruits and vegetables. However, the mechanism
of this striking behavior of the nanocomposite film has not been
reported. Therefore, there is a need to study the characteristics of the
nanocomposite film to fully understand its behavior. The objective of
this research was to synthesize and characterize the cassava starch-
zinc nanocomposite film based on its physical, mechanical, thermal,
and structural attributes.
162 Characterization of Cassava Starch-Zinc Nanocomposite Film for Food Packaging

7.2 Materials and Methods

7.2.1 Synthesis and Particle Size Analysis of

Nanoparticles
The nanoparticles were synthesized using the sol-gel method
described by Fadeyibi et al. [2, 7, 12] and Surya [13] at the processing
and storage laboratory, Federal University of Technology, Minna. In
this method, a 30 ml of distilled water was added to a solution of 20
ml triethanolamine and 2 ml ethanol, and mixed thoroughly to form
a homogeneous solution. This was transferred into a 500 ml beaker
containing a 0.5 M solution of 5.39 g zinc acetate di-hydrate and 50
ml distilled water. Another solution of 2 g ammonium hydroxide and
10 ml distilled water was added to the homogeneous mixture in the
beaker, which was placed on a Bunsen burner to heat for 20 min. A
white bulky precipitate was formed, which was washed 10 times
with distilled water before filtration to obtain a clean white residue
and dried in an air-circulated oven dryer for 8 h. Moreover, the size
distribution of the resulting nanoparticle was determined using a
Zetasizer equipment (ver. 7.01) at the Center of Genetic Engineering
and Biotechnology, Federal University of Technology Minna, Nigeria.
The size of the nanoparticles was found in the range of 4−6 nm.

7.2.2 Development of Nanocomposite Film

The nanocomposite film was developed by mechanically
homogenizing different proportions of cassava starch (1000 g),
glycerol (45–55%, w/w), and zinc nanocomposites (0–2%, w/w). The
choice of the glycerol instead of other types of plasticizers for binding
the starch and the nanoparticles together was basically because it did
not pose any health hazard when used to prepare materials for food
packaging [7, 14]. A dispersed mixture of 24 g of the products was
then mixed with distilled water (600 ml) and heated for 30 min at
boiling temperature to form a thermoplastic solution. The film was
formed in different sizes (15, 16 and 17 µm thickness) by casting the
solution on a 350 mm ×180 mm plastic mold of different depths (8,
10, and 12 mm). The film was thereafter carefully peeled off from the
mold and sealed in the polyethylene pack to avoid possible hydration.
The process flow diagram for the preparation of cassava starch
nanocomposite film is shown in Figure 7.1 [2, 15].
  Materials and Methods 163

48 hours at 50oC
Starch (1000 g)
Nanoparticle (0-15%) Oven
Glycerol (45-55 %)
Extruder
Grinder
Film casting with mould
Drying Nanocomposi tes
Casting solution after
24 hours at 60oC heating to 95oC
and 80% RH
Figure 7.1 Process flow diagram for the development of the nanocomposite
film.

7.2.3 Determination of Structural and Barrier

Properties
A multipurpose X-ray diffractometer was used to study the structural
properties, based on the full-width at half maximum and polymer
d-spacing of the nanocomposite film, at the Sheda Science and
Technology Complex (SHESTCO), Abuja, Nigeria. The range of
orderliness of the molecular constituents in the film as well as the
degree of intercalation and exfoliation processes in its structure was
determined [2]. The ASTM Standard method was used to determine
the permeability of the film due to water vapor [16]. This method
involves placing an 8.75 cm diameter sample of the nanocomposite
film inside a test dish filled with 50 ml deionized water at 100%
relative humidity (RH). The setup was subjected to a temperature
and RH of 25 °C and 65%, respectively. The test dish was arranged on
a rotating turntable to expose it to the same atmospheric conditions
for 2 h, before the initial weight of the sample was recorded. The final
weight of the sample of the film was obtained after every 15 min, and
average values and standard deviations were computed using the
expression in Eq. (7.1) [16, 17].
∆m
Wvpt = (7.1)
tA
where, Δm is change in mass (g), t is the time (min), A is the area of
the mouth of the test dish (m2), and Wvpt = water vapor transmission
rate (g−2s−1).
Thus, the water vapor permeability of each film sample was
computed using Eq. (7.2) [16].
164 Characterization of Cassava Starch-Zinc Nanocomposite Film for Food Packaging

Wvpt (7.2)
Wvp = ∆p ×T

where T is the thickness of the film sample (mm), Δp the partial

vapor pressure difference across the film, and Wvp the water vapor
permeability (g/m.Pa.s).
Furthermore, the method described by Fadeyibi et al. [2] was
used to determine the oxygen gas permeability of the nanocomposite
film. In this method, 2 g of the film sample was placed inside an
absorption column setup, which was stocked at one end, and stream
of oxygen gas was passed into the column via the open end at the top
[17, 18]. The concentration of the oxygen gas inside the column was
measured using an electronic weighing balance for 1 h at an interval
of 10 min. Thus, knowing the data of properties given in Table 7.1,
the average value and standard deviation of the oxygen permeability
of each sample of the nanocomposite film were computed using
Eqs. (7.3−7.8).

Table 7.1 Data of properties used for the calculation of oxygen permeability

Variable Symbol Value SI unit

1 Volume of column Vv 0.0174 cm3

2 Density of oxygen ΡO2 0.001331 g/m3

3 Atmospheric pressure P atm 101325 Pa

4 Saturated water vapor pressure PsatH2O 190.2× T °C Pa

5 Area of film sample A 0.000123 m2

6 Atmospheric temperature T 25 °C

mo2 (7.3)
[O2 ] = 1000M

RH × PsatH2O (7.4)
[O2 ]n = 100RT
O2
[O2]t% = [O ] × 100 (7.5)
2 n
Therefore,
Pt = Patm−PsatH2O × T (7.6)
  Materials and Methods 165

∆PO2 = ([O2 ]t−[O2 ]i)Pt (7.7)

∆m∆y
Op = (7.8)
A ∆t ∆PO2 )
where [O2]t is the oxygen concentration inside the absorption
column at time t, [O2]i the initial column oxygen content, the mass
of oxygen gas absorbed by the cassava starch nanocomposite film in
the column, M the molar mass of oxygen gas (16 g/mol), R the molar
gas constant, RH relative humidity (63%), T absolute temperature
(25 + 273 K), Op oxygen permeability (g/m.Pa.s), and Δy the thickness
of the film (μm).

7.2.4 Determination of Thermal and Rheological

Properties
A thermogravimetric analyzer was used to determine the thermal
properties of the nanocomposite film. The weight degradation or
loss of the film was determined by computing its difference in weight
after exposure to a laboratory-controlled temperature 30−950
°C for 30 min. The rheological properties of the nanocomposite
films were determined using a nano-mechanical testing machine
(Model: Hysitron TI750) at the SHESTCO, Abuja, Nigeria. A record
of the applied load on the film sample, depth of penetration of an
indenter, and the corresponding indented area were determined
by the machine’s response. The values of the young modulus,
hardness, activation volume, and tensile strength of the sample of the
nanocomposite film were thereafter computed from a graph of the
load versus the penetration depth or displacement (Figure 7.2.), and
using the empirical relationships in Eqs. (7.9−7.14) [19].

Figure 7.2 Load-displacement curve of a sample of nanocomposite film [19].

166 Characterization of Cassava Starch-Zinc Nanocomposite Film for Food Packaging

E = dP⁄dh (7.9)

S2 π
Yr = × (7.10)
2α Ai(ha)
Pmax
H= (7.11)
AP
d lnσ
m= . (7.12)
d lnδ
.
. 9kb T ln δ (7.13)
υ=
dH
Pmax
Ts = (7.14)
Ac
where dP/dh is the slope of the load displacement curve (N/m), S
stiffness of the contact of the indenter with film sample, α geometric
constant of the material (= 1), ha contact depth (μm), Ap projected
area of the indenter (μm2), Yr the reduced modulus of the film
sample (μN/mm2), H hardness of the film sample (MPa), Pmax the
maximum applied load (μN), σ flow stress of the film due to indenter
penetration (μN/mm2), strain or drift rate of the film under
indentation (nms−1), m stress strain sensitivity of the flow (μN/
mm2), kb Stephen Boltzmann’s constant, T temperature of the film
sample (°C), activation energy (kJ), Ac cross-sectional area of the film
sample (mm2), and Ts tensile strength of the film sample (N/mm2).

7.3 Results and Discussion

7.3.1 Permeability of Nanocomposite Film

The study of water vapor permeability of food packaging materials
is important for maintaining or extending the shelf life of the food
product. The water vapor permeability coefficient indicates the
amount of water vapor that permeates per unit of area and time
in the nanocomposite film. The results of the permeability of the
various categories of the nanocomposite film after 3 h exposure of
water and oxygen gas are presented in Table 7.2. The variation of the
water vapor and oxygen permeability with the concentration glycerol
  Results and Discussion 167

and the level of zinc nanoparticles are affected by the thickness of

the film. The amount of water vapor, absorbed by the film, decreases
with the concentration of the zinc nanoparticles and increases with
the concentration of the glycerol. The molecular absorption behavior
of the nanocomposite films may be influenced by the nanoparticles
used. The water vapor permeability is low for the film without the
nanoparticles and high for the film with 2% nanoparticles. The
reason for this may be associated with the higher water absorption
affinity of nanoparticles at higher concentrations. The addition
of the nanoparticles to the film may have caused a modification of
the polymer network of the film, thereby affecting its water vapor
permeability. An increase in the glycerol concentration from 45%
to 55% may even cause an increase in the mobility of the polymeric
chains of the film [20]. The overall effect of the composition of the
film on the water vapor permeability of the material can be enhanced
with the addition of more nanoparticles and glycerol. The addition
of more glycerol may decrease the intermolecular hydrogen bonds
between the polymer chains, thereby increasing the flexibility of the
nanocomposite film [20, 21]. The nanocomposite film is, therefore,
an ideal material for packaging low-moisture food products because
of its high-water vapor permeability coefficient.
The knowledge of oxygen gas permeability of the nanocomposite
film is essential for understanding the rate of product respiration
and shelf life. The amount of oxygen gas absorbed by the film
decreases with the increase in concentrations of zinc nanoparticles
and glycerol (Table 7.2). The oxygen permeability is generally higher
for the film without the nanoparticles, and this decreases with the
increase in level of nanoparticles and glycerol. The presence of the
nanoparticles in the film is likely to alter the gas mobility, as they
diffuse across the film. Although the reason for this behavior is
not yet known, it is likely that the decrease in the porosity of the
nanocomposite film as a result of an increase in amount of the
nanoparticles may be responsible for this observation. It may also
be related with the formation of a stable complex resulting from
the filling up of the empty d-spaces of the zinc nanoparticles with
the oxygen gas molecules [2]. Therefore, the rate of diffusion of the
oxygen gas across the film layers may reduce due to the decrease
in number of pore space or pinhole opening of the film. Thus, the
nanocomposite film can help reduce the amount of atmospheric
 168
Characterization of Cassava Starch-Zinc Nanocomposite Film for Food Packaging
Table 7.2 Permeability of cassava starch nanocomposite films for 3 h period

Permeability of cassava starch nanocomposite films (g/m.Pa.s)

Film of 15 µm Film of 16 µm Film of 17 µm
water vapor
OP = Oxygen
permeability:
Treatments permeability Treatments WVP [× 10−10] OP[× 10−11] Treatments WVP [× 10−10] OP[× 10−11]
WVP
OP[× 10−11]
[× 10−10]
45-0-15 2.240±1.076 1.568±0.084 45-0-16 1.723±0.101 1.521±0.018 45-0-17 0.613±0.023 1.240±0.002
45-1-15 2.360±0.049 1.530±0.016 45-11-6 1.730±0.119 1.500±0.017 45-1-17 0.797±0.006 1.109±0.082
45-2-15 2.450±1.027 1.437±0.030 45-2-16 1.837±0.112 1.287±0.081 45-2-17 0.813±0.053 1.192±0.008
50-0-15 3.170±0.001 1.347±0.041 50-0-16 1.840±0.008 1.169±0.009 50-0-17 1.221±0.003 1.151±0.043
50-1-15 3.380±0.001 1.320±0.087 50-1-16 1.873±0.001 0.886±0.004 50-1-17 1.323±0.002 0.633±0.058
50-2-15 3.420±0.000 1.280±0.011 50-2-16 1.874±0.002 0.789±0.005 50-2-17 1.340±0.001 0.614±0.063
55-0-15 3.450±0.000 1.184±0.020 55-0-16 2.032±0.001 0.657±0.004 55-0-17 1.424±0.003 0.502±0.004
55-1-15 3.640±0.001 0.917±0.050 55-1-16 2.040±0.001 0.589±0.017 55-1-17 1.428±0.004 0.486±0.014
55-2-15 3.680±0.003 0.807±0.075 55-2-16 2.059±0.002 0.481±0.006 55-2-17 1.513±0.001 0.456±0.023
Note: WVP, water vapor permeability; OP, Oxygen permeability.
  Results and Discussion 169

oxygen gas influx into the system of the packaged food product. This
may create a macro environment or modified atmosphere for the
ideal storage or packaging of the food product.
Thickness is structurally related with the permeability of the
nanocomposite film [22, 23]. The thickness of the film plays an
important role in its absorption behavioral and characterization.
Thus, the variations in barrier property of the nanocomposite film
with an increase in its thickness are shown in Table 7.2. There is a
clear decrease in the water vapor and the oxygen gas permeability
from 2.240 × 10−10 to 0.613× 10−10 g/m.Pa.s, with the increase in the
thickness of the film. The permeability of the film is slightly higher as
compared with the permeability of low- and high-density polyethene
materials of similar thickness [23]. In a related investigation, Islam
and Buschatz [24] observed an increase in the permeability of
polyamide films with the increase in their thickness. Thus, the
thinner the nanocomposite film, the higher will be the diffusion and
water vapor coefficients, due to the less restriction of particle influx
into the film layers.

7.3.2 Thermal Stability of Nanocomposite Film

A typical thermal degradation curve for different thicknesses of the
cassava starch nanocomposite film, which were obtained for the film
with 45% glycerol and 0% zinc nanoparticles, is shown in Figure 7.3.
Similar trends were observed for the remaining 26 film formulations.
Less than 2% of the weight of the film was degraded between 30 °C
and 85 °C. The residual weights of the film with 45% glycerol and
15−17 µm thickness were 14%, 12%, and 9% at 30 °C.

Figure 7.3 Thermal degradation curves of nanocomposite film.

170 Characterization of Cassava Starch-Zinc Nanocomposite Film for Food Packaging

The residual weights of the films with 45% glycerol and 1% zinc
nanoparticles were 13% for 15 µm, 10% for 16 µm, and 12% for 17
µm. The films containing 45% glycerol and 2% zinc nanoparticles
offered 17%, 16%, and 10% residual weight loss with the increase
in thickness. Also, less than 2% of the weights of the films were
degraded between 30 °C and 70 °C. Furthermore, only 2% of the
weights of the cassava starch nanocomposite films were degraded
between 30 °C and 50 °C, in the case of the films with 50% glycerol
and 1% zinc nanoparticles. In general, since more than 80% of the
films were degraded when subjected to temperature above their glass
transition range, the residual weight represented almost complete
decompositions of the films.
Beyond this temperature range, the cassava starch nanocomposite
film may become unstable and the weight loss of the film may increase
with the increase in temperature. The differences in the values of the
glass transition temperatures of the films and their residual weights
can be partly associated with their varied thicknesses, which affect
the physical states, volumes, and shapes of the samples at higher
temperature. It can also be argued that the increased concentrations
of the glycerol and the zinc nanoparticles are partly responsible the
difference in the glass transition temperature.This behavior agrees
with the low-density polyethylene film and other synthetic polymers,
which show a single mass loss step with significant decomposition
[25]. Therefore, the knowledge of thermal properties of the
nanocomposite film is necessary for understanding its decomposition
pattern for packaging application, especially in a high temperature
environment.

7.3.3 Mechanical Properties of Nanocomposite Film

The mechanical properties of the nanocomposite film may be
necessary for studying the influence of defects such as pinholes that
may affect other properties, such as the resistance to breakage and
abrasion. The effects of nanoparticles and glycerol concentrations
on the mechanical properties of the nanocomposite film are shown
in Table 7.3. The reduced modulus and the strain energy decrease
with the increase in the nanoparticles and glycerol concentrations.
Also, the hardness, drift rate, tensile strength, and deformation
increase with the increase in the concentrations of glycerol and
  Results and Discussion 171

zinc nanoparticles. Although the reason for this is not well known,
from previous research and preliminary investigation [26−30], the
morphology of the film and its displacement when load is applied
are evaluated. This may create a large interface between the film
constituents’, thereby affecting its molecular mobility and relaxation
behavior. This corroborates the findings of Park et al. [31], who
reported that the polymer structure, plasticizer selection and
concentration, molecular weight of the film forming materials, type
of solvents, and film thickness affect the mechanical properties.
Furthermore, the results of the effects of thickness on the
loading and unloading behaviors of cassava starch nanocomposite
films are typically shown in Figure 7.4. The variations of the
applied load on the cassava starch nanocomposite films with the
displacement, observed in the nano-indentation analyses, are also
shown in Figure 7.4. The strain energy absorbed by the cassava
starch nanocomposite film is higher for the 15 µm film than for the
16 µm and 17 µm, thus a magnitude of 190 pNm is released during
the loading part of the hysteresis loop. But, only 5 pNm of the
strain energy is dissipated as heat during the unloading part of the
hysteresis loop, as most of the energy is recovered in the process. It
is possible that the energy dissipated as heat during the unloading
part of the loop by the cassava starch nanocomposite films is
lower than those of the pure thermoplastic films, irrespective of
the concentration of the glycerol [32]. The energy dissipated also
decreases with the thickness of the films.

Table 7.3 Mechanical properties of cassava starch nanocomposite films

Variables Mechanical properties of the films

g np t E H ϕ d σt δ F
45 0 15 1.39 941.1 101.0 11.34 0.400 4040.2 50.00
45 1 15 2.47 765.6 80.80 3.862 0.000 3231.6 50.00
45 2 15 3.19 515.3 74.28 −7.63 0.000 2977.0 49.90
45 0 16 5.39 1.010 55.91 −1.57 0.000 2236.5 50.00
45 1 16 43.7 2.690 24.95 12.64 0.200 998.10 50.00
45 2 16 7.01 701.6 55.02 8.478 0.100 2200.7 50.00
45 0 17 2.76 163.7 103.3 −0.76 0.100 4132.8 50.00
45 1 17 6.34 14.11 155.4 −2.31 0.100 6214.7 50.00
(Continued)

172 Characterization of Cassava Starch-Zinc Nanocomposite Film for Food Packaging

Table 7.3 (Continued)

Variables Mechanical properties of the films
g np t E H ϕ d σt δ F
45 2 17 10.2 1.480 42.01 −3.60 0.100 1680.5 50.00
50 0 15 4.73 433.9 68.75 5.46 0.100 2749.9 50.00
50 1 15 5.09 311.3 33.11 −3.05 0.200 1324.4 50.00
50 2 15 5.62 286.5 75.94 −0.17 0.100 3037.6 50.00
50 0 16 5.52 1.110 54.82 11.72 0.000 2192.8 50.00
50 1 16 92.4 73.50 14.54 −1.54 0.100 581.50 50.00
50 2 16 11.3 1.090 43.49 6.90 0.100 1739.5 50.00
50 0 17 17.2 1.410 36.78 24.3 0.100 1471.2 50.00
50 1 17 12.2 391.3 61.28 −3.84 0.200 2451.0 50.00
50 2 17 13.5 4.040 34.22 25.4 0.100 1368.8 50.00
55 0 15 168 67.86 9.556 −0.28 0.200 383.00 49.90
55 1 15 60.7 5.600 18.67 −1.41 0.200 746.80 50.00
55 2 15 45.2 4.980 20.8180 −10.1 0.100 832.70 50.00
55 0 16 41.3 33.87 22.0480 −0.70 0.100 881.90 50.00
55 1 16 167 67.86 9.55590 −0.28 0.200 383.00 49.90
55 2 16 12.9 7.060 542.909 −7.47 0.1 3620.6 299.9
55 0 17 43.40 35.51 21.5030 −2.56 0.1 860.10 50.00
55 1 17 185.2 11.43 11878 4.88 0.4 475.10 50.00
55 2 17 84.32 9.070 15170 −1.55 0.2 606.80 50.00
Note: = Drift rate (nm/s), = Maximum force (μN), = Maximum depth (nm), = Tensile strength
(μN/mm2), = Hardness (MPa), = Reduced modulus (μN/mm2), = Strain energy (pNm), g =
Glycerol concentration (%, w/w), np = Concentration of nanoparticles (%, w/w), t = Thickness
of the film (μm).

Figure 7.4 Load-displacement profiles of nanocomposite film [29].

  Results and Discussion 173

7.3.4 Structural Stability of Nanocomposite Film

The results of some structural properties, showing the X-ray
diffraction patterns of the cassava starch nanocomposite films
of different thicknesses and concentrations of glycerol and
nanoparticles, are typically shown in Figure 7.5. The peak values
of the structural properties at 15 µm, 16 µm, and 17 µm film
thicknesses, which were deduced from the X-ray diffraction patterns,
are presented in Table 7.4.

a. 200
Intensity(counts)

150
X : 2 3 .6 7
Y : 1 6 3 .9
100

50

0
0 10 20 30 40 50 60 70 80

100
b.
80
Intensity(counts)

X: 21.34
60 Y: 79.2

40

20

0
10 15 20 25 30 35 40 45 50 55 60

150
C. X : 3 4 .2 9
Intensity(counts)

Y : 98

100

50

0
10 15 20 25 30 35 40 45 50 55 60
Diffraction angle(2Th)

Figure 7.5 Profile of nanocomposite film with 2% nanoparticles:

(a) 45% glycerol, (b) 50% glycerol, and (c) 55% glycerol.
174 Characterization of Cassava Starch-Zinc Nanocomposite Film for Food Packaging

Table 7.4 Peak values of cassava starch nanocomposite films

Structural properties of cassava starch

Nanocomposite films
Relative
Variables Position Height FWHM d-spacing intensity
g np t [°2Th] [cts] [°2Th] [Å] [%]
45 0 15 10.12 10.79 0.19 8.74 65.22
45 1 15 5.27 6.71 0.5 16.77 7.7
45 2 15 35.06 12.54 0.76 2.56 65.74
45 0 16 10.12 10.79 0.19 8.74 65.22
45 1 16 10.12 10.79 0.19 8.74 65.22
45 2 16 23.19 34.56 0.25 3.84 48.35
45 0 17 5.27 6.71 0.5 16.8 7.7
45 1 17 34.39 21.02 0.25 2.61 100
45 2 17 23.29 15.96 0.76 3.82 75.92
50 0 15 35.12 11.62 0.19 2.56 100
50 1 15 23.33 27.86 0.5 3.81 67.68
50 2 15 22.87 20.09 0.63 3.89 100
50 0 16 22.87 20.09 0.63 3.89 100
50 1 16 5.27 6.71 0.5 16.8 7.7
50 2 16 24.63 8.3 0.92 3.61 100
50 0 17 34.54 17.44 0.19 2.6 100
50 1 17 23.88 13.64 0.61 3.72 100
50 2 17 17.38 9.05 0.76 5.1 15.34
55 0 15 34.54 17.44 0.19 2.6 100
55 1 15 17.23 10.39 0.76 5.15 27.55
55 2 15 10.48 10.82 0.5 8.44 65.4
55 0 16 19.56 104.3 0.16 4.54 100
55 1 16 35.24 15.62 0.5 2.55 100
55 2 16 18.62 41.17 0.88 4.76 100
55 0 17 34.26 43.48 0.16 2.62 100
55 1 17 32.16 17.64 0.5 2.78 71.76
55 2 17 34.42 7.21 0.38 2.61 68.25
Note: FWHM, full width at half maximum; g, glycerol concentration (%, w/w); np, concentration
of nanoparticles (%, w/w); t, thickness of the film (μm).
  Results and Discussion 175

The X-ray diffraction is a commonly used technique for the evaluation

of crystal structure because it relies on coherent scattering from
many unit cells in a spatially time averaged fashion [33]. The effects
of the intensity of incident radiation on the pure thermoplastic films
of different thicknesses, containing 45% glycerol, are shown in Table
7.4. The diffraction patterns depicted show a defect in the 15 µm
thermoplastic film, which occurs at a diffraction angle of 19.68 °2Th,
unlike the other thermoplastic films that show no observable defect
with diffraction. The effect of the intensity of the incident radiation
on the nanocomposite film, which contains 45% glycerol, 1% zinc
nanoparticle with thickness in the range of 15 to 17 μm, was shown
in Table 7.4. The diffraction patterns depicted show defects in the 15
µm and 16 µm cassava starch nanocomposite films, which occur at
diffraction angles of 19.62 °2Th and 19.68 °2Th, respectively; unlike
the 17 µm film that shows no observable defect with diffraction.
The effects of the intensity of incident radiation on the cassava
starch nanocomposite films of different thicknesses, containing 45%
glycerol and 2% zinc nanoparticles, are also shown in Table 7.4. The
diffraction patterns depicted show defects in the 15 µm and 17 µm
cassava starch nanocomposite films, which occur at diffraction angles
of 23.2 °2Th and 19.44 °2Th, respectively; unlike the 16 µm film that
shows no observable defect with diffraction. It can be seen, from the
foregoing, that thickness is important in determining the crystalline
structures of cassava starch nanocomposite films, in terms of the
diffraction position along the films’ geometry. The observed patterns
for the variations of the intensity with the diffraction angles are
relatively homogeneous. The patterns show relatively sharp peaks,
which indicate that the nanocomposite film may be crystalline in its
structure. This resembles the structure of a face-centered cubic zinc
particle with a lattice constant of approximately 0.4085 nm and is
consistent with the available literature value (0.4086 nm) [2, 27].
The film-forming materials and especially their structural cohesion
have important effects on the structural properties of edible films
and coatings [27]. In addition, an area of almost 100% structural
defect intensity in the molecular structure of the nanocomposite film
is found, as shown in Table 7.4. The intensity of the structure of the
film depends on the material composition, as evident in the different
patterns exhibited by the various film categories and treatments. The
defect is more pronounced in the film with 55% glycerol than the film
176 Characterization of Cassava Starch-Zinc Nanocomposite Film for Food Packaging

with either 50% or 45% glycerol concentration. Also, the values of

the full width at half maximum can help further explain the size of the
observed crystals in the film. An understanding of this phenomenon
may be vital for the food packaging engineer in the designing of
systems for the food packaging application. It may also aid in the
understanding of barrier mechanism of nanocomposite film, which
is yet to be reported.

7.4 Conclusion

The service performance analysis of the cassava starch-based zinc

nanocomposite film is carried out to ascertain its suitability for
packaging application. This is done by characterizing the film based on
its mechanical, thermal, structural, and barrier properties. The results
show that the amount of water vapor absorbed by the film decreases
with the increase in concentrations of the zinc nanoparticles and the
glycerol. The molecular absorption behavior of the nanocomposite
films may be influenced by the nanoparticles used. The water vapor
permeability is low for the film without the nanoparticles and high for
the film with 2% nanoparticles. The residual weights of the films with
45% glycerol and 1% zinc nanoparticles are 13% for 15 µm, 10% for
16 µm, and 12% for 17 µm. The films containing 45% glycerol and
2% zinc nanoparticles offer 17%, 16%, and 10% residual weight loss
with the increase in their thickness. The reduced modulus and the
strain energy decrease with the increase in the nanoparticles and
glycerol concentrations. The hardness, drift rate, tensile strength, and
deformation increase with the rise in concentrations of glycerol and
zinc nanoparticles. The diffraction patterns depicted show a defect
in the 15 µm thermoplastic film, which occurs at a diffraction angle
of 19.68 °2Th, unlike the other thermoplastic films, which show no
observable defect with diffraction. Thus, the nanocomposite film
has a potential for use as an active packaging material in the food
processing.
 References 177

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Chapter 8

Review on Advanced Food Packaging

Materials Based on Functional
Biopolymer Matrix

Md. Aftab Alam, Rizwana Khatoon, Shamsul Huda, and Pramod

Kumar Sharma
Department of Pharmacy, School of Medical and Allied Sciences,
Galgotias University, Greater Noida, Uttar Pradesh, India
[email protected]

The chapter describes the functional food packaging materials based

on biodegradable polymeric moiety, with biological activeness that
can be suitable to use to their synthetic counterparts. Functional­
polymer-based have many characteristics to the subsequent materials
of packaging. In the present scenario of eco-preservation, the
polymeric systems are under great interest such as polysaccharides
(cellulose, starch, pullulan, alginate); proteins (gelatin, casein);
polyesters and polyhydroxy esters; and many more. Such bio­
functional polymeric alternatives to synthetic ones have significant
applications in the packaging industry, as safe materials to make
cleaner as well as greener world.

Biomaterials in Food Packaging

Edited by Mohd Yusuf and Shafat Ahmad Khan
Copyright © 2022 Jenny Stanford Publishing Pte. Ltd.
ISBN 978-981-4877-98-5 (Hardcover), 978-1-003-25678-6 (eBook)
www.jennystanford.com
182 Advanced Food Packaging Materials Based on Functional Biopolymer Matrix

8.1 Introduction

The main functions of food packaging are to protect food products

from deterioration, retaining and extending valuable impacts of
processing, and keeping food quality and security with extended
shelf life [1] and extensive external impacts on the growth of
the global food market, accessibility of raw materials, customer
demands, etc. [2].
Non-renewable, non-biodegradable packaging constituents have
severe environmental disadvantages. Consumers and environmental
activists regarded them as a significant source of strong waste and
environmental pollution [3−5]. To address this issue, businesses and
scientists worked on ways to create fresh packaging approaches
with eco-friendly, plentiful biodegradable packaging products
produced from natural renewable polymers [4, 6].
These polymers have elevated molecular weight, and are non­
metallic compounds [7]. They consist of repeating macromolecules
and, depending on their structure, they have different features. A
range of plastics is used as feedstock sources for contemporary
plastic products (both renewable and non-renewable). However,
plastics have created serious environmental concern [8].
Feedstock for renewable resources includes microbial-grown and
starch-extracted polymers. Such materials can be reinforced by
natural fibers from crops like hemp, flax, jute, and other sources
of cellulose [9].
The perfect biodegradable packaging constituents are
acquired from renewable bio-based resources, commonly
known as biopolymers, with outstanding mechanical and barrier
characteristics and end-of-life options [10−13]. The biopolymers
are a group of natural resource molecules that display distinctive
polymer characteristics. These are molecules consisting of
repeating units (aka monomers) in a specific order of the same or
distinct sort. Their molecular weight relies on the number of units
that are repeated [14, 15]. The ‘bio’ prefix indicates living organisms
as the sources of biopolymer, which is often biodegradable. The
biopolymers are considered as alternatives to petroleum-based
  Introduction 183

plastics because they are biodegradable, renewable, and available

in large quantity [16−19]. Figure 8.1 illustrates the categories and
sources of biopolymers.

Figure 8.1 Illustration of categories and sources of biopolymers.

The natural biopolymers can also be altered or functionalized

mildly tobiopolymers
The natural serve cana also
particular
be altered or purpose. Foodto serve
functionalized mildly hydrocolloids
a particular are
biopolymers with elevated molecular weight. They are usually
purpose. Food hydrocolloids are biopolymers with elevated molecular weight. They are used
in many food formulations as functional food additives. They are also
usually used in many food formulations as functional food additives. They are also used in
used in several applications in the food industry, including thickening,
stabilizing, encapsulating, gelling, and film-forming, the drug sector
depending on their molecular forms and weights [14, 20, 21].
Biopolymers have been used as food, apparel, and furnishings by
humankind since ancient times, based on biomaterials such as silk,
wool, leather, and cellulose. The increasing dependence on synthetic
polymers has raised several environmental and human health
problems. An emerging issue is the advancement of materials from
natural polymers, due to growing environmental concerns [22].
The biopolymers generated from multiple natural resources, like
starch, cellulose, chitosan, and various plant and animal proteins,
have been regarded as appealing options for non-biodegradable
184 Advanced Food Packaging Materials Based on Functional Biopolymer Matrix

plastic packaging products, as they are plentiful, renewable, cheap,

eco-friendly, biodegradable, and biocompatible [23−25]. Thus, they
will play a major part in the bio-economy and certainly shape the
packaging industry’s future [26].

8.2 Origin and Description of Bio-Based Polymers

Renewable resource-based polymers are gaining increasing attention

as environmentally friendly materials. The bio-based polymers,
depending on their sources and construction, can be split into three
primary classifications:
(i) Polymers obtained straight from biomass like polysaccharides
(such as starch, cellulose, and chitosan) and proteins (such as
caseinates, soy, zein, whey, and gluten) [27];
(ii) Synthetic polymers mainly derived from alcohols like polyvinyl
alcohol (PVA), polycaprolactone (PCL), copolymers of ethylene-
vinyl alcohol (EVA), and polylactic acid (PLA) [28−30]; and
(iii)Polymers generated by natural or genetically-modified microbes
like polyhydroxyalkanoates (PHAs) or bacterial cellulose
[31−33].
These bio-based materials are particularly helpful in food-related
applications in three primary fields: food packaging, food coating,
and food and encapsulation edible films.

8.3 Polysaccharides

Polysaccharides are polymeric structures in biological systems,

also known as carbohydrates. These are made up of numerous
monosaccharides, consisting mainly carbon, oxygen, and hydrogen.
There are five or six carbon atoms in the most prevalent kinds of
monosaccharide units [34].
They are used an attractive food packaging platform. Most
polysaccharide biopolymers are used to safeguard food from
pathogenic and spoilage microbes in active packaging. In the
food industry, many polysaccharides are discovered for food
packaging applications because they are non-toxic, biodegradable,
  Polysaccharides 185

environmentally friendly, biocompatible, and eatable particles. These

biopolymers depend on the bonds linking the sugar residues at
different positions [35].

8.3.1 Plant-Based Polysaccharides

8.3.1.1 Starch
Due to its commercial accessibility, intriguing property balance,
and industrial productivity, the starch is the most important
material for food packaging among all biopolymers (Figure 8.2)
[36]. It is the most widely used renewable raw material and a
natural resource that is easily biodegradable. It is acquired from
seeds, corn, wheat, rice, potato, cassava, and sweet potato [37, 38].
Starch is a biocompatible and biodegradable low-priced renewable
source material [39, 40] whose films can be manufactured either
by extrusion [41] or casting [42].

Figure 8.2 Chemical structure of starch.

Starch is composed of a combination of two α-glucose-linear

amylose (containing 200−20,000 glucose units) polymers and
amylopectin (heavily branched polymer with brief side chains of
30 glucose units connected along the chain to every 20–30 glucose
units) [43].
186 Advanced Food Packaging Materials Based on Functional Biopolymer Matrix

It can be used to make films that are eatable or biodegradable.

Dissimilar starch source, high amylose starch, and modified starch
[44−46] are used by casting from aqueous solution to create
self-supporting films. These films seem to have mild oxygen
obstacle characteristic, but bad humidity obstacle and mechanical
characteristics that restrict their broad uses. The chemical
starch alteration was proved more than 60 years ago by adding
butan-1-ol [47].
A fascinating theme regarding starch is the incorporation of
various guest molecules into hydrocarbons to create complicated
constructions for applied purposes [48]. In the food industry, the
distinctive starch structure has many applications, such as water
retention, gelling, thickening, stabilizing, and bulking agent [49].
In the industry, a partly degraded starch with particular enzymes
is used as low-calorie bulking agent [50]. The intake of low-calorie
sugars is a major problem in diabetes management [51].

8.3.1.2 Cellulose
In nature, cellulose is the richest occurring biopolymer and is a major
component of fibrous plants, and certain bacterial species including
the genus Agrobacterium, Gluconacetobacter, Sarcina, etc. (Figure
8.3) [52, 53]. It is biocompatible, low-cost, and intelligent biopolymer
with improved biological and chemical properties [54]. Cellulose
molecules are amphiphilic and have a large density of hydroxyl groups
and consist of a chain of residues of β-(1→4)-linked glucose [55]. The
cellulose is very hard to use in packaging because it has bad mechanical
characteristics in its raw form and is hydrophilic and crystalline.
Therefore, cellophane with excellent mechanical characteristics must
be treated with chemicals, such as NaOH, H2SO4, CS2, etc. [56].

Figure 8.3 Chemical structure of cellulose.

  Polysaccharides 187

There are several commercially available cellulose derivatives.

The most frequently used cellulose derivatives are carboxymethyl
cellulose, methylcellulose, ethylcellulose, hydroxyethylcellulose,
hydroxypropyl cellulose, and cellulose acetate (CA). However, CA
and its derivatives are chiefly used in food packaging applications
(boiled products and new products). The CA has comparatively small
moisture and gas barrier characteristics and its film production must
be plasticized [57, 58].
The cellulose derivatives can be generated through the derivation
of cellulose from the solved state by esterification or hydroxyl group
etherification. The incorporation of hydrophobic compounds is
one way to increase the humidity barrier property of the cellulose
derivatives, e.g. fatty acids into the matrix of cellulose to create a
composite film [59]. If this scenario is to alter, research is needed
to create effective handling techniques for the manufacturing of
cellulose derivatives.

8.3.2 Animal-Based Polysaccharides

8.3.2.1 Chitosan
Chitosan is a chitin de-N-acetylated derivative of amino polysaccharide
(Figure 8.4) [60−64]. Chitosan is, next to cellulose, the second most
abundant natural product, structurally made up of glucosamine and
N-acetylglucosamine units connected via the glucosidic bond β-1-4.
As chitosan is biodegradable, non-toxic, and easily biocompatible, it
has been widely researched for multiple applications in the food and
packaging industries [65, 66].

Figure 8.4 Chemical structure of chitosan.

188 Advanced Food Packaging Materials Based on Functional Biopolymer Matrix

It can also be acquired from the chitin element of fungal cell

walls (Aspergillus fumigates, Histoplasma farciminosum) and the
Saccharomyces cerevisiae fungus [64, 67]. Mucor rouxii forms
(filamentous and yeast-like) contain big amounts of chitosan [60].
Chitin is an outer skeleton structural polysaccharide of crustacean
creatures, such as crabs, shrimps, lobsters, insects, and some fungi
and algae cell walls [68, 69]. Chitosan forms films without adding
additives display good carbon dioxide and oxygen permeability, along
with outstanding mechanical and antimicrobial characteristics that
reduce the oxidation process and increase the food product’s shelf
life and quality [70−72]. Hydrophobic elements (vital oil, beeswax)
can be added to decrease the water vapor permeability of chitosan
films [73−76].

8.3.2.2 Pullulans

Pullulan, comprises a sequence of units of the sort of maltotry,

i.e. α-(1→6)-linked (1→4)-α-D-triglucosides, is a non-ionic
polysaccharide generated from linear, water-soluble, and
exopolysaccharide substrates by the fungus Aureobasidium pullulans
(Figure 8.5). Pullulan is easily soluble in water, but it is very sparingly
soluble in inorganic and non-water-miscible solvents. The pullulan
is currently used for numerous applications in food, medicine, and
cosmetic products [77−80]. It can be used efficiently in edible films
because of its applications [81−83].

Figure 8.5 Chemical structure of pullulan.

  Polysaccharides 189

8.3.2.3 Carrageenan
Carrageenan is found in red seaweed (Kappaphycusalvarezii, formerly
Eucheuma cottonii) [84] and has excellent gas barrier characteristic
(Figure 8.6) [85]. It is a linear anionic sulfate polysaccharide that
consists of alternate residue of d-galactopyranose connected via
α-(1→3) and β-(1→4) glycosidic linkages [86, 87]. Coatings based
on carrageenan have been revealed to extend shelf life of poultry
products [88, 89]. In addition, carrageenan-based products are being
utilized as thickeners
widely stated in the
in the literature. food
More dataindustry. Edible
on applying carrageenan-based
carrageenan as a layer is available
films are not widely stated in the literature. More data on applying
elsewhere [90].
carrageenan as a layer is available elsewhere [90].
OH
OSO3
OH H H
OH O
O H
H
O O
O O H O H
H
O O H H
O O
H OH
H OH H
H H
H H
OSO3

Figure 8.6 Chemical structure

Figure 8.6 Chemical structure of carrageenan.
of carrageenan.

Carrageenan is generally categorized into three industrially

appropriate kinds: λ-carrageenan, which is a heavily sulfated galactan
with a viscosity
Carrageenan enhancing
is generally characteristics;
categorized into ι-carrageenan,
three industrially appropriate which
kinds: λ-carrageenan,
forms smooth gels that are thermo reversible; and κ-carrageenan,
which is a heavily sulfated galactan with a viscosity enhancing characteristics; ι-carrageenan,
which provides water syneresis to make powerful and fragile
which forms smooth gels that are thermo reversible; and κ-carrageenan, which provides water
gels. There is also a hybrid type composed of κ- carrageenan and
ι-carrageenan.
syneresis to make Its existence
powerful in seaweed
and fragile gels. Thererelies
is also on the basis
a hybrid of algal,of κ-
type composed
harvest season, and process of extraction used [91, 92].
carrageenan and ι-carrageenan. Its existence in seaweed relies on the basis of algal, harvest
However, carrageenan biopolymers have a complicated
season, and process of extraction used [91, 92].
hybrid chemical composition consisting of monomers of λ-, ι-, or
However, carrageenan
κ-carrageenan biopolymers
together with have a complicated
monomers hybrid chemical
of non-gelling composition
biological
precursors like monomers
consisting of monomers of λ-, ι-, or of ѵ- or µ-carrageenan
κ-carrageenan [91]. ofDue
together with monomers to
non-gelling
powerful contact, the anionic character of the ι-carrageenan is
biological precursors like monomers of ѵ- or µ-carrageenan [91]. Due to powerful contact,
higher in water [93, 94]. More than 100 carrageen products are
the anionic character
accessible of the ι-carrageenan
today, worldwide, whichis exceeds
higher in the
watermanufacturing
[93, 94]. More than of 100
the agar products
carrageen [95, 96].are accessible today, worldwide, which exceeds the manufacturing of the

agar [95, 96].

8.3.2.4 Xanthan
190 Advanced Food Packaging Materials Based on Functional Biopolymer Matrix

8.3.2.4 Xanthan
Xanthan gum is a polysaccharide bacterium formed by the
bacterium Xanthomonas campestris aerobic fermentation (Figure
8.7) [97, 98]. The structure contains β-d-mannose (1→4) β-d-acetyl
glucose (1-2)-α-d-mannose backbone of β (1→4) C3 substituted
d-glucose.
The fragile gel is prepared in elevated viscosity of low-shear
rate. In essence, xanthan specimens enable process control like
spreading, pumping, pouring, and sparing. Xanthan thixotropy
has resulted in the growth of multiple dry-mix preparations like
desserts, gravies, and sauces, with their thermally stable textual
properties toward cooling and heating. Xanthan is the highest
gluten substitute. Galactomannan mixtures based on xanthan are
used to make thickened or gelled food [99].
CH2OH
CH2OH
O
O
OH O
O

OH
COOH
H3C O
OH
O n
R6
H3C O
O
R4 OH

R6 O COOH O

O
O OH
OH OH O

R4 O
OH

Figure 8.7 Chemical structure of xanthan.

Figure 8.7
It is a colorful, free-flowing white-to-cream powder that is soluble
in warm and cold water, but insoluble in most organic solvents
[100, 101]. Xanthan interacts with other components of food like
whey protein. These interactions result in a synergistic impact on
emulsifying capacity and an increase in emulsion droplet stability
against flocculation and coalescence [102].
  Proteins 191

8.4 Proteins

Proteins are complicated structures consisting of amino acids

connected via peptide bonds and organized in a three-dimensional
structure. It can be derived from crop sources (gluten, wheat, maize,
zein, and soy) and animal sources (whey, casein, keratin, and gelatin).
Because of the distinctive side chain in their structure, they are
extremely desirable to alter the necessary features of packaging
products. Moreover, due to their renewable nature, proteins and
protein-based materials are used in many industrial applications for
biodegradability and their outstanding gas barrier characteristics.
However, they are adversely impacted as starch-based polymers by
their hydrophilic nature. They, therefore, need to be mixed with other
polymers or must be changed chemically or microbiologically [77,
103].
Most protein biopolymers are used as hydrostatic agents, tissue
engineering scaffolds, suture biomaterials, and drug delivery cars in
many applications. Biopolymers based on proteins undergo natural
procedures of degradation [35].

8.4.1 Plant-Based Proteins

8.4.1.1 Soy protein
Since the 19th century, soy protein has been used in a various kind
of products. It occurs as soy flour and is used in adhesives, plastics,
and packaging materials manufacturing. It is a nice solution to the
pro polymers as well [104]. There has also been an extensive study
of soy proteins for their film-forming characteristics and use in the
production of biodegradable materials [105]. Soy proteins are now
accessible commercially from soybean processing plants in three
distinct forms: soy protein concentrate, soy flour, and soy protein
isolate, which include more than 90% protein and are acquired
through isoelectric rainfall of alkali solubilized protein dispersions.
Soy proteins consist of a combination of globular proteins, with the
two primary ones being beta-conglycinin (7S globulin) and glycinin
(11S globulin), representing 37% and 31%, respectively, of the
protein mix [106−108]. Additionally, glycerol and water significantly
192 Advanced Food Packaging Materials Based on Functional Biopolymer Matrix

enhance soy protein polymer’s flexibility, but significantly reduce

tensile strength [109].

8.4.1.2 Zein protein
Zein is a maize protein (Zea mays Linn.). It consists of an elevated
non-polar amino acid content that makes zein more hydrophobic.
This characteristic makes it an outstanding barrier to oxygen,
but has bad mechanical properties [110]. Different kinds of
thermophilic products have been developed [111]. Technically,
films produced from a protein like zein that is soluble in alcohol
have comparatively elevated barrier characteristics as compared
to other proteins. Zein has great characteristics of film-forming
and can be used to make biodegradable films. Zein-film is created
by lipophilic, hydrogen, and restricted disulfide bonds between
zein chains [112]. Table 8.1 depicts some example of biopolymer
matrix-enabled antimicrobial agents.
The formation of maize zein films involves the growth in film
matrix of lipophilic, hydrogen, and restricted disulfide bonds between
zein chains [113]. Corn zein is commercially generated by aqueous
alcohol extraction and dried into a granular powder. However, due
to the weak interaction between protein and glycerol molecules,
glycerol tends to migrate through the film matrix. Glycerol migration
results in the film’s loss of flexibility. It was shown that a combination
of glycerol and polyethylene glycol slowed the rate of migration in
zein films [114, 115].

Table 8.1 Some examples of biopolymer matrix-enabled antimicrobial agents

S. Biopolymeric Antimicrobial Microorganism Reference

no. matrix agent tested
1. Gelatin Olive leaf L. monocytogenes [136]
extract
2. Calcium Acetic acid L. monocytogenes, [137,138]
alginate S. Typhimurium,
and E. coli O157:H7
3. Cellulose Pediocin L. monocytogenes [139]
4. Borley bran Grapefruit seed E. coli O157:H7 and [140]
protein/ extract L. monocytogenes
gelatin
(Continued)
  Proteins 193

Table 8.1 (Continued)

S. Biopolymeric Antimicrobial Microorganism Reference
no. matrix agent tested
5. Whey protein Lactoperoxidase L. monocytogenes [141]
6. Wheat gluten Sorbic acid, P. notatum and L. [142−144]
Nisin monocytogenes
7. Chitosan Acetic acid S. liquefaciens, L. [145, 146]
Sakei, and
Enterobacteriaceae
8. Pullulan [147]
9. Corn zein Nisin L. monocytogenes [148, 149]
and S. enteriditis
10. Starch film Chitosan B. subtilis, E. coli, [150, 151]
and S. aureus
11. Corn zein Lauric acid L. monocytogenes [149]
and S.
enteriditis
12. Carrageenan Grapefruit seed Micrococcus luteus, [152]
extract L. innocua, S.
enteritides, E. coli,
and S. aureus
13. Soy protein EDTA L. plantarum and [153, 154]
Corn zein E. coli

8.4.2 Animal-Based Proteins

8.4.2.1 Keratin
The keratin protein has a significant structure that gives exterior
coverage to hair, wool, feathers, horns, and nails of most mammals,
birds, and reptiles. It is an organic, biodegradable polymer in which
biodegradation occurs due to powerful covalent bonds within its
composition and its continuous crosslinking [116−118].
Naturally, keratin is non-burning, lipophobic, biocompatible, and
biodegradable protein that can be used for chemical processing in
various respects. The keratin protein obtained from chicken feathers
can be used for biotechnological applications in various forms, such
as sponges, films, and fibers, alone or mixed with other natural or
synthetic polymers [119−124]. Keratin does not have excellent
194 Advanced Food Packaging Materials Based on Functional Biopolymer Matrix

mechanical characteristics, so it should be used in combination with

a synthetic polymer that is not biodegradable [125, 126].

8.4.2.2 Whey protein

Whey protein forms elastic films that are used as biodegradable packaging
materials [127−130]. It consists of several individual proteins, the
primary components being α-lactalbumin, β-lactoglobulin, bovine-serum
albumin, and immunoglobin [131, 132].
It contains a combination of enzymes like β-lactoglobulin (18kDa
molecular weight), α-lactalbumin (14kDa molecular weight), bovine
serum albumin, and immunoglobulins. β-lactoglobulin includes
about 57% of complete whey protein and two disulfide groups such
as free sulfhydryl group and lipophilic group. Approximately 20% of
complete whey protein is α-lactalbumin and it includes four disulfide
bonds. In aqueous solutions, whey protein film formation includes
heat denaturation. The denaturation breaks current disulfide bonds
and forms fresh hydrophobic and intermolecular disulfide bonds.
Relative humidity, type, and plasticizer concentration affect the water
vapor permeability of whey protein films [133−155].

8.4.2.3 Collagen

Collagen is the richest biopolymer and is an important element

of bone, cartilage, ligament, skin, and tendon [155]. It consists
of three parallel α-chains combined to create a triple-stranded
super helical structure. A repeated series of Gly-X-Y residues
(where X and Y are often proline and hydroxyproline, respectively)
dominates the amino acid sequence of collagen [156]. It is a flexible
polymer, but it hardly degrades and requires some therapy due to
the complicated and helical-fiber framework. Different techniques
of crosslinking using chemical agents are feasible to enhance
mechanical characteristics, decrease solubility, and improve
thermal stability of collagen-based films [157]. To date, 22 distinct
collagens have been recognized in the human. However, types I–IV
were widely studied collagens. Collagen is the best-selling edible
protein film. The films based on elevated hydrolyzed collagen have
more homogeneous surfaces [158−160].
  Proteins 195

8.4.3 Microbial-Based Proteins

8.4.3.1 PHA
Under unbalanced growth circumstances, PHA is a family of bacterial
polyesters with biodegradable and biocompatible nature. The
bacterial fermentation of sugar and lipids produces these polymers
in nature. The PHAs consist structurally of easy macromolecules
consisting of monomers of 3-hydroxy fatty acids. The thermo-
mechanical characteristics of PHAs are comparable to synthetic
polymers like polypropylene [161]. These polymers offer great
packaging films, either alone or in conjunction with starch or
synthetic plastic [162].
Hydroxybutyrate (PHB) and poly(hydroxy valerate) (PHV) are
the most prevalent forms of PHA. The PHAs with thermoplastic
characteristics and medium-chain length (PHAmcl) with
elastomeric characteristics are categorized as brief chain length
(PHAscl) [163]. The thermo-mechanical characteristics of PHAs
are comparable to synthetic polymers like polypropylene [164,
165]. Many microorganisms produce PHB, but Ralstoniaeutropha is
the most commonly researched bacterium because of its capacity
to produce large amount of PHB [166]. Other PHB-accumulating
microorganisms are Haloferax mediterranei, Halomonas boliviensis,
Bacillus megaterium, and others [167−169]. PHB-based polymers or
composites are currently used in the agriculture, medicine, and food
packaging industries [170].

8.4.3.2 Bacterial cellulose (BC)

Bacterial cellulose (BC) is a naturally occurring biomaterial of C-
and N-rich medium generated by certain bacterial species such as
exopolysaccharides including Komagataeibacter genus (formerly
Gluconacetobacter) [171]. So far, BC is unexploited extensively, but
it possesses great potential. Its chemical and physical composition is
the same as plant-forming cellulose. However, to remove lignin and
hemicellulose, plant cellulose must undergo severe chemical therapy.
The BC was generated by fermenting waste from the fermentation of
beer culture. Static cultivation on the grounds of manufacturing was
discovered to be superior to shaking cultivation [172]. In addition, it
can be used for multiple applications, including gelling, thickening,
196 Advanced Food Packaging Materials Based on Functional Biopolymer Matrix

and binding to water. It has been used to boost tofu gel power, to
avoid precipitation of cocoa in a chocolate drink and to maintain the
viscosity of the drink after heat treatment [173]. It is an outstanding
food packaging option, but sadly it does not have any antibacterial
and antioxidant characteristics to avoid contamination of the food
[170−172]. Its composites are therefore used to acquire these
characteristics [174].

8.5 Edible Films and Coatings

The thin layers of edible films and coatings usually <0.3 mm in

thickness are used to coat food products for increasing their shelf life
and these can be safely consumed along with the edible portion [6,
175, 176]. These also follow the general legislations and regulations
on food [106]. Unlike synthetic polymers, this form of the material
originates from natural sources and is biodegradable as well as
consumable safely [177−180]. The benefits of biopolymer-based
films to their synthetic ones are [181−186]:
manufactured from renewable resources;
• consumed in conjunction with the edible packed materials
and prevent solid waste;
• even if they do not consume with the packed products, create
no pollution/hazard due to biodegradable in nature;
• encourage the sensory features of packaged products by
incorporating multiple substances, like colors, flavors, and
sweetness;
• useable for individual packaging of tiny parts of food,
especially berries, beans, peas, and nuts;
• may complementing the product’s dietary significance;
• can provide active finishing to the food (antimicrobial and
antioxidant);
• useable in combination with inedible as part of multi-layer
packaging materials, where the edible film is in direct contact;
• can be used for heterogeneous food products to avoid
moisture and other components from migrating between
them, i.e. pies, sweets, and pizza; and
  Properties of Edible Films 197

• can be used successfully for substance microencapsulation

(mainly aroma) to effectively and accurately administer the
same dosage in the food.

8.6 Properties of Edible Films

8.6.1 Antimicrobial Activity
Packaging products with antimicrobial function have been
acknowledged as one of the most emerging active packaging
technologies, helping to enhance food security and shelf life by
destroying or inhibiting food-contaminating spoilage and pathogenic
microorganisms [187, 188]. In recent trend, nanomaterials are
smart alternates with high surface-to-volume ratio and enhanced
antimicrobial features, which are being the main reasons for
their effectiveness [189]. The addition of antimicrobial as well as
antioxidant agents to edible films is recognized very useful because
it provides the chance to release agents gradually and maintain a
critical concentration for an extended period [190−194].

8.6.2 Antioxidant Activity
The use of antioxidants in packaged food products is another
promising area to improve the oxidative stability of food toward
residual O2. The presence of residual O2 may results in texture change,
discoloration, microbial growth, formation of aldehydes, and dietary
losses with severe toxicity [195, 196], which are the main causes of
decreasing shelf life of meat, poultry, fish, and seafood products [197].
To solve this problem, the use of reactive-free radicals (hydroxyl,
peroxide, superoxide, alkoxy, etc.), non-radicals (hypochlorous, H2O2),
and various kinds of antioxidants have been employed [198, 199].
In the development of active packaging, both natural and
synthetic antioxidants are used that offer promising results. The
most frequently used synthetic antioxidant to form packaging films
is butylatedhydroxytoluene (BHT; E-321). Huang and Weng (1998),
when it integrated into polyethylene films, noted the efficacy of BHT
in stopping the oxidation of fish muscle and oil [200].
198 Advanced Food Packaging Materials Based on Functional Biopolymer Matrix

8.7 Alginate-Based Edible Films

Naturally occurring alginates are indigestible polysaccharides

produced either from algae or bacterial species [201, 202]. Alginates-
based films are currently being found appropriate in formation
of films due to their eco-safe, biodegradability, and non-toxicity
characteristics [201−204]. Edible films made from alginates have
excellent mechanical characteristics, but due to their hydrophilic
nature, they have bad water resistance [178].
Sodium alginate form water-soluble glossy gel, tasteless, and
odorless films with low permeability for oxygen and moisture
[205]. Amongst other alginate types, it is now commonly used as a
stabilizing, emulsifying, swelling, thickening, and chelating agent
[206, 207] and scavenger for various ions like Hg(II) [208], Cr(VI)
[209], Pb(II), Cu(II), Cd(II) [210]. Stem cell differentiation [211]
is efficient in alginate hydrogels in flame retardation, and barium
alginate films have shown promise results in this [212].

8.8 Protein-Based Edible Films

In general, proteins constitute structural components of various body

tissues composed of several amino acids joined by peptide bonding.
Protein-based biopolymers are used in several sectors, including
drug delivery and tissue engineering. Biopolymers based on proteins
undergo natural procedures of degradation [35].
Protein-directed films have been obtained from either animal-
sourced proteins, including egg white protein, keratin, collagen,
casein, gelatine, and fish myofibrillar protein, or from plant sourced-
proteins such as wheat gluten, soy, zein, and other proteins [213].
Because of the powerful cohesive energy density of the polymer,
protein films are fragile [211]. Addition of compatible plasticizers
enhances the films’ extensibility and viscoelasticity [214]. In recent
decades, protein-based edible films have gained interests, due to
their excellent use as safe edible packaging materials, over synthetic
films. Due to its outstanding biodegradable and biocompatible
nature, pectin is regarded as a wonder biopolymer of natural origin
[211], which is manufactured at commercial scale from citrus
  Fossil-Based Biopolymeric Blends 199

peels [215]. Additionally, wheat gluten, stored in wheat and maize,

is another permissible protein with brilliant effectiveness, and
it is a natural origin edible film and coating material [216]. After
successful assessment, wheat gluten is recognized as “green plastic
for future”, although more challenging applications are required in its
strengthening because wheat gluten-based films are fragile without
using plasticizers [217].
Gluten films have excellent barrier characteristics for oxygen and
carbon dioxide, but they have comparatively elevated WVP. Wheat
gluten is also used to maintain fruit and vegetable quality [217].
Consequently, Lee et al. (2005) investigated the impact of gamma-
irradiation on gluten film’s physicochemical properties [218]. The
absence of fundamental knowledge of the tertiary and quaternary
structures of gluten is one of the main challenges connected with
gluten processing to create packaging products [219].

8.9 Fossil-Based Biopolymeric Blends

The objective of mixing two or more bioactive polymers is to obtain a

mixture of each polymer’s favorable characteristics within the blend
[215]. The benefits of polymer blends are that these can be combined
into fresh compositions, thus obtaining products having specific
characteristics. This approach triggers the research and development
of new materials [220].

8.10 Future Perspective

Benefit of the biopolymers/bioplastics is that the disposal of used

products has a decreased environmental impact. The bioplastics are
generally biodegradable and thus enable the materials to be cycled.
These are the least environmentally toxic polymers among all the
plastics, and can decrease reliance on plastics based on petroleum.
The depletion of fossil fuels and increasing petroleum costs are the
major problems for the plastics industry’s long-term sustainability.
On the other hand, agricultural products must be regarded as
alternatives for the production of bioplastics, with the dwindling
supply of petroleum products.
200 Advanced Food Packaging Materials Based on Functional Biopolymer Matrix

Research involves the development of bacteria strains that

require distinct plant sources, as well as the genetic engineering of
a food crop with the capacity to create plastics or a biointermediate
from the plant’s stem for bioplastic manufacturing. Recently, studies
have been extended on film-forming and coating food products with
edible biopolymers. It is possible to use edible or biodegradable
films and coatings to maintain the quality during the product’s
shelf life. Furthermore, due to human responsibility toward the
production, research, and use of biodegradable polymers, their
demand is increasing. This is the primary driving force implementing
biopolymers that shows their enormous potential in the future.
Issues other than the effect on the environment and reliance on
fossil fuel influence the feasibility of replacing standard plastics with
bioplastics. The development of the bioplastics is presently limited
by factors such as economical and mechanical characteristics. There
are a few types of bioplastics being commercially produced, which
means that the production of bioplastics can be economical, but to
what extent it is unknown. The bioplastics are in their technological
infancy, while standard plastics have reached a degree of maturity,
since they were produced in the 1920s [221].

8.11 Conclusion

The growing awareness of the environment has resulted in rising

demand for biodegradable packaging, composed of raw materials
obtained from agricultural feedstock, marine sources, or agro­
food sector by-products. Biopolymers have a wide variety and
their applications in food packaging are therefore varied, as these
have less environmental impacts. Because biodegradable films are
produced from renewable feedstock and agricultural waste, these are
economical and widely used in packaging applications. Edible films
can be used for packaging products that require solubilization or
rehydration before use in the food industry and other related sectors.
The descriptions of the biopolymers; applications of the most
frequently researched natural polysaccharides such as starch,
cellulose, chitosan; and proteins such as collagen, keratin, and whey
protein, are given in this chapter. Recent developments in biopolymeric
products with antioxidant and antimicrobial characteristics, and
 References 201

extensive discussion of alginate-based, protein-based edible films

and coatings, are also included in the text.

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Chapter 9

Prospects of Nanomaterials in Active

Finishing of Food and Food Packaging:
A Review

Divya Bajpai Tripathy,a Anjali Gupta,b and Pooja Agarwalb

a Department of Forensic Science,

Galgotias University, Greater Noida, Uttar Pradesh, India

b Department of Chemistry, Galgotias University,

Greater Noida, Uttar Pradesh, India

[email protected]

Continuous advancements in the area of nanotechnology enable

the use of nanomaterials in vast range of sectors from electronizcs
to environment science, and from detergents to agriculture.
In almost each and every sector, research and development is
exploiting nanomaterials for different applications. Along with
the development of the smart and active packaging for agri-food,
nanomaterials have been used as nanosensors, nanofertilizers, and
nanopesticides. Various novel nanomaterials have proved promising
excellence and safety of food, crop growth, as well as in monitoring
environmental settings. A vast variety of nanomaterials, from
inorganic to nanoorganic materials, and from metal to metal oxides,
have been exploited in the food sector. In the present review, the
usage of nanomaterials in active finishing of food and food packaging

Biomaterials in Food Packaging

Edited by Mohd Yusuf and Shafat Ahmad Khan
Copyright © 2022 Jenny Stanford Publishing Pte. Ltd.
ISBN 978-981-4877-98-5 (Hardcover), 978-1-003-25678-6 (eBook)
www.jennystanford.com
220 Prospects of Nanomaterials in Active Finishing of Food and Food Packaging

are discussed that also involve the toxicological rudiments and

risk calculation of nanomaterials in food and food materials. More
emphasis has been taken to underline the sustainable development
of biologically-synthesized nanomaterials for their prospective
applications.

9.1 Introduction

Approximately all of the foodstuffs that are eaten and all types of
drinks that are consumed are packaged in some way. Maximum
of the food packaging materials formed by using non-degradable
synthetic polymers signify not only a serious global environmental
problem, but also have adverse effects on nutritional values of
food products. In addition, the dependence on fossil resources also
bounds the sustainability of food packaging and production. In the
packaging of food materials, the main purpose is the protection of
the products without disturbing their nutritional values and their
own shelf life as well as environmental concerns. The commerce of
the food packaging industry has to follow some protocol in order to
accomplish this target. The industry is continuously in quest of new
technologies for further improvement in critical parameters, such as
quality, safety, shelf life, and traceability of food material [1].
Recently, the introduction of nanotechnology has generated
more prospects for the improvement and exploitation of new
materials, such as nanomaterials, on food packaging. It is less
than two decades since nanomaterials have been found to have
applications in food packaging. The innovative technology for food
packaging claimed to have various value-added characteristics like
antimicrobial activity and active packaging [2]. Nanomaterials are
the particles that have size of less than 100 nm. These materials
are known to have various properties that make them suitable to
be exploited in varied food science applications. As the analysis
of nanomaterials in food matrices is on its initial stages, there is
still an increasing demand to emphasize on the modern analytical
  Food Packaging Applications of Nanomaterials 221

techniques that make nanomaterials to be exploited more

conveniently in this field [3]. Although, nanomaterials possess a
number of advantages over conventional food-packaging system,
there is a great disagreement about their production cost, and safety
and fitness of these materials when in contact with foodstuffs [4].
In the current review, properties, limitations, and current status of
different aspects of nanomaterials exploitation in food packaging
have been discussed.

9.2  FoodPackagingApplicationsof
Nanomaterials

Due to their nanosize and versatility, nanomaterials have widely been

exploited in food packaging applications (Figure 9.1) which can be
summarized as below:

Protective
finishing of
food
Enhancement
Bio-based food
of barrier
packaging
properties

Humidity
Active packaging
indicators
NANOMATERIALS IN
FOOD PACKAGING

Detection of
Intelligent or
spoilage and
smart
pathogenic
packaging
microorganisms

Antioxidant
Surface biocides
properties

Figure9.1 Applications of nanomaterials in food packaging.

222 Prospects of Nanomaterials in Active Finishing of Food and Food Packaging

9.2.1 ProtectiveFinishingofFood
Handling of food packs should be easy, and should appropriate to be
used in the food dispensing. Moreover, they also have many other
characteristics that are associated to the physical attributes of the
packaging stuff [5].
The exploitation of rods and nanofibers (nanosized in two
dimensions) can converse advantageous physical characteristics
to the food packaging. Specifically, the fibers with the size of >300
nm length to width are useful. Therefore, nanomaterials like carbon
nanotubes (CNTs) and cellulose nanowhiskers (CNWs) are integrating
innovative materials suitable for packaging purposes [4–6].

9.2.2 EnhancementofBarrierProperties
Food packaging must have properties to preserve freshness of food
materials and to shield the food against putrefaction through light
as well as oxidation of the products that leads to spoilage. Demands
of today are the light-weighting of stuffs and their added shelf life
in order to increase suitability and lower the food waste. In this
direction, the uses of nano-based coatings are becoming boon, as
they can provide enhanced barrier operation [7].
Nowadays, vacuum-deposited aluminum coatings applied on the
plastic films are one of the commonly used barrier materials used for
the packaging confectionery, snacks, fast food, and coffee. Thickness
of this aluminum coating that is permissible cannot be more than
50 nm, as only this limit of thickness makes it formally qualified as a
nanomaterial (as one dimension is on the nanoscale). In the similar
way, treatments of the glass made surfaces of containers that have
been used to contain food and beverages, such as jars and bottles,
using organosilanes through plasma or some other high-temperature
technologies, are reasonably appropriate for the purpose [8, 9].

9.2.3 Active Packaging

Conventional packaging is projected to be mostly “inactive” that
offers a protective approach for foodstuffs as a barrier to and from
  Food Packaging Applications of Nanomaterials 223

the outside environment. In contrast, active packaging concept

can be understood as the packaging system that provides spoilage
protection without alteration in composition of the food items. Nano­
enabled materials are being used for substitutes to conventional ones
and thus are very promising. Illustrations comprise nanomaterials
exploited for rummaging purposes to remove oxygen or taint
and/or odor generating chemicals from within the pack. Instead,
nanoencapsulation can be applied for releasing the additives for
preservatives or to provide instance colors onto the surfaces of food
materials, where the additives are required. This could decrease the
required quantity of chemical additives [10].

9.2.4 IntelligentorSmartPackaging
Smart or intelligent systems of food packaging enhance the
communication properties of the packaged items. These systems
exploit numerous advanced communication systems like oxygen
sensors, nanosensors, freshness indicators, time−temperature
indicators, etc. [10−12]. The insertion of nanosensors into food
packaging systems supports the detection of the spoilage-associated
changes, chemical contaminants, and pathogens, and hence provides
the exact scenario of freshness of the foodstuffs [13]. Nanosensors can
be defined as the nanotechnology empowered sensors categorized
with a range of variations. In general, nanosensors can be applied as
labels as well as coatings in order to enhance an intelligent function
to the food packaging to ensure the integrity of the package by the
leaks detection (specifically for the food items that are packed in an
inert atmosphere or in vacuum), indications of temperature−time
variations (i.e., freeze–thaw–refreeze), as well as microbial safety (in
order to protect the deterioration of foodstuffs by microbes) [14−16].
Working of optical-O2 sensors is based on the principle associated
with electromagnetic radiation, such as the law of absorbance changes
or luminescence quenching, which arises due to the straight contact
with the analytes; whereas, opto-chemical sensors are exploited for
checking the excellence of the products using sensing gas analytes
like CO2, H2S, and volatile amines. The exclusive studies have been
known for electro-optical and chemical characteristics of nanosized
224 Prospects of Nanomaterials in Active Finishing of Food and Food Packaging

particles [12, 14−18]. The examples of such changes are humidity

or temperature in storage rooms, stages of oxygen exposure, and
product dilapidation or microbial contagion. Furthermore, smart
packaging technology is curiously benefited for common customers,
food supervisors, and industry investors, evenly [17−20].

9.2.5 SurfaceBiocides
The term “surface biocides” is quite different from active packaging.
In surface biocides, the chemicals that have requisite biocidal agents
have been exploited in order to maintain the standard hygienic
condition for the food contact surface of packaging material by
preventing and/or reducing the growth of microbial colonies to
maintain ‘cleanability’. In this process, the main concern that has to
be taken, in addition, is that there should not be any preservative
impact of such material on the foodstuff [21].
These equipped materials may also have a character to show
in recyclable food containers like boxes and crates as well as inside
liners of freezers and refrigerators. Their one time use applicability
as throwaway packaging is under question. Compounds including
nano Ag and ZnO/MgO showed effectiveness, to be a surface biocide,
in the food contacted silicones, rubber, plastics, and others [22].

9.2.6 AntioxidantProperties
Some nanomaterials of metal/metal oxides have found less reactive
to behave as antioxidant carriers alone [23−25]. Introduction of
nanoparticle-polymer composites are recommended to be appropriate
for the encapsulation of the bioactive compounds (i.e. vitamins) as
well as to discharge them in acidic atmosphere [26]. In the same way,
SiO2-gallic acid-based nanoparticles as novel nanoantioxidants have
been established and verified on the basis of scavenging capability
of 2,2-diphenyl-1-picrylhydrazyl radicals [27]. In addition to that,
employability of antioxidant medications in association with the
comestible coating is the most common technique in order to control
oxidation and colouration of fresh-cut fruits [28]. The coloration of
fresh-cut fruits is an uninvited effect fetched by the transformation
of phenolic compounds into the dark-tinted organics during the
  Food Packaging Applications of Nanomaterials 225

storage and marketing. This transformation is due to the presence of

oxidative environment [29]. Though, there are only a few applications
of nanomaterials are known in which they can directly employed
as anti-browning agents. Active packaging based on nanosized-
ZnO coatings has been described to be a feasible substitute for the
betterment of the shelf-life properties of “Fuji” apples as a fresh-cut
product [30]. In this study, researchers reported that the activities
of pyrogallol peroxidase and polyphenol oxidase were significantly
low in fruits stored in nano-ZnO packaging. Furthermore, the initial
texture of freshly-cut Fuji apples was reserved, and the browning
index was prohibited in fresh-cut fruits stored in nano-ZnO packaging
with the browning index value of 23.9, which was found much lower
when compared to the control group with refractive index value of
31.7 on day 12. Zambrano and his coworkers [31] also described that
action of freshly-cut red colored delicious apples with nanocapsules
containing DL-tocopherol with poly-ε-caprolactone biopolymer
membrane expressively lowered the browning index.

9.2.7 DetectionofSpoilageandPathogenic
Microorganisms
In the USA, according to a report by the Centers for Disease Control
and Prevention (CDC), nearly 48,000,000 cases of food-borne
infections are reported yearly. It is assessed that little decrease of
1% in occurrence of food-borne infections would help save lives of
about 5 lacks individuals [32]. Generally, food-borne sicknesses are
occurred due to common microbes like fungi, bacteria, and viruses,
and are still a big concern for public health [33, 34]. Currently used
detection methods mostly investigate an immunological assay that
mainly depends on the selective interaction between the antibodies
and the antigens. Antibodies conjugated nanomaterials like quantum
dots (QDs) are specifically exploited in order to detect bacteria. The
QDs are used specifically owing to their high-distinctive sensitivity,
high-fluorescence efficiency, prolonged decay life-time, stability
for photobleaching, electronic behavior like continuum, and wide-
absorption spectrum and narrow-emission spectrum [34−36].
226 Prospects of Nanomaterials in Active Finishing of Food and Food Packaging

QDs and organic fluorescent compounds (OFCs) are further

categorized into two categories. The first category involves down-
conversion phosphors (DCPs) and second category contains up-
conversion fluorescent nanoparticles (UCNPs). The DCPs are
known to have ability to absorb energy at lower wavelength;
whereas they emit radiation at higher wavelength. On the contrary,
the excitation of UCNPs takes place as a result of absorption
of low-energy radiations in the range near infrared spectrum,
and gives emission spectrum at higher energy radiations in the
range of visible spectrum. These significant features help them
to overcome photodamage and auto-fluorescence-related issues.
In addition, UCNPs and QDs have found various applications in
labeling, imaging, and medicine. They are the potential candidates
to get exploited in the food packaging, predominantly for expected
progression in intelligent label for the pathogens and the detection
of toxins present in the food matrix [37].

9.2.8 HumidityIndicators
Quality of package and safety and quality of food items in package
are indicated by monitoring the humidity inside the package. Zhou
[38] developed humidity indicator using iridescent technology. The
dry iridescent film emits blue-green color, but when the same film
gets exposed to the environment of high humidity, it turns into red-
orange colored film.
Tian et al. [39] revealed another type of humidity color indicator.
These photonic crystal hydrogels have been designed by combining the
photo-polymerized acrylamide with photonic mono-dispersed latex
spheres made up of poly (styrene-methyl methacrylate-acrylic acid).
Hong and his co-workers [40] revealed that these photonic crystals
exhibit confrontation toward degradation and photobleaching that
enable them to be one of the best known constituents for photonic
crystals. Indicator based on photonic crystals is transparent at 20%
humidity and changes color first to violet then blue, then cyan, and
then green, and finally changes to red, as relative humidity increases
to 100%. Using a similar approach, Zulian et al. [41] developed an
emulsion radical method and described core-shell latex particles
  Nanotechnology: Environmental and Human Safety Prospects 227

along with the varied degrees of order, resulting in a range of

structural colors and different humidity levels.

9.2.9 Bio-BasedFoodPackaging

Barrier properties of packaging materials are important in maintaining

the quality of food and its shelf life without additional chemical
preservatives. Improved barrier behavior of packaging materials
thus can help reduce food wastage, and offer more reliable food
supply and better nutritive value of the food. Bio-based materials are
generally found to be inferior as packaging materials, as compared to
artificial polymers made up from oil or gas. Nanotechnology can help
understand properties of bio-based materials. The characteristics of
the bio-based materials can be upgraded by integrating nanomaterials
or by exploiting nanotechnology to improve production methods.
This can help in substituting synthetic polymers with locally obtained
bio-based materials for the purpose of packaging.

9.3  Nanotechnology:EnvironmentalandHuman
SafetyProspects

There are potential risks of nanoparticles from packaging being

absorbed by the food and thus impact its quality. Also, there are
concerns on the environmental impact on how the used package is
disposed of and how the presence of nanoparticle impacts recycling
processes [42]. Impact of consumption of nanoparticles in the human
body at organ level and as well as cellular and subcellular levels is
uncertain, as different studies have reported conflicting results
[43−49]. This challenge is faced not only by the packaging industry,
but by other industries, and thus needs further research to establish
safety of nanoparticles in human body [46, 50].

9.4  Conclusion

There are challenges in terms of lack of availability of techniques to

analytically measure the movement of nanoparticles from packaging
to food materials. There are risks of unwanted chemical reactions
228 Prospects of Nanomaterials in Active Finishing of Food and Food Packaging

during processing and fabrication of nanoparticles, owing to the high

surface area and high active chemistry of the nanoparticles. Research
needs to focus on the above challenges of adverse responses if any,
and characterization of nanoparticles toward human consumption
approaches and waste disposal, and thus to develop health-related
references for safety of these particles in human body. Though it can
be concluded that since nanoparticles are fixed and embedded in the
packaging, these are not likely to migrate and thus cause threat to
the humans.

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Chapter 10

Applications of Nano-Biocomposite
Materials as Antimicrobial and
Antioxidant Finishing Agents for
Packaged Food Products
Md. Aftab Alam,a Rizwana Khatoon,b Shamsul Huda,b Niyaz
Ahmad,c and Pramod Kumar Sharmaa
a Department of Pharmacy, School of Medical and Allied Science,

Galgotias University, Greater Noida, Uttar Pradesh 203201, India

b Department of Pharmacy, School of Medical and Allied Science,

Galgotias University, Greater Noida, Uttar Pradesh 203201, India

c Niyaz Ahmad, Department of Pharmacy, Division of Pharmaceutics,

College of Pharmacy, Dammam, Kingdom of Saudi Arabia

[email protected]

Today, nanotechnology is gaining great attention because of its

wide applicability in various sectors, including food packaging.
Nanomaterials possess antimicrobial as well as high gas barrier
properties with excellent physical and chemical characteristics,
and therefore, most market companies have increased investment
to develop food packaging alternatives. Innovative packaging
systems also facilitate communications at consumer level in the
forms of certain transit preservation and effective distribution. The
technological advances in food packaging are managed mainly by
nanotechnology. It manipulates and produces products of industrial
and scientific interest, on a nanometer scale. Specific nano-based
materials having active functional abilities increase shelf life of food
and its quality and safety. The food packaging industry has embraced

Biomaterials in Food Packaging

Edited by Mohd Yusuf and Shafat Ahmad Khan
Copyright © 2022 Jenny Stanford Publishing Pte. Ltd.
ISBN 978-981-4877-98-5 (Hardcover), 978-1-003-25678-6 (eBook)
www.jennystanford.com
234 Applications of Nano-Biocomposite Materials

the “nano” era to satisfy the growing need for safe and cost-effective
goods for customers. The review highlights the use of nanotechnology
in the processing and packaging of foods, with a concentrate on food
quality and safety.

10.1  IntroductiontoNanotechnologyinFood
PackagingSystems

Nanotechnology means guidance and usage of nano constituents of

size between 1 nm and 100 nm, with 1 nm being 1×10−9 m [1]. In
these nanosizes, the components have unique properties that were
not available until they were in their initial size. Nanoscientists
across the globe aim to understand these unique characteristics to
build new and advanced materials by green processes [2]. Three
options are mainly examined by nanotechnological strategies on food
packaging. Marketing, successful implementation, and responses
to various nanotechnological applications are based on consumer
views and the acceptability of newly launched technologies and their
submissions [3]. With various uses, nanotechnology has penetrated
into the agri-food industry. This is primarily used for production of
agri-food products; decreasing the use of consume supplements;
reducing the use of agrochemicals; manufacturing of novel food
items with enhanced flavors, texture, colors, and sensory properties;
nourishment with lowered fat or sugar content; and supplying of
supplements (i.e. minerals, vitamins, phenolics, etc.) [4].
Numerous unknown related danger features characterize the
latest scientific enforcement in nanotechnology for food applications.
The versatility of nanotechnology in foodstuffs defines its application
range. Based on their features, food nanotechnology can have an
impact on the bioavailability and nutritional benefits of the food.
It is understood that nanomaterials have highly dependent on
biological characterizations (including toxicological impacts), for
their physicochemical parameters [5]. The food industry is always
looking for new and inexpensive approaches for food production
and conservation. Recent developments in food wrapping relate to
nano reinforcement, nanocomposite active packaging, and smart
nanocomposite packaging [6].
  Introduction to Nanotechnology in Food Packaging Systems 235

Polymers are the replacement in food packaging for traditional

substances, such as card board, paper glass, metal films, ceramics,
etc. Nanocomposites in polymers typically have much stronger
interactions with polymer/filler than regular composites. With the
assistance of nano-reinforcement strategies, the gaps in packaging
substances are packed, which make them more sustainable with
improved tensile strength. Food wrapping gets great tensile strength
with the system of nano strengthening like nanoclay, cellulose, and
other food packaging materials. Improved feasibility and tensile
strength are the nano strengthening methods for the final products
[7]. Nanotechnology is capable of significantly improving food quality
and safety. Nanosensors targeting advanced pathogen identification
in food systems that are presently undertaken with considerable
efforts. Several e-companies have been using researched polymers
that are performing electrically. The same components can also
be used to develop sensors capable of detecting extremely low
concentrations of spoilage and food-borne microbes within seconds/
minutes. This system may identify components per trillion and
charges some 50 cents of output, according to scientists involved in
the project [8].
To enhance gas transfer into plastic film to remove harmful
carbon dioxide, which can reduce the overall life of the product,
nanotechnology is being used to build small molecules in the film
and offer barrier protection and prevent the deterioration of food by
gases such as oxygen and ethylene [9, 10]. Several food and pharmacy
investigators are now focusing on advanced nanotechnology to
enhance the supply of pharmaceutical drugs, vitamins, or delicate
micronutrients in daily foods by generating small, deliverable
capsule-based nanoparticles to specific places in the body, on order.
The health benefits will, therefore, be substantial for lowering the
risks of human diseases like stroke, heart attack, neurodegenerative
disorders, and even cancer [11, 12]. Instances of nanotechnology
used in the food industry are as follows [13]:
• Enhanced safety in the development, processing, and shipping
of food items with pathogens and contaminant identification
through sensors.
• Technologies to keep historical environmental data and to
track specific transactions in a specific product.
• Systems for monitoring food items (smart/intelligent
systems), localization, and remote controlling for improving
the efficiency and safety of food manufacturing.
236 Applications of Nano-Biocomposite Materials

• Encapsulation and distribution networks that transport,

safeguard, and supply food products to their specific sites.
Nanostructured foods cover a broad range of materials, from food
processing to food packaging. Nanostructures may be utilized in food
packaging applications and in particular as antimicrobial agents, anti-
caking agents, and fillers to boost mechanical strength and packaging
material’s durability [14].

10.2  PackagingTechnologiesBasedon
Nanotechnology

10.2.1 NanotechnologicalSystemsforActivePackaging
Effective compounds amalgamation, i.e. anti-microbial products,
preservatives, oxygen and water vapor absorbers, and solvent
extractors, makes nanomaterials more powerful in improving food
products’ shelf life and consistency [6, 15, 16]. Nanoparticles with a
very large surface region are very likely to trap or release chemicals.
They have large outcomes, for example, nano encapsulates may
be employed to expel ingredients on the surface of food; whereas,
ingredients such as colors and preservatives are required. A new
strategy for reducing microbial food contamination on surfaces is
the application of active substances in food packaging products.
There are certain nanomaterials, such as silver, gold, and zinc, have
antimicrobial property [17]. Thus, there are various industrial uses
of silver nanoparticles, due to their lower volatility and higher
temperature stability, and silver is a strong antimicrobial and anti-
fungal agent at a nanoscale.
In comparison with other antimicrobial agents, silver has many
benefits. Silver is poisonous to a wide range of fungal, bacterial, algae,
and some virus types. Certain antimicrobials, on the other hand, are
generally organism-specific (to different degrees). For an extended
time, silver is shelf constant. The effect of biofilm penetration,
which many molecular antimicrobials fail to attain, is also relatively
effective [18]. Nanomaterials are used to directly connect with the
food or the environment to ensure higher safety in active packaging
advancement. For instance, silver nanoparticles and silver coatings
having anti-microbial features are used in other components as oxygen
  Packaging Technologies Based on Nanotechnology 237

or ultraviolet scavengers. Furthermore, the use of nanomaterials to

impart active food packaging properties are commercialized, such as
nanosilver, carbon nanotubes, nanocopper oxide, nanomagnesium
oxide, and nanotitanium oxide [19−21]. Kodak Company launched
and commercialized antimicrobial packaging for food items that
consume oxygen [22]. Oxygen scavenging packages are also produced
by using enzymes from polyethylene films [23]. Once the product is
exposed and re-wrapped with an active film, there is also a need of
suitable treatment to stop microbial growth [24].

10.2.1.1 Antimicrobialpackaging
The dissolution of silver nanoparticles has documented the
antimicrobial activity of Ag+ ions [25]. The absorption and
decomposition of ethylene in silver nanoparticles have also
been stated to contribute toward the extension of the fruit’s and
vegetable’s shelf life [26]. Antibacterial characteristics of carbon
nanotubes were also reported [27]. Nanosensors designed for
this task may detect the complexity of packaged products and
the involvement of pathogens. They probably take on the shape
of “buttons” on the color-changing packaging [28]. Antimicrobial
activity of nanomaterials was researched for use as inhibitors to
microbial growth or as antibiotic carriers for use. In this regard, silver
nanoparticles have been recognized as popular antimicrobial agents
for food packaging applications, on account of their high toxicity for
a variety of pathogenic isolates with low volatile and temperature-
resistant nature [17, 29−34].

10.2.1.2 Oxygenscavengingpackaging
Generally, food and drinks that are prone to oxygen have been
packaged so that their sensitivity to oxygen is reduced. Such oxygen
may be inserted in the package when the package is closed or entered
by permeation or leakage during the storage. Several chemical
reactions concerning food degradation, like overcooking and rancid
flavoring, involve oxygen. The inclusion of O2 scavengers will achieve
extremely low levels of O2 in food packaging systems. The literature
has documented oxygen scavengers’ films with the application of the
TiO2 nanoparticles to various polymers [35].
238 Applications of Nano-Biocomposite Materials

There is strong clarity about TiO2 nanoparticles-based nanofilms

[10]. Oxygen leads to the degradation of many foods directly or
indirectly. Active oxidation reactions, for instance, cause fruit
browning and vegetable oils to be rancid. Food spoilage by aerobic
microbes is the passive activity of oxygen itself. Consequently, it
is possible to keep very low oxygen rate by incorporating oxygen
scavenger in the food pack, which is beneficial for many purposes,
as it increases food’s shelf life [36]. Numerous definitions of active
packaging focused on nanocomposite films for O2 and ethylene
scavenging have been examined or the direction of O2 diffusion has
been restricted [37−39].

10.2.1.3 UVscavengers

A film based on nanocrystalline titania (TiO2) is a generally used

content for UV absorption. Metal doping enhances the viewable
absorption of TiO2 and enhances the photocatalytic behavior under
ultraviolet rays. Doping TiO2 with silver was confirmed to have
significantly increased photocatalytic inactivation of bacteria. This
composition led to excellent antibacterial activities in nanocomposite
with PVC of TiO2/Ag+ nanoparticles [40−44].

10.2.2 NanotechnologicalSystemsforSmart/Intelligent
Packaging
For the sensation of biochemical or microbial changes in food,
nanomaterials in smart/intelligent packaging are used to detect
particular pathogens developed in foodstuffs or particular gases
caused food spoilage [28] that permit environmental protection
[45]. Several companies aimed to develop smart packaging for the
optimal protection of products using nanotechnology [46]. The
chemical sensors that identify colored changes are presently used by
Nestle, British Airways, and the MonoPrix Supermarket [47, 48]. The
interactional function of a product is improved by smart or intelligent
packaging systems. Such sophisticated packaging identifies all the
features of packaged food and uses different methods to document
and transmit information of food safety and digestibility as regards
  Packaging Technologies Based on Nanotechnology 239

to the current quality or condition. Such technology uses various

revolutionary methods, for example, oxygen sensors, nanosensors,
freshness indicators, time−temperature indicators (TTIs), and others
[16, 49, 50].

10.2.2.1 Nanosensors

The existence of pathogens, mycotoxins, and microbes in food can

be sensed with nanosensors [51]. Nanoparticle-based sensors,
array biosensors, nanocantilevers, nanoparticle in solution, and
nanotest strips are all used as various types of nanosensors in the
food packaging industry [52]. Advanced nanosensor packages to
alert the consumers about the spoilage or pathogens of products
use engineered nanosensors like electronic “noses” or “tongues” to
“taste” or “smell” aromas and flavors [22, 53−55].
Nanosensor packaging is helpful for tracking of external or
internal conditions across the food supply chain of food products,
pellets, and containers. In plastic packaging, nanosensors can identify
food gases when the food products are spoiled and when packaging
itself changes its color, to warn the customers. Also, silicate-packed
nanoparticles film can limit the O2 influx into the container, and it can
keep the food fresh while keeping the moisture out of its packaging.
Also, the mold development in the refrigerator can be prevented.
Escherichia coli contamination in packaged food has been detected
by sensors. Nanotechnology can minimize packaging disposal in
connection with packaged food and can also promote the protection
and enhance the shelf life of the fresh food. Modern technology
enables food products to identify microbial pathogens within 2−7
days. Consequently, it is also used for the detection of spoilage
microbes, pesticides, and toxins [52].

10.2.2.2 TTIs
The major factors that are liable for the decreased shelf life of food
are the temperature exploitations that affect food during transit and
distribution. TTIs are beneficial for monitoring thermal background
during the storage, handling, and distribution of food to counteract
240 Applications of Nano-Biocomposite Materials

different temperature abuses. TTIs enable distributors to assure that

food is kept at an appropriate temperature, to benefit consumers
to determine the food product quality they are buying, and to help
producers monitor the food supplied across the supply chain. TTIs
help in improving food products and services [3]. On the enzymatic
base and polymeric and biological reactions, various types of TTI
activities have been produced. It is important to check changes in
temperature and time parameters from the development of food
products to till they reach to the customers to assure the safety and
quality of the products that require a certain temperature [56].

10.2.2.3 Oxygensensors
Lee et al. (2005) established an ultraviolet-based colorimetric oxygen
indicator, used to decrease methylene blue in a polymer encapsulation
medium in the photosensitization of TiO2 nanoparticles for
triethanolamine [57, 58]. Ultraviolet irradiation responds to sensor
bleaching that stays colorless up to the oxygen exposure. The level of
color change is proportional to exposure of oxygen. Nanocrystalline
SnO2 was used by Mills and Hazafy (2009) [59] as a photosensitizer
and colorimetric oxygen indicator. They used glycerol as an electron
donor, hydroxyethyl cellulose (HEC) as encapsulating polymer, along
with methylene blue dye as an indicator. When the ultraviolet-B
light is exposed, the indicator is bleached and photoreduction the
coloration by SnO2 nanoparticles. Another study carried out by
Mihindukulasuriya and Lim (2013) [60] developed an electrospinning
approach for the activation of the ultraviolet-based oxygen indicator
membrane. The encapsulation in the electrospun polyfibers of active
ingredients like TiO2 nanoparticles, glycerole, and methylene blue
improves the membrane’s oxygen sensitivity [57−60].

10.2.2.4 Freshnessindicators

The product quality is demonstrated directly by a freshness

indicator. This is generally labeled on the container. The variable
is generally focused on detecting the first type of changes, such as
pH, composition of gas, etc. These modifications are identified by
the indicator and converted into a reaction that can be generally
measured by color and correlated to food’s freshness value. This
  Packaging Technologies Based on Nanotechnology 241

reaction may be affected by changes in microbes’ metabolism

substances, such as carbon dioxide, glucose, ethanol, organic amines
and acids, and volatile nitrogen and sulfur compounds in storage,
which indicate the growth of microorganisms [61]. Various kinds of
gas sensors are constructed, which translate chemical interactions
between particles on the surface into a reaction signal, depending
on applicable surface properties studies of materials. Many electro­
active conjugated polymers were produced that employed either
chemical or electrochemical oxidation reactions. Thus, they play an
important role in food preservation, due to their electronic, electrical,
optical, and magnetic characteristics linked to their conjugated pi-
electron backbones [28, 62].

10.2.3 NanotechnologicalSystemsforImproved
Packaging
Many nanoparticles that include polymers of up to 5% w/w
nanoparticles with clay nanoparticles with enhanced barrier
structures (80−90% lowered) are used in the manufacture of
containers and bottles (i.e. edible oils, carbonated drinks, beer drinks,
etc.) and films that have a range of nanoparticles (also known as
nanocomposites). The United States Food and Drug Administration
(USFDA) have authorized the use of nanocomposite in food contact
[9, 10, 19, 24, 47, 55]. Table 10.1 describes common nanomaterials
for food packaging applications.

Table10.1 Food packaging applications of some common nanomaterials

Application Description Key nanomaterial

Active packaging Integration of nanomaterials Ag, TiO2
with antimicrobial or
other characteristics (e.g.,
antioxidants, ultraviolet
absorption), which are
supposed to activate and
result in taste, freshness,
and shelf-life impact on the
packaged food.
(Continued)
242 Applications of Nano-Biocomposite Materials
Table10.1 (Continued)

Application Description Key nanomaterial

Smart packaging Nanosensors are integrated to ZnO, CNTs
track and report the status of
food (e.g., oxygen indicators,
freshness indicators, and
pathogen indicators).
Improved Nanomaterials are Clays, SiO2
packaging included in the packaging
to boost physical
presentation, robustness,
obstacle characteristics,
biodegradation,
biocompatibility, and climate-
friendly.

10.3 BiodegradableNanocomposites

Nanocomposites, a synthesis of conventional food packaging

materials with nanoparticles, are becoming more common in the
food packaging industry. It shows a strong mechanical efficiency and
difficult resistant, as well as its notable antimicrobial spectrum. In
a continuous or discontinuous stage, nanocomposites are typically
composed of a polymer matrix [15, 39]. Polymer nanocomposites
(PNCs), polymer’s mixtures of inorganic or organic additives with
specific geometries (fibers, flakes spheres, particulates), are less than
100 nm in size and currently introduced as new packaging materials
[63, 64].
A significant function is played by the aspect ratio of packaging
filler material (the proportion of the largest filler to the smallest).
Further, general surface areas with correlated high reinforcement
effects are available in fillers with a higher aspect ratio [65, 66].
Diverse nanomaterials, including silica [67], clay [68], organic
clay [69], grapheme [70], nanocrystals of polysaccharides [71],
carbon nanotubes [72, 73], chitosan-based [74], other metal
nanoparticles, for example, ZnO2 [75], colloidal Cu [76], or Ti, and
other nanoparticles, are thoroughly studied as fillers [77].
  Other Polymer Matrix-Based Nanocrystal Systems 243

It is interesting that nanocomposites based on biopolymers

can even have environmental benefits as compared to traditional
plastics. Othman (2014) looked at various forms, for the use of
biocomposite substances for food packaging activities, of nano­
sized fillers and biopolymers [78]. The theoretical production of
biodegradable nanocomposites using starch, poly-lactic acid (PLA),
or polyhydroxybutyrate (PHB) biopolymers was studied by Goyal
and Goyal (2012). Large numbers of nanocomposite biopolymers
are being utilized using several organic molecules, including nylons,
polyolefins, ethylene vinylacetate (EVA), polyamides (PA), polyimides
(PI), polystyrene (PS), copolymers, epoxy-resins, polyurethane
(PU), and polyethylene terephthalate (PET) [79]. Ray et al. (2002)
investigated that the polylactic acid-based bionanocomposite
has a speedier biodegeneration rate than polylactic acid without
such additives, when nanofillers are spread within bio-compatible
polymer polylactic acid [80].

10.4  OtherPolymerMatrix-BasedNanocrystal
Systems

Cellulose is a specific and widely available biomaterial possesses

a range of beneficial characteristics such as renewability,
biodegradability, and non-toxicity. It is a polysaccharide consisting
of repeating β-D glucopyranose units and highly functional with
three groups of hydroxyl per anhydrous glucose unit. In several
industries, like food and pharmaceutical, cellulose is widely utilized
in pure form or as a derivative in the manufacture of a broad
range of products [81]. In the 1950s, Ranby first obtained a liquid
colloidal solution of cellulose micelle by sulfuric acid treatment [82].
Mukherjee et al. reported first in 1953, the images of dried powdered
nano cellulose with needle shaped morphology. The term “nano
cellulose” was first used to characterize the gel-like substance of
wood pulp homogenization at high temperature and high pressure
at ITT Rayonier Lab in Whippany, New Jersey, the USA, in the late
1970s by Turbak et al. [83]. In the early 1980s, ITT Rayonier granted
several patents to explain how these cellulosic nanomaterials were
prepared and applied [84]. Table 10.2 depicts the list of identified
244 Applications of Nano-Biocomposite Materials

nanotechnologies used for food packaging and preservation utilized

in the food industry during past few decades.
In recent decades, scientists have identified unique features of
cellulose nanocrystals (CNCs) like excellent mechanical properties
[97], self-assembling capabilities, surface interface effect [98],
photonic properties, thixotropic function, and chemical reactivity [99,
100]. Several types of nano celluloses, including CNF, CNC, and BNC,
have been obtained up to now. Acid hydrolysis can produce CNC from
native fibers that lead to extremely crystalline and rigid nanoparticles,
which are shorter than the nano fibril obtained by homogenization,
microfludisation, or by grinding routes [101]. CNC has been studied
and a broad range of applications in a wide variety of fields have
recently been developed. It may be modified to meet new product
enhancement specifications or to produce new applications that have
previously been considered impossible. In the food industry, the quality
of food and beverage products is constantly increasing with the use of
nanocrystals [102, 103].
Various polymers were grafted onto the CNC surface using
the grafting-on approach to improve the dispersion and matrix
compatibility. Habibi et al. grafted a poly-caprolactone CNC (PCL)
with isocyanates coupling agent, and applied high modulus and
good ductility were shown in nanoscale films made with PCL-graffed
nanoparticles, which represent the strengthening of CNC’s polymer
matrix. The same approach has been taken by Cao et al. [104] with
CNC graft-borne polyurethane chains. In the presence of carbodimide
derivatives, Mangalam et al. used TEMPO oxidized CNCs in functional
groups using-COOH to graft tranded ADNs [105]. Ljungberg et al.
grafted maleate, a low molecular weight functionalized atactic
polypropylene on tunicate CNCs extract. Films cast using grafted
CNCs have demonstrated strong matrix compatibility and greater
transparency and tensile unit. Amina functionally administered
polyethylene glycol (PEG) has been grafted by Araki et al. [106] to
obtain high-stability CNC suspensions from the TEMPO oxidized
CNC by carbodimide chemistry. CNCs modified by the surface have
significant properties, including high-colloidal stability, increased
dispersion in polar and organic solvents, and thermo-reversible
aggregation [107].
There are basic requirements of applicable materials, such as
thermal and tensile properties; however, food packaging deserves
Table10.2 List of identified nanotechnologies used for food packaging and preservation utilized in the food industry

Nanotechnique Composition Application Advantage Reference

Nanoparticles Polymeric Food packaging Identified to be well-organized delivery systems and are [85]
nanoparticles and preservation bactericidal
Reduce moisture leakage [86−88]
Silicon dioxide Food packaging Used as drying and anticaking agents
and preservation Absorb hygroscopic interaction of water molecules in milk
Silver Food packaging Secure food from microbial infestation and act as [85,89]
nanoparticles and preservation antibacterial agents
Enhance fruit’s and vegetable’s shelf life through the
absorption and degradation of ethylene
Zinc oxide Food packaging Reduce the oxygen flow into the containers [89]
and preservation

 Other Polymer Matrix-Based Nanocrystal Systems

Nanocomposites Nanoclay (polymer Food packaging Used to build gas obstacles to reduce carbon dioxide [90]
and nanoparticles) leakage from carbonated drink bottles
Enzyme Food packaging Provide a wider area and quicker transfer [91]
immobilization
Nano core Food packaging Used in manufacturing of plastic beer bottles to prevent [92]
carbon dioxide from being emitted from beverages
NanoCeram PAC Food packaging Help quickly absorb unpleasant components that can [91]
cause foul smell and repulsive taste
Nanosensors Nano-smart dust Food packaging Find pollution of any kind [93]
Nanobiosensors Food packaging Identify viruses and bacteria [93]
Abuse indicators Food packaging Calculate optimal temperature [94]
Carbon black and Food packaging Detect carcinogens in food materials [95, 96]

245
polyaniline Identify pathogens transmitted from foodstuffs
Detect microorganisms that normally infest the food
246 Applications of Nano-Biocomposite Materials

more specific features. Food packaging is aimed at ensuring quality of

life and safety of nutrition. Barrier properties are therefore important
to slowdown the oxidation of water vapor and gas exchange between
the food and the atmosphere [108]. For this reason, the proposed
food safety materials are critical to water vapor (WVP) and oxygen
permeability (OP). Transparency is also important, as the customer
can see by visual inspection about the quality and condition of the
material. With, the use of CNCs in the biodegradable polymers, matrix
significantly improves the mechanical properties of the neat polymer,
which leads to improve the water and oxygen barrier properties.
Water resistance is also preferred because contacts with wet surfaces
can lead to the disintegration of the film [96].

10.5 ConclusionsandFutureProspects

Nanotechnology is becoming ever more important to the food

industry. It offers a variety of exciting advantages for food packaging,
including improved food quality and sanitation, enhanced food’s
shelf life, etc. With many innovative applications, its uses for food
packaging are promising as nano-based packaging materials
that provide excellent protection toward microbial attack, and
nanosensors are capable of detecting microorganisms or chemical
contaminants at extremely low levels. The future of food security
is largely dependent on nanotech progress, the integration of a
nanosensor in a food container and the breakdown of IP solutions.
This new systems can help detect, monitor, track, record, and
communicate through the supply chain.
The application of nanotechnology offers considerable
advantages even in the early stages to improve the properties of
packaging materials and requires continuing investment to finance
research and development to better understand nanotechnology’s
advantages and disadvantages in packaging system. In the range of
advanced functional properties, the use of nanotechnology to make
food packaging can offer numerous benefits. It can provide packaging
materials with improved processing functionalities, such as health
and packaging, transportability, and lower costs.
 References 247

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Chapter 11

An oxidant Finishing Enabled Packaging

for Improved Shelf Life of Food

Meenu Aggarwal,a Anjali Gupta,b Vanita Sapra,c

Meenakshi Singhal,d and Nisha Sainie
a Department of Chemistry, Aggarwal College, Ballabgarh, Faridabad, Haryana, India
b Department of Chemistry, Galgotias University, Greater Noida, Uttar Pradesh, India
c Department of Chemistry, GGDSD College, Palwal, Faridabad, Haryana, India
d Department of Chemistry, Aggarwal College, Ballabgarh, Faridabad, Haryana, India
e Department of Chemistry, Gargi College, University of Delhi, New Delhi, India

[email protected]

Antioxidants are valuable additives capable of preventing the rancidity

of food by preserving lipids from oxidation either by annihilating free
radicals or stealing oxygen so as to amplify the shelf-life expectancy
of the foodstuffs. Synthetic antioxidants regulate the oxidation by
sustaining the re ined oils and fats within the food products. But,
owing to deadliness and cancer-causing properties of certain man-
made antioxidants, they could be swapped by natural antioxidants.
The increased awareness of consumers toward products has shifted
the focus to use natural active agents. Biocomposite constituents,
come up with the packaging tool, retain the aspect, assurance, as
well as sensual equities of the foodstuffs; all together securing the
environment due to their biodegradable and renewable nature.
Thus, it is a necessity to include active agents into packingmaterials.

Biomaterials in Food Packaging

Edited by Mohd Yusuf and Shafat Ahmad Khan
Copyright © 2022 Jenny Stanford Publishing Pte. Ltd.
ISBN 978-981-4877-98-5 (Hardcover), 978-1-003-25678-6 (eBook)
www.jennystanford.com
258 Antioxidant Finishing Enabled Packaging for Improved Shelf Life of Food

Biocomposite reinforced with nanofibrillated cellulose (NFC) has

advantageous benefits in food packaging applications by taking the
place of petroleum-based typical plastics.

11.1  Introduction

This chapter is focused on the antioxidant compounds that currently

are pertinent to the food industry, worth mentioning them as food
additives employed in the most auspicious types of packaging.
Foodstuff packaging can be defined in many ways. The main job of
food packaging is to keep the foodstuff safe, amid repository and
shipping over the biological, chemical, and automated responses [1].
Thus, to control, ameliorate, and improve the packaging protective
properties, there is a need to first concentrate on food packaging
materials. Information about the properties of food products and
packaging materials allow to control, utilize, achieve, and experience
better packaging alternatives with new technological improvements
to enhance the mean life of the food products and protect them from
multiple external and internal changes [2].
So as to conserve the food products against deterioration beside
proximity to extraneous factors, certain features are connecting to
stock like being inactive, non-toxic, and impervious to pathogens,
and prerequisite to be explored while packaging. Due to ambiguities
in user and natural defense, the handling as well as uptake of food
packaging operations gets hindered in spite of the biggest proportion
of the running market [3].

11.2  CurrentChallengesinFoodPackaging
Industry

Plastic packaging was used, due to its low cost, stable, and oil
resistant properties. Consumers should be careful rather than
taking a risk and give away the plastic as much as possible as per
intensifying evidences collected against the safety of plastics.
[4]. Traditional packaging keeps elementary postulate “to stay as
passive as possible”, i.e. coaction amidst the food and packaging
should be minimum, nevertheless simultaneously it needs to offer a
defensive blockade to foodstuff from outside effects that guarantee
  Smart Packaging Systems 259

food management, in addition to safeguard the food excellence for a

definite time. Food packaging technology [5, 6] is constantly changing
in reaction leads to several challenges for the current society, which
is becoming more and more heterogeneous because of different type
of users like food processors, food producers, logistic operators,
retailers, and consumers. The changes include modifications in the
usage of materials that are novel and productive in food wrapping to
promise food security, value, and traceability.
Conventional packaging can be replaced by edible coverings
as well as films that improve the shelf life of foodstuffs. Thus,
development of new techniques for food storage act in lessening gas
interchange, respiration, moisture movement, etc., in the items like
vegetables, in addition to decrease metabolic disorders and depress
the proportion of oxidative reaction.

11.3 SmartPackagingSystems

In the 20th century, the development in packaging skills gives the

impression as intelligent or smart and active packaging (oxygen
scavengers, antimicrobic agents, breathing regulators, and odor
absorbers). The smart packing is efficient in sensing, recording,
tracing, or collaborating data about the value and/or status of
the creation during the whole food chain. The second packing is
constructed on the notion of accumulating definite constituents into
packaging structures that liberate or consume materials from or into
the packed food or the neighborhood area, in order to encompass
the shelf-life time along with strengthening the value, security, and
sensory features of the food products [7].
The smart packaging is sandwiched amid active and intelligent
packaging. Once it draws closer to active packaging, the technology
is grounded on the connections between the eatable and packaging
materials, along with the interior gaseous atmosphere. Typically, the
packing practiced in the food occupation comprises lively enzymes and
other constituents that can be the copycat procedures of a live system,
such as respiration. Eliminating oxygen from food packages is not an
easy-going approach. The oxygen can be detached through machine-
driven handling or additional techniques. Recently suggested method
for oxygen scavenging is phyllosilicate clay functionalized with iron,
which is produced in order to accomplish a tremendously active
260 Antioxidant Finishing Enabled Packaging for Improved Shelf Life of Food

oxygen scavenger. This process depends on the exclusion of oxygen

through passage and responding with the dispersed iron with the
purpose of generating iron oxide, which is captured inside the packing
and the clay acts as a barricade stopping any migration. The novelty
of active packaging is to cut the deterioration of food/beverage inside
the package and to influence constructive alterations to shelf life of
the foodstuffs inside the package. Active packages with assimilated
oxygen blockades or films with selective porous properties also have
potential applications in the storing of probiotic food products. This
is an open area of research for scientists and industry [8].
With the aim to fulfill the necessities of active packaging,
numerous specific additives are to be incorporated like oxygen
absorbers, materials producing or absorbing CO2 or sulfur dioxide,
antimicrobial substances, ethylene absorbers, moisture content
regulators, packaging releasing antioxidants, packaging releasing or
absorbing taste, and aroma compounds [9].
Table 11.1 depicts some commonly used absorber types,
compounds, and their applications in improving food’s shelf life.

Table11.1 Some commonly used absorber types, compounds, and their

applications in improving food’s shelf life [2−4, 10]

Type of absorber Compound Application

Oxygen absorbers Iron complexes, Cheese, bakery
ascorbic acid, metal products, sweets,
salts, glucose oxidases nuts, beans, cereals,
meat, powdered milk,
chocolate, tea
Moisture absorbers Silica gel, glycerol Bakery products,
meat, fish, poultry,
vegetables, fruits
CO2 absorbers Calcium, sodium or Roasted coffee beans
potassium
hydroxide
Substances exhibiting Encapsulated ethanol, Fats, cereal products
antimicrobial activities silver
containing
compounds, sorbic
and benzoic acids,
components of spices/
herbs
(Continued)
  Biopolymer Packaging: Edible Films and Coverings 261
Table 11.1 (Continued)
Type of absorber Compound Application
Ethylene absorbers Aluminum oxide, Fruits (apples,
active carbon, bananas, avocado),
potassium vegetables (carrot,
tetraoxomanganate potatoes, tomatoes,
cucumbers)
Absorbers of aroma Citric acid, cellulose Readily oxidizable
compounds esters, products, e.g. adipose
polyamide tissuein fish products,
fruit juices

11.4  BiopolymerPackaging:EdibleFilmsand
Coverings

Bio-based products and modern progression are receiving attention

in the food industry to reduce the dependency on fossil fuel and
transfer to a maintainable constituent’s base.

11.4.1 BioactivePackaging
A novel idea of so-called ‘bioactive packaging’ has been presented
when talking about food packaging. The dissimilarity amid active and
bioactive packaging lies in the fact that the active packaging aids to
attain as well as recover the state and security of deposited things,
whereas the bioactive packaging directly influences the well-being
of the user through the creation of healthier food packages [10, 11].
Edible coverings or films are well defined as continual patterns made
up of lipids, proteins, and polysaccharides, which are fit for human
consumption [12].
To improve security, constancy, sensory, and dietary properties
of food [13], functional food substances, such as antimicrobials,
antioxidants, flavoring agents, and nutrients, are incorporated.
Materials producing palatable films can be classified into four
categories: resins, biopolymer hydrocolloids, lipids, and composites.
Biopolymer hydrocolloids comprise proteins such as collagen, casein,
keratin, wheat gluten, soy protein, and polysaccharides (starch,
cellulose derivatives, and plant exudates); resins include wood rosin;
262 Antioxidant Finishing Enabled Packaging for Improved Shelf Life of Food

lipids comprise acylglycerols, waxes, and fatty acids; and composites

usually comprise lipids and hydrocolloid elements in the form of a
bilayer or else an emulsion [14]. Researchers are hitting more efforts
in the progress of green products by recycling and selecting eco­
friendly products in lieu of the growing moral mindfulness and ‘green
consumerism’ among the consumers [15, 16].
Edible films and coverings are coats of constituents applied to food
products, which provide antioxidants, nutraceuticals, antimicrobials,
flavoring agents, and numerous flavors that improve the value,
management, and reliability of the packaged items. Widespread
concern in the world is with the production of protein-based packing
by means of durable antioxidants besides antibacterial activities.
Suitable gelatin film integrated with carvacrol as appropriate
food packing material is made inclusive of strong antioxidant and
antibacterial properties [17].
Environment-friendly films can be produced by either wet
processing or dry processing. In wet processing method, film forming
ability can be produced from materials, which must be soluble in a
solvent like water and alcohol, further combined with plasticizers,
antimicrobial agents, and colors or flavors in this process. The dry
method does not include solvent dispersal as it depends on intrinsic
thermoplastic features of some biopolymers [12].
Eco-plastics are both bio-based and decomposable, such as
polylactic acid (PLA) or polyhydroxyalkanoate (PHA), poly-4­
hydroxybutyrate, and polyhydroxyvalerate, are widely used. The
plasticizers, prepared by esterifying tannic acid and gallic acid, can
be used for many applications like cosmetics, food preparation,
brews, and polymeric matrices [18]. Starch-based polymers are
having varied structures forming combinations with other polymer
components making the products particularly tough [19].

11.4.2 AntioxidantPropertiesinBiopolymerPackages
Antioxidant properties in biopolymer packages play a very important
role as antioxidant compounds present in the packages to decrease
the rate of oxidation of lipids as well as proteins. Thus, the antioxidants
[20−23] improve the shelf life of food products by preventing from
oxidation, so that the products can be preserved for a longer period.
  Biopolymer Packaging: Edible Films and Coverings 263

Thus, antioxidant agent in the polymeric matrix of film is the area of

interest in the packaging industry.
The various analytical methods of evaluation of the antioxidant
capacity fall into distinct categories like: DPPH, ABTS, FRAP, ORAC,
TRAP, etc., which help in determining the potential of an antioxidant
agent present in the biopolymer matrix of the film to destroy the free
radicals.
The oxidation of unsaturated lipids present in food product results
in the decrease of its nutritive value and at the same time makes it
tasteless. Further, antioxidants delay oxidation of lipids either by
annihilating free radicals or scavenging oxygen. Antioxidants are
broadly categorized into two types depending upon their mechanism
of action, i.e. primary antioxidants, which break the free radical
chain reaction initiated due to oxidation by hydrogen donation;
and secondary antioxidants, which control the rate of oxidation
by chelation mechanism, scavenging of oxygen, and destruction of
hydroperoxides [24].
The most commonly used synthetic antioxidants in the
food industry are butylated hydroxytoluene (BHT) and tert­
butylhydroquinone (TBHQ). Adverse effects of these synthetic
antioxidants on human being have increased the focus on the research
of natural antioxidants, which are particularly derived from plant
sources. The natural antioxidants can be obtained from varieties of
plants by adopting solvent extraction method.
Although plants contain ascorbic acid and tocopherols, but
they are also rich in phenolic compounds [25], thus offering a good
source of natural antioxidants, which are to be used in various food
applications [26]. Antioxidant compounds like anthocyanins, flavanols,
hydroxycinnamates, and carotenoids are present in fruits like apple,
blueberries, blackcurrant, cherry, cranberries, grapes, orange, peach,
plum, raspberries, strawberries, etc. [26]. Grape seed and grape seed
extract have the same antioxidant properties as present in propyl
gallate, butylated hydroxyanisole, and butylated hydroxytoluene [27].
Apart from grapes, even the rosemary, pomegranate, and cinnamon
also possess better antioxidant properties in comparison to synthetic
analogs. Thus, plant extracts can be used as natural antioxidants in
meat products, particularly for red meat [28].
Nowadays, worldwide, curiosity is increased over the extraction
of natural antioxidants from plants to overcome the adverse health
264 Antioxidant Finishing Enabled Packaging for Improved Shelf Life of Food

effects caused by synthetic antioxidants. Green tea, which is a natural

source of antioxidant, is highly useful for food product that contains
high percentage of polyunsaturated fatty acid because it is more
susceptible to oxidation. The green tea extract is extensively used
in dressing of salad, sauces, soups, mayonnaise, fat spreads, meat,
poultry, bakery products, frying oils, seafood, pizza toppings, cereals,
and snacks [29].
Chitin, a natural polysaccharide, is used for the synthesis of
bioactive polymer chitosan via deacetylation process. The biological
activities like antibacterial properties and non-toxicity make chitosan
and its derivatives a suitable candidate for numerous applications in
the food, pharmaceutical, and agricultural sectors [30−32].
Majority of snacks like nuts, cereals, dry fruits, chocolate, etc., that
employ ingredients containing high-antioxidant contents fall under
the ready-to-eat cereal category. Such snacks are being promoted to
target audience [33]. Aerated (black) tea’s antioxidant property as
well as its flavor is enhanced by the addition of spices. Research finding
has shown that some spices are required in higher concentration for
optimum taste, but aerated (black) tea give good results at lower
concentrations of spices [34]. As the spices are expensive, which can
increase the overall cost of the product, therefore in order to reduce
the quantity of spices added, focus is on the commercial production
of spiced aerated (black) tea by setting threshold levels of spices for
product development.
The antioxidative properties of milk and milk products like whey,
skim milk, and casein contribute significantly in maintaining high-
milk quality by preventing lipid peroxidation. This is all because of
high concentration of phenolic compounds in milk, which enhance
the oxidative stability of dairy products [35]. The incorporation of
plant-based antioxidants further decreases the rate of oxidation of
dairy products.
The natural antioxidants are used widely not only to improve
the shelf life of the food products, but also to prevent the human
beings from the adverse side effects of synthetic antioxidants. The
research is going on to find more and more antioxidant molecules
from a variety of plants, which can be used very safely in the dairy
industry [36].
The deficiency of vitamin C in human beings as well as in some
species of birds and fishes, which are not capable to synthesize it,
  Biopolymer Packaging: Edible Films and Coverings 265

suffer from the disease scurvy. Therefore, the citrus fruits such as
orange, kiwi, lemon, guava, grapefruit, papaya, and strawberries,
and vegetables such as broccoli, cauliflower, and capsicums, which are
rich in ascorbic acid, are highly recommended for daily consumption.
Vitamin C or ascorbic acid is a natural organic compound
presents in both plants and animals, enriched with antioxidant
properties. Ascorbic acid is a strong reducing agent, which allows it
to get oxidized easily to dehydroascorbic acid. This property makes
it suitable for scavenging free radicals such as hydroxyl radical,
hydrogen peroxide, and singlet oxygen. The free radicals are very
harmful for the humans, as they can damage tissues and speed up
the destruction of liver in people having hepatitis. This mechanism
is responsible for the reduction of major antioxidant, i.e. glutathione,
presents in the liver cells. Ascorbic acid promotes the assimilation of
the iron in the intestine as well as the detoxification caused by heavy
metals such as nickel, cadmium, and lead, to provide cellular defense
mechanism. The food industry is looking for some specific additive
of ascorbic acid and its salts, which possess strong antioxidant
properties to improve the quality of food products. The various
additives of ascorbic acid are: E300, ascorbic acid; E301, sodium
ascorbate; E302, calcium ascorbate; and ascorbyl stearate. The
ascorbic acid also prevents the meat products from getting oxidized
and discolored upon storage [37].
Also, fundamental element influencing lipid oxidation in
mayonnaise has been discussed in this chapter. In nutshell, oxidative
degradation of lipids in mayonnaise can be reduced by controlling
all those factors that increase rancidity such as reduction in storage
temperature, avoiding direct light, and improving chemical properties
of oils.
However, oxidation of mayonnaise can also be prevented by using
antioxidants. Keeping in mind the health of people, there is a tendency
of using natural antioxidants in food products. After reviewing the
literature, it can be interpreted that it could be possible to design a
mayonnaise with greater oxidative stability, by replacing synthetic
antioxidants with natural ones.
With several researches in the area of using natural antioxidants
in mayonnaise, it is decided that now focus is on elucidating the
mechanism of oxidation, exploring more natural antioxidants, as well
266 Antioxidant Finishing Enabled Packaging for Improved Shelf Life of Food

as to study the interfacial area of oil in water emulsion to decrease

the rate of oxidation. These all help in finding the best suited natural
antioxidant to be used in mayonnaise to decrease the side effects
caused by oxidation [38].
Now the consumer preference has been changed, i.e. more
inclination is toward organic and green food. So, the food industry
is also concentrating on the use of natural compounds, which are
the safest alternatives to synthetic products, but at the same time
they maintain the quality of food products and prevent them from
microbial spoilage, which are utmost importance.
The futuristic approach for the use of antimicrobial and
antioxidant properties of natural substances is not only helping
in the production of safer and healthier food, but also maintaining
the integrity of environment, as harmful chemicals are replaced by
natural analogs [39].
Nowadays, there is an increasing interest in nutraceutical
compounds based on natural sources being added for food coloring
as well as eco-functional properties [40]. However, the limited
development of novel nutraceuticals and bio-based food additives
is all due to the low production with poor yield upon purification,
specifically when these bioactive compounds are synthesized by
microbial fermentation. Thus, in the future, more projects will be
made compulsory for the research in the area of improvising the
production and purification of natural bioactive compounds to
maximize the yield for fulfilling the demand of increasing population.
It is also essential to establish regulatory authority to define rules and
regulations for the use of natural substances in the food, cosmetic,
and pharmaceutical industries [41].
According to the present invention, the food packaging materials
include polymeric materials and natural antioxidants. Typically, the
natural antioxidant is organic in nature and obtained from active
ingredient presents in a plant, which is responsible for providing
desired antioxidant effect. The active ingredient is obtained from
plant products by extraction process using a suitable solvent to
dissolve the active ingredient, in order to separate it from residual
plant material. The organic solvent extracts can be obtained by single
or successive extraction process from the plant. The extracts may
be used in aqueous, gel, or oil form in the food packaging material.
Aqueous solvents, alone or in alkaline and acidic medium; oils (palm
oil, coconut oil); and organic solvents like hexane, ethanol, methanol,
  Nanotechnology in Food Packaging Industry 267

acetone, tetrahydrofuran, chloroform, etc., are used in the extraction

process [42].

11.5 NanotechnologyinFoodPackagingIndustry

The elementary opinion in the usage of active packing based on the

integration of specific constituents inside the polymer and inherent
features of the polymer itself can be used in the food packaging
industry. Because of the size of nanoparticles, relatively larger surface
area, and cost-effectiveness, nanotechnology is applied to polymer
matrices.
Due to the changeable structures and shapes of nanoparticles,
these are used in formation of different nanostructured materials,
which are accountable as food packing constituents, mainly because
of their antimicrobic nature, in addition to oxygen-scavenging
capacities. The usage of biopolymers as packing films in the food
division has increased, owing to their extraordinary price and
mediocre implementations, as compared to synthetic polymeric
materials.
Nano-reinforcement that integrates the application of
nanoparticles and nanofibers, e.g. nano clays, metal oxides
nanoparticles, carbon nanotubes, and other fillers into a matrix of
the polymer, thus providing smart or active assets to the wrapping
arrangement by diffusing it in the form of nanocomposites [43].
Polymeric elements strengthening through nanoparticles have
unlocked a great space of prospects and upgrading by even spreading
of nanofillers in the polymer. The contact between nanofiller and
polymer, which is vital to accomplish healthier reinforcement, can be
augmented through insertion of parameters like amount, functional
moiety, quality of filler, polymer performance, and handling method.
However, cellulose is an actual fascinating accepted polymer. An
extremely auspicious segment of cellulose is NFC, which is broadly
exploited in abundant applications, precisely in the food packing
business. To recover the mechanical and barrier properties of the
composites, the nanocellulose is chiefly used to reinforce with the
polymer, which may supplement the mixture performance like
antimicrobic and antioxidant, in addition to mechanical features.
The composites with boosted properties may be well-matched for
conserving fruits, vegetables, and other foodstuffs in the food packing
268 Antioxidant Finishing Enabled Packaging for Improved Shelf Life of Food

industry. Consequently, problems mainly met by the food industry

will be overcome by the usage of nanocellulose-based polymer
composites [46].
Further, there are some shortages restraining their possibility
of uses, for instance, agglomeration as well as acquiescence with
hydrophobic polymeric matrices. These challenges can be overcome
by chemical treatment of NFCs, contributing novel functionalities
to these materials. Thus, the interfacial linkage between NFCs
and polymer matrices is extremely improved by means of filler
functionalization, which allows even nanoscale dispersal of the
reinforcing fillers within the matrices, therefore attaining the
persistent shelf life [47, 48]. Special emphasis has been given to
blends in the frame of packaging application [48−50].
Nanocomposite idea has technically acquainted with uniqueness
in production of a novel refinement of innovative polymeric
constituents possessing adaptable, exciting, and superior assets,
embracing thermo mechanical attributes though sustaining varying
polymer matrix transparency. These materials have also established
competence with respect to costing and effectiveness in several
applications especially in packaging.

11.6 ConclusionandFutureRemarks

Among the various types of active packaging, mainly for the food
industry, the antioxidants play the promising role to progressively
meet the necessities to encompass the shelf life, thereby generating
novel potentials for their applications. The use of synthetic
antioxidants will be substituted with natural antioxidants, which
are good synergists that can enhance the shelf life expectancy of
foodstuffs by including herbs and spices. The forthcoming scope
of bio-based packaging materials is hopefully very bright, due
to the environmental concerns and the global realization that
petroleum resources are limited and renewable resources will be
the solution. Bio-nanocomposites offer an opening for the use of
high performance, lightweight nanocomposite constituents, hence
substituting traditional non-biodegradable petroleum-based plastic
packaging materials. With regard to the upcoming visions of NFC
packaging materials, it is positively expected that simple packaging
systems will be substituted with high-tech intelligent packaging
 References 269

systems. Also, biosensing application not only protects food

against environmental factors, but also integrates properties to the
packaging materials, permitting quite a lot of budding choices in the
food packaging industry.

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Chapter 12

Active Finishing Agents for Food Bio-

Preservation Based on Natural Origin to
Prevent Microbial Risks

Smrita Singh,a Lalit Prasad,b Ashutosh Singh Chauhan,c and

Shafat Ahmad Khanc
a Bioexplore, Dimapur, Nagaland, India
b Division of Chemistry, School of Basic & Applied Sciences,
Galgotias University, Greater Noida, Uttar Pradesh, India
c Air Pollution & Stone Conservation Laboratory,

Archaeological Survey of India, Agra Fort, Agra, Uttar Pradesh, India

[email protected], [email protected]

Bio-preservation technique is used to enhance the shelf life of highly

perishable food of plant and animal origin. This process exploits
the antimicrobial property of naturally occurring agents and their
metabolites to prevent the spoiling of food. Several organisms of
biological and natural origin are used for preservation of the food
for longer time, without having any adverse effect on human health.
This process involves the use of several natural micro-floras of plant
and animal origin, as well as of microbial origin, such as bacteria,
bacteriophages, etc., under controlled environment. This natural
technique helps in reducing the volume of chemical preservatives
as well as other processes that may negatively affect the quality and
nutritional value of preserved food. Genetically modified micro-

Biomaterials in Food Packaging

Edited by Mohd Yusuf and Shafat Ahmad Khan
Copyright © 2022 Jenny Stanford Publishing Pte. Ltd.
ISBN 978-981-4877-98-5 (Hardcover), 978-1-003-25678-6 (eBook)
www.jennystanford.com
276 Active Finishing Agents for Food Bio-Preservation Based on Natural Origin

floras or their metabolites may also be used as bio-preservatives,

but the selection of substances to be used in bio-preservation should
be done carefully and judiciously keeping in view of all toxicological
and safety issues, is foremost important. New genetically
modified micro-floras and microorganisms are being developed
for better preservation of food, keeping in view of nutritional
value and organoleptic quality of food products. Nowadays, this
bio-preservation process is gaining acceptance due to its inert
benign approach.

12.1 Introduction

Bio-preservation is a method of extending shelf life of food by

exploiting ingredients derived from microorganisms, and metabolites
from microorganisms, flora, and fauna. Several ingredients derived
from plants, animals, and microorganisms have strong antimicrobial
property and inhibit the growth and survival of harmful pathogenic
microorganisms in food. Since ancient times, several herbs and
spices have been used for the preservation of food and inhibited the
growth of bacteria, fungi, mold, and other harmful microorganisms.
The choice of natural preservatives is logical one, as they help us
to avoid the use of excessive chemical preservatives and physical
treatments of the food for preservation. This method helps us to
retain the nutritional value of food products and makes them safe
for consumption.
Natural antimicrobials and their products/ingredients that can
be used as bio-preservatives can be broadly classified into following
three categories:
i. Active finishing agents of plant origin
ii. Active finishing agents of animal origin
iii. Active finishing agents from bacteria and other micro world.
This chapter provides a basic overview of natural active
finishing agents derived from bacteria and their use as bio-
preservatives of food.
  Active Finishing Agents from Bacterial World in Food Preservation 277

12.2  ActiveFinishingAgentsfromBacterialWorld
in Food Preservation

12.2.1MajorDerivedComponents

12.2.1.1 Bacteriocins
Bacteriocins are minute polypeptide molecules or protein, biosynthesized
within ribosomes that exhibit antimicrobial activity against several
closely related groups of bacteria and other unrelated groups of microbes.
Nowadays, bacteriocins are classified as heat-stable cationic peptides,
produced by mainly Lacto bacillus (lactic acid bacteria, LAB), which
show wide-spectrum antibacterial potential [1, 2]. Bacteriocins are
proven toxicologically safe, as they are produced by both Gram-positive
and Gram-negative species, which are an important part of the defense
system. Bacteriocins produced from Gram-positive bacteria are heat
stable and function at the wide range of pH and have broad-spectrum
antibacterial activity, while bacteriocins from Gram-negative bacteria are
heat labile (exception being Microcin V from E. coli) and have narrow
antibacterial activity range.

12.2.1.1.1  Classification of bacteriocins from

Gram-positive bacteria

On the basis of extensive studies performed previously [3, 4],

bacteriocins are categorized into four divisions:
Class I (The lantibiotics): These post-translationally modified
bacteriocins with molecular weight <5 kDa, having 19−50 (approx.)
amino acids, are referred to as variacin, cytolysin, subtilin, and nisin.

These lantibiotics are further divided into three types: Class Ia, Class

Ib, and Class Ic [5].

Class II (The unmodified peptides): These translationally unmodified

bacteriocins have molecular weight <10 kDa, e.g. pediocin PA-1 from
Pediococcus acidilactibci, enterocin 1071 from Enterococcus faecalis
BFE1071, and enterocin EJ97 from E. faecalis EJ97. These Class II
bacteriocins are further grouped into three types: Class Ia, Class Ib,
and Class Ic.
278 Active Finishing Agents for Food Bio-Preservation Based on Natural Origin

Class III: These heat-labile bacteriocins are large proteinaceous

molecule with molecular weight >30 kDa. Due to this, they are not
widely utilized in food bio-preservation, e.g. enterolysin A from E.
faecalis, dysgalacticin, streptococcin A-M57, helveticin J, etc. They are
sub-grouped into two types: Class IIIa - bacteriolysins and Class IIIb
- ornon-lytic bacteriocins.
Class IV (Circular peptides): These bacteriocins are unique in nature.
They joined by a circular peptide bond through the ligation of their
N-terminus to the C-terminus. Their molecular weight ranges from
5.5 kDa to 7.5 kDa. These circular peptide bacteriocins have lipid or
carbohydrate moieties, due to which they are complex proteins, e.g.

AS-48 from E. faecalis [1, 6].

Furthermore, the classification of bacteriocins based on their

molecular mass of Gram-negative bacterial colonies can be

separately countered. Bacteriocins produced from Gram-negative are

categorized based on their size. For example:

i. Colicins having high molecular mass (HMM) peptides with

molecular weight ranging from 20 kDa to 90 kDa.
ii. Microcins having low molecular mass (LMM) peptides with
molecular weight ranging from 1 kDa to 20 kDa.
iii. Tailocins having structure like a tail of bacteriophages and have
multiple subunits with high molecular weight.
The mode of action of bacteriocins varies depending on their
type. Bacteriocins are cationic and hydrophobic in nature and act
as membrane permeabilizers [6]; hence, form pores leading to the
efflux of ions (disruption of proton motive force) and other molecules
out of cells leading to permanent damage and death of cells. The
other mode of action of bacteriocins is inhibition of biosynthesis and
formation of cell wall.

12.2.1.2 Pediocins
Under the Class II of bacteriocins, pediocins are produced mainly by
the genus pediococcus of LAB. The main strains of bacteria producing
pediocins are Pediococcus acidilactici and Pediococcus pentosaceus
[7]. Pediocin inhibits the formation of cell wall of target cell by
inhibiting the absorption of amino acids required for the formation
of cytoplasmic membrane of the target cell. It is thermally stable and
  Active Finishing Agents from Bacterial World in Food Preservation 279

active at wide range of pH values and is resistant to several protease

enzymes. Pediocin SA-1, produced from P. acidilactici NRRL B 5627,
shows inhibition activity against bacteria that cause common food
spoiling, for example, Bacillus cereus, Micrococcus flavus, Salmonella
carnosus, Clostridium, Clostridium thiaminolyticum, Leuconostoc
mesenteroides, E. faecalis, Listeria monocytogenes, sporogenes, and
Lactobacillus brevis. The study carried out by Díez et al. (2012),
wherein the effect of PA-1 and combination of PA-1 with sulfur
dioxide and ethanol was investigated to assess the growth of a wide
collection of pathological strains (i.e. 16 yeast, 18 acetic acid bacteria,
and 53 oenological LAB) [8]. It was observed that PA-1 alone can be
used as a potential bio-preservative for winemaking. These days,
pediocins are being used as bio-preservatives in the preservation of
wine, baked products, dry sausage, and meat products, and reducing
cheese contamination [9].

12.2.1.3 Enterocins
Primarily Enterococcus species produce enterocins, including E.
faecium (enterocins A and B) and E. faecalis (enterocin AS-48).
In addition, a few of the entrocins, e.g. enterocin A derived from
Lactococcus lactis, are broad-spectrum antimicrobial bacteriocins.
Major enterocins, such as enterocin AS-48, enterocin 13, enterocin
416K1, enterocin L50A, and enterocin CCM4231, inhibit the growth
and survival of several food-spoiling microorganisms, such as L.
monocytogenes, Listeria innocua, Bacillus cereus, Staphylococcus
aureus, etc. [10]. Enterocins such as A, B, and AS-48 were found
effective to restrict the growth of Salmonella sp., E. coli [11, 12],
Stearothermophilus, several other Bacillus spp., Lactobacillus sakei,
and other food-spoiling lactic acid bacteria [1, 6]. They are mainly
used to preserve canned food, vegetable sauces, soybean sprouts,
skimmed milk, yogurt, frankfurters, fresh cottage cheese, raw fruits
and fruit juices, alfalfa and bean sprouts, green asparagus, infant rice-
based food and drinks, fish spread, etc.

12.2.1.4 Endolysins
Endolysins/lysins are the hydrolytic enzymes and are generally
murein hydrolases with strong antimicrobial effectiveness, produced
by the bacteriophages at the final stage their replication cycle, kill the
280 Active Finishing Agents for Food Bio-Preservation Based on Natural Origin

host microorganisms by cleavage and hydrolysis of peptidoglycan of

host cell wall. Four major types of enzymes that cleave peptidoglycan
moiety and degrade cell wall of the peptide glycan molecules by
rupturing of targeted areas are:
(i) glycosidases,
(ii) endopeptidases,
(iii) amidohydrolases, and
(iv) lytic transglycosylases.
Endolysin LysH5 has showed a bactericidal nature and used in
pasteurized milk to prevent spoilages from S. aureus [13]. Similarly,
polycendolysin has an eradicating effect on several varieties of food.
Endolysin’s application controls the spoilage of fruits by inhibiting
the growth of Erwinia amylovora, the organism responsible for fire
blight spoilage in fruits. Several endolysins are found active against
zoonotic and food-borne pathogens. In addition, phage-encoded and
engineered endolysins are recognized imparting broad-spectrum
inhibitory functions toward a number of pathogenic isolates in food
[14−16]. Lysing proteins Spp64 and Spp62 from bacteriophage
Spp001 show wide spectrum of inhibitory effect on Shewanella
putrefaciens, which is a common spoilage microorganism for seafood.
Endolysin, nowadays, finds wide applicability as antimicrobial, as
most of the bacteria are becoming resistant to common antibiotics.

12.2.2 Minor-DerivedComponents

12.2.2.1 Sakacins
Sakacins, an important class of bacteriocins, frequently come
together with other lactic-acid bacteriocins, are derived from
Lactobacillus sake. The major-isolated sakacins are sakacin A, G, K,
P, and Q; out of these, sakacins A and P are commonly used [17, 18].
Sakacins are revealed to inhibit the growth of several food-spoiling
microorganisms [19], e.g. Proteus vulgaris W7, Klebsiella aerogenes
N12, Staphylococcus aureus N16b, Bacillus cereus W18, B. subtilis
N20, E. coli N2, E. coli W4, Pseudomonas aeruginosa N7, Listeria
monocytogenes W6, etc. [6, 18, 19].
  Active Finishing Agents from Bacterial World in Food Preservation 281

12.2.2.2 Lacticin
Lacticin, derived from Lactococcus lactis sub sp. Lactis, is a
bacteriocidin with broad-spectrum antimicrobial properties with
many significant peptides having generally recognized as safe
(GRAS) status. Due to their broad-level antimicrobial prospects, they
are generally regarded safe for food bio-preservation and storage
[20−22]. Due to the high-inhibitory action against common food-
borne microorganisms and wide applicability, they have been utilized
in protecting the quality of packaged as well as fresh pork-sausage
[23, 24]. Moreover, in combination with nisin, lacticin can be used as
an effective bio-preservative.

12.2.2.3 Reuterin
Reuterin is recognized due to its valued safeness and stability over a
wide range of pH values, high resistance to heat, proteolytic and lipolytic
enzymes, and high solubility in water. Reuterin, composed of non-
hydrated, hydrated, and dimeric forms of 3-hydroxypropionaldehyde (3-
HPA), is derived from few strains of Lactobacillus reuteri. It is found very
effective cidal capacities against the molds and yeasts, Gram-negative
and Gram-positive bacteria strains, along with some protozoa [25, 26].
Reuterin was reported to have excelled inhibitory activity against many
microorganisms, such as S. aureus, S. choleraesuis, L. monocytogenes,
E. coli, Campylobacter jejuni, Yersinia enterocolitica, and Aeromonas
hydrophila, causing food spoilage [1, 6, 27, 28]. Therefore, nowadays,
reuterins have been used to impart preservative benefits for meat as
well several kinds of dairy products, as a smooth alternate for food
bio-preservation [29, 30]. Additionally, reuterin has assessed for its
preservative effects and found positive responses in various cooked pork
and beef sausage, alone or in combination with other bacteriocidins,
and possessed excellent antimicrobial potential and could be an ideal
contender to be effective and eco-safe preservative applicable for food
and dairy items.

12.2.2.4 Nisin
Nicin, a protein consisting 34 amino acids, is derived from Lactococcus
lactis and regarded as GRAS category. Some uncommon amino
282 Active Finishing Agents for Food Bio-Preservation Based on Natural Origin

acids are reported in nicin biomolecule, including ethyllanthionine

(MeLan), lanthionine (Lan), didehydroaminobutyric acid (Dhb), and
didehydroalanine (Dha) [30, 31]. The antimicrobial activity of nisin
is attributed to the interaction with phospholipids of host bacterial
cell, where disruption of normal cell membrane occurred by nicin. It
is found quite effective against the growth of several pathogenic and
harmful Gram-positive bacteria such as Listeria monocytegenes and S.
aureus. In addition, it inhibits the spore growth of many species of
Clostridium and Bacillus leading to their death. In combination with
heat treatment and chelator EDTA, nisin possesses considerable
effectiveness against the growth of spores of several Gram-negative
bacteria, e.g. Pseudomonas aeruginosa, E. coli, Salmonella enteritidis,
S. typhimurium, etc.
Several nisin derivatives have been developed by altering the
amino acid sequences, which show enhanced antimicrobial properties
for both Gram-positive as well as Gram-negative bacteria [26, 30]. As
sole or in combination with other naturally occurring biomolecule,
nicin found its potential to be used as food preservative, capable
of inhibition of few types of food-borne pathogen isolates [32]. In
combination with pediocin, reuterin or organic acids, lysozymes,
etc., nicin has shown its improved efficiency against pathogenic and
harmful bacteria such as E. coli, L. monocytogenes, B. thermosphacta,
and others [33].
Consequently, nisin can be used as an effective agent for preserving
several food products, such as cheese, juices, beverages, meat, etc.,
against several pathogenic microorganisms commonly causing food
spoilage [34]. On account of brilliant activity for suppressing the
growth of food-spoilage generative microbes, nicin is being used
in the making of biodegradable polymeric (especially based on
polylactic acid (PLA), whey protein isolate (WPI), pea protein isolate
(PPI), etc.) films for packaging food materials [35].

12.2.2.5 Natamycin
Natamycin is a naturally occurring compound obtained from
Streptomyces natalensis comes under GRAS consideration. It is used as
a broad-spectrum antifungal in the food industry, and dairy products and
beverages. Natamycin shows a high affinity toward ergosterol present in
the fungal cell wall. It binds irreversibly to this ergosterol, resulting in
the alteration of the permeability of cell wall toward leakage of essential
  Active Finishing Agents from Bacterial World in Food Preservation 283

ions and small peptides, thus leading to the cell death [36]. It is not much
effective against both Gram-negative and Gram-positive bacteria, as
it lacks sterols in its cell wall. A colloidal solution in water is applied
either by dipping or spraying on to the food surface. Natamycin is used
to control the growth of molds during the fermentation process and it
is used as a bio-preservative in beverage products, even it is stable at
low temperatures with sufficient effectiveness over a wide range of pH
values [37]. Natamycin shows strong inhibitory activity against a number
of molds, fungi, and bacteria, such as Penicillium chrysogenum, P.
camemberti, P. brevicompactum, P. glabrum, A. niger, A. versicolor, A.
flavus, Cunning hamella spp., Fusarium spp., Pseudalles cheriaboydii,
Mucorra cemosus, and Eurotium herbariorum. It is also very effective
against Cladosporium cladosporiodes, C. tenuissimum, Byssochla
mysnivea, Epidermophyton floccosum, Alternaria alternata, Candida
albicans, Acremonium spp, Trichophyton spp., Aspergillus carbonarius,
P. commune, P. corylophilum, and P. verrucosumetc [38, 39]. Natamycin
in combination with nisin [40, 41] is used in polymer packaging films, and
it inhibits the growth of Lactobacillus helveticus, Fusarium culmorum,
Listeria ivanoviı, and Penicillium expansum. A mixture containing
malic acid, nisin, and natamycin, inhibits the growth [42, 43] of several
food-spoiling microbes such as Penicillium aeruginosa, P. commune, P.
chrysogenum, Y. lipolytica, Penicillium, and L. monocytogenes. Natamycin
in combination with chitosan films shows considerable antimicrobial
activity against various food-spoiling pathogens and microbes [44]. As
an antimicrobial preservative, the property of chitosan has been proposed
at less than 6.0 pH to liquid and solid food products [45]. Chitosan shows
poor water solubility, therefore, glucosyloxyethylacrylated chitosan, a
water-soluble derivative is synthesized by using the Michael reaction of
chitosan with glucosyloxyethylacrylate derivative [46].

12.2.2.6 Bacteriophages
Bacteriophages are viruses that specifically infect and grow in bacterial
cell, just like a parasite replicates through the lytic or lysogenic cycle
within the cell. They can selectively control the population of food-
spoiling bacteria [47]. Their phages are grouped into 13 types, on
the basis of their specific sizes, shapes, and types of genetic material
(nucleic acid), presence/absence of an envelope (outer capsule), or
lipids in their internal structures [47]. Application of bacteriophages
to the food is known as phage therapy and this procedure is applied
284 Active Finishing Agents for Food Bio-Preservation Based on Natural Origin

to decontaminate the raw food materials, fresh vegetables & fruits,

and other eatables [48]. They may also be used as biosanitizers
for disinfecting contact surfaces and equipment. An important
application of bacteriophages is to extend the shelf life of perishable
food products. Reduction in colonies of Salmonella, Campylobacter,
and E. coli in chicken and meat products has been noticed after phage
therapy. It also inhibits the growth of S. aureus in dairy products
such as milk, curd, etc. Food-spoiling bacteria including Listeria
monocytogenes may be eradicated completely after surface treatment
of phage P100 in ripened cheese. Reconstituted infant milk can be
protected against Enterobacters akazakii and chicken frankfurters can
be protected against Salmonella typhimurium after the treatment with
bacteriophages. Certain bacteriophages are found to be active against
food-borne pathogenic bacteria B. cereus and Clostridium perfringens,
and therefore, can be utilized in making packaging films [47, 48].

12.2.2.7 Organicacids
Since ancient times, several organic acids have been widely used as a
preservative in the food of almost all kinds. Organic acids, such as lactic,
acetic, propionic, citric, and benzoic acids, exhibit a broad-spectrum
enzymatic activity and antimicrobial property against several food-
spoiling microbes, and are widely used in food preservation directly
or indirectly. These are produced as by-products during fermentation
by bacteria [49]. Following organic acids are commonly used in food
bio-preservation:
Organic acid Chemical formula
Acetic acid C2H4O2
Propionic acid C3H6O3
Formic acid CH2O2
Ascorbic acid C6H8O6
Lactic acid C3H6O3
Sorbic acid C6H8O2
Citric acid C6H8O7
Benzoic acid C7H6O2
Phenyllactic acid C9H10O3
  Toxicological and Safety Aspect 285

Ordinarily, the uncharged organic acids exist in un-dissociated

form at lower pH, and at certain pH, they exist in equilibrium between
un-dissociated and dissociated forms. Organic acids in un-dissociated
form can pass freely through the plasma membrane of the bacteria
or fungi. Once inside the cell, these organic acids begin to dissociate,
leading to the release of negatively charged anions and positively
charged protons. These charged ions exhibit toxicological effect in
the cell in different ways, such as disruption of essential metabolic
reactions, disruption in membrane formation, intracellular stress
due to pH change, and inhibition of production of essential enzymes,
which ultimately lead to cell death.
Acetic acid and lactic acid are generally cheap, easily available,
and environmentally friendly antimicrobial. Vinegar (the main
constituent is acetic acid) and lemon juice are used as decontaminants
in household for commodities, such as carrot, lettuce, and parsley.
Acetic acid is also used as emulsifier, firming agent, stabilizer, flavor
enhancer, and preservative. Furthermore, at low concentrations,
formic acid is used as a flavoring agent. Dicarboxylic acids, such as
adipic, fumaric, and succinic acids, and their calcium and magnesium
salts are used in beverage, feed, and food preservation. Alpha hydroxyl
acids, like citric, lactic, and malic, acids, have found application in the
beverage and food industry [50].
Several sugar acids, such as ascorbic, gluconic, lactobionic, and
tartaric acids, are used as preservatives in the milk and dairy industry.
Many salts of these organic acids are used as food preservatives and
antimicrobials and are used to extend the shelf life of food products,
e.g. potassium acetate, calcium and sodium propionate, sodium
sorbate, potassium sorbate, sodium benzoate, etc. The use of organic
acids in food bio-preservation should be used with the utmost care
and should be considered to be acceptable from a toxicological point
of view.

12.3 ToxicologicalandSafetyAspect

Preservatives are used to increase the shelf life of food and maintain
the quality for a longer time. In order to determine whether food
additives, including preservatives and antimicrobials, are suitable
for consumption, their toxicological and allergenic effect should be
286 Active Finishing Agents for Food Bio-Preservation Based on Natural Origin

considered. Naturally occurring and naturally derived compounds

are no exception to the harmful effect, as the term “natural” does not
necessarily mean “safe”. It is very essential to study the toxicological
effects and characteristics of these natural antimicrobials along with
their biological metabolites. A study should be done for possible
toxicity caused by the interaction of natural bio-preservatives with
food components, along with their allergic effect to the sensitive
individuals. Consumption of a particular type of bio-preservative
may not cause any adverse effects up to the certain levels present in
nature, but it might become toxic once it reaches at high concentration
in order to achieve antimicrobial activity or when consumed
continuously over a longer period of time. The adverse reaction
of preservatives can vary from very mild to life-threatening. The
adverse and long-term effects of preservatives if not suitable to some
person include eczema, nausea, vomiting, diarrhea, rhinitis urticaria,
angioedema, irritable bowel syndrome, bronchospasmic syndrome,
migraine, anaphylaxis, exfoliative dermatitis, hyperactivity, other
behavioral disorders, tumors, cancer, DNA damage, etc., and in long
run, they may act as mutagens [50]. The process of collecting data
and analysis of data about novel antimicrobial compounds should be
done keeping in view of their toxicity and acceptable thresholds for
food consumption.
In addition, the use of naturally derived materials [51, 52] with
antimicrobial characteristics endowed with high potential, not only
preserving food and beverages, but also impart color as well flavor,
thus extending their shelf life and appealing sense [53, 54]. Thus,
various regulating agencies should make laws and ensure that only
those food additives that are of GRAS status should be used; and in
the case, it becomes essential to use some food antimicrobials that
are not recognized as safe (Non-GRAS), the acceptable daily intakes
(ADIs) should be clearly mentioned and should not be exceeded the
limit and recommended quantity.

12.4 ConclusionandFutureOutlook

During these days, there is an increasing demand for natural

preservatives, either derived from animal, plant, or microbial
sources, to be used as food preservatives, to reduce the consumption
 References 287

of synthetic preservatives. There are a number of natural products

being used as bio-preservatives because of their effectiveness and
potent antimicrobial, biocompatible, non-toxic, and ecofriendly
properties. But still there are many unexplored natural sources and
their products that can be used as bio-preservatives. The unexplored
resources open up a large possibility of using these natural compounds
as novel antimicrobials. While natural antimicrobial opens up a large
possibility in the field of food bio-preservation, several factors should
be kept in mind before using a natural substance or its derivative as
food preservative, such as its compatibility and stability with the
target food, effectiveness against the undesirable microbes, safety,
etc. Further while exploring and using natural antimicrobials in food
bio-preservation, these newly explored natural compounds should
not interfere with the original nutritional value of the target food, and
in other words, the traditional value of food should be maintained and
have GARS status as well as effective against a broad range of harmful
microbes. More advance researches should be done to optimize their
processing and application in the field of food bio-preservation.
These advanced researches should be governed by strict laws and
have regulatory approval by concerned authorities, and furthermore
they should be cost effective.

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Chapter 13

Upsurgence of Bio-Based Packaging

Materials: Emphasis on Biodegradable
Plastics as a Greener Alternative

Divya Bajpai Tripathy,a Pinki Chakraborty,a Munesh Sharma,b

and Mohd Yusuf c
a School of Basic and Applied Sciences, Galgotias University, Uttar Pradesh, India
b Department of Chemistry, Faculty of Science,
J.V. College, Baraut, Baghpat, Uttar Pradesh, India
c Department of Natural and Applied Sciences, School of Technology,

The Glocal University, Mirzapur Pole, Saharanpur, Uttar Pradesh, India

[email protected]

In today’s world, there has been an enormous demand for

biopolymers like poly(butyrates) and polylactides, as they find
applications in major industries like pharmaceutical and food
packaging. The actual importance and significance of biodegradable
polymers have emerged, due to the environment-related issues in
the conventional food packing sector, including waste management,
and the way of composting these bio-based materials. The
biodegradability depends on various internal and external factors,
including degradation mechanism, suitability, and level of adoption.
Several sectors involve the use of biotechnology, as it plays an
important role in the treatment processes of different waste
materials. The treatment of hazardous contaminants is a promising
application of this technology, as it is cost effective and can result
in complete removal of hazard materials and their minerals. One

Biomaterials in Food Packaging

Edited by Mohd Yusuf and Shafat Ahmad Khan
Copyright © 2022 Jenny Stanford Publishing Pte. Ltd.
ISBN 978-981-4877-98-5 (Hardcover), 978-1-003-25678-6 (eBook)
www.jennystanford.com
294 Upsurgence of Bio-Based Packaging Materials

of the basic features of biopolymers includes their recyclability

and biodegradable nature. This article is a summary to provide
an overview regarding biodegradable polymers that are based on
bio-based recourses.

13.1 Introduction

From past few decades, many food packaging materials have been
utilized. They can be natural (i.e. wood, pulp, paper, etc.) or synthetic
(i.e. glass, plastics, metals, etc.). Over time, semi-synthetic and
composite materials have been developed with more environment-
friendly characteristics. In addition, these materials not only limited
to food packaging, but also are being utilized in other growing life care
sectors, including cosmetics, personal care, and domestic products
[1]. Many of these polymeric substances possess high stability/non­
biodegradability with less or non-compatibility to the environment.
Also, the huge amount of plastic litters and wastes (microplastics)
are being dumped annually to the environment, which particularly
gives rise to severe health-related problems by the action of food-web
with detrimental effects [2]. Consequently, the global environmental
concerns triggered the minimal usage of synthetic materials for food
packaging applications [3], as they enter to the municipal waste
streams after the end of their usage.
Recycling of these wastes is found another major problem.
According to an estimation, it was observed that during 1950−2015,
only 9% of the plastic-based wastes were recycled [4, 5]. To execute
this major concern, strict rules and regulations have been developed
to use better alternatives to materials produced from non-renewable
resources. In this context, several global regulatory bodies are involved
in setting standards for biodegradable and compostable plastics, for
example, the American Society for Testing and Materials (ASTM), the
European Committee for Standardization (CECS), the British Plastics
Federation (BPF), the US Composting Council (USCC), the American
Certification System of Biodegradable Products Institute (ACS-BPI),
the Environment & Plastics Industry Council (EPIC), and the Japan’s
Green Plaprogram (JGPla) [6].
In the habitat of living beings (land/aquatic), the existence of
plastic-fritters has imposed critical issues, which are being vigorously
exploited by the environmental lobby to demand solutions from the
 Types of Biodegradable Plastics 295

packaging industry. The solutions for the associated problems have

been proposed by scientific community, including incineration,
recycling, composting, and environmental degradation. Out of these
four, the last refers to both photodegradation (attack by photons of
ultraviolet radiation) and biodegradation using microbes (bacteria,
algae, or fungi) [2, 7]. In fact, the diversity of biodegradable materials
and their varying properties makes it difficult to describe so easily.
In this context, a common thought can be drawn as biodegradable
products are all ‘good’ or petrochemical-based products are all
‘bad’ [8, 9]. The chapter provides a literature on exploration toward
biodegradable plastic materials explaining their biochemical
characteristics, and economic viability with future trend and
applicability (Figure 1).

PLA-based Corn-based Cellulose-based

polymers as polymers as polymers as
packaging packaging packaging
materials materials materials
Cofee and tea,
beverages, fresh
salads, cut fruits, Milk chocolates, Cellulose-based kiwi,
organic tomatoes, etc. potato chipps, pasta,
whole fruits, bakery sweets, etc.
goods, potato chipps,
organic poultry, etc.

Companies using bio- Companies using bio- Companies using bio-

plastics as packaging plastics as packaging plastics as packaging
materials materials materials
KLM, Mossberger, Cadberry, Marks and Walmart, Birkel,
McDonalds, Delhaize, Spencers, Coop Italia, Boulder Canyon,
Pepsico, and others Iper supermarkets, and Thornton, and others
others

Figure 13.1 Common biopolymers, packaging applications, and companies

using them as packaging materials.

13.2 Types of Biodegradable Plastics

13.2 Types of Biodegradable
Nowadays, plastics are Plastics
seemingly ubiquitous and their regenerated
products are often used globally by consumers [10]. Chemically,
plastics are synthetic or semi-synthetic organic compounds in origin
that are malleable and can be transformed into a wide range of solid
objects. Commonest utilized plastics are depicted in Table 13.1 with
their broadly significant applications [11−13].
296 Upsurgence of Bio-Based Packaging Materials

Table 13.1 Most common plastics and their significant applications

Type of plastic Abbreviation Application/use

Polyamide or nylon PA Fibrous materials like
toothbrush bristles,
tubing, fishing line, fibers,
ropes
Polyimide PI Adhesives tapes
Polycarbonate PC Security windows,
traffic lights and lenses,
compact disks, eyeglasses
Polyester PES Fibers, threads, textiles
Polyethylene PE A wide range of
packaging and carrier
thin bags, bottles
High-density polyethylene HDPE Strong and thickened
bottles, milk jugs
Low-density polyethylene LDPE Floor tiles, shower
curtains and clamshell
packaging, cheap & light
weight portable furniture
Polyethylene terephthalate PET Transparent drinks
bottles, jars, packaging
films
Polypropylene PP Yogurt containers,
appliances, bottle caps,
drinking straws
Polystyrene PS Disposable cutlery,
cups, plates, CDs &
DVDs, cassette boxes,
plastic tableware, food
containers
High impact polystyrene HIPS Refrigerator liners,
vending cups, food
packaging containers
Polyurethane PU Leather looking
appliances, jackets,
belts, shoes, printing
rollers, cushion, thermal
insulation foams, surface
coatings

(Continued)
 Types of Biodegradable Plastics 297

Table 13.1 (Continued)

Type of plastic Abbreviation Application/use
Polyvinyl chloride PVC Electrical wire/cable
insulation, plumbing
pipes and guttering,
home appliances
Polyvinylidene chloride PVDC Food packaging
containers, strong films
Polyvinyl alcohol PVA Adhesives
Acrylonitrile butadiene ABS Cases for electronic
styrene equipment/appliances
(e.g. computer monitors,
printers, keyboards),
drainage pipes
Polycarbonate+acrylonitrile (PC+ABS) Mobile phone bodies,
butadiene styrene interior and exterior car
parts, etc.
Polyethylene+acrylonitrile PE+ABS Low-duty dry bearings
butadiene styrene
Polyepoxide Pepox Adhesives, potting agents
for electrical components,
matrix agents
Polymethyl methacrylate PMMA Contact lenses,
fluorescent/luminescent
light diffusers, rear light
covers for vehicles
Polytetrafluoroethylene PTFE Heat-resistant and low­
(Teflon) friction coatings, non­
stick surfaces
Phenol formaldehyde PF High modulus and
fire resistant polymer
coatings, thermally
insulation foams
Urea-formaldehyde UF Multi-colorable
alternatives to phenolics,
wood adhesives
Melamine formaldehyde MF Break-resistance
alternatives to ceramic
cups, plates and bowls,
decorated top surface
layer of paper laminates
(Continued)
298 Upsurgence of Bio-Based Packaging Materials
Table 13.1 (Continued)
Type of plastic Abbreviation Application/use
Polyetheretherketone PEEK Strong, chemical & heat-
resistant thermoplastic
moldings, medical
implanting applications,
aerospace moldings
Polyetherimide (Ultem) PEI Used in applications that
require high strength,
heat resistance, modulus
and broad chemical
resistance like making
of electric transmission
components, medical
instruments
Maleimide & bismaleimide MM & BMM High temperature-
resistant composite
materials
Furan resin FR Foundry sands,
biologically derived
composites
Polysulfone P(S) High-temperature
resistant materials like
water heater dip tubes,
membranes, filtration
media
Polydiketoenamine PDK A novel plastic variant
that can be dunked
in acid and reshaped
endlessly (under trial)
Silicone polydiketoenamine SPDKA Cooking utensils,
sealants, base resin for
industrial paints

Nowadays, due to the serious environmental concerns, vigorous

researches are going on to explore sustainable, eco-friendly plastics
that not only will have the negative impacts on the environment,
but also there will be no compromise with the applicability of the
products.
Some of the common bioplastic types, originated from natural
products are as follows [14]:
 Types of Biodegradable Plastics 299

13.2.1 Polyhydroxyalkanoates
Polyhydroxyalkanoates (PHAs) are the types of bioplastics, produced
by microbes like C. necator. Some particular types encompass
poly-3-hydroxybutyrate (PHB), polyhydroxyhexanoate (PHH), and
polyhydroxyvalerate (PHV). PHA is generally biosynthesized through
deprivation of organisms of some nutrients specifically in absence
of phosphorus, oxygen, and/or nitrogen like elements. This can be
attained through excess supply of carbon sources [15].
PHAs can be further divided into short chain length PHAs
(originated from short chain generally 3−5 carbons and produced
by various bacteria including C. necator and A. latus) and medium
change length PHAs (originated from short chain generally 6−14
carbons and produced by P. putida like microbes) [16, 17].

13.2.2 Polylactic Acid
Polylactic acid (PLA) is a type of thermoplastic aliphatic polyester
produced by microbes through fermentation of plant starch like corn,
sugarcane cassava, or sugar beet pulp. In 2010, PLA was reported to
have the highest utilization volume than any of the bioplastics used,
globally. Although as per the American and European standards, PLA
is considered as compostable rather than biodegradable, as it is not
found degradable outside the artificial composting environment [18].

13.2.3 Starch-Based Plastics
Starch blends belong to the class of thermoplastic polymers originated
as starch-plasticizer blends. These are biodegradable, but are not
applicable to all plasticizers, so their biodegradability depends on
the ratio of plasticizers in blends. Some such blends include starch/
polycaprolactone, starch/PLA, and starch/polybutylene-adipate-co­
terephthalate [19].
300 Upsurgence of Bio-Based Packaging Materials

13.2.4 Cellulose-Based Plastics

This class of bioplastics covers cellulose esters and their derivatives
along with celluloid. Cellulose needs extensive modification to yield
its thermoplastic form. Due to high manufacturing cost of cellulose-
based plastics, their exploitation for packaging purpose is not very
much promoted [20].

13.2.5 Lignin-Based Polymer Composites

These bioplastics consist of sustainable, biodegradable, and bio­
renewable natural aromatic polymers. Lignin can be obtained from
the by-product process involves in paper production. Due to its easy
availability, low weight, eco-friendly characteristic over conventional
counterparts, and comparable chemical properties with current
plastic chemicals, lignin-based polymer composites have been
produced in great quantities and are available for exploitation as
emerging eco-friendly polymers [21−23].

13.3 Bioplastics vs. Compostable Plastics

The basic difference between bioplastic and compostable plastic is

that the compostable plastic is a type of plastic that degrades through
biological pathways, and during the process, it releases carbon
dioxide, water, inorganic compounds, and biomass at a rate coherent
with other recognized compostable materials and does not leave any
visually distinct or noxious residues. So, this can be concluded that
all compostable plastics are bioplastics, but this cannot be claimed
in reverse.
Whereas, biodegradable polymers (BDPs) or bioplastics are the
polymeric stuff capable to decompose into carbon dioxide, methane,
inorganic compounds, water, or biomass, predominantly through
enzymatic activity of microorganisms [24].

13.4 Mechanism of Biodegradation

Biodegradation process is classified into three categories, such as

bio-deterioration and bio-fragmentation [24]. In the first stage of
biodegradation, i.e. bio-deterioration, surface degradation starts
  Mechanism of Biodegradation 301

that modifies the physical and chemical properties of materials.

The surface degradation mainly depends on outdoor and abiotic
factors, which involve initial external factors like light, temperature,
and chemical environment. The first and the second stages, bio­
deterioration and bio-fragmentation, are inter-related that is along
with bio-deterioration, the bio-fragmentation process occurs
parallelly. The bio-fragmentation mainly involves undesirable action
of living organisms on manmade materials, involving corrosion of
building materials and metals by microorganisms [23−25]. Aerobic
biodegradation is another important stage for biopolymers, which
generally means breakdown of organic contaminants into smaller
molecules with the release of oxygen. The main function of oxygen
in aerobic oxidation is the conversion of carbon containing species
into carbon dioxide and the rest of the hydrocarbon gets converted
into cell masses; whereas in anaerobic biodegradation, there are
many electron acceptor species, which act as substitutes for oxygen,
like nitrates, sulfates, and iron [26]. Most common electron acceptors
for anaerobic degradation are transition metals and even carbon
dioxide in some cases [27]. The anaerobic process is used for treating
wastewater with high concentrations of biodegradable organic
materials, such as concentrated domestic wastewater, biosolids,
animal manure slurry, and food processing wastes [25]. The overall
overview of the main stages of the degradation process is represented
in Figure 13.2.

• Microorganisms
• Enzymes (extracellulars)
PHASE-1

• Adherence to surface of polymer

• Cleavage of polymer bonding
PHASE-2

• Biodegradation
• End products
PHASE-3

Figure
Figure13.2 Flow
13.2 Flowchart of the
chart of thebiodegradation
biodegradation process.
process.
302 Upsurgence of Bio-Based Packaging Materials

13.5 Factors Influencing Biodegradation

13.5.1 External Factors

13.5.1.1 Physical parameters
Physical parameters play noteworthy impact on biodegradation of
bio-based food packaging materials. The parameters like polarity of
surface area, molecular weight, melting point, and elastic behavior
of polymers impart tremendous impact on the biodegradation of
the materials. Generally, branched chain polyesters degrade less
conveniently than the linear ones [7]. Furthermore, the morphological
properties of biopolymers influence greatly to the biodegradation rate.
Similarly, the melting temperature of the biopolymers also has great
impacts on the enzymatic or microbial polymer degradation. Higher
the melting point of the biopolymer, lower will be its degradation
[20, 23, 24]. Aliphatic polyesters with esters and/or polycarbonates
linkage are the polymers that have great assessments to be exploited
as bioplastics. This is because of their vulnerabilities to microbial and
lipolytic enzyme degradation. In this series, the aliphatic polyamides
and polyurethanes were claimed to be relatively less susceptible to the
degradation, as compared to aliphatic polyesters and polycarbonates,
due to their higher Tm (temperature of melting) values.

13.5.1.1.1 Moisture or water content

Moisture or relative humidity presents in the environment also leads
to the significant change in the rate of polymer biodegradation. It is
a well-known fact that water is essential for the development and
propagation of almost every microbial species [28].
Increase in moisture content presents in the environment raises
the activity of microbes, thus increases the rate of biodegradation
of polymers. Ho et al. disclosed that there was sharp increase
in the degradation rate with the rise in relative humidity of the
surroundings [27].

13.5.1.1.2 Temperature
Temperature is one of the most vital parameters that influences
the polymers degradation remarkably [29]. It is claimed that
 Factors Influencing Biodegradation 303

degradation of most of materials is almost impossible in the absence

of suitable temperature, as the extension of optimum temperature
for biodegradation is a reaction-specific modality. Generally, the
hydrolysis rate and the microbial activity increase with the rise in
temperature; but at an extended high temperature, the microbial
activity reduces and even can be halted [30, 31].
Usually, the activity rate of microbes increases with
temperature, since at a certain temperature range, the microbes
start dying. Same trends were obtained in another study, in which
the biodegradation of bioplastics has been studied by burying 0.5
g of each bioplastic sample in 30 g of normal soil. Same procedure
has been adopted for blank, where same amount of sterile soil has
been taken as control [32].

13.5.1.2 Chemical parameters
pH also plays an important role in the biodegradation of
biopolymers. Its type specifically depends on the reaction type. pH
value can alter the hydrolysis reaction rate as well as propagation of
microorganisms [28]. Hayakawa et al. (2014) revealed a progressive
relationship between enzyme activity of cellulose and pH that
leads to the conclusion that low pH value decreases the cellulose
degradation [33].

13.5.1.3 Environmental parameters
Besides the chemical composition and crystallinity, biodegradation
of biopolymers is also influenced by various environmental factors.
The illustration of “readily degradable” sugars can exist as such in soil
organic matter (SOM) for longer period even for centuries; whereas,
“intractable” lignin turnover can be somewhat more [34]. Climate can
also determine the rate of degradation. In contrast, Prescott (2010)
[35] published a review paper, encompassing 70 researches, in which
he revealed that carbon-to-nitrogen ratio had greater impact on
the decomposition rate. In this study, it has also been claimed that
the impact of climatic variations, due to global alterations on the
microbial cleavage, is probably to be little; until or unless the change
is modified or manipulated related plants species [36, 37]. In this
way, the plant species type is the utmost significant parameter to
determine the decomposition of biopolymers.
304 Upsurgence of Bio-Based Packaging Materials

13.5.2 Internal Factors

13.5.2.1 Composition

In addition to the other factors, composition of bioplastics also plays

a vital role in their decomposition. For instance, due to the chemical
structure and chemical composition, PHA shows tremendous
biodegradability [38, 39]. Its capability to degrade in natural
environment enables it to get listed in bioplastics. Microorganisms
on the degradation of PHA secrete extracellular enzyme, PHA
depolymerase. Besides this, chemical additives also influence the
biodegradation of PHA in a positive manner. Addition of chemical
additives has great impact on the degradation of PHA on both the
chemical scale and physical scale by inhibiting enzymatic cleavage.
In addition, non-degradable chemicals like co-polyesters subsidized
the area available to the interaction of enzymes and biopolymers.
For example, chain extenders and anti-fouling agents that are the
best-known used chemicals influence the biopolymer degradation
by reducing the extracellular enzyme activity or by minimizing the
availability of surface area to microorganisms to produce biocatalysts
[35]. Moreover, the microbial degradation of polyethylene decreases
reciprocally with the molecular size. Linear paraffin molecules
with less than or equal to molecular size of nearly 500 Da can be
easily degraded through various microbes [40]. In the same way,
microbial degradation of starch−polyethylene blend and their
chemically modified blends has been examined [41]. Result of this
study revealed that the removal of carbon from the blend of starch
and polyethylene was relatively low, comparing to the pure form of
starch. Same result has been concluded for linear low-density blend
of polyethylene with starch in the soil. Outcome of a simultaneous
biodegradation study on the cellulose, polycaprolactone (PCL) and
starch blend, and aliphatic–aliphatic co-polyester reflected that
cellulose was more rapidly degrade than PCL-starch blend, which
was consequently more degradable over co-polyester [42]. In
the same way, PVA blends-based films were claimed to have very
promising biodegradation properties [43].
  Economic Aspects 305

13.5.2.2 Crystallinity
Polymeric structure is indissolubly associated with crystallinity
impact and is also related with the effectiveness of biodegradability
[38, 41]. Final sample crystallinity of the polymer is also influenced
by the processing techniques of polymers, which also alter the
solvent casting and quenching like parameters [44]. For instance,
the biodegradation of PHA starts with the rise in mass losses and
intermolecular phase erosion on the sites of disordered chains prior
to the samples of well-ordered crystalline regions. On contrary,
amorphous area allows moisture and enzymes to enter into the active
site and results in increasing microbial degradation. This is due to the
more availability of surface area [45]. In case of PHA and PHB, due
to the greater extendibility to crystalline forms, less degradability
is expected.

13.6 Economic Aspects

The biodegradable polymers are widely used in the packaging

industry, and there are no mandatory regulations for customers
when it comes to the use or post-customer treatment.
The increasing urge for product improvement has opened up
new doors for packaging segments, such as cellulose products and
PLAs for packaging-related applications [46, 47]. The increasing
usage of biodegradable polymers in the packaging and medicinal
industries has enormously increased their productivity and these
are used widely in the preservation of food items [48]. Moreover,
from economic perspective, these biodegradable materials find their
applications in the chemical industry, as useful building materials.
Among all biodegradable materials, the demand for PLAs is
constantly increasing, as these are greener in nature, renewable, and
biodegradable products, which are resulting in constant growth over
the years of the production and innovation units [40, 44]. However,
one of the limitations of biodegradable polymers is that they are
expensive, and thus it is important to make them cost-effective.
Moreover, from both psychological and economic perspectives,
the research achievements in this area have resulted directly
306 Upsurgence of Bio-Based Packaging Materials

or indirectly in effective legislations, manufacturing practices,

directives, and sustainable cycles based for packaging procedures
[49]. The increased awareness and consciousness among the people
regarding the significance of recyclable and biodegradable polymers’
usage have also led to the enhancement in the economic aspects
of polymers. In most of the recent studies, it has been prioritized
that most of the USA and Canada customers generally are involved
in buying biodegradable household products rather than other
commercial goods and commodities. So, from economic perspective
till date, most of the uses of biodegradable polymers have been in
the field of fiber and non-fiber packaging; and in recent times,
these biodegradable polymers and plastics are combined with non­
renewable materials to be used in the production of oil-based plastic
materials [41, 48, 49].

13.7 Industrial Aspects

Due to the increasing environmental pollution levels and rising uses

of biodegradable polymers, these materials have gained a lot of
importance in the automobile, agricultural, and medicinal industries
[42]. Biodegradation of automotive waste, such as polyester and
polyurethane foam, can take place by using Pseudomonas chlororaphis
[50]. In these industries, majorly of biodegradable polymers are
used for the conversion and production of less toxic and harmful
environmental species. Moreover, plastic pollution has become one
of major concerns all over the world, which has ultimately resulted in
increasing demand for biodegradable polymers [47].
PHA and PLA are the two most promising biodegradable
polymers. The PHA is price-competitive and offers a challenge for
some commercial petroleum-based plastics. Whereas, the PLA has
already replaced a number of non-biodegradable polymers in the
food packaging and carrier bag markets, but its biodegradation is still
much slower than those of other biodegradable polymers. However,
in terms of properties and usability for certain applications, a very
few commercial non-biodegradable polymers can be replaced by
known biodegradable polymers. It is, therefore, possible to only
slightly reduce the current environmental problems by using known
  Conclusion and Future Outlook 307

biodegradable polymers for some low-level applications. Thus, a lot

of researches are still needed to develop biodegradable polymers or
polymer blends that will have the necessary properties to replace
most of the current non-biodegradable polymers [47−50].

13.8 Conclusion and Future Outlook

This review has covered mainly the biodegradation chemistry

and degradability studies. The influence of polymer chemistry on
environment can be both positive and negative, and can also result
in different environmental issues. This factor has been the driving
force for the wide area of researches on renewable resources and
their applications. Composting with organic wastes is one of the
major ways to enrich soil and also increases the soil longevity and
stability. This article reveals that the use of biodegradable polymers is
beneficial for both environment and industries. Therefore, in respect
to other polymers, the use of biodegradable polymers is of utmost
importance from commercial perspective.

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 Index

α-lactalbumin 140, 194 antimicrobial agents 51, 53,

acceptable daily intake (ADIs) 30, 56, 58, 85, 107, 115, 147,
192–193, 236, 262
286
antimicrobial food packaging
acetic acid 91, 192, 284–285
system 129
active agents 24–26, 55, 257
antimicrobial packaging 129, 237
active biopackaging 55 antimicrobial properties 8, 114,
active component 23–25, 52 129, 236, 275, 284
active finishing 196, 219–220, antimicrobials 6–7, 18, 28–29, 53,
222, 224, 226, 228 56, 60, 115, 125, 130,
196–197, 233, 236, 241,
active finishing agents 276–277,
261–262, 266, 280, 283, 285
279, 281, 283
natural 31, 150, 276, 286–287
active packaging materials (APMs)
84–85, 114 antioxidant activity 145, 148–149,
197
ADIs, see acceptable daily intake
antioxidant agents 197, 263
adsorption, physical 26–27
antioxidant compounds 130, 258,
agri-food products 234 262–263
agriculture 1, 138, 195, 219 antioxidant finishing enabled
agro-polymers 3–4 packaging 258, 260, 262,
264, 266, 268
alginate-based coatings and films
149 antioxidant properties 127, 224,
262–263, 265–266
alginates 4, 27, 54, 65, 90, 144,
antioxidants 6, 18, 28, 50–51,
149, 181, 183, 198
56, 61, 69–70, 85, 115, 127,
sodium 144, 146 196–197, 200, 241, 257,
structure of 65 261–265, 267–268
amino acids 4, 69, 109, 191, 198, natural 257, 263–266, 268
277–278, 281 synthetic 197, 257, 263–264,
antibodies 93–94, 225 268
APMs, see active packaging
antimicrobial activity 197, 220,
materials
237, 260, 277, 282–283, 286
ascorbic acid 260, 263, 265, 284
314 Index

β-lactoglobulin 140, 194 biodegradable films 50, 53–54,

Bacillus cereus 143, 279–280 138, 141, 160–161, 192, 200
biodegradable materials 10, 34,
bacteria 65, 114, 225, 238, 245,
57, 191, 295, 305
275–280, 283–285, 295, 299
starch-based 160
food-spoiling 283–284
biodegradable organic materials
bacterial cellulose (BC) 2, 113, 301
183–184, 195
biodegradable packaging 34, 200
bacteriocins 66, 277–278, 280 biodegradable plastics 33, 293,
bacteriophages 275, 278–279, 295, 297, 299
283–284 biodegradable polymers packaging
baked products 59, 63, 279 33
barrier properties 18, 34, 105, biodegradable products 295, 305
109, 111–113, 163, 169, 176, biodegradation 9, 32, 105, 114,
221–222, 246, 267 193, 242, 295, 300–303, 306
gas 111–112 factors influencing 301–303
beverages 125, 222, 245, 282, biological processes 8–9
285–286, 295 biomass 1, 3, 9, 32, 50, 105, 107,
128, 183–184, 300
bio-based materials 112–113, 184,
227, 293 biomaterial-based packaging 3,
29, 31
bio-based packaging materials
biomaterials
268, 293–294, 296, 298, 300,
302, 304, 306 biodegradable 33
categories of 3, 5, 7
bio-deterioration 300–301
degradation of 8–9, 11
bio-fragmentation 300–301
disadvantages of 8
bio-nanocomposites 143, 268
thermoplastic 19
bio-plastics 295
bioplastics 106, 111, 113, 145,
bio-preservatives 276, 279, 287 199–200, 299–300, 302–304
biodegradability 22, 32–33, 106, biopolyesters 3–4, 8, 10, 12, 16,
110, 114, 145, 191, 198, 243, 34, 107, 109–110
293, 299, 304–305 biopolymer hydrocolloids 261
biodegradable 1, 10, 32–35, 50, biopolymer packaging 261, 263,
53–54, 57, 60, 65, 67, 69, 265
105–106, 110–111, 116, 130, biopolymeric matrix 192–193
138, 140–142, 150, 160–161, biopolymers 51, 57, 105–109,
181–187, 191–196, 198–200, 111–114, 116, 130, 182–183,
242–243, 246, 257, 268, 282, 185–186, 191–192, 198,
293–295, 297, 299–301, 200, 243, 262, 267, 293–294,
305–307 301–304
 Index 315

biodegradation of 303 235, 240, 243–244, 258, 261,

carrageenan 189 267, 295, 300, 303–305
categories of 183 carboxymethyl 108, 187

functional 105–106, 108, 110, ethyl 108

112, 114, 116 nanofibrillated 258
natural 183 structure of 58–59
sources of 182–183 cellulose acetate (CA) 16, 108, 187

biosensors 93–94, 129 biodegradable 34

cellulose-based coatings and films
biotechnology 83, 162, 293
147
BPF, see British Plastics Federation
cellulose degradation 303
British Plastics Federation (BPF)
cellulose derivatives 4, 34, 59,
294 187, 261
cellulose esters 261, 300
CA, see cellulose acetate cellulose fibers 58, 108
carbon 9–10, 184, 245, 299, 301, cellulose micelles 243
304 cellulose nanocrystals 22, 143,
carbon dioxide (CO2) 2–3, 9, 16, 147, 244
32, 50–51, 57, 70, 85, 89–91, chitin 15, 60–61, 147, 187–188,
95–96, 107, 111, 114–115, 264
125, 131, 141, 150, 188, 199, chitosan 27, 29, 54, 57, 60–61, 88,
223, 241, 245, 300–301 143–144, 146–149, 183–184,
carrageenan 4, 147, 189 187–188, 200, 264, 283
chemical structure of 189 structure of 60
casein 107, 109, 140, 181, 183, chitosan coating 147
191, 198, 261, 264 chitosan films 147, 188, 283
cassava starch 159, 161–162 chitosan nanobiofilm (CN) 61, 127
cassava starch nanocomposite
CN, see chitosan nanobiofilm
films 162, 165, 168–171,
173–175 CO2, see carbon dioxide

cassava starch-zinc nanocomposite coatings

film 159–162, 164, 166, alginate-based 150
168, 170, 172, 174, 176
biodegradable 138
casting 17–19, 159, 162, 185–186
cellulose 51
cell walls 114, 278, 280, 282–283
gelatin-based 144
cellulose 2–4, 16, 22, 27, 34, 51,
polysaccharide-based 57, 139
54, 58–59, 106–108, 113,
143–145, 147, 181–184, starch-based 145
186–187, 192, 195, 200, 222, whey-based 140–141
316 Index

collagen 4, 67, 143–144, 183, 194, endolysins 279–280

198, 200, 261 enterocins 277, 279
corn 62–63, 108, 149, 183, 185, Escherichia coli 94, 140, 143–145,
299 151, 192–193, 239, 277,
corn starch 63, 145, 161 279–282, 284
European Food Safety Authority
dairy products 264, 281–282, 284 (EFSA) 30–31
degradation 5–7, 9–10, 27, 96,
114, 160, 191, 198, 226, 238, FAO, see Food and Agriculture
245, 301–303 Organization
microbial 304 FDA/USFDA, see U.S. Food and
denaturation 19–20 Drug Administration
diffraction 175–176 Food and Agriculture Organization
(FAO) 32
food bio-preservation 275–276,
EC, see edible coating
278, 280–282, 284–287
edible coating (EC) 15, 31, 49–54,
food coatings 6, 14, 184
56–68, 70–72, 130, 137–140,
142–144, 146–152 food containers 246, 296
edible film (EF) 15, 51–55, 57–58, food hydrocolloids 183
70–71, 112, 130, 137–145, food industry 1, 26, 28, 32, 57,
147, 149–150, 175, 184, 188, 60–61, 65, 67–69, 71, 84,
196–200, 261–263, 265 98–99, 121, 129, 137–139,
biodegradable 138, 140 147, 183–184, 186, 189, 200,
234–235, 244–246, 258, 261,
edible films
263, 265–266, 268, 282, 285
properties of 197
food nanomaterials 32
protein-based 139, 141, 143,
food nanotechnology 234
198
food packaging
edible films and coatings 130,
137–139, 141, 143–145, 147, bio-based 221, 227, 301
149–150, 175, 196 biomaterial-based 3
polysaccharide-based 144–145, biomaterials for 1–2, 4, 6, 8, 10,
147, 149 12, 14, 16, 18, 20, 22, 24, 26,
EFSA, see European Food Safety 28, 32, 34–36, 49, 83, 105,
Authority 121, 137, 159, 181, 219, 233,
257, 275, 293
electrospinning 2, 23–26, 240
food packaging industry 66, 97,
core-shell 23, 25
111–113, 195, 220, 233, 239,
emulsion 23, 25 242, 258, 267, 269
 Index 317

food packaging materials 1, 16, 21,

gellan gum (GG) 15
87, 110, 112, 125, 130–131,
gels, fragile 189–190
166, 220, 235, 242, 258, 266,

generally recognized as safe

294

(GRAS) 30–31, 51, 281–282

food packaging products 33, 236

GG, see gellan gum

food-packaging techniques 106

glycerol 140–143, 145, 147,

food preservation 66, 123, 241,

159–160, 162–163, 167,

277, 279, 281, 283–285

169–176, 191–192, 240

food preservatives 285–286 grapefruit 138–139, 192, 265

food processing 95, 123–124, 129,
GRAS, see generally recognized as

176, 236
safe

food processing wastes 301

food quality 83–87, 97, 114, 116,
hemicellulose 3, 195

121, 123, 126, 137–138, 182,

human body 227–228

234–235, 246

humidity 9, 16–17, 111–112, 224,

food spoilage 33, 127, 238,

226

281–282

food storage 61, 259

immobilization, chemical 26–27

food supply chain 85, 94, 97, 239

intelligent devices 85, 93, 98

food wrapping 234–235, 259

intelligent packaging materials

fossil-based biopolymeric blends

(IPMs) 85, 131

199

intelligent packaging systems 83,

fruits 28, 49, 51–52, 56–58,

85, 87, 100, 238

69–70, 92, 131, 138–139,

144, 147–150, 199, 225, 237,

intelligent packaging techniques

245, 260–261, 263, 280, 284,

(IPT) 86–87, 89, 91, 93–95,

295
97, 99–100

coated 149
IPMs, see intelligent packaging

materials

fresh 70, 131, 138–139

IPT, see intelligent packaging

fresh-cut 224–225

techniques

uncoated 147–149

functional/active packaging
114–115 κ-carrageenan 189

keratin 191, 193, 198, 200, 261

gas concentration indicators keratin protein 193

99–100
gas indicators 87, 89–90 lactic acid 8, 30, 34, 91, 109, 183,

gelatin 4, 19, 21, 29, 67–68, 109,

284–285

141, 143–144, 181, 183,

lacticin 281

191–192

gelatin films 262

318 Index

LDPE, see low-density polyethylene monocytogenes 143, 151,

Listeria monocytogenes 149, 151, 192–193, 279–284
279 monomers 8–9, 23, 31, 105, 107,
low-density polyethylene (LDPE) 110, 182, 189, 195
13, 17, 110
luminescence sensors 93 nano-biocomposite materials
233–234, 236, 238, 240, 242,
244, 246
MAP, see modified atmosphere
applications of 233–234, 236,
packaging
238, 240, 242, 244, 246
mayonnaise 264–266 nanocellulose 243–244, 267
meat 28, 58, 91, 140, 142–143, nanoclays 30–32, 235
151, 197, 260, 264, 281–282
nanocomposites 21–23, 30, 141,
meat products 91, 144, 263, 265, 159, 163, 234–235, 238,
279, 284 241–243, 267–268
metabolites 275–276 biodegradable 242–243
methylcellulose 147, 187 nanocrystal systems, polymer
microbes 1, 10, 91, 109, 114, 123, matrix-based 243, 245
129, 138, 150, 223, 235, 239, nanofibers 23, 25–26, 222, 267
241, 277, 283, 287, 295, 299, cellulose 147
302–304
surface loading of 23, 26–27
food-spoiling 283–284 nanofibrillated cellulose (NFC)
spoilage 125, 128–129, 184, 239 258, 267–268
microbial activity 144, 303 nanofilms 24, 238
microbial growth 87, 89, 91, nanomaterials 29–32, 128–129,
128–129, 197, 237 197, 219–228, 233–234,
microorganisms 4, 8–11, 50, 60, 236–238, 241–242
66, 88, 105, 107, 110–111, cellulosic 243
114, 116, 130, 183, 192–193, nanoparticles 8, 18, 29–31, 129,
195, 245, 276, 281, 300–301, 159–163, 167, 170, 173, 176,
303–304 227–228, 236, 239, 241–242,
food-spoiling 279–280 244–245, 267

modified atmosphere packaging silver 236–237

(MAP) 96, 123, 130–131 nanosensors 129, 219, 223, 235,
237, 239, 246
moisture barrier 55–56, 58, 113
nanotechnology 29, 31–32,
moisture barrier property 113
128–129, 219–220, 223, 227,
moisture loss 58, 63, 115, 233–239, 241, 246, 267
148–149
natamycin 282–283
molds 148, 162, 276, 281, 283
 Index 319

NFC, see nanofibrillated cellulose pectin-based coatings 149

nisin 143, 193, 277, 281–283 pectin-based films 148
pediocins 278–279, 282
organic acids 56, 91, 282, 284– permeability 7, 13–15, 53, 55, 95,
285 113, 163–164, 166, 169, 282
oxidation 56, 114–115, 127, 197, PGA, see poly(glycolic acid)
222, 246, 257, 262–266 PHA, see polyhydroxyalkanoate
oxygen 2, 10, 16, 55, 64, 85, 111, photonic crystals 226
115, 131, 160, 164–167, 184, PLA, see poly-lactic acid
192, 198–199, 223, 235–238, plastic films 222, 235
240, 259–260, 263, 299, 301
plasticizers 17–19, 27, 55, 58, 106,
oxygen permeability 16, 55, 141, 108, 139–140, 145, 161–162,
144, 164–169, 188, 246 198–199, 262, 299
oxygen scavengers 107, 115, plastics 2, 13, 16–17, 53, 105–106,
259–260 116, 182–183, 191, 199–200,
oxygen scavenging 29, 237, 259 224, 258, 294–298, 300, 306
oxygen sensors 223, 239–240 cellulose-based 300
synthetic 1–3, 8, 10, 12–13,
15–16, 28, 30, 33, 35
packaging, bioactive 261
poly-lactic acid (PLA) 8, 10, 12,
packaging films 14–15, 20–21, 29,
16, 27, 29–30, 34, 106–107,
34–35, 113, 141, 284, 296 109–110, 112, 130, 183–184,
packaging materials 243, 262, 282, 299, 305–306
bio-based 302 poly(glycolic acid) (PGA) 8, 10
biodegradable 50, 69, 142, 194 polybutylene succinate (PBS) 34
functional 181 polycaprolactone/poly(ɛ-
multilayer 53 caprolactone) (PCL) 8, 10,
12, 34, 184, 244, 299, 304
synthetic 1
polycarbonates 14, 296–297, 302
pathogenic bacteria 139, 142–143,
polyester 14, 113, 181, 183, 296,
284
306
pathogens 94, 223, 226, 235, 237,
polyethylene 2, 13, 17, 110, 112,
239, 245, 258, 280, 282
296–297, 304
PBS, see polybutylene succinate
polyethylene films 197, 237
PCL, see polycaprolactone/poly(ɛ- polyhydroxyalkanoate (PHA) 2,
caprolactone) 8, 10, 17, 29, 107, 110–111,
pea protein isolate (PPI) 282 183–184, 195, 262, 299,
pectin 4, 63–64, 140, 144, 146, 304–306
148–149, 183, 198
320 Index

biodegradation of 304–305 natural 127, 276, 286

degradation of 304 printing 2, 13, 27–28
polyhydroxyalkanoates (PHA) 2, printing technology 27–28
17, 107, 184, 262, 299 protein-based films 109, 139, 144
polylactic acid 2, 17, 106, 184, proteins 1, 3–4, 20–21, 53–55, 62,
243, 262, 282, 299 65–67, 69, 106–107, 109,
polymer films 21, 95 137, 139, 143, 160, 181,
polymer packaging films 94, 283 183–184, 191–195, 198, 200,
261–262, 277, 281
polymers 3–5, 9–11, 13, 18–22,
29, 33–35, 50, 53, 56, 62, 94, fibrillar 143

105–107, 110, 112–113, 116, globular 139–140, 191

127, 144, 170, 182–185, 191, potato 139–140

193, 195–196, 199–200, 220,
pullulan 4, 58, 64–65, 181, 183,
227, 235, 237, 241, 244, 246,
188, 193
262, 293–295, 299–300, 302,
305–307 structure of 64

bio-based 107, 184

biodegradable 33–35, 50, 67, QACCP, see Quality Analysis and
106, 110, 193, 200, 246, 293, Critical Control Points
300, 305–307 QDs, see quantum dots
synthetic 10–11, 13–15, 110, Quality Analysis and Critical
170, 183–184, 193–196 Control Points (QACCP) 126
polyolefins 13, 243 quantum dots (QDs) 225–226
polypropylene 2, 16–17, 110, 195,
296 relative humidity (RH) 28,
polysaccharide 1, 3–4, 21, 53–54, 163–165, 194, 226, 302
56–58, 60, 63–65, 107–109, reuterin 281–282
137, 139, 144–147, 149–150,
RFID systems 98
160, 181, 183–185, 187–190,
242–243, 261, 264 RFID tags 98–99

polysaccharide-based films 109, RH, see relative humidity

137
polystyrene 2, 17, 110, 112, 243, sakacins 280
296 seafood 264, 280
PPI, see pea protein isolate sensors 28, 84, 86–87, 92–96, 100,
preservatives 125, 130, 223, 236, 129, 235, 239

285–286 electrochemical 93

 Index 321

shelf life 28, 50, 56–57, 64, 71,

thermoforming 19–20

83–85, 100, 106, 111–113,
thermoplastic films 159, 171,

122–125, 128, 131, 137–138,

175–176

143, 147–150, 166–167, 189,

thin films 94

196–197, 220, 222, 227, 233,

236, 239, 259–260, 262, 264,

time temperature indicator

268, 275, 284–286

(TTIs) 88–89, 99–100, 128,

239–240

silver 236, 238, 245, 260

TiO2 nanoparticles 237, 240

simple temperature indicator (STI)
88
tomatoes 138–139, 149, 161, 261

smart-food packaging 28–29

TTIs, see time temperature

indicator

biomaterial-based 28

smart interactive active packaging
28
UCNPs, see upconversion

fluorescent nanoparticles

snacks 222, 264

upconversion fluorescent

soy protein 4, 19, 109, 142–143,

nanoparticles (UCNPs) 226

183, 191, 261

U.S. Food and Drug Administration

soy protein isolate (SPI) 142–143,

(FDA/USFDA) 31, 33–34,

191

51, 111, 241

SPI, see soy protein isolate
spices 115, 260, 264, 268, 276

vacuum packaging (VP) 123

Staphylococcus aureus 140, 143,

vegetables 16, 28, 49, 89, 131,

145, 151, 193, 279–282, 284

138–139, 141, 150–151, 161,

starch 4, 8, 19–21, 27, 29, 34, 54,

259–261, 265, 267

62–64, 68, 106–108, 130,

shelf life of 58, 144, 237, 245

144–146, 160–163, 181,

183–185, 195, 200, 243, 261,

vitamins 69, 149, 224, 234–235,

299, 304
264–265

starch blends 17, 161, 299, 304

VP, see vacuum packaging

STI, see simple temperature

indicator
wastewater 301

strawberries 144, 147, 149–150,
water vapor 55, 69, 150, 160,

263, 265
163–164, 166–167, 169, 176,

structural matrix 51, 53

246

sustainable packaging 34, 130

water vapor permeability 16, 139,

141, 144–145, 147–148, 163,

166–168, 176, 188, 194

thermochromatic inks 99–100
322 Index

wheat 63, 141–142, 183, 185, 191,

whey protein isolate (WPI) 141,

199
282

wheat flour 59
WPI, see whey protein isolate
wheat gluten 19, 109, 141–142,

183, 198–199, 261

xanthan 2, 4, 183, 189–190

whey 109, 140–141, 183–184,

chemical structure of 190

191, 264

xanthan gum 190

whey protein 4, 19, 140–141, 190,

194, 200, 282

zinc nanoparticles 161, 167,

whey protein films 194

169–171, 175–176