Invited Review

Journal of Reinforced Plastics

and Composites

Recent advances in epoxy resin, natural 0(0) 1–24

! The Author(s) 2015
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DOI: 10.1177/0731684415618459
their applications jrp.sagepub.com

Naheed Saba1, Mohammad Jawaid1,2, Othman Y Alothman2,

MT Paridah1 and Azman Hassan3

Abstract
The versatile characteristic of epoxy and its diversity made it suitable for different industrial applications such as
laminated circuit board, electronic component encapsulations, surface coatings, potting, fiber reinforcement, and adhe-
sives. However, the pervasive applications in many high-performance field limited the epoxy use because of their
delamination, low impact resistance, inherent brittleness, and fracture toughness behavior. The limitations of epoxy
can be overcome by incorporation and modification before their industrial applications. Currently, modified epoxy resins
are extensively used in fabrication of natural fiber-reinforced composites and in making its different industrial products
because of their superior mechanical, thermal, and electrical properties. Present review article designed to be a com-
prehensive source of recent literature on epoxy structure, synthesis, modified epoxy, bio-epoxy resin, and its applica-
tions. This review article also aims to cover the recent advances in natural fiber-based epoxy composites and
nanocomposites research study, including manufacturing techniques and their different industrial applications.

Keywords
Natural fibers, epoxy resin, bio-composites, nanocomposites, applications

been known for the processing of thermosets by the

Introduction
Environmental concern is stimulating the scientific
research toward the design and proposal of new engin-
eered materials for construction, packaging, furniture,
and automotive industries involving modified thermo-
set polymer.1 A thermosetting resin and thermoset
composite once formed is highly cross-linked, which
once catalyzed, cannot be reversed, remolded,
reshaped, or reformed.2 It also cannot be cured or set
using heat and pressure or heat and light irradiation.
Thus, due to the developed high cross-linking density,
the long chain macro movement or slippage get
restricted in cured epoxy. The higher flexibility for tai-
loring desired ultimate and high-performance products
for industries leads to its strength, high modulus, dur-
ability, and better thermal and chemical resistances.3–6
Most of the large volume thermosetting systems are
melamine formaldehyde, urea formaldehyde, phenol
formaldehyde, resorcinol formaldehyde, polyurethane,
polyesters, and epoxies.7 Different techniques have
researchers. Molding is one of the best and widely
used techniques for the fabrication or processing of
thermosets. It includes compression molding, transfer
molding and injection molding based on the types of
material to be processed and end application of the
products.7
1
Department of Biocomposite Technology, Institute of Tropical Forestry
and Forest Products (INTROP), Universiti Putra Malaysia, Serdang,
Selangor, Malaysia
2
Chemical Engineering Department, College of Engineering, King Saud
University, Riyadh, Saudi Arabia
3
Department of Polymer Engineering, Faculty of Chemical Engineering,
Universiti Teknologi Malaysia, Skudai, Johor Bharu, Malaysia
Corresponding author:
Mohammad Jawaid, Department of Biocomposite Technology, Institute of
Tropical Forestry and Forest Products (INTROP), Universiti Putra
Malaysia, 43400 UPM, Serdang, Selangor, Malaysia.
Email: jawaid@upm.edu.my; jawaid_md@yahoo.co.in

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2 Journal of Reinforced Plastics and Composites 0(0)
Epoxy
Epoxy is the thermosetting matrix or resin materials,
having at least one or more epoxide groups in the mol-
ecule. The epoxide also termed as oxirane or ethoxyline
group and is regarded as representative unit of epoxy
polymer.7,8 Most of the commercially available epoxy
resins are oligomers of diglycidyl ether of bisphenol A
(DGEBA).9,10 These oligomers when react with the
hardener, the epoxy resin get cured and becomes a
thermosetting polymer.10 There are mainly two families
of epoxies non-glycidyl and glycidyl epoxies. Glycidyl
epoxy resins can be further defined as either glycidyl-
amine, glycidyl-ester, or glycidyl-ether. Non-gylcidyl
epoxy resins are also called cyloaliphatic or ali-
phatic resins (http://composite.about.com). The most
common glycidyl epoxy resins is synthesized by reacting
bisphenol A (BPA) with epichlorohydrin molecules.
Novolac-based epoxy resin is the other type of epoxy
that are also frequently used in certain industries.11
Nowadays, epoxies are combined with a large range
of co-reactants/curing agents/hardener, such as anhyd-
rides, amines, and amides,2,12 perhaps the amine-based
hardener is quite common. Epoxy resins usually require
the higher amount of curing agent in the ratio of resin
to hardener (1:1 or 2:1), compared with polyester or
vinyl ester resins, where the resin is catalyzed with a
small (1–3%) addition of a catalyst (http://composite.
about.com). Like other thermoset resin, cured epoxy
systems indicates low fracture toughness, inherently
low impact resistance, unaltered shaped after curing/
polymerization, and reduced resistance to crack initi-
ation and propagation.13–16 The advantage and limita-
tions of epoxy resins can be preset by the chemical
structure of the resin and hardener, as well as by the
network achieved after curing.13 Curing results 3 D
(tridimensional) covalent network with properties
Figure 1. (a, b) The three-dimensional oxirane ring of epoxy and resulting cross-linked structure of cured epoxy
(www.3me.tudelft.nl).
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depending on the extent-density of crosslinking
curing kinetics and their chemical composition.12 It is
possible to vary their mechanical and physical proper-
ties ranging from extreme flexibility to high strength
along with improved adhesive strength, hardness,
chemical resistance, electrical resistance, and heat
resistance.14,17
Structure, chemistry, and synthesis of
epoxy resin
DGEBA is a typical commercial epoxy resin. The oxi-
rane functional group (a three-member ring formed
between two carbon atoms and an oxygen) is the
main feature of the epoxy monomer. Figure 1(a) and
(b) shows the 3-D oxirane ring of epoxy and resulting
cross-linked structure of cured epoxy. Because of the
different electronegativity of carbon and oxygen,
the carbon atoms of the ring are electrophilic. This
atomic arrangement shows enhanced reactivity because
of their high strain, compared with common ethers.
Thus, epoxies or epoxy functions are highly reactive
and readily undergoes ring-opening reactions with
nucleophiles such as hydroxyl. The polarity of the oxi-
rane ring can be detected by IR spectroscopy to reveal
the epoxy chemistry shown in Tables 1 and 2. Epoxy
resins, depending on their backbone structure, may be
of low- or high-viscosity liquids or solids. In low-visc-
osity resin, a decent wetting of fibers by the resin with-
out using high temperature or pressure can be achieved.
But the impregnation of fibers with high-viscosity resins
is usually done through high temperature and
pressure.13
Nowadays, almost 90% of the world production of
epoxy resins is based on the reaction between BPA and
epichlorohydrin in the presence of a basic catalyst, pro-
ducing major DGEBA.2,18–20
Saba et al. 3

Table 1. Characteristic bands of DGEBA in the mid-IR.11

Commercial applications of epoxy resin
1
Resin Band (cm ) Assignment
Epoxy resin, being inexpensive has superior properties,
DGEBA 3500 O–H stretching is extensively used as indispensable insulating material
3057 Stretching of C–H of the oxirane ring in heavy apparatuses and as a dielectric materials field.
2965–2873 Stretching C–H of CH2 and CH These properties lead it to extremely versatile materials
aromatic and aliphatic rings that range from laminated circuit board, structural
1608 Stretching C ¼ C of aromatic rings fiber-reinforced composites, electronic component
1509 Stretching C–C of aromatic rings encapsulations, and as adhesives.25,26 Some of the
1036 Stretching C–O–C of ethers
important applications involving epoxy resins21,22,27,28
are as follows:
915 Stretching C–O of oxirane group
831 Stretching C–O–C of oxirane group
. Adhesives for general purposes
772 Rocking CH2 . Binder in cements and mortars
DGEBA: diglycidyl ether of bisphenol A. . Making rigid foams
. For non-skid coatings
. Solidifying sandy surfaces in oil drilling
Table 2. Characteristic bands of DGEBA in the near IR.11 . Industrial paintings and coatings
. Potting and encapsulating media
Resin Band (cm–1) Assignment . Fiber-reinforced plastics
DGEBA 7099 O–H overtone
6072 First overtone of terminal
CH2 stretching mode Green or sustainable epoxy resins
5988–5889 Overtones of –CH and –CH2 stretching
Recent years have witnessed a huge interest in develop-
5244 Combination asymmetric stretching
ing the polymers derived from renewable resources
and bending of O–H
in industrial applications because of growing environ-
4623 Overtone of C–H stretching of the
mental issues, waste disposal, and depletion of
aromatic ring
non-renewable resources.29–31 The advantages of bio-
4531 Combination band of the second
polymers includes low production cost and their
overtone of the epoxy ring stretching
with the fundamental C–H stretching possible biodegradability.32,33 The BPA is one of the
highest volume chemicals produced worldwide.
4066 Stretching C–H of aromatic ring
Current estimates indicate that more than 4 million
DGEBA: diglycidyl ether of bisphenol A. tons of BPA are produced annually and approximately
100 tons get released into the atmosphere each year.34
The negative impact of BPA on human health35–40
includes alterations in both immune and reproductive
Advantages of epoxy over thermoplastics
systems along with the modification in brain chemis-
Epoxy resins have distinct advantages compared with try.41–43 Moreover, BPA has been known to have estro-
other traditional thermoplastic or thermoset resins,21–24 genic properties,44,45 thus currently several efforts are
such as the following: being made to replace the traditional DGEBA by bio-
based epoxy monomer or oligomer with comparable
. Minimum shrinkage during curing high-performance materials.46 The chemical bonds
. Relatively cheaper and abundant between BPA in polymer structures are quite not
. Improved mechanical and fatigue strength stable, thus enabling the polymer to release a small
. Outstanding moisture resistance amount of BPA, with time, which is toxic to living
. Outstanding chemical resistance organisms. In some countries like Canada or France,
. Better electrical properties the growing environment impact implies the researches
. Good adhesion with many substrates to focus for the substitution of BPA.46 Thus, currently
. Non-magnetic properties several efforts are being made by the researchers to
. No Volatile Organic Compounds (VOCs) replace the traditional DGEBA by bio-based epoxy
. Long shelf life monomer or oligomer with comparable high-perfor-
. Perfect damage tolerances mance materials.45,46
. Impact resistant The DGEBA is derived from BPA and epichlorohy-
. Corrosion resistant (anticorrosive) drin; thus, the easiest way to obtain a partially

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4 Journal of Reinforced Plastics and Composites 0(0)
bio-based DGEBA is to use epichlorohydrin from bio-
based glycerol, an abundant and inexpensive polyol.
Such bio-based epichlorohydrin is commercially avail-
able. The challenge to obtain a wholly bio-based epoxy
pre polymer still persists, as the molar mass of DGEBA
is dominated by BPA, whereas the epichlorohydrin
parts accounts only for 20%, but it can be overcome,
by replacing BPA with a bio-based polyol.45 In the for-
mation of sustainable epoxy resins, natural polyphenols
(condensed tannins, lignin, gallo-tannins) and polysac-
charides are the most abundantly available renewable
natural resources (forest/agricultural biomass or resi-
dues) in large quantities.30 Table 3 tabulates the list
of bio precursor for epoxy resin. Generally, bio-based
epoxy resins were synthesized from a catechin molecule
or condensed tannins, one of the repetitive units in nat-
ural flavonoid biopolymers with improved thermal and
mechanical properties.48 More particularly, non-func-
tionalized gallic acid (produced from hydrolysis of
gallo-tannins), glycerol-based epoxy precursors such
as glycerol polyglycidyl ether (GPE) and polyglycerol
polyglycidyl ether (PGPE)47 are industrially available
and are quite inexpensive for the bio-based epoxy
resins formulations.30 The methanol soluble lignin
extracted from unused bamboo are also used by some
researchers.65 Currently, researchers are attracted
toward the epoxidized plant oils and fatty acids to util-
ize it as a potential alternative, because they display
interesting and comparable thermal properties to the
commercial DGEBA.46,66–68 However, traditionally,
epoxidized plant oils are used as stabilizers and plasti-
cizers for PVC, painting, and in coating formula-
tions.69,70 The investigation of curing and conversion
of epoxidized oils into flexible, semi-flexible, and rigid
cross-linked resins with various approaches and meth-
ods is successively made by several researchers.71,72
Modification of epoxy resin
The potential use of epoxy thermosets in many high-
performance applications is limited because of some of
their structural drawbacks.2,73 However, to overcome
the epoxy resins weak point, virtually all of the epoxy
resins are modified/amended with various additives and
fillers, such as reactive oligomeric compounds, low
molecular weight polymers, plasticizers, nano-particles,
nano-fillers, and carbon nanotube.9 Significant prop-
erty improvements are made by,
(i) Using curing agents, resins, and co-monomers with
new backbone chemistries.
(ii) Modification with thermoplastic polymer, elasto-
mers, inorganic particles, continuous or chopped
fibers (glass, carbon, aramid, or natural fibers), dif-
ferent geometry (particles, fibers, or platelets) and
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of different size (micro and nano). Incorporating
tough thermoset or thermoplastic films in the
form of interpenetrating network systems.74
(iii) By adding reinforcements of different nature to
provide additional mechanical energy absorption
mechanisms in the epoxy to make it fire
retardant.7
Extension in the applications of the obtained mod-
ified epoxies in the civil infrastructure and transporta-
tion sector are reconnoitered.75,76
Fire retardant epoxies
Thermoset polymers based on petroleum are highly
flammable and combustible. Epoxies like other
thermoset resins, on exposing to high temperatures
(300–400 C), decomposes releasing smoke, heat,
toxic volatiles, and soot from the organic matrix of
the cured epoxy laminate.77,78 Epoxy resins will
become fire retardant either by incorporating fire
retardant additives or by copolymerization with react-
ive fire retardant like other thermoset.79 The main
fields where fire retardancy of epoxy resins is required
are electronics (semiconductor encapsulation and
printed wiring boards), transportation (automotive,
high speed trains, military and commercial aircraft),
composite structure, and in furnishing elements.
Table 4 displays the list of fire retardants added
to modify the epoxy resin. The introduction of
boron-,90 phosphorus-,91,92 and silicon-containing78
compounds also proved to be beneficial and valuable
to enhanced fire retardancy of epoxy resins systems.
Recently, some ecological and friendly flame retard-
ants involving natural mineral (montmorillonite, kao-
linite, and aluminum hydroxide) have been developed
for improving burning resistance of epoxy resins.93,94
In another work, fire retardant epoxy resins are
synthesized by incorporating tris (2-hydroxypropyl)
borate (THPB) and Oap POSS (octaaminophenyl
polyhedral oligomericsilsesquioxane) having boron
and silicon in the cured system by the researchers.81
Researcher found an increase in the LOI (limited
oxygen index) value of epoxy resin together with the
improved heat-resistant char layer formation and low-
ered release rate of flammable gases.
Natural fiber-based epoxy composite
Incorporation of natural fibers is also the most
attractive way to modify the epoxy resin. During last
few years, the interest and applications of using nat-
ural fibers as reinforcement in polymers has increased
dramatically in both areas of engineering and research
technology.95–97 Researchers and scientists also shows
Saba et al. 5

Table 3. List of some of the bio-based precursors for sustainable epoxy polymer.

Bio precursors References Chemical structure

47
GPE and PGPE

45
SPE and PSPE

48
GEC

49–55
Soybean oil, linseed oil, and castor
oil (vegetable oils)

56–59
Wood powder, alcohol liquefied wood
(wood alcohol)

(continued)

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6 Journal of Reinforced Plastics and Composites 0(0)

Table 3. Continued

Bio precursors References Chemical structure

60,61
Cardanol (cashew phenol)

45
Sorbitol, maltitol

62,63
Vanillin (wood-derived compound)

48
Condensed tannins (catechin molecule)

46
Gallic acid and gallo-tannins

(continued)

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Saba et al. 7

Table 3. Continued

Bio precursors References Chemical structure

64
Tannic acid

more emphasis on the use of renewable resources

based on the issues of safer environment, waste dis- Table 4. Showing the list of some important fire retardant
posal, and the depletion of nonrenewable resources.98 materials for epoxy resin.
Many research studies has been carried out based on Fire retardant material References
the reinforcement of natural fibers (such as vakka 80
(Roystonea regia), date palm, coir, oil palm empty OPS and DOPO
81
fruit bunch (OPEFB), ramie, bamboo, hemp, flax, THPB and Oap POSS
82
sisal, jute, kenaf, etc.), which are a potential substitute TMT
83
or alternatives for synthetic fibers (glass and carbon TGIC-DOPO
fibers) in the composite applications.17,99 Table 5 illus- Co3O4–graphene and SnO2–graphene 84

trates the list of nature fiber reinforcement in epoxy Cyclotriphosphazene 85

polymeric matrix to fabricate composites. In the com- Graphene nano sheets 86

posite industries, epoxy is used as binder to hold the CNT via the sol–gel method. 87

reinforcing materials in its place. Generally, natural Hydrotalcites 88

fiber is used in advanced polymer composites in
three forms by considering their aspect ratio. The
first utilization of natural fiber as filler (powder)
in polymer is to enhance the desired properties of
composite compared with the initial pure or virgin
resin. The second form is by using short fiber and
randomly arranging in designed volume content per-
centage. The third one is by using continuous bio fiber
in polymer composites.111 Research study is also done
to determine the possibilities of introducing new nat-
ural fibers as fillers in a polymeric matrix to develop
economic and light weight structural materials.138,139
High-performance composites with improved proper-
ties, based on thermosetting polymers can be achieved
by simultaneously improving fiber, resin, and their
interfacial properties.140 Natural fibers-based epoxy
composite shows the unique combination of great ver-
satility, high performance, and processing advantages
at promising cheaper rates compared with thermoplas-
tics.24 Researchers claimed that, in most of the cases,
the mechanical and physical properties of the poly-
meric matrix get improved with the incorporation of
natural fibers such as jute, kenaf, OPEFB, etc.1,141,142
Research study elaborated that most of the thermoset
composite involving epoxy are fabricated by manual
layup and spray-up techniques.2
80
OPS, OAPS, and DOPO
89
PFR
Oap POSS: octaaminophenyl POSS; POSS: polyhedral oligomeric silses-
quioxanes; OPS: ctaphenylsilsesquioxane; TMT: maleimido-substituted
aromatic s-triazine; THPB: tris (2 hydroxypropyl) borate; OAPS: octaa-
minophenylsilsesquioxane; PFR: poly(DOPO substituted phenyl dimetha-
nolpentaerythritol diphosphonate); DOPO: 9,10-dihydro-9-oxa-10-
phosphaphenanthrene-10-oxide; TGIC: 1,3, 5-triglycidyl isocyanurate;
CNT: carbon nanotube.
Hybrid epoxy composites
Several research studies has been made to modify the
properties of epoxy resin by reinforcing natural fiber
along with other fillers or other natural fiber to fabri-
cate the hybrid epoxy bio-composite. Reported work
on hybrid composites are tabulated in Table 6 along
with their references.
Nano epoxy composites
The development of nano-particle-reinforced polymer
composites is currently one of the most promising
approaches in the field of future hi-tech engineering
applications with an appropriate or minimal amounts

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8 Journal of Reinforced Plastics and Composites 0(0)

Table 5. Showing the reinforcement of different types of natural fiber in epoxy composites.

Reinforcement Fabrication techniques References Modifications in properties

100
UTCSE and TCSE fiber Hand layup followed TCSE composite showed higher mechanical properties, higher
by compression storage modulus, lowered damping parameter (Tan ), and less
molding char yield. The TCSE shows higher thermal stability compared
with UTCSE composite.
101
Alkaline-treated kenaf Initial hand layup fol- Alkali treatment increased the mechanical properties, storage, and
fiber lowed by vacuum the loss moduli. Also a notable reduction of tan  or damping
bagging factor peaks are observed.
102
Sundi wood dust Hand layup The tensile and flexural properties of the polymeric resin
improved by the reinforcement of wood dust.
103
Recycled cellulose Hand layup The flexural modulus, flexural strength, fracture toughness, and
fiber impact strength increased as the fiber content increased. But
flexural modulus, strength and fracture toughness decreased as
a result of moisture absorption of the composite.
104
Treated and untreated Hand layup and com- Treated fiber-reinforced composite has improved dynamical and
short Agave fiber pression molding thermo-mechanical properties compared with untreated short
Agave fibers-reinforced composite.
105
Flax fiber Hot platen press Tensile strength and Young’s modulus are affected by the hygro-
thermal aging of composite.
106
Unidirectional flax Hot press The void content decreases and mechanical properties of com-
fiber posite increased by reinforcements
107
Treated and untreated Hot press Flexural modulus and flexural strength were improved by 79% and
kenaf fiber 24.7%, respectively, and the impact strength by 14.7% by the
reinforcement of treated kenaf fiber.
108
Lantana camara fiber Hand layup Increase in flexural and tensile strength observed with increase in
fiber content up to 30%.
109
Unidirectional long Hand layup The reinforcement of epoxy with treated kenaf fibers increased
kenaf fiber the flexural strength of the composite by about 36%, whereas
the untreated fibers introduced 20% improvement. The por-
osity of the treated kenaf fibers/epoxy composite is lower than
the untreated fiber/epoxy composites.
110
Non-woven kenaf fiber Hand layup The composite tube with b ¼ 60 exhibited local buckling failure
mode and displayed the highest specific energy absorption
capability equal to 9.2 J/g compared with neat epoxy.
111
Unidirectional kenaf Hand layup The void content, tensile modulus, and tensile strength of unidir-
fiber ectional kenaf fiber epoxy composite increases.
24
Bi-directional jute fiber Hand layup Pronounced positive effect of fiber loading on physical (surface
hardness increases, inter-laminar shear strength ILSS increases,
void content decreases) and mechanical properties are
observed.
1
Woven jute fibers Compression molding Mechanical behavior improved by increasing the number of woven
jute fiber layers.
112
Luffa cylindrica Hand layup Treated mat fiber-reinforced composites have better thermal
stability and mechanical properties than pure epoxy.
113
Alkali-treated woven Hot platen press An improvement in the fibers/matrix adhesion by alkali treatment
flax fiber in the composite are observed.
114
Woven hemp fiber RTM The tensile–tensile fatigue behavior increases by reinforcement of
woven hemp fiber.
115
Natural flax fabric Hand layup The PU foam-filled flax/epoxy tubes has the capability of spreading
the deformation under lateral compression and enhance the
energy absorption of the tubes during flattening process.
116
Hand layup
(continued)

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Saba et al. 9

Table 5. Continued

Reinforcement Fabrication techniques References Modifications in properties

Phormium tenax leaf The quasi-unidirectional fibers reinforcement improved both

fibers strength and modulus for tensile and flexural loading compared
with neat epoxy.
117
Bamboo fibers Hand layup Adhesive wear resistance and friction performance of BMBFRE
composite is higher than pure epoxy resin.
118
Flax fiber Hand layup followed Glycerol and polyglycerol addition increases the damping
by vacuum bagging coefficient of flax composites by 10–13% and 21–25%,
respectively, by DMTA and acoustic testing. The damping
coefficients of the polyol-treated flax composites were larger
than those of the non-treated flax and the aramid- or CF
composites prepared under similar conditions.
105
Quasi-unidirectional Hot platen press Young’s modulus and tensile strength are affected by the hygro-
flax fiber thermal aging as a significant reduction in Young’s modulus,
while tensile strength decreases much less for water-saturated
composites.
119
NS Vacuum bagging NS/epoxy/coremat possess better load bearing capability than
other sandwich configurations. NS/epoxy/foam specimen
showed more energy attenuation capability among other con-
figuration and NS/epoxy.
120
CFF Hot press The electrical resistivity of the CFF composites are two to four
orders of magnitude higher than that of E-glass fiber compos-
ites. The dielectric constant of the composites decreased with
CF contents.
121
Alkalized and silanized Hand layup The blend increases the impact strength by 163% compared with
woven sisal fiber neat epoxy resin. Flexural strength of all composites are lower
than that of the blend but get improved after addition of sali-
nized sisal fiber.
122
Coir fiber Compression molding The coir fiber volume fraction, curing time, and compression load
perfectly influence the tensile strength of the resultant
composite.
123
Alkali treated and Hand layup Kenaf fibers reinforcement slightly improves both the charring and
untreated kenaf thermal stability of the epoxy composite. Alkalization reduces
fiber the decomposition temperature of the kenaf fiber/epoxy
composite and produces lesser char than untreated composite
124
Palm tree fiber Contact method In addition to the relaxation associated to the glass transition of
the epoxy resin matrix and ionic relaxation caused by the
mobility of electric charges, the presence of cellulose fibers in
the composite gives rise to the other relaxation associated to
the MWS interfacial polarization.
125
APF Hand layup The aged specimens have higher tensile strength compared with
the original specimens, by 50.4%. The aged APFREC composite
shows increased ductility and the resistance toward deform-
ation also get decreased.
126
Jute fiber Hand layup Treated (with sodium hydroxide and the addition of silane cou-
pling agents) jute fiber enhances the interfacial interaction and
mechanical properties between jute fibers and an epoxy matrix
in the composite.
127
Sugar palm fiber Melt mixer and hot The fracture toughness of seawater immerses specimen register
press better fracture toughness than other type of treatments.
Improvement of mechanical properties by the reinforcement of
sugar palm fiber in epoxy matrix is also observed.
128
Untreated and alkali Hand layup Alkali treatment generally improved composite strength, better
treated short strength at high fiber contents for long fiber composites.
(continued)

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10 Journal of Reinforced Plastics and Composites 0(0)

Table 5. Continued

Reinforcement Fabrication techniques References Modifications in properties

(random and Composites with 65 wt% untreated, long aligned fiber were the
aligned) and long strongest with a TS of 165 MPa, Young’s modulus of 17 GPa,
(aligned) hemp fiber flexural strength of 180 MPa, flexural modulus of 9 GPa.
129
Unidirectional abaca RTM Salinization and slight mercerization (1.0 wt% NaOH solution,
fiber 5 min) enhance fiber–resin interface strength, whereas a heavy
mercerization leads fiber–resin interface modification and also a
diminish of lumen size and weakening of interface between
elementary fibers. The TCC of the composite also increases
with decrease in void content.
130
Piassava fibers Hand layup Alkali treatment of piassava fiber results in the removal of pro-
trusions as well as the surface wax on the fibers. Thus, the
flexural and elastic moduli steadily increase for piassava fiber
contents in the composite.
131
Flax fiber Compression molding The mechanical performances of unidirectional composites
increases and is linked to the elementary fibers as well as to the
composites microstructure. The composites homogeneity are
confirmed by the Rosen model, used for calculation of inter-
facial shear strength measurements.
132
Bamboo cellulose fiber Casting method Both silane coupling agent modification and NaOH aqueous
solution of bamboo cellulose fiber apparently improved the
tensile strength and the values of elongation at break of the
fiber-reinforced composite. Compared with the untreated cel-
lulose-filled epoxy composites, the NaOH solution treatment
increased the tensile strength by 34% and elongation at break
by 31%. The silane coupling agent treatment produced 71%
enhancement in tensile strength and 53% increase in elongation
at break.
133
Arundo Donax fillers Hand layup Composites exhibit higher tensile moduli, comparable flexural
moduli, and lower strength properties in comparison with the
neat resin.
134
Flax fiber Compression molding The stiffness, damping, and permanent strain of the composite are
higher compared with the neat epoxy resin.
135
Ramie fabric VARIM Hot compaction can significantly improve the mechanical proper-
ties of ramie fabric composites (tensile and flexural properties
range from 18.0 to 41.5%).
136
Unidirectional kenaf Hand layup The tensile properties (tensile strength and modulus of elasticity)
fiber increased as the fiber volume increased in the composite. The
composite shows reductions in the modulus of elasticity com-
pared with neat resin.
137
Unidirectional kenaf Hand layup Fiber content ratios were found to affect fatigue life strongly on
fiber the low cycle fatigue regime as illustrated with stress level
versus cycles to failure. It is found that kenaf fiber-reinforced
epoxy composites with higher fiber content possess higher load
carrying capacity and degradation rates.
UTCSE: untreated (raw) coconut sheath fiber-reinforced epoxy; TCSE: treated coconut sheath fiber-reinforced epoxy; PBT: polybutylene terephthal-
ate; SMC: sheet molding compound; RTM: resin transfer molding; VARIM: vacuum-assisted resin infusion method; VARTM: vacuum-assisted resin
transfer molding method; NS: natural silk; CF: carbon fiber; CFF: chicken feather fiber; APF: Arenga pinnata fiber; MWS: Maxwell–Wagner–Sillars; TS:
tensile strength; TCC: transverse thermal conductivity.

and dispersion of nano-particles.171 Currently, a lot of as carbon nanotubes173,174 and carbon nano fibers.175
approach and research study has been made to enhance A nano-modification of the epoxy matrix leads to
epoxy properties to overcome its shortcomings by rein- novel products with enhanced new features such as
forcing nano-sized inorganic particles or fillers172 such matrix-dominated mechanical properties, physical

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Saba et al. 11

Table 6. Showing the reinforcement of different types of natural fiber and filler in hybrid epoxy composites.

Reinforcement Technique References Modifications in properties

143
Glass fiber/sisal/ Hand layup The results indicated that the incorporation of sisal fiber with
jute fiber GFRP exhibited superior properties than the jute fiber-rein-
forced GFRP composites in tensile properties. Also, the jute
fiber-reinforced GFRP composites performed better in flexural
properties.
144
Banana/Flax/ Hand layup Thermal properties of hybrid composites of flax and banana with
Glass fibers GFRP have better thermal stability and flame resistance over
flax, banana with GFRP single fiber hybrid composites. The
hybrid composite also shows far better properties than single
fiber glass-reinforced composite under impact and flexural
loads. Hybrid composite have better strength as compared with
single fiber composites.
145
Banana/sisal Hand layup The addition of sisal fiber in banana/epoxy composites of up to
fiber 50% by weight results in increasing the mechanical properties
and decreases the moisture absorption property.
146
Oil palm EFB/ Hand layup Hybrid composites were fabricated by incorporation of modified
jute fiber oil palm EFB and jute fibers into an epoxy matrix by the hand
lay-up technique. Mechanical (flexural and impact) and mor-
phological properties of modified hybrid composites were
measured. Results indicated that flexural and impact properties
of modified fiber-reinforced hybrid composites improved as
compared to untreated hybrid composites.
147
Oil palm EFB/ Hand layup The tensile and flexural properties of pure EFB composite get
jute fiber improved by hybridization with woven jute fiber as extreme
woven jute fiber mat. Also, the tensile and flexural properties of
hybrid composite is higher than that of EFB composite but less
than woven jute composite.
148
Kenaf/glass fiber Modified sheet Thermoplastic toughening improves the epoxy impact property
molding with a low thermo-mechanical defect. The impact property of
developed hybrid kenaf/glass epoxy composite is greater than
pure epoxy. Also, the impact property improved by 54% com-
pared with non-toughened bio-composite.
149
Jute fiber/poly- Compression The results show that the jute-reinforced epoxy composite
ester/epoxy molding exhibited better mechanical properties (tensile and flexural
properties) than jute-polyester composite.
150
Kenaf/glass fiber Modified SMC The results indicate that some mechanical properties such as
tensile strength, Young’s modulus, flexural strength, and flexural
modulus are similar to GMT and are thus suitable for some car
structural components such as bumper beams.
151
OPEFB/jute Hand layup The addition of fibers and coupling agent considerably improved
fiber the thermal stability of the hybrids. The impact properties show
good enhancement in case of EFB/jute/EFB type of laminate as
compared with jute/EFB/jute with coupling agent, respectively.
152
Banana/sisal Compression The flexural properties were enhanced on banana–sisal fiber with
fiber molding two layers of glass fibers rather than three layers and the
laminate with sisal and three glass ply offers better impact
strength. The tensile strength, flexural strength, and impact
strength also get increased by the addition of two and three
layer of glass fiber by a factor of 2.34 and 4.13, respectively.
153
Sisal/henequen Hot compres- Tensile strength increases by joint geometry in the case of uni-
fiber sion molding directional-reinforced high strength natural fiber composites
for the manufacture of engineered structures.
(continued)

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12 Journal of Reinforced Plastics and Composites 0(0)

Table 6. Continued

Reinforcement Technique References Modifications in properties

154
Woven kenaf Hand layup The hybrid Kevlar/woven kenaf (78/22) composite possess better
fibers/Kevlar mechanical properties than kenaf/epoxy and Kevlar/epoxy
Laminates composite as a function of fiber content.
155
Bamboo/coco- Twin screw The flexible epoxy surface treatment improved impact property of
nut/Vetiver extruder bamboo fiber/PLA and coconut fiber/PLA composites when
grass fiber/ compared against the untreated composites.
PLA
156
Woven kenaf– Hand layup The tensile properties of hybrid composites improved in three-
Kevlar layer composites compared with four-layer composites. Hybrid
laminates composite with Kevlar as outer layers display a better mech-
anical properties as compared with other hybrid composites.
Tensile and flexural properties of treated hybrid composites are
better than non-treated hybrid composites. The impact
strength of kenaf/Kevlar hybrid composites is also not affected
by the water aging.
157
Luffa fiber/ Hand layup The mechanical property values of luffa–groundnut–reinforced
ground nut composite were slightly higher than that of luffa fiber-reinforced
composite. The alkali-treated composites possessed higher
values of mechanical properties as the alkali treatment
improves the adhesive characteristics of the surface of the luffa
fibers and groundnut.
158
Jute/banana Conventional To improve the mechanical properties, jute fiber are hybridized
fiber hand layup with banana fiber, with various weight ratios (100/0, 75/25, 50/
50, 25/75, and 0/100). The addition of banana fiber in jute/
epoxy composites of up to 50% by weight results in increasing
the mechanical and thermal properties and decreasing the
moisture absorption property.
159
Long kenaf/ Hand layup and The rates of the moisture uptake by the composite increases with
woven glass compression immersion time and exhibit non-Fickian behavior. Exposure of
molding the natural fiber composite material to environmental condi-
tions such as distilled water, sea water, and rain water results in
decreasing of fracture toughness.
160
Date palm/ Conventional The addition of the graphite is highly recommended to reduce the
graphite filler hand layup friction, which thus enhances the wear characteristics of the
date palm epoxy composites. The hybrid composite also shows
better mechanical and tribological performance.
161
Abaca/jute/glass Hand layup The abaca–jute hybrid composite has better properties than the
fiber abaca fiber alone in tensile and shear. The abaca composite is
superior to hybrid composite in flexural and impact strength
and also from neat epoxy. Also, the hybrid composite with-
stands more strain before failure in tensile testing than the
single fiber composite.
162
Banana/hemp/ Hand layup It has been observed that the banana–hemp–glass fibers reinforced
glass fiber hybrid epoxy composites exhibited superior properties and can
be used as an alternate material for synthetic fiber-reinforced
composite materials.
163
Hemp fiber/ VARTM Both flexural and tensile modulus increases when lignin was added
lignin up to 2.5% w/w. An increase in impact properties of the fab-
ricated composites with the energy absorbed by the composite
containing 5% w/w lignin being 145% higher than the composite
with no lignin are also noticeable. The addition of lignin
increased the structural properties of the composites to some
degree when compared with composites with no additional
lignin.
(continued)

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Saba et al. 13

Table 6. Continued

Reinforcement Technique References Modifications in properties

164
Hemp/basalt Compression The impact and flexural strength properties of hybrid composites
fiber molding carried out and hybrid composites have better residual flexural
strength and impact properties compared to non-hybrid
composites.
165
Flax/CF Compression An advanced new CF/flax/epoxy hybrid composite with a ‘‘sand-
molding wich structure’’ as a substitute for metallic materials for
orthopedic long bone fracture plate applications and in ortho-
pedic trauma treatments are found. The developed hybrid
shows improved fatigue or cyclic loading.
166
Bamboo/glass Hand layup fol- Bamboo-based composites exhibit relatively better erosion wear
fiber/red mud lowed by performance than that of the glass fiber-reinforced composites.
light com- The incorporation of red mud particulates results in improve-
pression ment of erosion wear resistance of both the bamboo and glass
molding fiber composites.
167
Rice husk par- Hand layup The rice husk modifies the tensile, flexural, and the interlaminar
ticulates/glass shear strength of the glass-epoxy composites. The microhard-
fiber ness and density of the composites are also greatly influenced
by the content of these fillers. The multiphase hybrid composite
filled with rice husk particulates in glass fiber/epoxy composite
thus has better mechanical properties and lowered erosion
wear properties compared with unfilled samples. The impact
velocity, filler content, impingement angle, and erodent size
influence the wear rate significantly of the developed hybrid
composite.
168
Rice husk par- Hand layup The micro-hardness of the composite is increasing while tensile
ticulates/glass and flexural properties are decreasing with addition of rice husk.
fiber The effective thermal conductivity (Keff.) and CTE of neat epoxy
are reduced by 74.38% and 22%, respectively, and the Tg is
increased by 14 C with addition of (15 wt%) rice husk content.
169
Unidirectional Vacuum bagging A significant increase in tensile strength and modulus observed
hemp/paper when the paper layer is used as core in hemp/paper/epoxy and
and flax/ flax/paper/epoxy composites. A significant increase in tensile
paper/epoxy strength and modulus also obtained compared with the tensile
properties of epoxy matrix.
148
Kenaf/glass Modified SMC PBT toughening with the modified SMC process improved the
fiber/PBT impact properties of hybrid kenaf/glass epoxy composite. The
impact property improved by 54% over the impact property of
the non-toughened bio-composite. Developed hybrid com-
posite is intended to be used in the car bumper beam and
strengthening ribs of the auto-car.
170
Basalt/flax/ Vacuum infusion The mechanical performance of all the hybrid laminates appears
hemp/glass superior to pure hemp and flax fiber-reinforced laminates and
fiber inferior to basalt fiber laminates. Among the hybrids, the best
properties obtained by adding glass and flax to basalt fiber-
reinforced laminates in epoxy.
PLA: polylactic acid; SMC: sheet molding compound; VARTM: vacuum-assisted resin transfer molding method; OPEFB: oil palm empty fruit bunch; CF:
carbon fiber; GMT: glass mat thermoplastic.

properties, and an anisotropic electrical epoxy resins with nano-particles could endow the
conductivity.171,176 materials with some superior properties such as
Table 7 tabulates the recent study with different modest increase in the glassy modulus, broadening of
types of nano-particles reinforcements in epoxy and the glass transition temperatures, low dielectric con-
their method of fabrication. The modification of stant, and significant improvement in key mechanical

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 14
Table 7. Nano-reinforcement in epoxy and its modification by different manufacturing techniques.

Nano-reinforcements Techniques References Modifications in properties

177
Biomass-based CB Hand layup Improvement in tensile and electrical properties observed by the incorporation of 5% CB
(bamboo stem, coconut shell, OPEFB) into the epoxy resin. The CBs-epoxy com-
posites exhibited better flexural properties than the neat epoxy, which was attributed
to better adhesion between the CBs and the epoxy resin. TGA also governed the
improvement in thermal stability of the CB-filled composites compared with the neat
epoxy resin.
178
CNWs Phase-inversion The storage modulus (G0 ) of WTME/CNWs nanocomposites increased with the increase
emulsification of CNWs content. The Young’s modulus and tensile strength of the nanocomposites
were significantly reinforced by the addition of CNWs. The glass transition tempera-
tures (Tg) of WTME/CNWs nanocomposites slightly decrease with the increase of
CNWs content.
179
NGF Stirring and The iso-conversional method show that the effect of conversion on activation energy (Ea)
direct mixing is negligible for both the neat resin and epoxy/(NGF)-filled system. The Ea of epoxy/
NGF are lower than those of the systems without NGF and the reaction get slower in
the presence of NGF.
180
CNTs/glass fiber VARIM The CNT reduces the crack initiation and propagation sites in the epoxy resin. The
addition of pristine CNT in the stoichiometric matrix composition has shown
improvement by 26% in tensile modulus, 42% in tensile strength, 50% in flexural
modulus, and 74% in flexural strength. While with amino-functionalized CNTs, the
flexural modulus and strength increased by 36% and 46%, respectively, as compared
with neat epoxy composite properties.
181
Glass-fiber/organo-modified Hand layup and An average of 11.7% improvement in the ultimate tensile strength, 10.6% improvement in
surface nanoclay compression tensile modulus, and 10.5% improvement in tensile ductility compared with mechanical
properties obtained for the pristine material are observed. The nanoclay-reinforced
composite had a 7.9% greater fatigue strength and a fatigue life over a decade longer or
1000% greater than the pristine composite when extrapolated to 109 cycles or a
simulated 10-year cyclic life.

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182
MWCNTs Hand layup The addition of CNTs increases both the flexural strength and strain to failure by 45%.
Moreover, with the pre-curing step, the nanocomposite with 0.25 wt% CNTs presents
an increase of flexural strength by 58% and strain to failure by 68% regard to neat
epoxy resin.
183
Nano clay/sisal fiber VARIM A dramatic decrease in water mass uptake of nanoclay-filled composites is obtained.
Tensile, DMA, and wear studies for micro-clay filled and unfilled composites decreased
before and after placing in the water medium. However, it improved significantly for
nanoclay-filled composites.
184
Nano-clay platelets/HNTs/(n-SiC) particles Hand layup Addition of the nano-fillers into epoxy matrix decreases both water uptake and diffusivity
compared with unfilled epoxy. Flexural strength and modulus of epoxy-based
(continued)
Journal of Reinforced Plastics and Composites 0(0)
 Saba et al. 15

exposing to water. The presence of nano-fillers increased both fracture toughness and

VARIM: vacuum-assisted resin infusion molding; RTM: resin transfer molding; WTME: waterborne terpene–maleic ester type epoxy resin; HNTs: halloysite nanotubes; n-SiC: nano-silicon carbide; CB: carbon
fracture toughness and impact strength of all types of nanocomposites increases after
Table 8. Manufacturing techniques used in different
nanocomposites also decreases. The addition of nano-fillers enhanced the flexural
strength and modulus of nanocomposites compared with wet unfilled epoxy. The
applications.

Manufacturing techniques Applications fields

Compression molding  Aircraft parts

impact strength of nanocomposites compared with wet neat epoxy.  Skis and snow-boards

black; OPEFB: oil palm empty fruit bunch; CNWs: cellulose nano-whiskers; NGF: nano-glass flake; MWCNTs: multi-walled carbon nanotubes; DMA: dynamic mechanical analysis.
 Skate boards
 Circuit boards
 Prepreg and autoclave
 Aerospace components
 Bicycle frames
 Hockey sticks
 Vacuum Infusion
 Boats and ships
 Wind turbine blades
Pultrusion  Insulator rods
 Arrow shafts
Filament winding  Pressure vessels
 Pipes
 Rocket housings
Modifications in properties

Conventional hand layup
and compression molding
Source: http://composite.about.com
References
 Recreational equipment
 Hard-tissue applications
(skull reconstruction, bone
fracture repair, total knee,
ankle, hip, and other joint
replacements)
 Dental applications (ortho-
dontic arch wires, brackets,
and dental posts)

properties.185 However, in certain cases, nano-particles

commonly shows agglomeration after reinforcing,
which lowered the interfacial interaction between the
nano-particles and matrix.186–189 Surfactant has been
successfully applied to address this challenge to
improve the dispersion and interfacial interaction of
Techniques

nano-particles (such as carbon nanotubes) in epoxy

resin matrix.

Applications of fiber-reinforced epoxy

composite
The lowered viscosity and the absence of aromatic rings
in aliphatic epoxies enables them UV resistant, thus
making suitable for various exterior/outdoor applica-
tions.11 Currently, the manufacturing industries are
promoting natural fiber-based bio-composite and
hybrid composite applications especially in automotive,
building construction, packaging, marine, sporting,190
Nano-reinforcements
Table 7. Continued

aerospace,103 and in furniture to utilize plant fibers

instead of the non-renewable and harmful reinforcing
materials.191,192 Moreover, fiber-reinforced polymer
composites are the most widely used multiphase mater-
ials in orthopedics, artificial limbs.193 In dental appli-
cations, composite resins are fully replacing the

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16 Journal of Reinforced Plastics and Composites 0(0)

Table 9. Reported work on nanocomposite applications in different scientific field.

Nanocomposite Applications field Reasons/improvement in properties References

195
Nano calcium Painting, plastics, and rubber As anti-chemicals, varnishing, and excellent elec-
carbonate/ industries trical isolation.
PMMA
196–204
Nanoclay In packaging material, food pres- Fresh juice packaging (printable and flexible
ervation, interior coatings, technology), electronic packaging, industrial
and processing technology for packaging, and bioactive
beer bottles, beverage, car- packaging. Paperboard juice cartons, injec-
bonated drinks, and thermo- tion-molded bottles, Cast and Blown films
formed containers interior coatings applications
205
CNT In aerospace and automotive Airplane interiors, fuel tanks
industries
205
CNT Electrical and electronic Components in electrical or electronic parts,
industries resistors, capacitors, and inductors
206–211
Inorganic nano- Textiles and soap-cosmetic Modification of textiles properties such as anti-
particles industries bacterial, UV blocking, super hydrophobic,
(gold, silver) anti-fungal, flame retardant, UV absorber,
antistatic and chemical absorber, antimicro-
bials, waste materials removal from the skin
and control sebum
212
Nanoclay Bio medical and membrane Anti-bacterial efficiency, sterilizing effect, Toxins
coatings adsorption
205,213
Layered silicate Heavy and electrical industries Insulating materials for generators, rotators, and
switchgear; SIS; and GIS
205
Nano inorganic Ceramics industries Embedded capacitor having high dielectric
particles constant
200,213
Polymer-layered Automobiles, aerospace, con- Gasoline tanks, bumpers, interior and exterior
silicates struction, and electronics– panels, etc.; flame retardant panels and high-
(MMT, hec- pigment industries performance components; building sections
torite, and and structural panels; printed circuit boards
saponite) and electric components
214–217
Transparent and LED industries, solar cells, and Optically functional and transparent materials (all
optical digital watches optical switches), switching, amplification, high
industries refractive index applications (solar cells to high
refractive index lenses). Visible light transpar-
ency and UV light shielding efficiency in win-
dows for automobiles, trains, and ships and in
precision optical devices
MMT: montmorillonite; CNT: carbon nanotube; SIS: solid insulated switchgear; GIS: gas insulated switchgear; PMMA: Poly(methyl methacrylate).

conventional restorative materials such as amalgam,
gold, alumina, and zirconia.194 Some common prod-
ucts of different applications fields and manufacturing
methods for fiber-reinforced epoxy are tabulated in
Table 8.
Nanocomposite applications
Nanocomposite based on nano technology shows
diverse applications globally. Table 9 shows the com-
piled nanocomposite applications with their important
properties that are applied in different field. Currently,
70% of nanoclay composite structures shows
enhanced applications in many different field of food
preservation, innovative packaging, and processing
technology owing to their great potential tendency
for reducing flavor scalping, increased heat resistance
and improved food quality, safety, and respective sta-
bility.197,199,204 CNT epoxy composite has also been
widely used in aero-automotive, electrical, and elec-
tronics field.205 Layered silicate epoxy nanocomposite
has been exclusively used as insulating materials in
heavy apparatus of auto-aero industries and for elec-
trical insulation.205,213

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Saba et al.
Conclusions and future perspectives
Epoxy matrix regarded as 3-D polymer networks
formed by the chemical reaction between monomers
with some constraints. The curing and aging of epoxy
resins are complex phenomena and are highly decisive
for many industries from many decades. The modifi-
cation of epoxy is critically important to improve its
brittleness, toughness, wear, and fire resistances, and
to widespread its practical applications in many areas
of outdoor, construction buildings, engineering, and
technology sectors. The introduction of natural fiber
reinforcement as an alternative to synthetic fibers
in the epoxy matrices results in lower density,
weight, and cost, accompanied with the better renew-
ability and biodegradability. We concluded that
physical, mechanical, and thermal properties of nat-
ural fiber-reinforced epoxy composite and nanocom-
posite display better performance for manufacturing
of high-performance automotive and aerospace
products and their components. Moreover, it seems
that reinforcing of nano-sized inorganic particles or
fillers in epoxy are gaining more attention from the
academicians and industrialists globally for the
manufacturing of high-performance engineering
materials.
This review article hopefully provide valuable litera-
ture information for further investigations and in the
elaborative study of novel natural fiber-based epoxy
macro–micro composites and nano epoxy composite
as compared with other thermosets and thermoplastic
composites.
The future work would be the production of innova-
tive green nanocomposite materials with biodegradable
epoxy polymeric resin and nano cellulosic fiber having
enhanced properties both for structural and nonstruc-
tural applications. The other forthcoming perspective
would be the development of natural fiber-reinforced
flame-retarded nano epoxy composites to further con-
dense its shortcomings for renewable and/or biodegrad-
able structural materials in construction, automotive,
and aircraft producers industry. Furthermore, investi-
gations of tribological properties along with other
properties of epoxy nanocomposites made from con-
ventional materials obtained directly from agriculture
and bio-wastes, such as jute sticks, coconut pith, rice
husk, ground nut husk, wheat straw, flax straw, and
reed, would be the prime interests of researchers and
scientists.
Declaration of conflicting interests
The author(s) declared no potential conflicts of interest with
respect to the research, authorship, and/or publication of this
article.
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17
Funding
The first author acknowledges the International Graduate
Research Fellowship (IGRF) UPM-Malaysia grant support
to this work. The authors are also thankful to the Universiti
Putra Malaysia for supporting this research study through
Putra Grant Vot No. 9420700.
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