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Active and intelligent biodegradable packaging films using food and food waste-
derived bioactive compounds: A review

Nitya Bhargava, Vijay Singh Sharanagat, Rahul S. Mor, Kshitiz Kumar

PII: S0924-2244(20)30605-1
DOI: https://doi.org/10.1016/j.tifs.2020.09.015
Reference: TIFS 2959

To appear in: Trends in Food Science & Technology

Received Date: 5 July 2020

Revised Date: 8 September 2020
Accepted Date: 19 September 2020

Please cite this article as: Bhargava, N., Sharanagat, V.S., Mor, R.S., Kumar, K., Active and intelligent
biodegradable packaging films using food and food waste-derived bioactive compounds: A review,
Trends in Food Science & Technology (2020), doi: https://doi.org/10.1016/j.tifs.2020.09.015.

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 Active and intelligent biodegradable packaging films using food and food
waste-derived bioactive compounds: A review

Nitya Bhargavaa, Vijay Singh Sharanagata,*, Rahul S Mora,*, Kshitiz Kumarb

a
Dept. of Food Engineering, National Institute of Food Technology Entrepreneurship and
Management, Sonepat, India
b
Dept. of Food Processing Technology, A. D. Patel Institute of Technology, New Vidynagar,

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Gujarat, India
[*Corresponding authors, Email: [email protected] (VSS),

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[email protected] (RSM)]
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(Co-author’s Email: [email protected], [email protected])
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Authors contributions
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Nitya Bhargava studied the literature and drafted this manuscript; Rahul S Mor monitored and
directed the manuscript preparation; Vijay Singh Sharanagat, Kshitiz Kumar supervised the
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framework and content. The final edited manuscript was proofread and accepted by all the
authors.
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Declaration of competing for interest

The authors declare no conflict of interest.

*
Corresponding authors address
Dept. of Food Engineering, National Institute of Food Technology Entrepreneurship and
Management, Sonepat, India.
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1 Active and intelligent biodegradable packaging films using food and
2 food waste-derived bioactive compounds: A review
3

4 ABSTRACT
5 Background
6 The growing environmental concern of plastic packaging disposal has led to the innovation of
7 biodegradable biopolymers. Consumer demand and health concern further necessitate the

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8 emergence of active and intelligent packaging system to monitor the quality of packed food.
9 Whereas, the use of chemical dyes as an indicator in smart packaging is not suitable for food

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10 packaging because of their high toxicity and harmful effects on human health and the
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12
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environment. Hence, the researchers are focused on natural pigments derived from plants and
food waste as indicating substance in biodegradable packaging and also for the valorization of
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13 food waste.
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14 Scope and Approach

15 This paper summarizes the research on the utilization of naturally derived food- and food waste-
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16 based pigments (anthocyanins, curcumin, betalains, carotenoids, chlorophyll, brazilin, quercetin,

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17 etc.) with biopolymeric matrices (starch, cellulose, chitin, gums, agar, etc.) to fabricate “smart
18 biodegradable films”, for effective monitoring of spoilage and quality of meat products, seafood,
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19 milk, and others.

20 Key Findings and Conclusions

21 The results show that the smart packaging material developed by the biopolymers with plant-
22 based pigment has the potential to replace the traditional plastic packaging materials. The
23 extracted from food and food waste act as an indicator in smart packaging and promotes the
24 valorization of food waste. The biodegradable packaging is economical, safe, non-toxic,
25 sensitive, and natural pigments act as a quality indicator in packaging systems. Further, these
26 packaging films can be optimized and commercialized and to be employed as active and
27 intelligent packaging for visual quality evaluation of fresh food products.

28 Keywords: Active packaging; Intelligent packaging; Food waste; Bioactive compounds

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29 1. Introduction
30 Food packaging performs three basic functions: containment, preservation of quality, and
31 protection from environmental, physical, and microbiological factors (Barska & Wyrwa, 2016;
32 Ghaani et al., 2016). In recent times, the role of packaging has increased beyond its basic
33 function with changing consumer preferences and expectations. Now, it is also contributing
34 towards extending the shelf life and acts as a quality indicator of the packed food products. The
35 focus is also on the development of more interactive packaging systems, and are classified as
36 active and intelligent packaging (Dobrucka & Cierpiszewski, 2014). In active packaging,
37 deliberately added materials (absorber or emitters) interact with the inner environment of the

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38 package to enhance the shelf life of the food. Whereas, in intelligent packaging, deliberately

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39 added materials interact with the packaging environment and monitor the state (storage time,
40 temperature, shelf life, etc.) of the packaged food products (Commission Regulation (EU)
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41 450/2009). These can detect and provide an alert on spoilage or any potential problem in
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42 packaged food, termed as ‘Smart Packaging’ and ‘Clever Packaging’ (Yam, 2012; Ahvenainen
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43 & Hurme, 1997). These systems act as quality indicators to ensure food safety (Zhai et al., 2017)
44 and are broadly classified as direct (humidity, time-temperature, freshness and damage, and
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45 biosensor) and passive (traceability and tracking) indicators (Dobrucka & Cierpiszewski, 2014).
46 The variation in the qualitative information provided by these indicators varies due to chemical
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47 reactions or microbial growth with time and processing. The reaction between the metabolites
48 generated due to microbial growth and indicator substances provides visual indication and
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49 information regarding deterioration or quality of food (Fang et al., 2017).

50 Plastic polymer materials are widely used for packaging due to their flexibility for molding, low
51 cost, good printability, and good resistance against different environmental and mechanical
52 factors. However, these packaging materials pose a burden on the environment as these take
53 years to degrade and pose a risk of releasing chemicals that may render the quality of food
54 (Horodytska et al., 2018). Hence, the environment and health concern promote to use
55 biodegradable packaging in place of plastic packaging. Now, these days naturally derived
56 biopolymers, including protein, lipids, and polysaccharides, are commonly used as the base
57 materials for biodegradable packaging. These are recyclable, decompose in a short period, non-
58 toxic, and environment friendly (Zhang et al., 2020; Ma & Wang, 2016; Mohammadalinejhad et
59 al., 2020; Talukder et al., 2020; Yao et al., 2020).

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60 Numerous synthetic pigments and dyes are used in developing smart packaging systems, such as
61 chlorophenol, cresol and methyl red (Dong et al., 2008), bromocresol green (Pacquit et al.,
62 2007), bromocresol blue (Andreou & Clonis, 2002) and xylenol (Soliman et al., 2016). These
63 compounds may be potentially toxic and mutagenic, which may be released from the packaging
64 material and thus are unsuited for food packaging (Zhai et al., 2017). Hence, recent research
65 focuses on the incorporation of naturally derived pigment from plant products and food wastes,
66 which are readily available, non-toxic, economical, sensitive, safe, reliable, fast, non-destructive,
67 and non-invasive (Kuswandi et al., 2012). Plant and food materials are rich in pigments
68 including anthocyanins (Zhang et al., 2020), curcumin (Musso et al., 2017), betalains (Yao et al.,

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69 2020), chlorophyll (Chavoshizadeh et al., 2020), carotenoids (Kanatt et al., 2020), tannins (Lee et

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70 al., 2020) and others like brazilin and quercetin (Kurnianto et al., 2020; Masek et al., 2018).
71 These can be used for the development of smart biodegradable packaging material. When the
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72 smart packaging systems are exposed to different storage and processing conditions, these
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73 produce metabolites (volatile amines and organic acid) due to the microbial deterioration of food
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74 products in the packaging. These metaboils reacts with the packaging system and makes
75 significant visible changes. Though these systems act as real-time visual indicators, exhibiting
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76 changes in their color due to high sensitivity, monitoring the spoilage and quality of the food.
77 Previous review studies have summarized the potential of natural dyes/pigments/food colorants
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78 as indicators used in intelligent packaging systems (Latos-Brozio & Masek, 2020; Balbinot-
79 Alfaro et al., 2019; Tichoniuk et al., 2017), and still, there is a need to summarize the
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80 information on plant- and food waste-based pigment used for biodegradable packaging and its
81 effect on the quality of food. Hence, this paper summarizes the different food waste-derived
82 natural indicators used and recent research on the effective application of biodegradable smart
83 packaging films containing naturally derived pigments for the quality monitoring of meat
84 products, seafood, milk, etc., their advantages and disadvantages along with the prospects for
85 commercialization.

86 2. Food waste and its utility for smart packaging

87 Food waste such as peel, pulp, husk, seeds, bagasse, barks, oil cake, etc. are readily available and
88 constitute about 30-50% of the total food weight. The utility of food waste can be evaluated by
89 its composition and cost of extraction of valuable compounds. The waste products may be

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 90 composed of bioactive compounds like flavonols, polyphenols, and tannins that may contribute
91 towards the antioxidant and antimicrobial potential of the packaging system (Jönsson & Martin,
92 2016; Rojas-Graü et al., 2009). Many compounds such as anthocyanins, curcumin, betalains,
93 tannins, chlorophyll, brazilin, and other phenolic compounds can be extracted from food waste.
94 These compounds act as an indicator when mixed with a biodegradable polymer matrix and
95 provide significant results (Rai & Mehrotra, 2016). The polyphenols derived from agricultural
96 and industrial food wastes are environmentally appealing. Also, the prospects of value addition
97 or valorization of food wastes, which otherwise have no economic value, would make this a cost-
98 effective option. These films can also be presented as an eco-friendly and sustainable packaging

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99 material. Recent research studies have been carried out by employing bioactive polyphenolic

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100 pigments from food waste incorporated in biopolymeric films (Table 1).
101 Black rice milling by-product (bran) contains high amounts of polyphenolic anthocyanins (Pang
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102 et al., 2018) and has potential as a functional food. Gelatin based intelligent films containing
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103 black rice bran anthocyanins have been effectively used as freshness indicators for seafood and
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104 pork (Wu et al., 2019; Ge et al., 2019). In the blueberry juice processing, a large amount of
105 residual pomace rich in valuable phenolic compounds like antioxidants, anthocyanins are
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106 generated (Zhao et al., 2015). Blueberry agro-waste containing films based on corn/cassava
107 starch exhibited good pH sensitivity and could potentially be used in the monitoring of food
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108 freshness (Andretta et al., 2019; Luchese et al., 2018; Luchese et al., 2019). Kurek et al. (2018)
109 evaluated blackberry pomace along with blueberry residue incorporated in the chitosan matrix.
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110 Anthocyanins extracted from black bean and black soybean seed coat extracts were added to
111 corn starch and chitosan matrix, respectively (Ganesan & Xu, 2017). The films could be
112 potentially used in the packaging of perishable high protein foods given highly sensitive to pH
113 (X. Wang et al., 2019; Prietto et al., 2017). Grape skin is rich in cellulose, pectin, anthocyanins,
114 and other polyphenolic compounds. Ma & Wang (2016) used grape skin extract anthocyanins in
115 the cellulose matrix to monitor the spoilage of milk, and Chi et al. (2020) incorporated it in the k-
116 carrageenan film to monitor pork freshness. The husk of Vitis amurensis, a grape species used in
117 white wine manufacturing, is rich in phenolic compounds. It has been used to produce tara gum
118 films for visual monitoring of fish quality (Ma et al., 2017b).
119 Jambolan peel consisting of a large amount of anthocyanin (Zulfajri and Muttakin 2018) was
120 added to agarose based films to evaluate their potential to indicate the quality of packaged

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121 chicken patties (Talukder et al., 2020). Pomegranate peel, the non-edible part of the fruit,
122 contains tannins and phenolic acids (Ismail et al., 2012). Pomegranate peel extracts were added
123 to k-carrageenan based films, and these films were found suitable to be employed as freshness
124 indicators for perishable foods (Liu et al., 2020). Betalain extracts from red pitaya peels were
125 added to starch/Polyvinyl alcohol (PVA) and glucomannan films used to check the quality of
126 shrimp and fish, respectively (Qin et al., 2020; Apriliyanti et al., 2018). The amaranthus leaf
127 extracts, which are rich in betalains, chlorophyll, and carotenoids, have been effectively used in
128 the monitoring of fish quality when added into the gelatin/PVA matrix (Kanatt et al., 2020).
129 Turmeric residue flour, which is rich in curcuminoids possessing antioxidant properties, in

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130 combination with glycerol, exhibited desirable characteristics for active and intelligent

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131 packaging (Maniglia et al., 2015). Cashew nut reddish-brown covering skin or testa contains
132 tannins possessing high free radical scavenging activity (Nnaji et al., 2014). Lee et al. (2020)
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133 prepared cashew nut films with sugarcane to produce pH triggered release mechanism, active
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134 packaging. Brazilin extracts derived from Sappan wood were added to glucomannan/PVA films
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135 and were used to examine the quality variation of bananas (Kurnianto et al., 2020).
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136 3. Bioactive compounds and their utility

137 3.1 Anthocyanin
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138 Anthocyanins are bioactive compounds, part of the phenolic family, which contributes to various
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139 colors (red, orange, blue, and purple) in flowers, fruits, and vegetables (Yousuf et al., 2016).
140 Anthocyanins are water-soluble pigments exhibiting strong antimicrobial and antioxidant
141 properties and the ability to change in color with the change in pH, rendering them as a suitable
142 agent for active packaging (Kurek et al., 2018; L. Wang et al., 2019). The changes in color are a
143 result of modification of the chemical structure of phenolic substances in anthocyanin due to pH
144 variations (Shahid & Mohammad, 2013), and thus can be effectively used in the development of
145 intelligent pH-sensitive packaging to evaluate food freshness and quality (Zhang et al., 2019;
146 Sohail et al., 2018; Choi et al., 2017). The anthocyanin source greatly influences its functional
147 and physical properties. Red cabbage anthocyanins (RCA) showed optimal performance due to
148 high sensitivity to pH (Liang et al., 2019). RCA in chitin-polyvinyl alcohol (PVA) based films
149 exhibited good mechanical properties, rapid changes in color with varying pH, and was
150 successful in monitoring the spoilage of pork slices (Vo et al., 2019). RCA also caused distinct

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151 changes in color in response to ammonia (NH3) sensitivity and thus could be used in quality
152 monitoring of foods rich in protein (Zhang et al., 2020; Liang et al., 2019; Silva-Pereira et al.,
153 2015). The films based on agar and potato starch with purple sweet potato (PSP) anthocyanins
154 were found to be non-toxic and showed variation from brick pink (pH 2) to dark green (pH 10),
155 presenting relevant results. These can be used as a reliable method for visual detection of quality
156 variations of meat products (Choi et al., 2017). PSP films with chitin displayed better antioxidant
157 properties (Li et al., 2019). Jiang et al. (2020) suggested that starch-based PSP films are highly
158 sensitive to ammonia and can be used in the efficient monitoring of the freshness of fish and
159 shrimp.

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160 Packaging film based on blueberry (Andretta et al., 2019; Luchese et al., 2017) and blackberry

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161 pomace (Nogueira et al., 2019) in combination with biodegradable polymers showed variations
162 in color with varying pH and also exhibited high antioxidant potential (Kurek et al., 2018).
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163 Roselle anthocyanins have been reported to be suitable raw materials in combination with
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164 biodegradable polymers for monitoring the freshness of fish (Zhai et al., 2017) and meat
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165 products (Zhang et al., 2019). Eggplant extracts are also suitable for the development of
166 intelligent bio-based packaging, because of high anthocyanin content, to monitor food spoilage
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167 (Bilgiç et al., 2019; Yong et al., 2019c). Extracts from black rice bran in chitosan-based
168 biodegradable films were reported to be influential in the development of pH-sensitive films for
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169 monitoring the quality of seafood and restraining spoilage due to high antioxidant properties
170 exhibited by films (Ge et al., 2019; Wu et al., 2019; Yong et al., 2019a). Studies mentioning
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171 color variations on exposure to different pH levels in films based on biopolymers containing
172 anthocyanins from various sources (Figure 1) such as from Jambolan fruit (Merz et al., 2020),
173 Butterfly pea flower (Ahmad et al., 2020), Black carrot (Amiri et al., 2020; Goodarzi et al.,
174 2020), Prunus maackii (Sun et al., 2019), Chinese bayberry (Yun et al., 2019), Haskap berries (J.
175 Liu et al., 2019), Hibiscus (Peralta et al., 2019), Mulberry (Y. Liu et al., 2019), Purple corn (Qin
176 et al., 2019b), Lycium ruthenium murr (Qin et al., 2019a) and Ruellia simplex flower (Listyarini
177 et al., 2018) have been reported.

178 3.2 Curcumin

179 Curcumin is a di-phenolic, hydrophobic compound extracted from the roots of Curcuma longa
180 (Turmeric) (Pan et al., 2014). It has been added to different biodegradable packaging films for
181 the development of active and intelligent packaging. Curcumin added to gelatin-based films

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182 produced packaging systems with high antioxidant properties, which could provide information
183 on spoilage. This information is achieved by sensing the pH of the media and is depicted by a
184 change in color. Liu et al. (2018) reported the use of curcumin in combination with carrageenan
185 to produce indicative pH films with good barrier properties and thermal stability for evaluating
186 shrimp and pork freshness. It is observed that curcumin, in addition to tara gum and PVA based
187 films, exhibits ammonia (NH3) sensing property with a visible change in color. This can be used
188 in monitoring the freshness of seafood and meat (Ma et al., 2017a). Cellulose-based curcumin
189 films were sensitive to fish spoilage exhibiting a change in color and can also be used as
190 freshness indicators for food products (Tichoniuk et al., 2017). Curcumin incorporated in

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191 composite films based on pectin containing sulfur nanoparticles depicts variations in color due to

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192 changes in pH (Ezati & Rhim, 2020). Casein/zein nanocomposite films incorporated with
193 curcumin using pH driven method ( formation of hydrophobic curcumin loaded protein
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194 nanoparticles without the requirement of organic solvents or heat ) exhibit potential application
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195 as edible food packaging (L.Wang et al., 2019).
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196 3.3 Betalains

197 Betalains are water-soluble phenolic pigments that are obtained from plants like red pitaya,
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198 amaranth, beetroot, and prickly pear (Polturak & Aharoni, 2019). It contains antimicrobial,
199 antioxidant, anti-lipidemic, anti-diabetic, and anti-cancer properties (Gengatharan et al., 2015). It
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200 can be used as a suitable substance for the development of active and intelligent packaging
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201 (Jamroz et al., 2019a). Red pitaya peel (RPP) or dragon fruit peel, which constitutes 18-24% of
202 the fruit, is a rich source of betalains (Chew et al., 2019). Apriliyanti et al. (2018) reported that
203 RPP betalains added to glucomannan and PVA based films successfully monitored fish freshness
204 as the developed intelligent films exhibited sensitivity to ammonia. The color of the films
205 changed from purple to yellow in eight days, when used for fish packaging, due to an increase in
206 the total volatile basic nitrogen (TVB-N) content.
207 Similarly, starch-based films with RPP extracts displayed enhanced mechanical and antioxidant
208 properties, along with sensitivity to ammonia, suitable for monitoring shrimp spoilage (Qin et al.,
209 2020). Chitosan/PVA based films with cactus pear peel extracts are reported to be ideal in
210 monitoring the freshness of shrimp as the volatile compounds released from shrimp depicted
211 variations in the film color (Yao et al., 2020). Betanin is the major betalain in red beetroot extract
212 (Scheiber et al., 2001), but its addition to carboxymethyl cellulose and glycerol-based films did

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213 not depict significant sensitivity to change in pH, temperature, light, or ammonia levels. Thus, it
214 may not be used as intelligent packaging (Tichoniuk et al., 2017).

215 3.4 Chlorophyll

216 Chlorophyll pigment is found in plants, cyanobacteria, and mosses, possess antioxidant
217 properties and high nutrient values. It prevents the oxidative damage of cells by eliminating free
218 radicals and helps to dispose of carcinogens by binding them in the gastrointestinal tracts and
219 resists cancer cell growth (El-Sayed et al., 2013). It is reported that chlorophyll acts as a time-
220 temperature indicator in the temperature range of 50˚C to 70˚C (Maciel et al., 2012). Amaranthus

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221 leaf extract in gelatin/PVA based films is reported to monitor the quality of chicken and fish
222 effectively, as it is sensible to the detection of volatile amines (Kanatt et al., 2020). Green tea and

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223 basil extracts consist of chlorophyll, which imparts a yellow-green color and undergoes a change
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in color at different pH (Lee, 2012). Basil contains antioxidants like chlorogenic acid, methyl
chavicol, linalool with stability at high temperatures, suitable for film casting (Suppakul et al.,
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226 2008). Medina-Jaramillo et al. (2017) stated that films based on cassava starch films containing
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227 green tea and basil extracts exhibit good antioxidant potential and undergo a change in color on
228 exposure to varying pH and can be used as food quality indicators.
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229 Furcellaran and gelatin films blended with Pu–Erh and green tea extracts were employed to
230 fabricate active and intelligent films. Green tea extract films showed color variations during the
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231 tests for fish spoilage and thus can be used as spoilage indicators in the food industry. Both green
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232 tea and Pu-erh tea extract films showed a change in color with varying pH (Jamróz et al., 2019b).
233 Spinach extracts in cassava-based films did not exhibit significant variations in color at different
234 pH (Veiga Santos et al., 2010). Chavoshizadeh et al. (2020) observed that gluten films with
235 chlorophyll could result in the shelf life extension of sesame oil and also changed color, sensing
236 the oxidation of oils and thus can be used as smart sensing to detect the expiration of oils.

237 3.5 Carotenoids

238 Carotenes are lipophilic bioactive pigments (orange, yellow, and red), which are obtained from a
239 variety of fruits, vegetables, flowers, and green plants. The carotenoids exhibit antioxidant
240 properties because of their ability to quench singlet oxygen, free radical scavenging, and
241 photosensitizers (Christaki et al., 2013). Polylactic acid films modified with titanium dioxide and
242 lycopene (carotenoid) were reported to change colors for different oxidation conditions and

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243 exhibit adequate antioxidant capacity (Asadi & Pirsa., 2020). Lutein and β-carotene are naturally
244 occurring carotenoids found in various fruits (cantaloupe, apricots, grapefruit) and vegetables
245 (carrot, squash, sweet potato, red and yellow peppers, broccoli, green leafy vegetables).
246 Biodegradable films incorporated with β-carotene and lutein were examined under the influence
247 of thermooxidation aging and weathering. It is reported that both the films exhibited a change in
248 color and thus can be used as intelligent films for indicating the storage life of food products for
249 a short period (Latos-Brozio & Masek., 2020). The extracts of green tea and basil contain an
250 abundance of carotenoids to bring a change in the color of cassava starch-based films when
251 exposed to varying pH. Thus, these films may be employed as indicators to depict the quality of

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252 food (Medina-Jaramillo et al., 2017). Amaranthus leaf extract also contains carotenoids and,

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253 when incorporated in gelatin/PVA effectively monitored the spoilage of chicken and fish (Kanatt
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3.6 Tannins
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256 Tannins are complex bioactive phenols and heterogeneous secondary metabolites and can be
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257 effectively employed in active packaging films. Limited studies have been reported on the
258 utilization of tannin for the development of smart packaging. Cashew nut testa extract is rich in
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259 tannin, gallic acid, and other valuable compounds (Nnaji et al. 2014; Rajini, 2011). It is usually
260 separated and discarded in the processing of cashew due to its astringent and bitter flavor. Lee et
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261 al. (2020) successfully developed a cellulose-based film from sugarcane bagasse incorporated
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262 with cashew nut testa extract with high antimicrobial, antioxidant properties, and pH sensitivity.
263 The edible, as well as non-edible parts of pomegranate fruit, contain polyphenols in abundance,
264 such as tannins, phenols, and flavonoids (Ismail et al., 2012). Liu et al. (2020) developed
265 packaging films from pomegranate peel and flesh extract incorporated in the k-carrageenan
266 matrix with enhanced mechanical properties and high antimicrobial properties. It is reported that
267 the films containing pomegranate flesh extract were more pH-sensitive than peel extract films
268 and could be effectively used to evaluate food quality in active and intelligent films.

269 3.7 Others bioactive compounds used for packaging

270 3.7.1 Brazilin

271 Brazilin is a bioactive polyphenol that exhibits sensitivity and instability to pH and is also used
272 as an active ingredient in smart packaging. Studies were limited to the utilization of sappan wood

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273 brazilin. The sappan wood consists of red-toned water-soluble brazilein flavonoid possesses
274 antibacterial, antioxidant activities, and pharmacological activities (Athinarayanana et al., 2017;
275 Nirmal et al., 2015). Kurnianto et al. (2020) investigated the ability of PVA/Glucomannan films
276 containing sappan wood extract to monitor the freshness of climacteric fruits like banana. The
277 films turned ruby red from yellow, caused by pH varying from 4.5 to 5.1, as the storage time
278 increased and could thus be successfully used as smart packaging for the detection of banana
279 deterioration.

280 3.7.2 Quercetin

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281 Quercetin is the most abundant flavonoid compound derived from plants (tea), fruits (grapes,
282 berries, apples, citrus), vegetables (onion, broccoli), grains (quinoa). They function as

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283 antioxidants in the body and prevent inflammation, have anti-cancer properties, help in lowering
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blood pressure, and curb the effect of many other diseases (D'Andrea, 2015). It is found that
oxidation causes a change in the color of quercetin and thus could serve as a colorimetric
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286 indicator compound for aging (Giteru et al., 2015). Masek et al. (2018) observed that quercetin
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287 containing cycloolefin copolymer films exhibited changes in color with variations in climatic
288 factors like weathering and thermo-oxidation. These films can thus be effectively used as an
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289 aging time indicator in the food industries.

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290 4. Characteristics of active and intelligent films

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291 4.1 pH Sensitivity

292 The change in pH is a major indicator of the freshness and state of the food product. The
293 spoilage of food is followed by a change in the pH values (Medina-Jaramillo et al., 2017). Thus,
294 a relationship can be established between the freshness or quality of food and pH values, owing
295 to the microbial spoilage (Golasz et al., 2013). In the case of fruits, vegetables, and dairy
296 products, pH changes due to variations in the concentrations of organic acids during storage.
297 Similarly, the development of volatile nitrogen compounds like dimethylamine, trimethylamine,
298 histamine, tyramine causes pH change in high protein foods (meat, seafood, etc.) as a result of
299 metabolism and microbial growth (Bulushi et al., 2009). Recently, several studies have focused
300 on the development of smart packaging systems as visual indicators for monitoring fresh food
301 quality based on pH variations (Silva-Pereira et al., 2015). Chemical dyes like chlorophenol red

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302 and bromophenol blue were utilized as pH indicators. However, they are not found fit for food
303 applications. Thus, natural pH sensing pigments and dyes are used in intelligent packaging due to
304 non-toxic, safe, and readily available (Zhang et al., 2014).
305 Anthocyanins, when exposed to alkaline or acidic conditions, change their chemical structure
306 and respond to it with color variation. Under the acidic condition, a predominance of flavylium
307 cation is exhibited, contributing to the red and pinkish colors whereas, at pH 4-5, a predominance
308 of pseudo base carbinol is present, causing a transparent indicator. As the pH escalates to 6-7, the
309 quinoidal structure causes the purple color. The blue color is exhibited due to anionic form, as
310 pH increase to 7-8, and yellow color chalcone is formed at pH 8-9, as the central ring opens

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311 (Ananga et al., 2013). Chitosan, starch, and carboxymethyl cellulose biopolymers films,

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312 containing PSP, showed color variations with varying pH from 2-12 as red (2-3), pink (4-6),
313 purple (7), blue (8), green (9-10), and yellow (11-12) (Jiang et al., 2020). The pH-sensitive films
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314 containing RCA in combination with chitin/chitosan/starch/glycerol and gum-like biopolymers
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315 exhibited color variation with pH change (Wu et al., 2020; Liang et al., 2019; Vo et al., 2019).
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316 Sun et al. (2019) stated that k-carrageenan films containing prunus maackii juice discolored
317 within 10 sec on exposure to buffer solutions and showed a substantial variation in the color
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318 from deep red at lower pH to blue-grey color with an increase in pH. The color of roselle
319 anthocyanin films based on biodegradable polymers is observed to be pink at pH less than 5,
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320 purple at pH 6 & 7, which gradually changed at alkaline pH of 8-9 to blue and to yellow at pH 10
321 -12 (Zhang et al., 2019; Zhai et al., 2017). Haskap berries anthocyanins films based on fish
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322 gelatin were observed to change from pinkish-red at pH 3-5 to the color of chestnut at pH 6-8
323 and finally to purplish-grey color at pH 9-12 (J. Liu et al., 2019). Chitosan films containing
324 purple corn extract displayed notable changes in color, from purple at pH 3-6 to blue at pH 7-10
325 (Qin et al., 2019b). Lycium ruthenicum – starch films were observed to vary their color from
326 red/purple in acidic solutions to green in alkaline solutions (Qin et al., 2019a). Mulberry extracts
327 in k-carrageenan films attributed to the pH sensitivity and changed film color from red (pH 2-3)
328 to purple (pH 4-6) to green-blue (pH 7-13) (Y.Liu et al., 2019).
329 Food wastes and residues derived anthocyanins have also been added in biodegradable films for
330 the assessment of pH sensitivity. Blueberry residue containing anthocyanins when added to corn
331 and cassava starch-based films were found to transit from rose (pH 2), red wine (pH 4) and
332 purple (pH 6) in acidic condition to intense gray (pH 9) black (pH 10) and brown (pH 12) at

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333 alkaline pH because of anthocyanin degradation (Andretta et al., 2019). Intelligent pH-sensitive
334 films with black rice extract in chitosan matrix/chitosan nanocrystals showed visible variations in
335 color from rose-carmine to pink, then purple and gray-blue and finally yellow-green as pH
336 increased from 2-12 (Ge et al., 2019). Black bean seed coat extract anthocyanin and corn starch
337 blend films showed immediate color variations within five seconds when exposed to different pH
338 buffer solutions from red to green as pH increased from acid to alkaline (Prietto et al., 2017). The
339 color of films of black soybean coat extract anthocyanins in chitosan matrix, on exposure to
340 varying pH, changed from bright red at pH 3-6, then kermesinus to brown at pH 6-7 and finally
341 turned to blue at pH 8-10 (X. Wang et al., 2019). The pH indicator films containing blackberry

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342 pomace extracts, rich in phenolic compounds in the chitosan matrix, changed from bright red

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343 (pH 2-4) to violet (pH 5-7) and dark blue (pH 10-12) (Kurek et al., 2018). The wastes from wine
344 manufacture: grape skin powder films in combination with k-carrageenan and tara gum turned
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345 pink on exposure to acidic pH (2-4) and green on exposure to alkaline pH (10-12) (Chi et al.,
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346 2020; Ma et al., 2017b). Liu et al. (2020) reported that the color of k-carrageenan films
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347 containing pomegranate flesh extracts varied from red at pH 3-5 to green at pH 7-9 and yellow at
348 pH 11 due to change in anthocyanin structure.
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349 Curcumin is also unstable when exposed to varying pH and has the potential to be used in pH-
350 sensitive intelligent packaging films. Bovine gelatin films containing curcumin showed
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351 immediate response on exposure to pH. The films which were yellow at pH 6 get transitioned to
352 orangish-red when pH increased to highly alkaline, while the films which were orangish red at
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353 pH 11 when exposed to acidic media, turned yellow (Musso et al., 2017). In the case of k-
354 carrageenan films with curcumin, the films were yellow at pH 3-4 and turned to a red color
355 palette as the pH became more alkaline (Liu et al., 2018). The color of extracted brazilein varies
356 with varying pH conditions, exhibiting different colors at each pH level. The color varies from
357 pearl ruby red at pH (6-7), that is, at neutral pH and transforms to purple red – wine red as the
358 pH increases (Ulma et al., 2018). Glucomannan/PVA based films incorporated with brazilein
359 extract derived from Sappan wood showed a yellow color at pH (3-5), converting to orange at
360 pH (6), then to red at pH (7-8) (Kurnianto et al., 2020). Chlorophyll and carotenoids can impart
361 yellow-green color to various plant products. On exposure to acidic pH, chlorophyll degrades to
362 form pheophorbide and pheophytin, which results in a yellow or olive green color (Andrés-Bello
363 & Barreto-Palacios, 2013), whereas the degradation is inhibited at alkaline pH. At high pH,

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364 chlorogenic acid is oxidized, forming chlorogenic acid quinines that are highly reactive and
365 change the color to green, brown, or yellow (Wildermuth et al., 2016). Basil extract containing
366 film on exposure to pH 3, immediately changed to white with a slight yellow tone from a
367 greenish-yellow color to a clear, bright yellow color in basic medium. Furcellaran gelatin-based
368 films containing green tea extract turned to white on exposure to acidic pH (pH 3) and orange in
369 alkaline pH (pH 12) (Jamróz et al., 2019b).
370 Betalains are reported to exhibit stability in a broader pH range as compared to anthocyanins.
371 These show greater stability at pH 3-7, optimum pH being around 4-6; however, under alkaline
372 conditions, betalains turn from red to yellow, as they undergo a structural transformation

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373 (Rodriguez-Amaya, 2019). Thus, betalains are considered to be suitable for the development of

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374 intelligent food packaging films.

375 4.2 Time – Temperature sensitivity -p

Temperature is an essential criterion, affecting the safety and quality of various foods products
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376
377 throughout their processing, storage, and transportation (Tsai et al., 2002). The changes in the
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378 quality of food and information about the shelf life can be indicated by Time-temperature
379 indicators (TTIs) by recording and monitoring the effects of temperature on the product (Tsironi
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380 et al., 2017). TTI’s can be embedded as a part of the food package that provides information
381 about the product quality at temperature and specified period. It should provide a continuous and
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382 clear, irreversible reaction in response to temperature variation (Ellouze et al., 2009). The time
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383 duration from activation of TTI to termination, depicted by variations in color, corresponds to the
384 shelf stability of the food product (Kim et al., 2016). TTIs are categorized as chemical,
385 biological, and physical based on the cause of variations in color. The dyes used can be synthetic
386 such as bromothymol blue or methyl red; however, recent studies have been concentrated
387 towards the use of naturally derived dyes from food wastes and products, especially for food
388 packaging (Rachmelia and Imawan, 2018).
389 Anthocyanin phenolic compounds can be used in TTI as it exhibits sensitivity to changes in the
390 temperature (Markakis, 1982). Anthocyanin structures changes upon thermal degradation, which
391 depends on the severity and conditions of heating. Black corn anthocyanins incorporated in the
392 chitosan matrix were found to have greater color stability at temperatures 10˚C and 25˚C than at
393 40˚C (Rachmelia & Imawan, 2018). Paraffin wax films containing black carrot anthocyanins

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394 when exposed to different temperatures (-5˚C to 25˚C) for 48 h responded differently with more
395 significant color variation at a higher temperature (Amiri et al., 2020).
396 Echium amoenum in bacterial cellulose films were assessed for color stability at varying
397 temperatures (-18 to 25 ˚C) for 2-6 days. The highest values of ΔE were exhibited at room
398 temperature at all times. The changed color had great stability. Nogueira et al. (2019) subjected
399 starch-based edible films containing freeze-dried blackberry particles to sterilization at 127 for
400 15 min. The films underwent a significant change from red to brown color. Maciel et al. (2012)
401 exposed chitosan films containing anthocyanin at 20˚C to 60˚C for a period of 72h. At 60˚C or
402 temperatures generally above 50˚C lead to significant visual color change. The most significant

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403 changes were observed in the range of 20˚C to 37˚C attributed to anthocyanin degradation.

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404 Black been seed coat extracts, and red cabbage anthocyanins were exposed to time and
405 temperature combinations. The former showed a change in color towards yellowness, and the
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406 instability increased as the time increased, whereas the latter remained stable (Prietto et al.,
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407 2017). This could be attributed to the fact that the di-glucoside (cyanidin-3.5-diglucoside)
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408 anthocyanin present in red cabbage are more stable compared to the monoglucoside (delphinidin-
409 3-Glucoside) in the black bean seed coat which is due to the limited sugar formation of
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410 intermediates (unstable) that undergo degradation into aldehydes and phenolic acids (Fleschhut
411 et al., 2006). A paper-based colorimetric indicator containing Ruellia simplex flower
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412 anthocyanins was subjected to varying temperatures (13˚C, 25˚C & 40˚C) for 24 h. It is observed
413 that after 2 h of storage, the color of the films changed to purplish-blue from purplish pink for all
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414 temperatures. The color remained relatively stable at 13˚C, not showing any significant changes
415 in the 24 h duration. However, after 17 hours, the color changed to greenish-grey for films at
416 25˚C and 40˚C and further degraded to a yellowish grey color after 24 h. (Listyarini et al., 2018).
417 Glucomannan/PVA films with brazilin pigment were monitored for 6 days during storage.
418 Initially, the film remained yellow and then transformed its color to a pale yellow on the second
419 and fourth day, and on the final day, they turned orange following the ∆E values recorded
420 (Kurnianto et al., 2020).

421 4.3 CO2 sensitivity

422 Active and intelligent packaging is also employed for the sensing of carbon dioxide (CO2) and
423 oxygen levels. CO2 is a major indicator of the quality evaluation of packaged products
424 (Puligunda et al., 2012). The spoilage of food begins soon after it is packaged due to the growth

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425 of microorganisms accompanied by the generation of CO2. The visual sensors employed for the
426 detection of CO2 can be classified as 1st: luminescent dye-based sensors, which upon exposure to
427 CO2, change fluorescence; 2nd: pH indicators based on colorimetric dyes that respond by
428 variation in color on exposure to CO2 (Puligunda et al., 2012). Colorimetric indicators use
429 cheaper ingredients and require no separate instrumentations; however, they are less sensitive in
430 general. Saliu & Della Pergola (2018) assessed films based on poly-lysine and RCA mixture
431 label indicators for their CO2 sensitivity by exposing them to different CO2 levels (2.5% to
432 100%). When 100% of the label indicator was exposed to CO2, the color changed to purple from
433 an initial azure within a few minutes, whereas lower levels of exposure (5%) showed no

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434 significant change in color, which could be because of the high amount of the indicator. Also, the

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435 label indicators, under refrigerated conditions (0˚C to 5˚C) remained stable for an extended
436 period but responded well to small variations in CO2 concentration. Kurnianto et al. (2020) also
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437 suggested a change in the color of colorimetric films on exposure to CO2. They tested
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438 PVA/glucomannan films containing brazilin extracts for banana storage and observed that the
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439 release of CO2 during the deterioration of banana brought about a change in color of the yellow
440 mustard films to dark red in six days.
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441 4.4 Ammonia sensitivity

442 The process of proteolysis of high protein foods like meat and seafood (fish, shrimp), during
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443 storage, produce volatile amines like ammonia and di/trimethylamine together called total TVB-
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444 N (Kanatt et al., 2020). TVB-N acts as an indicator in assessing the freshness of high protein
445 food as their concentration increases with an increase in the decomposition during storage, which
446 is caused by enzymes and bacteria (Sun et al., 2019). Presently, chemical methods, such as FTIR
447 Spectroscopy and Kjeldahl, have been used for the determination of TVB-N. These methods are
448 time-consuming, cause sample destruction, and are inconvenient for consumers as they fail to
449 accommodate timely monitoring of packaged fresh food products (Cai et al., 2011). Whereas, pH
450 elevation in the packaging headspace of meat/fish products due to the accumulation of volatile
451 organic amines within the packaging film can be easily detected by pH indicators (Pirsa and
452 Shamusi 2019). Thus, due to their TVB-N sensing ability and to overcome the drawbacks of the
453 chemical methods used, various pH indicators have been employed in evaluating fish and meat
454 quality. Colorimetric pH indicators incorporated in the packaging headspace when exposed to
455 TVB-N released by the product package, change their color specifically, imitating gas sensors

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456 (Azmi et al., 2012). The diffusion of ammonia into the film matrix produces alkaline
457 surroundings resulting in a color variation of immobilized pH sensing dyes in the film (Zhang et
458 al., 2019).
459 Anthocyanins have been reported to be effectively used in the determination of volatile ammonia
460 released by packaged foods high in protein content. The color variations are attributed to the
461 mechanism that volatile ammonia diffuses into the film matrix and combines with water
462 molecules in the film, forming NH3.H2O, which further hydrolyzes to NH4+ and hydroxyl ions
463 (OH-) and responsible for the alkaline environment of the film. This modifies the anthocyanin
464 structure to chalcones, and thus brings about a change in color (Zhang et al., 2019).

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465 Purple sweet potato anthocyanins starch-based films exhibited sensitivity to ammonia as the

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466 color difference (∆E) increased with an increase in storage time and color changes to the green
467 from red (Jiang et al., 2020). It is reported that starch/PVA films containing roselle anthocyanins
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468 showed high sensitivity against ammonia, changing from pink to purplish-black as the storage
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469 time increased ( Zhang et al., 2019; Zhai et al., 2017). Liang et al. (2019) reported red cabbage
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470 anthocyanin in carboxymethylcellulose films is highly sensitive to ammonia and, on exposure,

471 intensified in color. Prunus maackii juice incorporated k-carrageenan films demonstrated a
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472 visible change in color on exposure to ammonia (Sun et al., 2019). The pH increase due to
473 ammonia resulted in anthocyanin losing its cation to quinone (blue), causing a reduction of color
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474 concentration. Thus, the film changed its color from red to blue (Peralta et al., 2019). Chen et al.
475 (2020) suggested that starch/PVA/glycerol-based packaging films containing anthocyanin
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476 (purple sweet potato) showed high sensitivity to ammonia in terms of ∆E values and those with
477 curcumin, in terms of relative color change (S) value. The presence of glycerol improves water
478 vapor permeability of the film (Farhan and Hani, 2017), thus enhancing its sensitivity to
479 ammonia. Cassava starch-based films containing anthocyanins from Chinese bayberry turned
480 blue from purple red color when exposed to ammonia for 5 minutes and olive green after 35
481 minutes (Yun et al., 2019). Mohammadalinejhad et al. (2020) observed that echium amoenum
482 containing films based on bacterial cellulose, when exposed to ammonia vapor, showed color
483 variation to yellowish-brown from purplish to black (Table 2).
484 Betalains containing intelligent packaging have shown sensitivity to ammonia depicted by color
485 variations. These color variations can be attributed to the degradation of betacyanin to betalamic
486 acid (yellow ), to cyclo-Dopa 5-O-(malonyl)-β-glucoside (colorless) (Qin et al., 2020). Chitosan

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487 films containing cactus pear betalains depicted sensitivity to ammonia, visible by color variations
488 from purple to yellow (Yao et al., 2020). The color of dragon fruit peel anthocyanin films based
489 on starch started to fade from the pink color on exposure to ammonia for 10 min. The color of
490 the films further deteriorated with exposure time and finally turned to yellow after 60 minutes
491 (Qin et al., 2020). Jamroz et al. (2019a) reported that furcellan films containing elderberry,
492 beetroot, and blackberry extracts, exhibited variations in color when exposed to ammonia.

493 4.5 Antimicrobial /Antibacterial ability

494 Food borne pathogens majorly affect food quality and hurt humans health (Fang et al., 2017).

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495 Antimicrobial packaging becomes necessary to prevent these pathogens. In active packaging, the
496 antimicrobial activity is attributed to the barrier and blocking functions that suppress or inhibit

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497 microbial growth in the packaged product (Camo et al., 2008). Antimicrobial agents added in
498 -p
food packaging can enhance the shelf stability of food as it minimizes microbial count and
extends the lag phase (Kuorwel et al., 2011). Anthocyanin phenolic compounds exhibit strong
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499
500 antimicrobial properties and act as good additives in the packaging (X. Wang et al., 2019). Sun et
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501 al. (2018) observed that anthocyanins could damage the bacterial cell membrane, affecting the
502 pathogenic biosynthesis, which leads to bacterial decomposition and, finally, death. Wu et al.
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503 (2020) examined the antibacterial activity of glucomannan films containing red cabbage
504 anthocyanins against Escherichia coli (E.coli) and Staphylococcus aureus (S.aureus), and the
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505 film showed hindrance to pathogenic growth. Anthocyanin rich purple corn exhibits great
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506 antimicrobial activity (Yang & Zhai, 2010). Chitosan and k-carrageenan based films containing
507 purple corn and pomegranate flesh and peel anthocyanins respectively were analyzed for
508 antimicrobial effect against S.aureus, E.coli, Salmonella, and Listeria monocytogenes
509 (L.monocytogenes). The films depicted strong antimicrobial ability against all four bacterial
510 strains (Liu et al., 2020; Qin et al., 2019b).
511 Curcumin exhibits intense antimicrobial activity, which is attributed to the phenolic hydroxyl
512 groups that covert to phenoxyl groups, thereby removing free radicals (Zhang et al., 2019). A
513 study suggested that the impaired cell wall permeability is responsible for curcumin’s
514 antimicrobial mechanisms (Tyagi et al., 2015). The antimicrobial activity of curcumin containing
515 gelatin films is assessed against E.coli (gram-negative) and L.monocytogenes (gram-positive)
516 that reduced the bacterial growth rate for both strains (Ezati & Rhim, 2020). The aqueous
517 curcumin extract had low inhibitory effects at 2-32g/L concentration for E.coli and S.aureus

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518 strains (Niamsa & Sittiwet, 2009). The alcoholic curcumin extract has a minimum inhibition
519 effect at 30 ppm concentration for S.aureus (Lawhavinit et al., 2010). The interactions between
520 gelatin and curcumin may also be the cause of lacking antimicrobial activity (Salgado et al.,
521 2012).
522 Betalains exhibit excellent antimicrobial properties. It is stated that betacyanins can cause cell
523 death as they affect the permeability of cellular membranes (Gengatharan et al., 2015).
524 Chitosan/PVA films containing cactus pear anthocyanins were evaluated for antimicrobial
525 properties to counter four strains: E.coli, S.aureus, L.monocytogenes, and Salmonella
526 Typhimurium and found to be useful for all strains except E.coli (Yao et al., 2020). Cactus pear

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527 extract betalains did not contribute towards the inhibition of growth rates of E.coli and thus,

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528 showed no antimicrobial activity (Melgar et al., 2017). Red pitaya peel extracts in cassava
529 starch-based films were assessed by agar diffusion method for countering four pathogenic
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530 strains: Salmonella, E.coli, L. monocytogenes, and S.aureus. The films exhibited an enhanced
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531 antimicrobial activity against all the tested strains, which increased with an increase in
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532 anthocyanin content (Qin et al., 2020). The antimicrobial ability of Gelatin/PVA films containing
533 amaranthus extract is assessed by disc diffusion against Pseudomonas fluorescens, E.coli,
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534 S.aureus, and Bacillus cereus. It is found to be maximum for gram-positive strains: S.aureus and
535 Bacillus cereus, whereas, for gram-negative strains: E.coli and P.fluorescens, lower
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536 antimicrobial activity was observed, which could be because of lipopolysaccharide membranes
537 that are present, preventing active compounds from transferring across it (Kannat et al., 2020).
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538 Catechins, especially epigallocatechin gallate, are responsible for the green tea extract’s
539 antimicrobial potential (Friedman, 2007). The mechanism involves inhibition of RNA and
540 DNA cell synthesis, the function of the cytoplasmic membrane, and the disturbance of bacteria’s
541 energy metabolism (Tsuchiya et al., 1994). Furcellan gelatin films added with Pu-erh and green
542 tea were monitored for antimicrobial ability against pathogenic strains: S.aureus & E.coli and
543 yeast strains: Candida albicans and Hanseniospora uvarum. The films depicted great
544 antimicrobial property for S.aureus and E.coli, lesser against the latter due to membrane
545 differences. However, the films did not show any antimicrobial effects on Candida albicans and
546 Hanseniospora uvarum species (Jamróz et al., 2019b).

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547 4.6 Antioxidant
548 In fresh packaged food products, the oxidation reaction encourages the development of off-
549 flavors caused by rancidity, accompanied by discoloration and, thereby, adversely affecting the
550 appearance, quality, and nutritional content of food (Liu et al., 2017). Active antioxidant
551 packaging has become popular for avoiding oxidative reactions. The synthetic oxidants
552 traditionally used, such as butylated hydroxytoluene and hydroxyanisole, may be substituted by
553 natural, plant-derived pigments that are effective in controlling oxidation reactions and are safe
554 for consumers’ health (Shahid & Mohammad, 2013). Phenolic compounds derived from plants
555 act as antioxidants (Shahidi & Ambigaipalan, 2015), based on their ability to chelate metal ions

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556 and scavenge reactive oxygen (Pisoschi & Pop, 2015). Hence, polyphenols like flavonoids and

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557 phenolic acids are added to biopolymer films to develop active packaging (Bai et al., 2019).
558 Anthocyanins rich compounds possess great antioxidant properties that are important in the
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559 maintenance of stability and extension of shelf life (Wrona et al., 2015). The antioxidant activity
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560 of black rice anthocyanins are widely researched (Boue et al., 2016). The antioxidant potential of
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561 black and purple rice extract anthocyanin containing chitosan films is determined by 2,2-
562 diphenyl-1-picrylhydrazyl (DPPH) scavenging activity (Yong et al., 2019a; Wu et al., 2019; Ge
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563 et al., 2019). The composition of phenolic extracts influenced the DPPH (free radical
564 scavenging) activity. Red cabbage anthocyanins added to glucomannan films also reported
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565 strong antioxidant ability (Wu et al., 2020). Zhang et al. (2019) evaluated roselle anthocyanins
566 incorporated in chitosan/PVA films exhibiting a low antioxidant activity due to the possibility of
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567 chitosan to change the film towards a basic setting, reducing the film’s phenolic content (Kanatt
568 et al., 2012). Liu et al., (2019) evaluated gelatin films containing haskap berry extract and
569 observed an enhanced DPPH scavenging activity, attributed to the antioxidant activity of
570 phenolic anthocyanins (Rasid et al., 2018). The antioxidant ability is observed to be proportional
571 to anthocyanin content in the film (Liu et al., 2017). Purple corn extract anthocyanin containing
572 chitosan films exhibited a strong DPPH scavenging activity due to its phenolic compounds (Qin
573 et al., 2019b). Liu et al. (2019) added mulberry extracts in the k-carrageenan matrix and
574 observed high antioxidant ability, which is due to the release of phenols from the film (Liu et al.,
575 2017). Sun et al. (2019) developed a green film containing Prunus maackii juice extracts
576 incorporated in the k-carrageenan matrix and observed an enhanced DPPH scavenging activity.
577 Liu et al. (2020) suggested that incorporating pomegranate flesh and peel extracts in k-

19
578 carrageenan films elevated the antioxidant activity due to the release of polyphenols and
579 abundant hydroxyl groups present in the extract. Black soybean coat extract anthocyanins added
580 to chitosan-based films also showed good antioxidant properties (Wang et al., 2019). Kurek et
581 al. (2018) evaluated the antioxidant ability of blackberry and blueberry extracts as well as the
582 developed films. The films containing anthocyanin extracts showed enhanced antioxidant
583 activities. The DPPH scavenging ability of starch films elevated on adding Lycium ruthenicum
584 extracts and increased with the increased amount of extracts (Qin et al., 2019a). The grape skin
585 anthocyanins exhibited the greatest antioxidant activity (Rockenbach et al., 2011). Cellulose and
586 k-carrageenan films containing grape skin extracts exhibited excellent antioxidant properties

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587 (Chi et al., 2020; Ma & Wang, 2016).

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588 Curcumin has been used as a spice and is also used in pharmacological and medical applications
589 due to its strong antioxidant properties (Ak & Gülçin, 2008). The antioxidant ability of gelatin
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590 films containing curcumin is assessed (Musso et al., 2017). It is reported that the incorporation
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591 of curcumin enhanced the antioxidant properties of gelatin films. It is reported that as the
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592 curcumin’s chemical structure modified with variation in pH, the interaction between curcumin
593 and gelatin also differed, thus inducing different antioxidant abilities. The antioxidant abilities of
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594 betalains have been researched through various studies (Gengatharan et al., 2015). Gelatin/PVA
595 films containing amaranthus leaf extract were tested using the DPPH method and showed good
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596 antioxidant abilities (Kanatt, 2020). Studies have shown that cactus pear extracts contain an
597 abundance of betalains, and thus possess excellent antioxidant properties (El-Mostafa et al.,
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598 2014). Yao et al. (2020) observed that chitosan/PVA films with cactus pear extracts exhibited
599 good antioxidant properties when assessed by the DPPH method, which is attributed to
600 betacyanins hydrogen atom donating capacity (Ciriminna et al., 2018). Starch/PVA films added
601 with dragon fruit peel extracts were assessed. It is stated to exhibit enhanced DPPH radical
602 scavenging activity due to the phenolic hydroxyl group’s electron donating activity (Qin et al.,
603 2020).
604 Chlorophyll, due to excellent nutrition values and antioxidant properties, is considered as a
605 nutrient food. It protects against oxidative damage to the cells by eliminating free radicals. It is
606 observed that in the gastrointestinal tract, chlorophyll binds to the carcinogens and disposes of
607 them. It also prevents the growth of cancer cells, acting as an antioxidant (El-Sayed et al., 2013).
608 Chlorophyll containing wheat gluten packaging exhibited great antioxidant potential and

20
609 prevented oxidation of sesame oil, enhancing the shelf stability (Chavoshizadeh et al., 2020).
610 Jamróz et al. (2019b) evaluated Furcellan/Gelatin films containing tea extracts for their
611 antioxidant abilities by using ABTS, DPPH assays, and Total Phenolic Content (TPC). DPPH
612 and ABTS method influenced the most significant scavenging activity. Pu-erh tea contains
613 phenolic compounds in its water extracts that are responsible for the prevention against oxidative
614 damage and nitric oxide scavenging (Duh et al., 2004).

615 5. Applications
616 Food quality continuously deteriorates during storage until the product becomes inedible. The

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617 metabolites produced by spoilage microorganisms adversely affect the taste, nutritional value,

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618 and flavor (Ma & Wang, 2016). Thus, it is essential to innovate effective indicators for food
619
620
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quality. The real-time quality evaluation of perishable products like fish, meat, fruits and
vegetables, milk, and dairy product, is in great demand that is fulfilled by intelligent packaging
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621 systems (Liu et al., 2017). Meat and seafood product spoilage is attributed to the production of
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622 nitrogenous substances, causing an increased pH (Musso et al., 2017), whereas fruits and
623 vegetables and dairy products on spoilage release organic acids (Goodarzi et al., 2020), reducing
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624 pH inside the food package. Several research studies have been carried out for the freshness
625 monitoring of meat and seafood, milk, oil, etc. (Table 2).
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626 5.1 Seafood

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627 Microbial spoilage is the leading cause of deterioration in seafood, which results in the
628 development of off-flavors and foul taste. Total volatile basic nitrogen (TVB-N) includes
629 ammonia di and trimethylamine etc. which cause the enzymatic and microbial degradation of
630 protein-rich foods, leading to pH variations in packaged foods (Zhai et al., 2017). These
631 variations can be monitored by employing a pH indicating intelligent film that assesses the
632 product deterioration (Musso et al., 2017).
633 Fish is highly susceptible to enzymatic and microbial deterioration, which decreases its nutrition
634 value and leads to various food borne diseases (Chun et al., 2014). It is highly perishable due to
635 its high contents of protein and water (Zhai et al., 2017). Freshness, a major characteristic in
636 monitoring fish spoilage, can be determined by the release of TVB-N. The concentration of
637 TVB-N increases due to the enzymatic decay of trimethylamine oxide by microorganisms, which

21
638 increases the pH (Jiang et al., 2020). The focus of several studies has been to develop real-time
639 indicators to determine fish spoilage. Anthocyanins from PSP for grass carp monitoring (Jiang et
640 al., 2020), roselle anthocyanins for silver carp (Zhai et al., 2017), black carrot anthocyanins for
641 rainbow trout (Amiri et al., 2020), RCA (Silva-Pereira et al., 2015), Vitis amurensis (Ma et al.,
642 2017b) and dragon fruit peel (Apriliyanti et al., 2018) for fish fillets, black rice anthocyanins for
643 Hairtail (Ge et al., 2019), PSP & curcumin for bighead carp (Chen et al., 2020), amaranthus leaf
644 extracts for spade nose shark (Kanatt, 2020) and red beetroot, elderberry and blackberry for
645 atlantic mackerel has been used (Jamroz et al., 2019a). All the composite films displayed a
646 change in color on the spoilage of the fish products, acting as a visual spoilage monitoring film

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647 for fish spoilage.

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648 The freshness of shrimp determines its suitability for consumption. Shrimp quality can be
649 evaluated by determining the microbial levels of shrimp, sensory methods, and total viable count
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650 or TVB-N (Olafsdottir et al., 2004). The easiest way is sensory evaluation, but it is hindered in
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651 the case of a packaged product. Also, the determination of TVB-N levels requires a long time
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652 and laboratories (Kuswandi et al., 2012). Hence, the generation of a practical and simple method
653 for determination of shrimp quality, directly incorporated into the packaging, is necessary.
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654 Studies have reported various researches on the development of colorimetric indicators for
655 shrimp quality determination based on natural pigments. Black rice anthocyanins (Wu et al.,
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656 2019; Ge et al., 2019), Echium amoenum (Mohammadalinejhad et al., 2020), haskap berries (J.
657 Liu et al., 2019), Jambolan fruit anthocyanins (Merz et al., 2020), Ruellia simplex flower
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658 (Listyarini et al., 2018), PSP and RCA (Zhang et al., 2020), Curcumin (Ezati & Rhim, 2020; Wu
659 et al., 2019; Liu et al., 2018; Ma et al., 2017a), cactus pears (Yao et al., 2020) and red pitaya peel
660 (Qin et al., 2020) has been used. All these films were sensitive to the volatile compounds
661 generated on the spoilage of shrimp and showed visible color change.

662 5.2 Meat

663 Meat and meat products mainly spoil due to microbial and enzymatic deterioration leading to the
664 production of various volatile amines by protein degradation. These changes result in the
665 variation of pH in the packaged food material (Sun et al., 2019). The fresh pork meat is very
666 susceptible to contamination by microorganisms and enzymatic deterioration when exposed to
667 the atmosphere. The proteins present in meat are prone to mildew and bacteria (Xiaobo, 2008).
668 The deterioration process can release a high amount of TVB-N, including ammonia and amine,

22
669 that bring about a variation in the pH of pork packaging (Liu et al., 2018). Anthocyanins from
670 (Yong et al., 2019a), Chinese bayberry (Yun et al., 2019), grape skins (Chi et al., 2020), PSP
671 (Choi et al., 2017), Prunus maackii (Sun et al., 2019), RCA (Vo et al., 2019), roselle anthocyanin
672 (Zhang et al., 2019), Lycium ruthenicum (Qin et al., 2019a) and curcumin from turmeric (Liu et
673 al., 2018) have been used as quality indicators in meat products. These films effectively sensed
674 pork spoilage, exhibiting their indicator potential through visual color change. Poultry meat has
675 high water content and protein content, which supports microbial growth, rendering the food
676 products highly perishable. (Shukla et al., 2016). Jamun fruit skin extract anthocyanins (Talukder
677 et al., 2020) and amaranthus leaf extract (Kanatt, 2020) are useful for determining the spoilage of

of
678 chicken.

ro
679 5.3 Milk
680 -p
Dairy products are known to be highly susceptible to chemical and microbial deterioration
during storage and distribution; thus it is essential to find a cost-effective, real-time indicator to
re
681
682 monitor these products visually. The variation in acidity and corresponding pH are the most
lP

683 reliable spoilage indicators. Many pH indicator films have been employed in the visual
684 monitoring of milk with anthocyanins from various sources: carrot (Goodarzi et al., 2020), grape
na

685 skins (Ma & Wang, 2016), purple and black eggplant extracts (Yong et al., 2019c), PSP (Liu et
686 al., 2017), and mulberry (Y. Liu et al., 2019). These studies observed that on spoilage, the acidity
ur

687 of milk increases because of the production of organic acids, thus decreasing pH and brings
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688 about a change in color of the pH sensing intelligent films.

689 5.4 Others

690 5.4.1 Oil
691 The rancidity of oil is caused by fat oxidation and results in off-flavor and odor. Wheat gluten
692 films with chlorophyll used to assess the oil oxidation showed high sensitivity to oxygen and
693 also prevented oxidation by exhibiting strong antioxidant properties (Chavoshizadeh et al.,
694 2020).

695 5.4.2 Banana

696 It is observed that glucomannan films containing brazilin extracts are effective in monitoring the
697 spoilage of banana. The banana starch converts into soluble sugars due to respiration, enzymatic,

23
698 and microbial deterioration. This increases the pH and leads to color variations in films,
699 monitoring the quality of banana (Kurnianto et al., 2020).

700 6. Advantages and Disadvantages

701 6.1 Advantages
702 The intelligent packaging films with natural bioactive polyphenols have been effectively
703 evaluated for different perishable food materials. The pigments incorporated in films are highly
704 sensitive to pH, temperature, light, time, and ammonia that enable the composite films to act as
705 an indicator in monitoring the spoilage of packaged food products. These pigments are also

of
706 easily available at a very low cost. These films possess immediate sensing abilities and thus

ro
707 provide real-time freshness monitoring. It has been observed that these films offer excellent U.V
708
709
-p
radiation and light barrier properties, which may otherwise cause deterioration of the product.
Also, the incorporation of pigments increased the film thickness, when compared to
re
710 biodegradable films without the pigments, due to effective cross-linking between the matrix and
lP

711 pigments. Since the bioactive pigments used are rich in polyphenols that exert excellent
712 antioxidant and antimicrobial properties, they are effective in preventing deterioration of the
na

713 packaged food against oxidative reactions and various food borne microorganisms. These films
714 are also characterized by low moisture content and represent better integrity of the
ur

715 microstructure. Overall, the active and intelligent packaging films developed with plant-derived
Jo

716 natural pigments are safe and non-toxic, to be effectively used in food packaging.

717 6.2 Disadvantages

718 Although the packaging films developed with biodegradable polymers and naturally derived
719 pigments are effective in food packaging, they also possess certain drawbacks. The films are
720 prone to thermal degradation as well as degrade with time and illumination. Most of the films
721 exhibit high oxygen and water vapor permeability due to compact inner structures that are not
722 desirable characteristics of a food packaging material and may lead to product deterioration. The
723 values observed for tensile strength and elongation at break were also not desirable for many
724 composite films, presenting dissatisfactory mechanical properties. Low swelling capacity is
725 observed with the increase in the content of polyphenols that affect the color response efficiency
726 of the films. The major drawback is that these phenolic pigments do not remain active for an

24
727 extended period. These drawbacks may present a hindrance and maybe overcome through further
728 research.

729 7. Future Prospects

730 The results of numerous research studies have established the potential of effectively employing
731 active and intelligent packaging systems containing natural plant extracts for quality monitoring
732 of various perishable products. Further improvements can be focused on enhancing safety, and
733 research can be carried out to ensure the prevention of toxicity in the films, which may be caused
734 due to degradation when exposed to the natural environment, and thus produce stable packaging.

of
735 Most of the natural products and the waste generated through them consist of bioactive

ro
736 polyphenols in abundance. Food wastes from different processing industries and inedible parts of
737
738
-p
plants can be researched upon as effective sources for deriving phenolic compounds that could
further be used for the development of real-time indicators. The valorization of otherwise waste
re
739 substances would generate great economic value and provide more sustainable packaging. Also,
lP

740 different combinations could be assessed by employing various biodegradable polymers with
741 varying pigments. Since most of the studies are focused on high protein foods and milk, there is
na

742 a scope of research towards fruits and vegetables that are highly perishable and require non-toxic
743 intelligent indicators for visual spoilage monitoring. These packaging films can be optimized
ur

744 further and commercialized to be employed as active and intelligent packaging for visual quality
Jo

745 evaluation of fresh food products.

746 8. Conclusion
747 The effective potential of active and intelligent biodegradable films containing naturally derived
748 pigments in the real-time quality monitoring of perishable foods has been demonstrated by
749 several recent research. The packaging developed has displayed great sensitivity towards pH and
750 ammonia, showing variations in the color of the films and thus, exhibiting prospective use as a
751 visual indicator. Moreover, the polyphenolic bioactive compounds present in the films contribute
752 towards antioxidant and antimicrobial properties, which further enhances the shelf life of the
753 packaged foods. The use of food waste-derived pigments also contributes to the valorization of
754 waste food materials. The ease of availability and non-toxicity of these materials makes them a
755 suitable option to be used as food packaging. These packaging films also provide an added

25
756 advantage of attracting consumers due to the vibrant colors presented. Smart packaging systems
757 containing naturally-derived pigments from food and food wastes, thus, offer a simple, easy to
758 fabricate, safe, and cost-effective solution for the continuous, real-time monitoring of fresh
759 perishable food products, with an opportunity for commercialization.
760
761 Acknowledgment
762 All the authors are thankful to the National Institute of Food Technology Entrepreneurship and
763 Management, Haryana, India, for infrastructural and financial support to conduct the present
764 study.

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765

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41
Table 1. Bioactive compounds, sources and extraction methods/form

Bioactive
Category Sources Method of Extraction/Form of Use References
Compounds
Powdered PSP (50 g) in 500ml, 40% ethanol solution Jiang et al., 2020
Stirred (60˚C for 6h), filtered, and concentrated (50˚C).
Extract - freeze-dried (vacuum).
HCl solution of PSP anthocyanins. Liu et al., 2017
PSP powder (100 g ) in 1litre, 40% ethanol (12h at 60˚C) with Choi et al., 2017
Potato Sweet stirring. Filtered and evaporated (50˚C). Freeze-dried (2 days).
Potato HPLC-MS method – 100g PSP (powdered) in 500ml 80% ethanol Yong et al., 2019b
solution with 1% HCl ( 4˚C , 24h). Centrifuged (8000 x g, 20 min),
concentrated (35˚C) and lyophilized.
Purple Potato PSP powder (25 ) in 500ml acidified ethanol solution. Ultrasound Li et al., 2019
assisted extraction (270W, 50˚C, 30 min). Filtered and evaporated
(45˚C). Extract- freeze-dried (vaccum).
PSP & Red PSP(100g) & Red Cabbage (350g) soaked in 500ml, 70% ethanol Zhang et al., 2020

of
Cabbage solution. Adjust pH (2) with 1M HCl. Stored (4˚C,24 h) Centrifuge

ro
(4000 x g,10 min), filter, concentrate (50˚C) and freeze dry.
Red cabbage is crushed and blended with 85% ethanol. pH (2) Wu et al., 2020

-p
adjusted with 1M HCl (24h at 4˚C) in dark. Centrifuge (4000 rpm),
filtered and neutralized (pH 7) with 2M NaOH. Concentrate (40˚C)
re
and lyophilize (4˚C).
Red Cabbage powder (50 g) in 1litre of 50% ethanol solution. Treat Liang et al., 2019,
lP

Ultrasound treatment (540 W, 1h, 50˚C). Filter, concentrate and dry ( Vo et al., 2019
Red Cabbage 100˚C).
Food Products

Cabbage (25g) homogenized in 50ml, 10% ethanol solution, and Saliu & Della
na

refrigerated (20 min). Stirred (5 min, 800 rpm), filtered and purified Pergola, 2018
with resin. Freeze-dried (48h). Kept under nitrogen
(-20˚C).
ur

Red cabbage (150g) macerated with 80ml of 70% ethanol solution. Silva-Pereira et al.,
pH (2) adjusted with 1M HCl. Stored (5˚C, 24h). Filtered and 2015
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centrifuged (103 x g,10 min). Filtered and neutralized (pH 7) with

2.5 M NaOH.
Black and Rice (1kg) was ground and extracted thrice (3 liters of 80% ethanol Yong et al., 2019
Purple Rice solution and 1% HCl). Extract was filtered, centrifuged (8000 x g,
4˚C ,15 min)concentrated and vaccum dried (45˚C, 3 days).
Carrot (900g) was blanched (100˚C, 3 min) and added to Amiri et al., 2020
demineralized water (1L). Equal volume of HCl solution was added
(19:1). The suspension was cooled (0˚C, 3h; 27 ˚C, 8h) Filtered and
Black Carrot conditioned (2L methanol & 2Lwater). Methanol/glacial acetic
solution to wash anthocyanin. Store extract (4˚C in dark).
Water-soluble powder Goodarzi et al., 2020
Roselle calyx was dried and powdered. Powder (1g), 80% ethanol Zhang et al., 2019
(15ml) was added and pH (2) adjusted with 1M HCl. Heat (50˚C, 1h)
and centrifuge (3000 rpm, 6min). Evaporated (50˚C) in dark and
Anthocyanin
Roselle calyx freeze-dried
Dehydrated Roselle calyx was crushed and blended with 75% Zhai et al., 2017
ethanol solution (1:10, solid-liquid ratio) (2h, 25˚C). Centrifuge
(8000 rpm, 20 min). Evaporated (35˚C) in dark. Freeze-dried
(vaccum) and stored (4˚C).
 Echium Crushed flowers (10g) added to 200ml, 80% methanol, and stirred Mohammadalinejhad
amoenum (30 min, 30˚C). Extract - filtered and concentrated to 20 ml (37˚C). et al., 2020
Refrigerated under dark conditions
Chinese Chinese bayberries (250g) were ground and extracted with 1000ml of Yun et al., 2019
Bayberry 80% ethanol solution containing 0.5% HCl (4˚C, 24h). Extract was
centrifuged (8000 x g, 20min). Purified, concentrated (40˚C) and
vacuum dried.
Butterfly Pea Powder (5g) was added to 100ml distilled water and extracted (60˚C) Ahmad et al., 2020
with stirring for 1h and homogenized for 15min. Filtered and stored
(4˚C) in dark.
Haskap Haskap berries (100g) were extracted in ethanol solution (400ml) Liu et al., 2019a
Berries with 1% HCl (24h, 4˚C). Extracts are centrifuged (8000 x g, 20min).
Concentrated (35˚C) and dried (vaccum)
Hibiscus Dry hibiscus flowers (3g) were dispersed in distilled water (27g) and Peralta et al., 2019
stirred (100rpm) in an incubator shaker (25˚C, 4h) and filtered.
Jambolan fruit Jambolan was washed and dried (20˚C, 4h). The pulp and seeds were Merz et al., 2020

of
separated. Pulp was lyophilized (-18˚C) milled and stored (4˚C).
Dried pulp (1g) was added to acidic water solution (200ml) and

ro
agitated (100rpm; 30, 60, and 80 min; 35˚C).
Lycium Dried fruit (200g) was extracted with 400ml, 80% ethanol solution Qin et al., 2019a
ruthenicum
Murr
-p
with 0.5% HCl (4˚C, 24h). Filtered and centrifuged (8000 x g,
10min, 4˚C. Purified, concentrated, and vacuum dried.
re
Purple Corn Purple corn kernels (1kg), extracted with 80% ethanol with 0.5% Qin et al., 2019b
HCl ( 4˚C, overnight). Filtered, evaporated, and purified. Extracts
lP

were vacuum dried and stored (-20˚C).

Ruellia Washed and weighed flowers (80g), and blended, then added to Listyarini et al.,
na

simplex 100ml of 70% ethanol solution and macerated. pH (2) adjusted with 2018
flower HCl, filtered and stored (5˚C, 24h) in a dark bottle.
Mulberry Mulberry (100g) was ground and extracted with 80% ethanol with Liu et al., 2019b
ur

1% HCl solution (4˚C, 24h). Centrifuged (10000 x g, 30min),

supernatant concentrated (50˚C) and vacuum dried.
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Prunus Fruit were washed, squeezed and centrifuge (3000rp, 5min). Sun et al., 2019
maackii Separated from supernatant and stored in a sterile glass bottle (5˚C).
Juice (10ml) was dried (100˚C) till constant weight.
Red Radish Radish was cleaned, cut, and dried (65˚C) under vacuum. Crushed Zhai et al., 2018
and added to 80% ethanol solution. Stirred (35˚C, 6h), filtered and
supernatant concentrated (45˚C) in dark. Extract was freeze-dried and
stored in dark bottles (4˚C), under nitrogen
Anthocyanins Purple Sweet PSP slices dried (50˚C), milled, ethanol solution of powder (1:20) for Chen et al., 2020
& Curcumin Potato and 3h at 50˚C. Curcumin powder added
Curcumin
1% curcumin solution in 10ml of 25% ethanol solution. Wu et al., 2019
0.04% w/v solution of curcumin in the ethanol-water mixture. Musso et al., 2017
Curcumin Turmeric
Curcumin Powder. Liu et al., 2018
Dissolution of curcumin in 1M NaOH solution. Ma et al., 2017a
40mg of curcumin in 10ml ethanol Wang et al., 2019
Betalains Cactus Pears Fruits were juiced and immersed in 2L, 60% ethanol solution (4˚C, Yao et al., 2020
12h). Centrifuged (30min, 10000 x g) and concentrated. Extract was
purified and vacuum dried.
 Diana Co. Chlorophyll Solution 30% (w/w) Chavoshizadeh et
(UK) al., 2020
Spinach Spinach was blanched (15min) and crushed at high speed ( 4 min). Veiga-Santos et al.,
Chlorophyll Aqueous solution wasstored in a plasma freezer (-30˚C) 2010
Green tea & Tea powder (2g) was mixed in 200ml distilled water, controlled Jamróz et al., 2019
Pu-erh tea (90˚C, 20min) and filtered.
Chlorophyll & Green Tea & Green tea and basil leaves were immersed in 100ml distilled water Medina-Jaramillo et
Carotenoids Basil and heated (100˚C, 40min). The extracts were cooled, filtered, and al., 2017
stored in dark bottles.
Chlorophyll, Latos-Brozio &
Lutein, β- Food Colours Powders Masek, 2020
carotene & (Poland)
Curcumin
Quercetin Sigma- Masek et al., 2018
Aldrich, Powder
Germany

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Myoglobin Meat Scraps The meat scraps were blended with distilled water (1:2), followed by Santos et al., 2020
centrifugation (1600 rpm, 5min, 25˚C) and filtration.

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Blueberry The baggase was frozen (-40˚C) before lyophilization, milled and Luchese et al., 2017
Agro-waste sieved to obtain the extracts.

Blueberry
-p
P omace was separated by filtration, freeze-dried, milled and sieved Luchese et al., 2018
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pomace
Blueberry Blueberry residue powder Andretta et al., 2019
lP

residue
Blackberry & Microwave extraction (2450MHz, 2min), 75% stirring, ventilation Kurek et al., 2018
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Blueberry after extraction (2 min). Extraction (50˚C) with ethanol as solvent -

Pomace microwave ( 600W, 10 min). Extracts were cooled, filtered and the
solvent evaporated. Stored (18˚C).
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Black rice bran was ground and blended with ethanol: 1M HCl Wu et al., 2019; Ge
Black Rice mixture (85:15) at a solid-liquid ratio of (1:30) for 24h under dark. et al., 2019
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Bran Extracts are centrifuged (4000rpm, 20 min) and neutralized (pH 7)

with 1M NaOH. The extract is concentrated (40˚C) and lyophilized
Food waste

(4˚C)
Jamun Fruit Jamun fruits were washed and peeled. Peels were dried (48hours, Talukder et al., 2020
Skin 27˚C), macerated and added to 10ml of 1% HCl-ethanol mixture.
50ml slurry is added to a centrifuge tube and refrigerated overnight.
The slurry was centrifuged ( 2000 x g, 15min). The supernatant was
Anthocyanin transferred to colored bottles and refrigerated, to avoid discoloration.
Grapes were washed and peeled. Grape skin was freeze-dried for 3 Chi et al., 2020
days, milled and sieved.
Grape skin Grape skin powder was macerated with 12M ethanol solution and pH Ma & Wang, 2016
(2) was adjusted with 1M HCl. Refrigerated (24h) and centrifuged (5
min, 3000rpm). Solvent was evaporated (50˚C) and diluted with
buffer solution. Dried (100˚C) till constant weight.
Black Seed coats (50g) were added to 1L of 80% ethanol with 1% HCl Wang et al., 2019
Soybean Seed (4˚C, 24 h). The extract was centrifuged (5000 x g, 4˚C, 15min).
Coat Supernatant was concentrated and lyophilized
Eggplant peel extracts were added to 100ml of water or 70% ethanol
solution and pH (2) was adjusted by acetic acid solution. Extraction Bilgiç et al., 2019
was done by stirring at room temperature (24h) and then
 Egg Plant ultrasonicated (30min). Filtered and concentrated (40˚C). Stored (-
Peels 18˚C).
Peels (100g) were extracted in 500ml of 80% solution with 1% HCl Yong et al., 2019a
(4 ˚C for 1 day). Centrifuged (8000 x g, 15 min, 4˚C), condensed
(35˚C) and vacuum dried
Vitis Husk was dried. Powdered and macerated with 70% ethanol solution Ma et al., 2017b
amurensis and pH (2) was adjusted with 1M HCl. Refrigerated (24 h) and then,
husk centrifuged (3000, 5min). The solvent was evaporated (50˚C) and
extract obtained.
Black Bean Black bean seed coat (1g) was added to 30ml of acidified ethanol and Prietto et al., 2017
Seed Coat agitated (1h). Supernatant was separated and 20ml of acidified
ethanol was added. Extracts were filtered and diluted with acidified
ethanol.
Turmeric Turmeric residue was obtained by the Soxhlet method (47˚C, 3h). Maniglia et al., 2015
Residue Ethanol/Isopropanol mixture was used as a solvent. The residue was
Curcumin subjected to steeping, milling, sieving, and drying. The liquid

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fraction obtained was centrifuged and further dried to obtain turmeric
flour.

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Peels (300g) were minced and extracted twice with 800ml of 30% Qin et al., 2020
Dragon Fruit
Peel
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ethanol solution (4˚C, overnight). The solution was filtered and
centrifuged (8000 x g,15min, 4˚C). The extract was purified,
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concentrated and vacuum dried
red pitaya peel (50g) was extracted with 50ml boiled distilled water Apriliyanti et al.,
lP

Betalains (5 min) and filtered. 2018

Amaranthus The leaves were separated, washed, and dried in a hot air oven Kanatt et al., 2020
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Leaf (45˚C). Powdered, added to distilled water containing 0.1M citric

acid (1:10), and agitated (150 rpm,18h). Centrifuged (12100 x g, 30
min). Supernatant was filtered and the extract was obtained.
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Cashew Nut Testa was milled (500rpm,1 hour) and MilliQ water was added Lee et al., 2020
Testa (1:10). The mixture was stirred and incubated in a water bath for (1h,
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37˚C). Centrifuged (10000 x g, 10min, 4˚C ). Supernatant was

filtered and freeze-dried.
Tannins Pomegranate Pomegranates (500g) were washed, and flesh and peel were Liu et al., 2020
Peel separated. The flesh and peel were individually ground and then
extracted (4˚C, 24h) with 1L ethanol solution with 1% HCl. The
extracts were centrifuged (8000 x g, 20min), evaporated (50˚C) and
vacuum dried.
Brazilin Sappan Wood Sappan wood (100g) was macerated with 200ml of 30% ethanol (1h) Kurnianto et al.,
and filtered. 2020
PSP – Purple Sweet Potato

HCl – Hydrochloric Acid

NaOH – Sodium Hydroxide

HPLC-MS – High-Performance Liquid Chromatography-Mass Spectrometry

Table 2. Properties and Applications of bioactive active compounds

Bioactive Activation Indication

Source Base Film Application Properties References
Compound Mode (color change)
Carboxymethyl pH Fish Light Purple to Film Thickness, Jiang et al., 2020
Purple Sweet cellulose/Starch (TVB-N) Blue Black TS, Light Barrier
Potato Agar/ Potato Starch pH Pork Red to Green ___ Choi et al., 2017
(TVB-N)
Potato Starch/PVA pH Milk Purple – Deep Antimicrobial, Liu et al., 2017
(Acid) Red Mechanical
Properties (TS &
EAB)
Purple Sweet Starch /PVA pH Shrimp Light Purple- Film Thickness, Zhang et al., 2020
Potato & Red (TVB-N) Bright Red- Light Barrier,

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Cabbage Blue- Green Thermal Stability
Chitosan /PVA pH Pork Pink to Mechanical Vo et al., 2019

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(TVB-N) Yellowish/Pale Properties ( TS &
-Green EAB)
Red Cabbage Carboxymethyl
Cellulose
-ppH
(TVB-N)
Protein-
Rich Foods
Light Purple to
Green
Thermal Stability,
Light Barrier
Liang et al., 2019
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Ethyl Cellulose CO2 Poultry Blue to Pink Stable for several Saliu & Della
weeks under cold Pergola, 2018
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Anthocyanin storage.
Chitosan/Corn Starch pH Fish Pink –Blue - Thermal Stability, Silva-Pereira et
(TVB-N) Yellow Light Barrier al., 2015
na

Chitosan/Starch/PVA pH Pork Red-Green- TS, Antioxidant Zhang et al., 2019

Roselle calyx (TVB-N) Yellow
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Starch/PVA pH Fish Purple-Green- Film Thickness, Zhai et al., 2017

(TVB-N) Yellow EAB
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Agarose Solution pH Chicken Pink to Yellow ___ Talukder et al.,

Jambolan Fruit (TVB-N) 2020
Chitosan pH Shrimp Pink-Red-Blue Film Thickness Merz et al., 2020
(TVB-N)
k-carrageenan pH Pork Purple to Green Hydrophobic, Chi et al., 2020
Grape Skin (TVB-N) Light Barrier,
Film Thickness
Tara Gum/Cellulose pH Milk Purple to Dark Oxygen Barrier, Ma & Wang,
(Acid) Red Light Barrier, 2016
EAB
Cellulose-based paper Time- Fish Deep Blue to Amiri et al., 2020
Temperature (Rainbow Wine Red ___
Black carrot Trout)
Potato Starch pH Milk Blue-Black to Water Resistance Goodarzi et al.,
(Acid) Light Purple 2020
Echium Cellulose pH Shrimp Violet –Grey- ___ Mohammadalinej
amoenum (TVB-N) Yellow had et al., 2020
Prunus maackii k-carrageenan pH Lard (Pork) Purple Red – Antioxidant, Sun et al., 2019
(TVB-N) Blue – Blue Mechanical
Grey Properties (TS &
EAB), Oxygen
 Barrier, Thermal
Stability, Light
Barrier
Egg Plant Chitosan pH Milk Blue-Purple Film Thickness, Yong et al.,
Extracts (Acid) Mechanical 2019c
properties (TS &
EAB), UV-vis
Light Barrier,
Antioxidant
Chitosan/Chitin pH Seafood Purple – Grey UV- Barrier, Wu et al., 2019
(TVB-N) Blue - Brown Antioxidant
Black Rice Bran Gelatin/oxidized chitin pH Shrimp & Purple – Grey Water and Ge et al., 2019
crystals (TVB-N) Hairtail Blue - Brown Oxygen barrier,
UV-Barrier,
Antioxidant

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Black and Purple Chitosan pH Pork Blue - Purple Film Thickness, Yong et al.,
Rice (TVB-N) EAB, Light 2019a

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Barrier,
Antioxidant
Vitis amurensis Tara Gum
-p
pH
(TVB-N)
Fish Purple- Green Oxygen Barrier,
Water Barrier
Ma et al., 2017b
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Haskap Berries Fish Gelatin pH Shrimp Brown to Antioxidant, J. Liu et al., 2019
lP

(TVB – N) Green Mechanical

properties (TS &
EAB), Water
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vapor Barrier,
UV-vis Barrier
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Lycium Starch pH Pork Pink – Purple- Antioxidant, Film Qin et al., 2019a
ruthenicum Murr (TVB-N) Green/Yellow Thickness, TS,
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Thermal Stability,
Water Barrier,
UV-vis light
Barrier
Mulberry k-carrageenan pH Milk Greenish black Film Thickness, Y. Liu et al., 2019
(Acid) to Pink TS, Water
Barries, UV-vis
Light Barrier,
Thermal Stability,
Antioxidant
Chinese Cassava Starch pH Pork Purple/Light Film Thickness, Yun et al., 2019
Bayberry (TVB-N) Blue-Orange- Water Barrier,
Yellow/Brown TS, UV-vis Light,
Antioxidant
Ruellia simplex Cellulose-based paper pH Shrimp Purple –Blue – ___ Listyarini et al.,
flower (TVB-N) Greenish Grey 2018
Butterfly Pea Sago Powder pH Chicken Blue to Green Film Thickness, Ahmad et al.,
Flow (TVB-N) Low water 2020
solubility
Red Radish Gelatin pH Milk/Fish Red to Dark Mechanical Zhai et al., 2018
 (Acid/TVB- Red/Orange- properties (TS &
N) red to Green to EAB), Oxygen &
Yellow-Green Water Barrier,
UV – vis Light
Barrier
Anthocyanin Purple Sweet Starch/PVA pH Big Head Yellow to Chen et al., 2020
& Curcumin Potato & (TVB-N) Carp Grey-Brown ___
Curcumin
k-carrageenan pH Shrimp and Yellow to Red TS, Oxygen and Liu et al., 2018
Curcumin Turmeric (TVB-N) Pork Moisture Barrier,
Light Barrier
Chitin pH Meat/Shrim Yellow to Antioxidant, TS, Wu et al., 2019
(TVB-N) p Orange - Red Water Barrier,
Light Barrier
Tara Gum/PVA pH Shrimp Yellow to EAB, Water Ma et al., 2017a

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(TVB-N) Orange-Red Barrier, Thermal
Stability

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Pectin powder/Glycerol pH Shrimp Yellow to Film Thickness, Ezati & Rhim,
(TVB-N) Brown Light Barrier, 2020

-p Water Barrier,
Thermal Stability,
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Antimicrobial,
Antioxidant
lP

Amaranthus Leaf Gelatin/PVA pH Chicken/Fis Red to Yellow Film Thickness, Kanatt et al.,
(TVB-N) h Antioxidant, 2020
Betalains Antibacterial, TS,
na

Oxygen, and
Water Barrier,
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Low Solubility
Cactus Pears Chitosan/PVA pH Shrimp Purple – Film Thickness, Yao et al., 2020
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(TVB-N) Orange - Antioxidant,

Yellow Antimicrobial,
Mechanical
Properties (TS &
EAB), UV – vis
light Barrier,
Water Barrier
Glucomannan/PVA pH Fish Pink to yellow ___ Apriliyanti et al.,
Red Pitaya Peel (TVB – N) 2018
Starch/PVA pH Shrimp Purple to Film Thickness, Qin et al., 2020
(TVB – N) Yellow Mechanical
Properties (TS &
EAB),
Antioxidant,
Antimicrobial,
UV-vis Light
Barrier, Water
Barrier
Chlorophyll Plants Wheat Gluten Oxygen Sesame Oil Green to Mechanical Chavoshizadeh et
Yellow properties (TS al., 2020
 &EAB),
Antioxidant
Brazilin Sappan Wood Glucomannan/PVA CO2 Banana Yellow to ___ Kurnianto et al.,
Ruby-Red 2020

TS – Tensile Strength

EAB – Elongation at Break

TVB – N – Total Volatile Basic – Nitrogen

UV – vis – Ultraviolet visible

PVA – Polyvinyl alcohol

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Fig. 1. Sources of bioactive pigments

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Highlights
• Smart packaging with naturally derived pigments facilitate real-time fresh food monitoring
• Utilization of food waste in biodegradable packaging helps in valorization of food waste
• Easy to fabricate, safe and cost-effective solution for continuous visual monitoring

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