Review Not peer-reviewed version

Biobased Filler Materials in Polymeric

Composites: A Comprehensive Review
of Epoxy and Polyurethane Systems

Stanley Chibuzor Onwubu * , Deneshree Naidoo , Zodidi Obiechefu , Thabang Hendrica Mokhothu

Posted Date: 17 February 2025

doi: 10.20944/preprints202502.1233.v1

Keywords: Biobased fillers; polymeric composites; epoxy resin; polyurethane foam; sustainability; natural
reinforcements; mechanical properties; thermal stability; eco-friendly materials; waste valorization

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Review

Biobased Filler Materials in Polymeric Composites:

A Comprehensive Review of Epoxy and Polyurethane
Systems
Stanley Chibuzor Onwubu 1,*, Deneshree Naidoo 1, Zodidi Obiechefu 1 and Thabang Hendrica
Mokhothu 1
1 Department of Chemistry, Faculty of Applied Sciences, Durban University of Technology, Durban, South
Africa
* Correspondence: [email protected]

Abstract: Polymeric composites, particularly epoxy and polyurethane systems, have gained
significant attention due to their excellent mechanical, thermal, and chemical properties. However,
the environmental concerns associated with petroleum-based polymers have driven research
towards biobased alternatives. This review explores the integration of biobased filler materials
derived from agricultural and marine waste into epoxy and polyurethane matrices to enhance their
performance while promoting sustainability. The empirical review of epoxy and polyurethane resins
reinforced with natural fillers highlights the significant role of bio-based additives in enhancing
mechanical properties while promoting sustainability. Findings from reviewed studies demonstrate
that natural fillers such as jute, sisal, lignin, and rice husk fish scales improve tensile strength, flexural
strength, and wear resistance of polymer composites. However, excessive filler content can lead to
agglomeration, reducing mechanical integrity. Optimal filler content varies depending on polymer
type, with moderate concentrations yielding the best mechanical performance. Additionally,
chemical modifications, such as silane treatment and alkalization, enhance filler-polymer adhesion,
further improving material properties. Despite their advantages, challenges such as moisture
sensitivity and long-term durability require further investigation.

Keywords: Biobased fillers; polymeric composites; epoxy resin; polyurethane foam; sustainability;
natural reinforcements; mechanical properties; thermal stability; eco-friendly materials; waste
valorization

1. Introduction
Polymeric composites are materials composed of a polymer matrix reinforced with fillers or
fibers to improve their mechanical, thermal, and chemical properties. These composites are
extensively used in industries such as aerospace, automotive, and construction due to their
customizable properties, lightweight nature, and high strength-to-weight ratios [1,2]. Among
commonly used polymer matrices, epoxy resins and polyurethane foams (PUF) stand out due to their
versatility and superior performance. Epoxy resins are renowned for their excellent chemical
resistance, mechanical strength, and thermal stability, but their intrinsic brittleness limits their impact
resistance [3,4]. Similarly, PUF materials are prized for their flexibility, biocompatibility, and tunable
mechanical properties, making them suitable for applications ranging from insulation to automotive
interiors [5].
Despite their widespread applications, traditional polymer production heavily relies on
petrochemical derivatives, raising significant environmental concerns [6,7]. Furthermore, the
mechanical properties of bio-based alternatives, such as soy-based PU, often lag behind their
petroleum-based counterparts [5]. To mitigate these challenges, researchers have increasingly
explored the incorporation of natural fillers and reinforcements to enhance the mechanical and

© 2025 by the author(s). Distributed under a Creative Commons CC BY license.

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thermal properties of polymeric composites while advancing sustainable materials development [8].
Biobased fillers derived from agricultural and marine waste are gaining attention for their
renewability, cost-effectiveness, and environmental benefits [9]. Previous studies have shown that
natural fibers such as wood fiber [10], sawdust [11], eggshells [12], and coconut husks [13] among
others can significantly enhance the mechanical properties of polymer composites.
In the polymer industry, the growth in bio-based, biodegradable, and recycled materials has a
huge positive impact on the environmental research and development field [14]. With a massive
growth in the development of science especially in polymer fields, it is of good concern to develop
and synthesize new and improved methods and materials used in our daily lives for cost-
effectiveness, reducing toxic pollutants such as emissions and using up waste products of everyday
human lifestyle to develop newer biomaterials [14]. As many of the polymers currently used in
different industrial applications are harmful to the environment [15,16], it is necessary to incorporate
eco-friendly and recycled ways to manufacture polymeric materials to improve the quality
(strengthening) of the product and reduce the build-up of food product waste causing numerous
environmental factors.
Besides, the versatility of polymer composites comes from the ability to tailor their properties by
selecting appropriate matrix materials and reinforcements [17]. The main function of these
reinforcements is to enhance the mechanical properties of the composite, including strength, stiffness,
and durability, without adding significant weight [18–21]. Reinforcements work by distributing loads
more efficiently throughout the composite [22,23]. Nilagiri Balasubramanian and Ramesh [24] note
that better improvement in mechanical, thermal, and electrical properties could be attained along the
filler-aligned direction. Fibers, for instance, align along the direction of applied stress, allowing the
composite to bear heavier loads and resist deformation. The inclusion of powders or particulate
fillers, such as silica or calcium carbonate, can also improve the hardness and wear resistance of the
composite, contributing to its longevity in demanding applications [25,26].
Given the beneficial properties of reinforcement in enhancing the properties of polymeric
materials, this review highlights the role of biobased reinforcement materials in enhancing the
mechanical, thermal, and chemical performance of polymer composites. By summarizing current
developments and research trends, the paper aims to provide a foundation for further studies,
particularly the potential of incorporating recycled biobased materials, as fillers to reinforce epoxy
and polyurethane polymers. This approach aligns with the broader goal of advancing eco-friendly
and high-performance composite materials.

2. Epoxy Resin and Polyurethane as Matrix Materials

Two of the most widely used matrix materials in polymer composites are epoxy resin and
polyurethane, both of which provide a range of desirable properties for industrial applications.

2.2.1. Epoxy
Epoxy resin is a thermosetting polymer known for its excellent mechanical strength, chemical
resistance, and adhesive properties [27]. It forms a highly cross-linked structure when cured, making
it highly resistant to environmental factors such as moisture, heat, and chemicals. Because of its
strength and durability, epoxy resin is commonly used as a matrix material in high-performance
composites, especially in the aerospace, automotive, and construction industries. Epoxy polymers
stand out as popular polymer matrices for composite applications owing to their exceptional
mechanical properties, chemical resistance, and thermal stability [1,28]. Despite these strengths,
epoxy polymers exhibit limitations such as low impact resistance, poor toughness, and susceptibility
to crack propagation [3]. To improve the physical and mechanical properties of this polymer,
several current reinforcing materials such as natural fibers, glass, and graphite have been added to
epoxy to such an extent that epoxies can be used in many structural applications [29].
Epoxy resins are widely used in composites reinforced with glass or carbon fibers, where they
enhance the material's tensile and flexural strength. In aerospace and automotive applications, epoxy-
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based composites provide a lightweight yet strong alternative to traditional metals, contributing to
fuel efficiency and improved performance. Additionally, the biocompatibility of epoxy resins makes
them suitable for use in biomedical devices such as prosthetics, implants, and medical adhesives.
According to Fink [30], epoxy resins are favoured in composite manufacturing because of their low
shrinkage upon curing, excellent adhesion to a wide variety of substrates, and superior mechanical
performance under a broad range of conditions. From a chemistry perspective, epoxy resins represent
a crucial and highly adaptable category of cross-linkable polymers, derived from monomers
containing at least two oxirane groups [31]. These strained-ring structures, composed of one oxygen
and two carbon atoms, are attached to a diverse array of aliphatic or aromatic organic molecules [31].
The majority of commercially significant epoxy resins are synthesized through the reaction of
polyphenolic compounds or other active hydrogen-containing molecules (such as amines or aliphatic
alcohols) with epichlorohydrin in basic conditions. Among these, bisphenol A (diphenylolpropane)
is one of the most widely used phenolic compounds, forming the foundation for an entire family of
epoxy resins with a characteristic general structure (Figure 1).

Figure 1. Structure of epoxy resins.

2.2.2. Polyurethane
Polyurethane (PUF) is another versatile polymer matrix widely used in composites. Unlike
epoxy resin, which is primarily a thermosetting polymer, polyurethane can be either thermosetting
or thermoplastic, depending on its formulation. Polyurethane composites are known for their
flexibility, abrasion resistance, and impact strength, making them useful in both structural and non-
structural applications. Polyurethane foams (PUF), widely used in various industries, are versatile
materials known for their lightweight nature, insulation properties, and affordability [32,33]. In
engineering, for example, PUF is widely used due to its tunable mechanical and biocompatible
properties which can be tailored by the type and composition of their components [5]. In the
construction industry, polyurethane-based composites are used for insulating panels and coatings
due to their thermal insulation properties. In the automotive and transportation sectors, polyurethane
composites provide shock-absorbing components such as bumpers and seat cushions. The
biocompatibility of polyurethane also allows it to be used in medical devices such as catheters and
artificial organs, where flexibility and durability are essential.
Polyurethane (PUF) polymers are synthesized through a reaction between diisocyanates and
polyester diols[6,33], a fundamental process in the polyurethane industry. The PUF macromolecule
consists of alternating non-polar segments: the hard segment (HS), derived from aliphatic or aromatic
isocyanates, and the soft segment (SS), typically derived from macrodiols such as polyester,
polyether, or polycarbonate-based compounds (Figure 2). Each segment contributes distinct
properties to the polymer. The HS imparts stiffness, abrasion resistance, and film-forming
capabilities, while the SS enhances elastomeric properties [34]. The chemical composition of these
segments significantly influences the overall characteristics of PUF materials [35]. For instance,
aliphatic isocyanates in the HS improve environmental stability compared to their aromatic
counterparts [36]. Similarly, polyester-based polyols in the SS provide high tensile strength and
excellent resistance to light and aging, while polyether-based polyols enhance chain flexibility and
elasticity but are more susceptible to degradation by heat, light, and oxygen. Polycarbonate-based
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polyols, on the other hand, offer superior hydrolysis and aging resistance, along with good
mechanical strength [37].

Figure 2. Polyurethane chemical structure (source: Patti, Costa, Perrotti, Barbarino and Acierno [35].

2.3. Natural Fillers in Polymer Chemistry

Natural fiber-reinforced polymer composites have a long history of use in civil engineering
construction due to their advantageous properties and suitability for various applications [38].
Ancient civilizations used natural materials like mud and straw in construction, and early composite
products such as pottery and boats utilized straw for reinforcement. The modern development of
composite materials began during the chemical revolution of the late 19th century, with the creation
of synthetic resins and the introduction of fiberglass in the early 20th century marking significant
advancements [38]. Synthetic materials like vinyl, polystyrene, phenolic, and polyester offered
improved performance compared to their predecessors. Natural fiber composites have since gained
prominence as eco-friendly alternatives to synthetic materials, offering benefits like low density, cost-
effectiveness, and renewability, despite challenges such as high moisture absorption requiring
chemical treatments [38,39].
Table 1 provides a comprehensive overview of the application of natural filers in polymers.
Natural fibers, such as plant fibers (e.g., jute, hemp) and animal fibers (e.g., wool, silk), have been
extensively studied as reinforcements in polymer composites due to their renewability, low cost, and
biodegradability [39,40]. These natural fibers offer advantages such as high specific strength and
stiffness, good thermal insulation properties, and reduced environmental impact compared to
synthetic fibers [39,40]. Natural fibers play a critical role in polymer chemistry, offering numerous
advantages and applications [41].Sourced from renewable materials like plants and animals, these
fibers are valued for their renewability, biodegradability, and enhanced mechanical properties [40].
Incorporating natural fibers into polymer matrices improves composite materials' overall
performance by enhancing strength, stiffness, and toughness [42].

Table 1. Comprehensive Overview of Research Papers on Natural Fibers/Fillers in Polymer Composites.

Type of natural Application of Historical dates

Research paper title Reference
fibers/fillers fiber/filler found and used

Cotton, wool, silk, Pre-20th

From natural to synthetic Textiles, clothing,
[43–45] jute, flax, wood century to
fibers construction materials
fibers or straw present

Plastics materials: Early plastics

Cellulose, wood
introduction and historical [46,47] formulations or their 1930s-1940s
fibers
development contemporary
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applications in
biocomposites

Plant-based natural fiber

Automotive,
reinforced composites: a Fibers like jute,
[48] construction, 1950s
review on fabrication, hemp, flax, bamboo
packaging
properties, and applications

Bioengineering and
Natural fiber-reinforced
environmental
composites for
engineering soil
bioengineering and Jute, coir, sisal,
[49] erosion control, 1960s
environmental engineering bamboo,
biodegradable
applications" by Hoi-yan
materials, wastewater
Cheung.
treatment

Fibers like jute, Automotive parts,

Natural fiber-reinforced
[39] kenaf, hemp, flax, construction materials, 1970s
polymer composites"
sisal packaging

Cellulose,
Recent advances of natural Structural components,
hemicellulose, and
fibers based green rubber consumer products, Late 20th
lignin. Ute, ramie,
composites: properties, [50] building, construction, century to
hemp, kenaf, silk,
current status, and future packing, and present
wool, angora,
perspectives automotive industries
mohair

A review: nanomaterials as a
Carbon nanotubes, Aerospace, electronics,
filler in natural fiber- [51] 21st century
graphene automotive
reinforced composites

Influence of filler material on

Epoxy, Marine, automotive,
properties of fiber-reinforced [52] Present
polyurethane civil engineering
polymer composites: a review

Recent progress on natural

fiber hybrid composites for Tailored performance Present and
[53] Hybrid composites
advanced applications: a requirements future
review

Previous research has focused on optimizing processing techniques, surface modification of

fibers, and compatibility with polymer matrices to maximize the mechanical performance of natural
fiber-reinforced composites [39,40]. The dispersion and alignment of these fibers within the polymer
matrix significantly influence the mechanical properties, underscoring the importance of optimizing
filler dispersion for maximum performance [41]. Additionally, natural fibers contribute to
lightweight and cost-effective composite materials, making them suitable for various industrial and
consumer applications [54]. With their biocompatibility and thermal insulation properties, natural
fibers are also utilized in medical devices and building materials [14]. In addition, the applications of
natural fiber-reinforced polymer composites span various industries, including aerospace,
automotive, construction, and packaging [55]. These composites find utility in manufacturing
household furniture, fencing, windows, decking, flooring, sports equipment, and lightweight
automobile components, among others [56,57]. Overall, the utilization of natural fibers in polymer
composites aligns with sustainable practices and offers versatile solutions for addressing
environmental and performance challenges [58].

2.4. Mechanical and Physical Properties of Composites with Bio-Based Reinforcements

The mechanical properties of polymer composites are significantly influenced by the
incorporation of bio-based reinforcements, such as natural fibers, and biopolymers. These materials
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offer sustainability, biodegradability, and favourable mechanical performance, making them

attractive for various industrial applications. This section examines empirical studies focusing on
tensile strength, flexural strength, impact strength, hardness, and other relevant mechanical
attributes.

2.4.1. Tensile Strength

Tensile strength is a critical mechanical property that determines how a composite material can
withstand pulling forces without failure [59]. It is typically defined as the maximum force that can be
applied in this manner before the material fractures [60]. Saba, et al. [61] note that tensile strength
evaluates the force needed to fracture a composite or plastic specimen and determines how much the
specimen stretches or elongates before reaching the breaking point. According to Ismail, Khulbe
and Matsuura [60], a tensile test is conducted using standard testing equipment following the ASTM
D638-10 method for measuring the tensile properties of plastics. Saba, Jawaid and Sultan [61] clarified
that tensile testing of composites typically involves basic tension or flat-sandwich tension testing,
following standards such as ISO 527-4, ISO 527-5, ASTM D638, ASTM D3039, and ASTM C297. These
tests generate stress-strain diagrams that are used to calculate the tensile modulus. An example of
tensile testing is illustrated in Figure 3.

Figure 3. Tensile testing machine.

When a material is exposed to a tensile pulling force, it stretches until it fractures. The results
are displayed as a curve illustrating the material's response to the applied forces [60]. Tensile testing
also measures properties such as tensile strength (both at yield and break), tensile modulus, tensile
strain, elongation, and percent elongation at yield, as well as percent elongation and elongation at
break [61]. These parameters help evaluate a material's appropriateness for specific applications [62].
Numerous empirical studies have shown that bio-based reinforcements, particularly natural fibers
can enhance the tensile strength of polymer composites [59,62]. For instance, Khan et al. (2020)
investigated the tensile properties of epoxy composites reinforced with jute fibers. The results
demonstrated a significant improvement in tensile strength and modulus compared to pure epoxy.
The tensile strength increased by 25% with the inclusion of 20% jute fiber, attributed to the effective
load transfer from the matrix to the fibers due to good interfacial adhesion. Jute fibers in epoxy
matrices demonstrated a 10.06% increase in tensile strength, showcasing the reinforcement's
effectiveness (Shah et al. 2023)
Mohammed et al. (2021) assessed the tensile behavior of composites reinforced with sisal fibers.
The tensile strength increased by 30% with 15% fiber addition, although the performance was highly
dependent on fiber-matrix bonding quality. Sisal fiber-reinforced epoxy composites achieved a
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tensile strength of 69.1 MPa, significantly outperforming neat epoxy (Huzaifa et al. 2024). Sisal fiber
reinforced with polyurethane composites enhanced tensile strength by up to sevenfold (17.0 MPa)
compared to neat polyurethane resin, with dry fibers improving fiber-matrix adhesion while humid
fibers offered higher elongation (11.3%) (Milanese, Cioffi and Voorwald 2011).
Kenaf/Epoxy composites exhibited the highest tensile strength, 3.1 times greater than the neat
resin, and achieved the highest Young's modulus at 50% fiber volume fraction (Hafizah et al. 2014).
Hybrid composites of bi-directional glass fiber and rice husk (RH) fiber in epoxy matrices achieved
the highest tensile strength (215.42 MPa) and modulus (1.8 GPa) with 25 wt.% glass fiber and 5 wt.%
RH fiber. Increasing RH content to 15 wt.% weakened interfacial bonding, reducing tensile properties
by 25% (Ismail et al. 2020). A more recent study by Onwubu et al. (2024) analyzed collagen-extracted
fish scale-reinforced epoxy composites. The addition of 5-10% fish scale collagen improved tensile
strength by 18% compared to the neat epoxy. The improvement was largely attributed to efficient
load transfer between the particulates and the polymer matrix.

2.4.2. Flexural Strength

Flexural strength indicates a material's ability to resist deformation under bending forces [63],
and bio-based reinforcements have shown considerable potential in enhancing this property in
polymer composites. The data is frequently utilized to choose materials for components that must
bear loads without bending [61]. The most common methods for flexural testing of plastics, polymer
composites, and large fiber-reinforced plates are three-point and four-point bend tests, conducted
following ISO 14,125, ISO 178, ASTM D790, and ASTM D6272. These tests provide valuable insights
into material properties and ensure their suitability for specific applications under various
conditions. Flexural properties testing delivers both raw and adjustable data, including flexural stress
and strain at yield, flexural stress and strain at break, flexural stress at 3.5% deflection (ISO) or 5.0%
deflection (ASTM), flexural modulus, and stress-strain curves. The flexural modulus serves as a
measure of a material's stiffness when subjected to bending [61].
An empirical study by El-Shekeil, et al. [64] on thermoplastic polyurethane (TPUF) reinforced
with 20–50 wt.% kenaf fibers reported increased flexural strength from 6.55 MPa (PUFre TPUF), with
higher fiber content improving both strength and modulus. Bamboo fiber-reinforced epoxy
composites demonstrated superior flexural strength compared to virgin epoxy and jute fiber
composites, with optimal performance at 5% NaOH-treated fibers [65]. Alkali-treated sugar palm
fiber-reinforced epoxy composites achieved the highest flexural strength (96.71 MPa, a 24.41%
improvement) with 10 wt% reinforcement using 0.25 M NaOH for 1 hour. Flexural modulus reached
6948 MPa (a 148% increase) with 0.5 M NaOH for 4 hours [66]. Bi-directional glass fiber and rice husk
(RH) fiber composites showed the best flexural strength (275.51 MPa) and modulus (9.79 GPa) with
25 wt.% glass fiber and 5 wt.% RH fiber, decreasing by 27% and 32%, respectively, at 15 wt.% RH
fiber [67].

2.4.3. Impact Strength

Impact strength is the material's ability to absorb energy during a sudden force or impact [61]
The impact test is specifically designed to assess the toughness, brittleness, notch sensitivity, and
impact strength of engineering materials in their ability to withstand high-rate loading [68,69]. Bio-
based reinforcements, including natural fibers and collagen-based materials, have been found to
enhance the impact resistance of polymer composites in various studies. In an empirical study by
Ribeiro, et al. [70], hemp fiber-reinforced epoxy composites showed an increase of 7.5% in impact
strength compared to the unreinforced epoxy. This improvement was due to the fibers' ability to
dissipate energy during impact, thus enhancing toughness. Similarly, Venkatachalam, et al. [71]
tested the impact of coir fiber-reinforced epoxy composites. The result reveals the maximum Impact
strength (98.35 J/m2) by combining coir fibre (5 wt.%), and coir fiber powder size (225 µm).
Furthermore, hybrid composites of bi-directional glass fiber and RH fiber achieved peak impact
strength (447.19 J/m) with 25 wt.% glass fiber and 5 wt.% RH fiber, outperforming other
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configurations [67]. The impact strength of Moringa oleifera bio-filler-reinforced epoxy composites
increased up to 12% v/v bio-filler content but declined beyond 16–24% v/v due to filler agglomeration
(Sridevi and Giri 2024). Epoxy-based composites with 3 wt.% Rohu fish scale residue powder
achieved an impact strength of 1908.2 J/m², a 54.72% increase over neat epoxy (Kumar, Bansal and
Singh 2019). Impact strength peaked at 22.22 kJ/m² with 30 wt.% fiber content in thermoplastic
polyurethane composites but decreased beyond this level due to fiber breakage (Radzi et al. 2017).

2.4.4. Hardness
Bio-based reinforcements offer other mechanical properties such as hardness, toughness, and
wear resistance. Hardness indicates a composite's resistance to surface deformation. The hardness of
polymer composites reinforced with bio-based materials was investigated by Martins et al. (2021),
where bamboo fiber-reinforced polyester composites showed a 12% increase in hardness compared
to pure polyester. The bamboo fibers' inherent stiffness and rigidity contributed to the improved
surface hardness, making the composites more resistant to indentation. In addition, an empirical
study by Agnihotri et al. (2022) examined the wear of bio-based hybrid composites reinforced with
hemp and silk fibers in an epoxy matrix. The wear rate was reduced by 30% compared to the neat
epoxy, highlighting the reinforcing effect of the bio-based fibers in reducing material loss under
friction.
Sisal-glass fiber-reinforced epoxy composites exhibited the highest hardness value (24.73 RHN)
(Huzaifa et al. 2024). Bamboo-coir epoxy resin composites achieved the highest Rockwell Hardness
Number (38 RHN), outperforming bamboo epoxy (20 RHN) and bamboo-jute epoxy (37 RHN)
composites (Bansal, Ramachandran and Raichurkar 2017). WPC with 50% finely ground wood filler
achieved the highest indentation hardness (56 MPa, a 125% improvement) and indentation modulus
(0.77 GPa, a 201% increase). Coarsely ground wood filler exhibited a hardness of 49 MPa (99%
increase), while slate fillers achieved 40 MPa (62% increase). These enhancements highlight the role
of filler type and content in improving WPC properties for applications such as tiling and window
frames (Dočkal et al. 2020).

2.5. Thermal Properties of Composites Reinforced with Particulate Fillers

According to Haque, et al. [72], the mechanical properties of polymers are significantly
influenced by temperature. Specifically, as temperature increases, the elastic modulus and tensile
strength decrease, while ductility improves [73]. To address these challenges, extensive research has
focused on enhancing the thermal properties of various polymers and developing heat-resistant
polymers for high-temperature applications requiring reliable performance[72].
Thermo-gravimetric analysis (TGA) is a widely used method to evaluate the thermal stability of
materials. TGA measures changes in a material’s physical and chemical properties as a function of
increasing temperature at a constant heating rate or over time at a constant temperature or mass loss
[74]. This technique provides insights into chemical processes such as desolvation (e.g., dehydration),
decomposition, and solid-gas reactions like oxidation or reduction. It also identifies physical
phenomena, including phase transitions, vaporization, sublimation, absorption, and desorption [75].
Sahu, Mondloe and Upadhyay [75] highlighted that TGA is instrumental in assessing the
thermal stability of polymers, ensuring their physical and chemical properties remain unchanged at
elevated temperatures. Researchers use TGA to determine the temperature at which a composite
begins to degrade, the weight loss with temperature increase, and the residue left behind [74].
Thermal stability within the desired temperature range is characterized by negligible mass loss and
minimal slope on the TGA curve. Additionally, TGA determines the upper application temperature
beyond which a material starts degrading [75].
Numerous studies have employed TGA to analyze epoxy composites. For instance, Wang, et al.
[76] investigated the thermal stability of pure epoxy and epoxy composites filled with 4.5 wt.%
KH550@EG. They observed initial decomposition temperatures of 318, 329, and 348 °C for untreated
and treated samples, respectively, concluding that surface treatment enhances compatibility and
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thermal stability. Similarly, Gu, et al. [77] examined graphene nanoplatelets (GNP) and functionalized
graphene nanoplatelets (f-GNP) composites. Their findings revealed improved thermal stability with
increasing f-GNP content, with heat resistance indices rising from 192 °C for pristine epoxy to 203 °C
for composites with 30 wt.% f-GNPs.
Xu and Chung [78] analyzed TGA data for composites filled with boron nitride and aluminum
nitride particles, comparing surface-treated samples with those treated using acetone or acids. They
reported that silane-treated samples exhibited higher weight loss compared to acid- or acetone-
treated samples. Liang and Wong [79] studied nanocomposites with 1 wt.% SiO2 or Al2O3 fillers and
hybrid composites containing 1 wt.% nano-fillers and 20 wt.% micro-fillers. Their results showed that
both micro- and hybrid composites exhibited significantly lower weight loss compared to neat epoxy,
with SiO2-filled samples displaying similar behaviour to Al2O3-filled specimens.
Hani, et al. [80] explored the thermal properties of fishbone-based (FBP) epoxy composites using
TGA and DSC. Their results demonstrated that incorporating FBPs enhanced thermal stability
compared to neat epoxy. The onset decomposition temperature (Tonset) increased with FBP content,
peaking at 345 °C for composites containing 10 wt.% and 15 wt.% FBPs. Furthermore, composites
with thermally treated FBPs (TFBPs) exhibited an additional 21 °C increase in Tonset for 10 wt.% TFBPs.
Differential scanning calorimetry (DSC) analysis revealed that the glass transition temperature (Tg)
of epoxy composites improved with FBP incorporation, rising from 58 °C for neat epoxy to 72 °C for
composites with 10 wt.% FBPs.
The above studies collectively highlight the importance of optimizing filler content and surface
treatment to enhance the thermal stability and mechanical performance of polymer composites.
Cognisance of the effect of filler content is critical for optimum reinforcement.

2.6. Empirical Review of Polyurethane and Epoxy Resins Reinforced with Natural Fillers
The integration of bio-based fillers into polymer matrices has garnered significant attention due
to their potential to enhance mechanical properties while promoting sustainability. Table 2
summarises empirical studies investigating the effects of different bio-based fillers on epoxy and
polyurethane properties. The narrative is presented as cases.
Case 1: Enhancing mechanical properties of epoxy composites using natural fillers
Shah, et al. [81] explored the incorporation of jute fibers at 30% weight in epoxy resin and
observed a 10.06% increase in tensile strength and a 4.70% improvement in flexural strength. This
enhancement demonstrates better load-bearing capabilities attributed to the strong interfacial
bonding between jute fibers and the polymer matrix. Similarly, Huzaifa, et al. [82] utilized sisal glass
fibers (50%) in epoxy, achieving a tensile strength of 69.1 MPa and a high hardness value of 24.73,
indicative of superior resistance to deformation. These results highlight the suitability of natural
fibers for structural applications where high strength and durability are critical.
Boopalan, et al. [83] studied a hybrid composite of jute and banana fibers (50%) in epoxy,
reporting enhanced mechanical and thermal properties, along with reduced moisture absorption. The
reduction in moisture uptake is significant as it improves the composites' durability and dimensional
stability, making them more viable for applications in humid environments. These findings align
with prior studies emphasizing the benefits of hybrid natural fibers for synergistic improvements in
polymer performance [84].
Wood, et al. [85] investigated the addition of lignin (1–10%) in epoxy, finding the highest tensile
and flexural strengths at 2.5 wt.% filler (86.16 MPa). The decline in strength at higher filler content
suggests filler agglomeration, leading to stress concentration and matrix disruption. This underscores
the importance of optimizing filler content for achieving peak mechanical performance, a recurring
observation in polymer-filler studies [86].
Majhi, et al. [87] introduced rice husk (5–20%) in epoxy and observed a 10% reduction in abrasive
wear loss, with wear resistance maximized at optimal filler content. The use of surface-treated rice
husk further amplified these benefits, emphasizing the role of chemical modifications in enhancing
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filler-polymer interactions. Such treatments mitigate filler incompatibility with hydrophobic

matrices, improving composite properties [88,89].
Hani, Firouzi, Islam and Sumdani [80] investigated the effect of thermal treatment on the
mechanical and thermal properties of fishbone-based epoxy composites (FBPs). The study revealed
significant improvements in both tensile and flexural strength, with increases of 30% and 200%,
respectively, compared to the neat epoxy (NE). These enhanced properties were attributed to the
thermal treatment of the FBPs. The authors observed that when FBPs were embedded in epoxy, they
formed mechanical interlocks with the epoxy molecules, resulting in a strong interfacial layer.
Additionally, epoxy molecules formed a bonding layer at the interface with the FBPs, further
reinforcing the composite structure. This combination of factors contributed to the superior
mechanical performance of the thermal-treated FBPs.
Case 2: Enhancing the mechanical properties of Polyurethane Composites using natural fillers
Członka, et al. [90] added grounded clove (1–5%) to polyurethane, achieving an 18% increase in
compression strength, 11% improvement in flexural strength, and 8% enhancement in impact
strength at 1–2 wt.% filler. However, beyond this range, diminishing returns were noted, aligning
with findings from Fan, et al. [91], who investigated glass microsphere and nanoclay fillers (1–7%) in
biobased rigid polyurethane. Although foam volume increased with filler content, compressive
strength decreased at 7% filler due to lower density and weaker cell wall structures. The impact of
fiber type and content on polymer properties is exemplified by Głowińska, et al. [92], who
incorporated sisal fibers (5–15%) into polyurethane. While hardness improved at lower filler
contents, tensile strength and elongation properties declined at higher percentages, attributed to poor
dispersion and matrix weakening. Husainie, et al. [93] also reported similar trends with cellulose,
chitin, hazelnut, and eggshell fillers (1–5%), where tensile strength peaked at 1 wt.%, but properties
such as split tear strength deteriorated significantly at higher concentrations.
Ozgur Seydibeyoglu, et al. [94] demonstrated the potential of the olive kernel and nutshell fibers
(2.5–7.5%) in polyurethane, with the highest compressive strength recorded at 2.5 wt.% olive kernel
filler, enhancing structural performance. This improvement highlights the strategic role of rigid fillers
in boosting foam stability and load-bearing capacity, which is critical for lightweight structural
applications.
Naidoo, et al. [95] investigated the incorporation of fish scale powder (FSP) into polyurethane
foam, examining its effect under varying temperature conditions. Their study revealed that at a
concentration of 0.5 wt% FSP, there was an 18.8% increase in tensile strength and a 15.7% increase in
elongation at break at room temperature. Additionally, the inclusion of FSP significantly enhanced
the tear resistance of the foam, with a 22% improvement at 0.5 wt% FSP and a remarkable 37%
increase at 1 wt% FSP, particularly under heat aging conditions. These results suggest that FSP can
effectively improve the mechanical properties of polyurethane foam, making it a promising
reinforcing agent.

Table 2. Summary of empirical work on enhancing mechanical properties of epoxy and polyurethane with
natural fillers.

Type of Bio- Polymer

Authors & Year Weight % Outcome of Mechanical Properties
based Fillers Material
Shah, Ahmad, Abid, Tensile strength increased by 10.06%, while
Arif, Khan, Khan and Jute fibers 30% Epoxy flexural strength improved by 4.70%,
Djavanroodi [81] highlighting better load-bearing capabilities.
Achieved a tensile strength of 69.1 MPa,
Huzaifa, Zahoor,
demonstrating superior strength, and
Akhtar, Abdullah,
Sisal glass fibers 50% Epoxy recorded the highest hardness value of 24.73,
Haider, Khan and
indicating excellent resistance to
Alam [82]
deformation.
Boopalan, Niranjanaa Jute/banana Enhanced mechanical and thermal
50% Epoxy
and Umapathy [83] fiber properties with a notable reduction in
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moisture absorption, improving durability

and stability.
Tensile and flexural strengths significantly
Wood, Coles, Maggs,
increased at 2.5% w/w filler, reaching 86.16
Meredith and Kirwan Lignin 1-10% Epoxy
MPa. Strengths declined at higher filler
[85]
content.
Abrasive wear loss was reduced by 10%
Majhi, Samantarai with improved wear resistance at optimal
Rice husk 5-20% Epoxy
and Acharya [87] filler content. Surface-treated rice husk
enhanced these effects.
Compression strength increased by 18%,
Członka, Strąkowska,
flexural strength improved by 11%, and
Strzelec, Kairytė and Grounded clove 1-5% Polyurethane
impact strength enhanced by 8% at 1-2 wt.%
Kremensas [90]
filler content.
Foam volume increased with filler content.
Glass Biobased
However, compressive strength decreased at
[91] microsphere and 1-7% rigid
7% filler due to lower density and weaker
nanoclay fillers Polyurethane
cell walls.
Hardness slightly improved at 5% filler
Głowińska, Datta and
Sisal fibers 5-15% Polyurethane content, but tensile strength and elongation
Parcheta [92]
decreased with higher filler percentages.
At 1 wt.%, tensile strength and elongation
Husainie, Khattak, cellulose, chitin,
improved. However, properties, including
Robinson and Naguib hazelnut, and 1-5% Polyurethane
split tear strength, decreased significantly at
[93] eggshell
5 wt.%.
Ozgur Seydibeyoglu,
The compressive strength of polyurethane
Demiroğlu, Erdoğan, olive kernel and
2.5-7.5 % Polyurethane foam increased at 2.5 wt.% olive kernel,
Akın, Ayvalık and nutshell fibers
enhancing structural performance.
Karavana [94]
Tensile strength polyurethane form increases
by 18.8% increase and a 15.7% increase in
Naidoo, Onwubu, elongation at break at 0.5 wt% (room
Mokhothu, Mdluli Fish scale 0.5-1% Polyurethane temperature). Tear resistance exhibited
and Mishra [95] significant improvements under heat aging,
with a 22% increase (0.5 wt%MFSP) and a
remarkable 37% increase 1 wt%
The tensile and flexural strength of the
composites were improved by 30% and
Hani, Firouzi, Islam
Fish bone 10-15% Epoxy 200%, respectively, compared to the neat
and Sumdani [80]
epoxy (NE) as an effect of the thermal
treatment

3. Discussion
The empirical review of epoxy and polyurethane resins reinforced with natural fillers highlights
the significant role of bio-based additives in enhancing mechanical properties while promoting
sustainability. The findings from the reviewed studies underscore critical trends and challenges
associated with natural filler incorporation.
Mechanical Performance Enhancement
From the review, it was evident that the integration of natural fillers into epoxy and
polyurethane matrices improve tensile strength, flexural strength, and wear resistance. Shah, Ahmad,
Abid, Arif, Khan, Khan and Djavanroodi [81] and Huzaifa, Zahoor, Akhtar, Abdullah, Haider, Khan
and Alam [82] demonstrated that jute and sisal glass fibers significantly enhance tensile and flexural
strength, reinforcing their suitability for structural applications. The work of Boopalan, Niranjanaa
and Umapathy [83] further supports the advantage of hybrid fiber composites, where combining jute
and banana fibers results in superior thermal stability and moisture resistance.
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These results align with previous studies [84,86] that emphasize the importance of fiber-matrix
adhesion in determining mechanical performance. However, the findings by Wood, Coles, Maggs,
Meredith and Kirwan [85] and Majhi, Samantarai and Acharya [87] highlight a critical limitation:
excessive filler content leads to agglomeration, which weakens the composite structure due to stress
concentration. This issue suggests that optimization of filler content is crucial to achieving the desired
balance between strength and durability, a factor consistently observed in polymer-filler research
[88,89].
Role of Filler Content in Property Optimization
The studies reviewed indicate that optimal filler content varies depending on the type of
polymer and filler material. In epoxy composites for example, the highest mechanical performance
was observed at moderate filler percentages, such as 2.5% for lignin [85] and 10% for rice husk [87].
This suggests that bio-fillers effectively reinforce polymer matrices within a specific concentration
range before the drawbacks of excessive filler loading, such as brittleness and reduced tensile
strength, outweigh the benefits.
Similarly, in polyurethane composites, Członka, Strąkowska, Strzelec, Kairytė and Kremensas
[90] and Fan, Tekeei, Suppes and Hsieh [91] found that filler loadings between 1-2% resulted in
maximum compression and flexural strength, while higher concentrations led to diminishing returns.
The results obtained by Husainie, Khattak, Robinson and Naguib [93] and Głowińska, Datta and
Parcheta [92] further emphasize that while natural fillers can improve rigidity and hardness, they
may simultaneously reduce elongation and flexibility at excessive loading levels.
These observations are consistent with broader studies on polymer composites, where optimal
filler dispersion is a key determinant of improved mechanical properties [94]. The findings suggest
that tailored filler percentages should be adopted for specific engineering applications, ensuring an
optimal balance between strength, stiffness, and flexibility.
Chemical Modification and Interfacial Adhesion
A recurring theme in the reviewed literature is the role of chemical modifications in improving
filler-polymer compatibility. As seen in the study by Majhi, Samantarai and Acharya [87], surface-
treated rice husk resulted in better adhesion, enhancing wear resistance. This is supported by similar
findings in the work of [88] and [89], which stress that untreated fillers often exhibit poor dispersion
within the polymer matrix, leading to performance degradation.
The studies suggest that chemical modifications, such as silane treatment or alkalization, can
mitigate the inherent hydrophilicity of natural fibers, improving adhesion to hydrophobic matrices.
This insight has implications for polymer composite manufacturing, where pre-treatment processes
can be standardized to optimize mechanical properties across different polymer-filler systems.

4. Conclusions
The empirical review provides compelling evidence that natural fillers enhance the mechanical
properties of epoxy and polyurethane composites. However, the effectiveness of these fillers is highly
dependent on content optimization, dispersion techniques, and interfacial bonding strategies. The
findings have significant industrial and environmental implications, emphasizing the need for
further research into sustainable polymer reinforcement technologies. Particularly, more research is
needed on the aging behavior of bio-based composites under real-world environmental conditions.

Author Contributions: Conceptualization, S.C. and D.; validation, S.C., Y.Y. and Z.Z.; formal analysis, S.C.;
investigation, S.C. and D; resources, S.C. and D; data curation, S.C and D.; writing—original draft preparation,
S.C. and D; writing—review and editing, S.C and Z.; visualization, S.C and T.H.; supervision, S.C. and TH;
project administration, S.C.; funding acquisition, S.C. All authors have read and agreed to the published version
of the manuscript.

Funding: This research was funded by National Research Fund (NRF) [CSUR230519107827].
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Data Availability Statement: Data can be made available by the author on request.

Acknowledgments: The authors acknowledge the support from NRF.

Conflicts of Interest: The authors declare no conflicts of interest.

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