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A Review on Peanut Shell Powder Reinforced Polymer Composites

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DOI: 10.1080/03602559.2018.1471720

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A Review on Peanut Shell Powder Reinforced

Polymer Composites

Nor Fasihah Zaaba & Hanafi Ismail

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Powder Reinforced Polymer Composites, Polymer-Plastics Technology and Engineering, DOI:
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POLYMER-PLASTICS TECHNOLOGY AND ENGINEERING
https://doi.org/10.1080/03602559.2018.1471720

A Review on Peanut Shell Powder Reinforced Polymer Composites

Nor Fasihah Zaaba and Hanafi Ismail
School of Materials and Mineral Resources Engineering, Universiti Sains Malaysia, Nibong Tebal, Malaysia

ABSTRACT KEYWORDS
Recently, the critical discussion about the innovation of superior properties of engineering Chemical modification;
products that produced from natural resources has led to the renewed interest worldwide, mechanical properties;
concerning renewable and environmental issues. Rigorous study has been conducted on the peanut shell powder;
thermal properties
natural fillers by both academicians and industrial researchers. Amongst the various sorts of
natural resources, peanut shell powder has been considerably utilized over the past few years.
Therefore, this study raises an overview with a specific focus on the improvements made in the
scope of peanut shell powder reinforced polymer composites in various type of polymer matrices
(i.e. thermoplastic, thermoset and natural rubber).

GRAPHICAL ABSTRACT

Introduction predominantly those from renewable resources and par-

ticularly that of polymers obtained from agro resources
Petroleum based plastics caused a serious environmental
such as natural filler has long been recognized. This type
problem owing to its properties of superior resistance to
of polymer could be an attractive solution to preserve
environmental effects. By the reasons of their backbones
petroleum resources by substituting some petroleum
are uniquely composed of hydrogen and carbon atoms,
based polymers and to defeat the higher cost of petro-
this makes this polyolefin versatile and highly durable to
chemical resources. In fact, they contribute to the reduc-
sunlight, heat, humidity and microorganisms [1]. The
tion of CO2 emission as well [6]. As stated before, the
resolution of the waste management problem caused by
growing anxiety concerning the discarding of plastic
non-degradable plastic materials can be achieved by the
waste as well as the necessity for multipurpose plastic
partial replacement of polyolefin with natural fillers.
materials have commanded to increase the attention in
Determinations have been carried out to discover the
combination of degradable materials with synthetic mate-
opportunity of consuming natural fillers as a reinforcing
rials. For the purpose of degradability, the conventional
element in polymer composites [2–4]. Besides that,
plastics are normally incorporated with biodegradable
endeavor is undertaken on the utilization of natural poly-
polymers (i.e. natural filler). This may support the
mers such as starch, cellulose, lignin, chitin and chitosan
approachability of the plastics to oxygen and
[5]. Biodegradable polymers or biopolymer

CONTACT Hanafi Ismail ihanafi@usm.my School of Materials and Mineral Resources Engineering, Universiti Sains Malaysia, 14300 Nibong Tebal,
Penang, Malaysia.
Color versions of one or more of the figures in the article can be found online at www.tandfonline.com/lpte.
© 2018 Taylor & Francis
2 N. F. ZAABA AND H. ISMAIL

microorganisms. Modified plastics have been proved to to fabricate a naturally degradable and eco-friendly
be met the requirements and assured at least partial composite from these types of fillers as reinforcing
degradation [7]. Though, it has been discovered that the components in polymer composites without affecting
inclusion of natural filler as a lower element in the syn- its rigidity [15]. Apart from the above mentioned ben-
thetic polymer affects a decrease of the mechanical prop- efits, natural fillers have appealed to increase the inter-
erties owing to the immiscibility caused by the dissimilar est among researchers due to their ease of separation,
polarity of the filler and matrix [8]. non-abrasive to equipment, renewability and carbon
dioxide sequestration [2, 16–18].
Consumption of high loading natural fillers results in
Natural filler composites high stiffness [19, 20]. In Europe, the thermoplastic/nat-
Current attentiveness in decreasing the environmental ural filler composites have been conquered by an auto-
effect of plastic materials is leading to the growth of motive application while in the USA, more prominence
newer plastic materials or products. Apart from that, on rail and decking products. Applications for these
due to the lack of petroleum sources and stress for composites comprise dashboard, car roofs, seat panels,
reducing the dependency on petroleum products, interior panels, headliners, acoustic panels and parcel
there is an increasing attention in exploiting the use shelves. Besides that, in China and other parts of Asia,
of renewable materials [9, 10]. As described before, the the natural filler/thermoplastic composites are starting to
inclusion of natural filler as reinforcements is one of involve with pallets, doors, and architectural moldings. In
the fascinating methods to develop the performance of fact, many determinations have been paying attention on
the polymer composite materials which met the the use of natural polymers which are inexpensive, renew-
requirements in engineering applications. That is why, able and also biodegradable [21–23]. Efforts are ongoing
the concern for natural filler reinforced composites to determine unconventional resources for biopolymers.
have been improved drastically in the last few years, Corn stover, wheat straw and cotton stalk, soy protein as
especially for numerous commercial applications [11, well as wheat gluten are amongst the agricultural by
12]. Combining natural fillers with thermoplastic is products and agricultural co-products that have been
becoming one of the biggest areas of research [13]. By explored for their potential use as a matrix [14].
addition of natural fillers to thermoplastics can reduce The rising quantity of publication throughout the
the cost of the final product. Somehow it can increase latest years reveals the rising interest regarding this nat-
the performance of the final product. Moreover, most ural filler polymer composite [1, 4, 21–28]. Presently, a
of the researchers concentrated on improving the final rough indication of the increasing interest among
properties of this natural filler/thermoplastic plastic researchers on this topic have been recognized. Table 1
product by using additives such as compatibilizer, cou- presented the chemical compositions of some common
pling agent or chemical treatment. As reported by cellulosic or lignocellulosic fillers [29]. Most of the
Ragunathan et al. [4] in their previous study on the
compatibilizing effect of polypropylene maleic anhy- Table 1. Chemical compositions of various natural fillers [1–3].
dride (PPMAH) on polypropylene (PP)/acrylonitrile Cellulose Hemicellulose Lignin Waxes
butadiene rubber (NBR)/palm kernel shell (PKS) com- Filler (wt. %) (wt. %) (wt. %) (wt. %)
Baggase 55.2 16.8 25.3 -
posites, where the results presented that, the compati- Bamboo 26–43 30 21–31 -
bilized composites showed a higher tensile strength and Flax 71 18.6–20.6 2.2 1.5
Kenaf 72 20.3 9 -
tensile modulus as compared to uncompatibilized com- Jute 61–71 14–20 12–13 0.5
posites. In another publication, Reddy and Yang [14] Hemp 68 15 10 0.8
Ramie 68.6–76.2 13–16 0.6–0.7 .
reported in their research work that the developed soy Abaca 56–63 20–25 1–9 3
protein-jute fiber composites showed a relatively high Sisal 65 12 9.9 2
Coir 32–43 0.15–0.25 40–45 -
tensile strength and modulus. Oil Palm 65 - 29 -
Natural fillers have some benefits compared to tradi- Pineapple 81 - 12.7 -
Curaua 73.6 9.9 7.5 -
tional fillers and reinforcing materials even though it is Alfa 45.4 38.5 14.9 2
not as popular as mineral or inorganic fillers. The main Banana 63–67.6 10–19 5 -
Cotton 82.7–90 5.7 <2 0.6
benefits of consuming lignocellulosic fillers as fillers/ Henequen 60–77.6 4–28 8–13.1 0.5
reinforcements in plastics are non-abrasive, low densi- Isora 74 - 23 1.09
Nettle 86 10 - 4
ties, biodegradable, low energy consumption, low cost Peanut 35.7 18.7 30.2 -
and easily recyclable. Besides, it is an efficient approach Piassava 28.6 25.8 45 -
 POLYMER-PLASTICS TECHNOLOGY AND ENGINEERING 3

natural fillers, comprise of cellulose, hemicelluloses and Peanut shells consist of cellulose, hemicelluloses, and
lignin, while pigments, pectins and extracts can be lignin microfibrils. The chemical compositions of pea-
obtained in minor quantities [30]. nut shell fillers are cellulose (35.7%), hemicelluloses
(18.7%), lignin (30.2%), protein (8.2%), carbohydrate
(2.5%) and ash content (4.7%) [34]. Hence, the con-
Mechanical and physical properties of various sumption of peanut shell as natural fillers in thermo-
natural fillers plastic/natural filler composites tends to raise a new
Instead of chemical composition, the cellulosic fillers’ application path in the transformation of agro wastes
properties are significantly affected by their morphologi- to beneficial resources in plastic industries [25].
cal factors for instance the microfibril angle, internal fiber
structure, defects and dimensions of the cell [30]. It is
expected that the mechanical properties of natural fillers Structure and chemistry of peanut shell powder
are influenced by the microfibrillar angles. In relation, the
higher cellulose content, higher degree of polymerization Figure 1 shows the structure of lignocellulose. The
of cellulose, longer cell length and lower microfibrillar primary constituent of this lignocellulose is glucose
angle leading to increase the mechanical strength [31]. molecules with beta(1–4)-linked chain which is also
Table 2 illustrates the physical and mechanical properties known as cellulose [11, 35]. The crystalline cellulose
of various natural fillers as available in the literature. is resistance to degradation which is contributed by
Owing to the different fillers were used, different testing hydrogen bonds between different layers of the
methods were employed and different moisture condi- polysaccharides. Besides that, the second most abun-
tions were presented, the properties of natural fillers dant constituent of lignocellulose is hemicellulose
might be vary among the cited work [32, 33]. which consists of various 5- and 6-carbon sugars
such as glucose, mannose, xylose, arabinose and
galactose. Lignin comprises three main phenolic ele-
Peanut shell powder as natural filler ments, namely sinapyl alcohol (S), and p-coumaryl
Peanut (Arachis hypogaea) is one of the world’s main alcohol (H) and coniferyl alcohol (G) [36, 37].
edible crops. It is grown principally for its fruits. It is Generally, hemicellulose is used as tablet binders,
frequently named as groundnuts due to their husks (shells) gelling agents and viscosity modifiers [38, 39]. The
grow underground. The top growing country of peanut is polymerization of these three components synthe-
Africa following by USA, China, and India. Peanut is able sized lignin. Lignin structure is very dense compris-
to produce waste shell with bulky volumes. Several deter- ing of three-dimensional structure of phenyl
minations to discover the utilization of these waste materi- propane units [40, 41]. The ratio of these compo-
als have led to limited or low-value application. nents is varied within different plants, cell wall
layers and wood tissues [42]. Microfibrils are
formed by cellulose, hemicellulose and lignin. Its
Table 2. Mechanical and physical properties of various natural
structured into macrofibrils that facilitates structural
fillers [1, 4].
Tensile
stability in the plant cell wall [43].
Strength Young’s Elongation at Density Membrane of the cell wall in fillers is not homo-
Filler (MPa) Modulus (GPa) break (%) (g/cm3) geneous. It is complex and built up with layered
Baggase 290 17 - 1.25
Bamboo 140–230 11–17 - 0.6–1.1
structures. Figure 2 shows the molecular structure
Flax 345–1035 27.6 2.7–3.2 1.5 of cellulose. As can be seen from Figure 2, the
Kenaf 930 53 1.6 -
Jute 393–773 26.5 1.5–1.8 1.3 layered structures comprise with a primary wall
Hemp 690 70 1.6 1.48 which is the first layer positioned through cell growth
Ramie 560 24.5 2.5 1.5
Abaca 400 12 3–10 1.5 surrounding by three layers of secondary wall [35].
Sisal 511–635 9.4–22 2–2.5 1.5 The mechanical properties of the fillers are controlled
Coir 175 4–6 30 1.2
Oil palm 248 3.2 25 0.7–1.55 by this thick central layer of secondary walls. The
Pineapple 1.44 400–627 14.5 0.8–1.6 long chain of cellulose molecules forms a series of
Curaua 500–1150 11.8 3.7–4.3 1.4
Alfa 350 22 5.8 0.89 helically wound cellular microfibrils which are com-
Banana 500 12 5.9 1.35 pleted as middle layer [11]. During the filler produc-
Cotton 287–597 5.5–12.6 7–8 1.5–1.6
Henequen 430–570 10.1–16.3 3.7–5.9 1.2 tion, several factors such as filler supply stage,
Isora 500–600 - 5–6 1.2–1.3 extraction stage, harvesting stage, and plant growth
Nettle 650 38 1.7 -
Peanut 55–70 1–5 2.7–10 - that can effected the overall quality of the natural
Piassava 134–143 1.07–4.59 7.8–21.9 1.4 cellulosic fillers [44].
4 N. F. ZAABA AND H. ISMAIL

Figure 1. Structure of lignocellulose (adapted from www.nature.com).

Figure 2. Structure of lignocellulose (adapted from www.nature.com).


Processing of peanut shell powder reinforced
composites
Preparation of peanut shell powder
According to Zaaba et al., the peanut shells were firstly
subjected to a grinding process, that produced a range
between 70–250 μm of particle size. By using a vacuum
oven, PSP was then dried at 70°C for 3 hours before being
used in subsequent PSP/recycled polypropylene compo-
site fabrication [45]. While for the preparation of PSP by
Prabhakar et al., the PSP was begun with washed in water
to remove dirt, sand and other contaminations. Next, by
using distilled water, it was washed with several times.
Then, lignin and greasy substantial from the shell were
eliminated through soaking them for 30 min in 2% of
NaOH solutions. Later, the PSP was washed in distilled
water. To eliminate the moisture content, it was dried for
2 days under the sunlight and then for 1 day in an oven at
120°C. Subsequently, the dried PSP was ground using a
kitchen grinder and sieved with yielded 200–300 μm of
particle size before being used in PSP/epoxy composites
fabrication [46]. Besides that, PSP was also prepared by
Chamaiporn Yamoum and Rathanawan Megaraphan for
the PSP/PLA composites fabrication, where the PSP was
firstly washed by water and dried at 80 °C for 3 days.
Then, the PSP was ground by using a grinder and sieved
by 200 mesh in order to obtain uniform filler. The yielded
particle size was 66.8 ± 13.2 μm [47]. While for PSP
preparation in polyethylene matrix reported by Obasi,
300 μm of average particle size was obtained. Also, PSP
was prepared by Sareena et al. in natural rubber matrix,
where the powdered PSP was sieved into 45–90 μm of
particle size [48].
Melt mixing and compression molding
For the preparation of PSP/thermoplastic composites, to
obtain a homogeneous sample, the PSP reinforced compo-
sites were prepared using an internal mixer (Haake
Rheomix Mixer, Model R600/610) with speed of 50 rpm
and at a temperature of 180°C. Initially, the thermoplastic
resin was placed in the mixer and melted for 4 min. Next,
the PSP was added and the composites were mixed for
8 min while waiting for the mixing torque stabilized. The
total mixing time was 12 min for all samples. Later, the
compounded samples were cooled down for 24 hours
before subjecting to shaping process. An electrically heated
hydraulic press (Kao Tieh Go Tech Compression Machine)
with a temperature of 180°C were then used to compres-
sion molded (hot press) the processed samples into a 1-
mm-thick sheet. Melt mixing and compression molding
are broadly recognized as one of the conventional
POLYMER-PLASTICS TECHNOLOGY AND ENGINEERING 5
techniques in fabricating PSP/thermoplastic composites
due to its ease and efficient processing method [49–53].
Whereas, PSP/thermoset composites were also pre-
pared, where the PSP and thermoset resins were firstly
mixed in a container and stirred well for 5–7 minutes.
To obtain a homogeneous mixture, the mixture was
again stirred for 10 minutes after adding the hardener
and catalyst. The glass mould (120 mm x 120 mm x
4 mm) was used to place the mixture. To polish the
glass mould, a releasing agent/wax has been used, in
order to avoid the composites from sticking onto it
upon removal. Then, the mixture was compressed uni-
formly after placed in the mould. This set up permitted
for curing and finally, the composite was taken out
from the mould. Different resins will have different
curing time [46, 54, 55].
Besides that, PSP/natural rubber composites were
also prepared. Firstly, all chemicals were powdered
and weighed precisely. Compounding was done via a
two-roll mill at 27°C. To prevent sticking of the rubber
compound to the mill rolls, the total mixing time has
been kept to a minimum (12 minutes). Precaution was
taken by using cooling to avoid that the mill-roll tem-
perature increases too high, that is beyond the set
temperature. This is to prevent any cross-linking dur-
ing mixing [56].
Challenges for peanut shell powder as
reinforcement in polymer composites
As mentioned previously, natural fillers/thermoplastic
composites offer a lot of benefits over the other materials
for example easy processing, flexibility, considerable
toughness, eco-friendliness as well as recyclability [41,
57]. However, there are few crucial drawbacks of the
usage of the lignocellulosic filler that limit its applications.
The main problem is the compatibility between the
hydrophobic thermoplastic and the high hydrophilic nat-
ure of natural fillers in composites. The mechanical prop-
erties of composites are depending strongly on the
interfacial adhesion between the filler and the matrix
components. However, this can be solved by enhancing
the adhesion and interaction between the fillers and the
matrix. The first approach that can be used to improve the
interfacial adhesion is by using coupling agents. Coupling
agents can modify the polymer matrix and enhance the
interfacial strength and mechanical properties of the pro-
ducts. Apart from that, filler treatment before mixing
process also can be used to improve the interfacial adhe-
sion [58]. Since the presence of hydroxyl groups in lignin
and cellulose, natural fillers have a decent potential for
chemical treatment. Hydroxyl groups reaction are able to
alter the polarity and surface energy of the natural fillers
6 N. F. ZAABA AND H. ISMAIL
[59]. Besides that, the possibility of lignocellulosic to
degrade and volatile emissions during processing also
limit its applications. Consequently, the processing tem-
perature should be limited to 200°C. Due to these pro-
blems, the types of thermoplastics that can be used are
also limited. For instance, only PE, PP or PS can be used
in processing with natural fillers. Another drawback is the
high moisture absorption of the natural fillers due to the
high hydroxyl groups in lignocellulosic. This results in
fillers swelling and finally affected the properties of com-
posites. Nevertheless, the moisture absorption of the fil-
lers can be lessened through chemical modification of
hydroxyl groups present in the fillers [60, 61].
While for the preparation of natural fillers/thermoset
composites, it offers few advantages such as easy proces-
sing and less temperature is required compared to the
thermoplastic composites. This is due to the liquid form
of the initial resin system. Thus, the natural fillers can be
easily mixed with the resin. Low pressure is required and
simple low cost or self-made is needed for these compo-
sites systems. Besides, natural fillers can be easily wet, as
well as higher fillers loading can be achieved depending to
the viscosity of polymer resin [35, 36, 62–64]. Instead of
the advantages, these thermoset polymer matrix compo-
sites also have major drawbacks such as non-recyclable
and high curing time [11, 38–40, 65].
Besides, the major drawback using natural rubber as
polymer matrix is the rigidity of natural rubber. In fact,
due to the unbearable degradation in a realistic period
causes it inappropriate for creating a degradable material.
Though, the incorporation of natural filler supports fab-
ricating an improved biodegradable and environmental-
friendly products. Numerous studies have been carried
out regarding natural rubber composites reinforced with
different fillers [66–72]. Nevertheless, only minor studies
have reported in natural rubber/peanut shell powder
composites [48, 56, 73].
Chemical modification
Due to the hydroxyl groups in cellulose and lignin, the
natural fillers are capable to modification. However, the
contribution of hydroxyl groups in hydrogen bonding
within the cellulose molecules causes the decrement of
effectiveness of natural fillers towards the polymer matrix
(interfaces). Mechanical and physical properties of com-
posites are depending on the interfaces between elements.
Though chemical/physical treatments or specific interfa-
cial additives can be utilized to improve the interfacial
adhesion through triggering these groups and offering the
new moieties that can proficiently interconnect between
the fillers and the polymer matrix [4, 38, 74]. In addition,
traditional chemical treatments for instance extraction
with alcohol, benzene, or sodium hydroxide (NaOH)
(delignation and bleaching) can also be applied.
Through various chemical modifications of natural fillers,
a distinctive stage of attainment in improving adhesion
and strength between the fillers and the matrix can be
achieved [1]. Below are the brief clarifications of several
significant chemical modifications of natural filler which
can be applied.
Compatibilization with poly(ethylene-co-acrylic
acid)
Poly(ethylene-co-acrylic acid) (PEAA) is synthesized via
free radical copolymerization of acrylic acid and ethylene
with high pressure. It is also known as carboxylated ethy-
lene copolymer [75]. The principal monomers, acrylic
acid and ethylene determine the properties of PEAA
copolymers. Many olefinic polymers consist of ethylene
as a basic monomer. Polyethylene is hydrophobic in nat-
ure which is composed of only carbon and hydrogen.
Likewise, its symmetric structure lets it to crystallize
under suitable circumstances. While for acrylic acid, the
pendant carboxylic acid group permits it to absorb water
even though it also has a backbone of carbon and hydro-
gen. Hydrogen groups opposite the acrylic acid group
tend to backbite during polymerization, hence imparting
itself to branching [76, 77]. Free radicals of the cellulose
molecules may initiate the acrylation reaction. High
energy radiation can be used to treat cellulose, thus gen-
erate radicals and chain scission [78]. In natural fillers
surface modification, acrylation lead to strong covalent
bond formation, thus slightly increased the tensile
strength and tensile modulus of treated fillers [79, 80].
Equation 1 exhibits the complete reaction between cellu-
lose-OH groups and acrylic acid from PEAA [81].
Fillers
OH þ CH2 CH
COOH !
(1)
Fillers
O
CO
CH
CH2 þH2 O
Filler modification by polyvinyl alcohol
In 1924, the first polyvinyl alcohol (PVOH) was prepared
by Hermann and Haehnel via hydrolyzing polyvinyl acet-
ate in potassium hydroxide and ethanol. Usually, PVOH
is produced using a continuous process from polyvinyl
acetate [82]. In the presence of aqueous sodium hydroxide
or anhydrous sodium methylate, acetate groups are
hydrolyzing using ester exchange with methanol. Degree
of hydrolysis and degree of polymerization are important
to determine its specific functional uses and physical
characteristics. PVOH is a powder with tasteless, odorless,
translucent, white or cream colored. The applications of
PVOH in food supplement tablets is as a moisture barrier

while in natural filler/thermoplastic composites applica-
tion, PVOH can be used in natural fillers modification.
This is because PVOH is a hydrophilic polymer. It has a
hydroxyl group on each of its repeating units, thus pro-
motes the interaction of hydrogen bonds with hydroxyl
and carboxyl groups of cellulose fillers. Equation 2 shows
a result of filler treatment by PVOH.
Fillers
OH þ CH2
CH
OH !
(2)
Fillers
O
CHCH2 þH2 O
Alkaline peroxide pre-treatment
Another considerable modification of natural fillers is
through alkaline peroxide pre-treatment. The procedure
is via the interference of hydrogen bonding in the network
structure [61, 83–85]. In this treatment, fillers is immersed
in sodium hydroxide (NaOH) solution for a period of time
[40, 86]. Subsequently, a certain amount of lignin, wax and
oils that are protecting the external surface of the fillers cell
wall are removed, short length crystallites are exposed
while celluloses are depolymerized [87]. The addition of
aqueous NaOH to natural fillers allowed the ionization of
hydroxyl groups to alkoxide [88]. Owing to that, the expo-
sure of celluloses on the fillers surface is increased and the
mechanical interlocking is improved [1]. Thus, promotes
natural fillers wetting and increased the number of possible
reaction sites. Additionally, in order to increase the
mechanical properties of polymer composites, previous
researches have been done regarding alkaline treatments.
20
15
Tensile strength (MPa)
10
0
0 5 10
Peanut husk (wt.%)
Figure 3. Tensile strength of compatibilized and uncompatibilized PHF/LDPE composites [7].
POLYMER-PLASTICS TECHNOLOGY AND ENGINEERING 7
For example, John et al. [89] studied the effect of alkali
treatment on properties of hybrid filler composites. The
results of alkali treatment showed that the fillers surface
area effectiveness in contacting the polymer matrix tends to
increase through breaking the fillers bundle into smaller
size of fillers. Above and beyond that, Sreekala et al [90].
and Mukherjee et al. [91] stated in their results that after
the partial removal of lignin and hemicellulose by alkali
modification of cellulose fillers, the interfibrillar region
becomes less dense and less rigid. Equation 3 illustrates a
result of alkaline treatment [92].
Fillers
OH þ NaOH ! Fillers
O
Na þ þ H2 O (3)
Properties of peanut shell powder reinforced
composites
Mechanical properties
Mechanical characteristics such as tensile properties can
present the performance and properties of polymeric
materials. These characteristics will influence the physical
capability particularly under critical and extreme circum-
stances, whereas related to the performance of engineer-
ing. From previous years, several findings have been
reported on PSP/thermoplastic composites, with aims to
entirely illustrate its mechanical performance [25, 47, 54,
55]. Furthermore, the tensile properties of PSP reinforced
composites involved: tensile strength (the maximum
engineering stress in tension that may be sustained before
breaking), elongation at break (the ability to resist changes
Compatibilized composites
Uncompatibilized composites
15 20 25
8 N. F. ZAABA AND H. ISMAIL

25

Compatibilied composites
Uncompatibilied composites
20

Elongation at break (%) 15

10

0
0 5 10 15 20 25
Peanut husk (wt.%)

Figure 4. Elongation at break of compatibilized and uncompatibilized PHF/LDPE composites [7].

of shape without crack formation) and Young’s modulus Table 4. Tensile properties of PSP/natural rubber composites
(tensile elasticity). For example, Obasi [25] reported that [6].
the addition of peanut husk filler (amorphous in nature) PSP Tensile strength Tensile modulus Elongation at break
(phr) (MPa) (MPa) (%)
reduced the tensile strength and elongation at break 10 22.75 2.6 1184
which continuously decreased with increasing filler con- 20 18.81 3.1 1020
tent (Figures 3 and 4). The reduction might be due to 30 14.81 3.5 603
40 12.09 4.1 580
poor adhesion between the filler and the matrix caused by
filler-filler interaction, which turn out to be more distinct
than that of the filler-matrix interaction. Besides that, increment of filler content as agreement with other
different polarities between the polar cellulosic filler and reported studies [98–101]. Accordingly, numerous
the non-polar matrix which could initiate and propagate researchers have revealed that the addition of compatibi-
sites for failure. However, addition of maleated polyethy- lizers improve the interfacial adhesion through steric sta-
lene (MAPE) as compatibilizer improved the tensile bilization, good wetting and reduction in surface tension
strength and elongation at break of peanut husk filler/ [102, 103].
low density polyethylene (PHF/LDPE) composites. While for PSP/thermoset composites, the tensile
Numerous studies have reported the reasonable improve- strength and tensile modulus results showed in Table 3.
ment on properties of natural filler composites by adding According to Prabhakar et al. [46], the modification of
MAPE coupling agent [93–95]. While for tensile modu- PSP with alkali offers substantial enhancement in filler-
lus, the presence of fillers might hindered the polymer matrix adhesion along with overall mechanical properties
chain mobility of polymer matrix, in addition to the of the composites. Obviously, the addition of modified
stiffness of the composites [96, 97]. The rigidity of the PSP has produced the reinforcing effect which is reliable
composites could be linked to the cellulose contents of for the increment of tensile strength. Obviously from
peanut shell fillers. Tensile modulus increases with the Table 4, the tensile strength (from 33.20 MPa to
35.36 MPa) and tensile modulus (from 1890 MPa to
1960 MPa) were regularly improved with addition of
Table 3. Tensile strength and Young’s modulus of PSP/epoxy
composites after alkali treatment [5]. PSP loading. Owing to the well bonded and dispersed
PSP (gm) Tensile strength (MPa) Tensile modulus (MPa) between the PSP and the epoxy matrix, leading to an
5 33.20 1890 improvement in interfacial adhesion between the filler
10 34.71 1920 and the matrix. Thus, increase the tensile strength of the
15 35.56 1960
composites [46, 55]. In addition, it was also reported by
 POLYMER-PLASTICS TECHNOLOGY AND ENGINEERING 9

most of the researchers where the tensile modulus
increases as the filler loading increased [104–107]. This
behavior may possibly due to the increment of the stiff-
ness of the reinforcing particles than the matrix materi-
als [46].
Table 4 shows the effect of PSP loading on tensile
properties of PSP/natural rubber composites. Apparently,
the tensile strength shows a maximum value at 10 phr of
PSP loading. The increment of the PSP loading manages to
reduce the tensile strength of PSP/natural rubber compo-
sites. This showed that at 10 phr of PSP loading, a uniform
distribution of PSP in natural rubber matrix can be
achieved. Thus, resulting in better interfacial adhesion
between the filler and the matrix, leading to increase the
tensile strength of the composites. However, as PSP loading
increases, the tensile strength tends to reduce. Indeed, at
higher filler loading, the weak interaction and bonding
between the fillers and the matrix leads to filler agglom-
erate and subsequently deteriorate the tensile strength
of the composites [56]. Contradictory, the elongation at
break tends to reduce as increasing the filler loading
(Table 4). This was due to the reduction of the deform-
able rubber portion in the composites, which is known
as dilution effect [108, 109]. The increment of filler
loading may harden and stiffens the natural rubber
compounds. Owing to that, the resilience and tough-
ness decreased, which ultimately lower the elongation
at break of the PSP/natural rubber composites. Similar
to tensile strength, the tensile modulus of PSP/natural
Table 5. Various value of tensile strength and Young’s modulus
of PSP with different polymer matrix done by others researcher.
Tensile strength Young’s modulus
Composites (MPa) (MPa)
PSP/PE 13.0 2000.0
PSP/PP 20.0 1000.0
PSP/Epoxy 24.0 1600.0
PSP/Polyester 58.0 2500.0
PSP/PLA 60.0 2100.0
PSP/Natural 21.4 2.5
Rubber
rubber composites also tends to increase as the filler
loading increased. (Table 4). In fact, fillers are well-
known to offer the increment of rigidity and stiffness
of the materials. Therefore, as more filler particles were
introduced into the rubber, the elasticity of the rubber
were decreased, resulting in higher tensile modulus of
PSP/natural rubber composites. Table 5 shows the var-
ious results (at 10 wt.% of PSP loading) of tensile
strength and tensile modulus of PSP with different
polymer matrix reported by other researchers.
Thermal properties
Thermal properties are another essential characteristic
that requires to be counted in order to observe the
overall behavior of PSP reinforced polymer composites.
For this purpose, two common characterization
approaches were used which are Thermo Gravimetric
Analysis (TGA) and Different Scanning Calorimetric
(DSC). In fact, numerous important parameters could
be considered form the DSC scans result, for instance
the melting temperature, crystalline level, glass transi-
tion temperature (Tg) and oxidation [110]. In the
meantime, the mass of the sample as a function of the
temperature can be obtained from the TGA analysis.
Usually, changes of mass take place during magnetic or
electrical transformation, decomposition, evaporation,
chemical reaction, and sublimation of the material,
which are precisely correlated to thermal stability [111].
Predominantly for PSP/thermoplastic composites,
Chamaiporn Yamoum and Rathanawan Magaraphan
[47] were implemented both TGA and DSC on poly-
lactic acid/peanut shell (PLA/PNS) biocomposites with
Reference
aims to investigate their thermal characteristics. From
[7, 8]
[9–11] the DSC analysis as shown in Table 6, the Tg of bio-
[5, 12] composites PNS are lower than that of PLA. This was
[13, 14]
[15] due to the hydrolytic degradation of PLA chains that
[6, 16, caused by the moistures in PNS. Besides that, the Tg
17]
was also influenced by plasticizing effect that triggered

Table 6. Thermal properties and density of PLA and the (PNS) biocomposites [15].
Density (g/cm3)
Tg Tcc Tm1; Tm2
Sample Run (°C) (°C) ΔHcc (J/g) (°C) ΔHm (J/g) Xc (%) Theory Experiment
PLA 1st 56.9 120.4 13.1 152.5 16.8 3.98 1.25 1.25
2nd 51.1 128.4 4.6 152.7 8.3 3.98
10PNS 1st 56.1 103.6 20.2 144.6; 151.6 21.9 2.03 1.27 1.25
2nd 51.9 109.3 23.9 145.4; 153.4 28.1 5.02
20PNS 1st 51.6 106.8 27.0 144.1; 153.4 29.6 3.49 1.31 1.31
30PNS 2nd 51.1 107.2 25.2 143.9; 153.3 30.0 6.45 1.34 1.35
40PNS 1st 54.9 105.9 22.1 148.3 18.1 27.80 1.37 1.28
2nd 51.7 87.6 18.5 143.8; 153.1 28.0 9.06
1st 36.0 143.4 24.7 44.26
2nd 127.5; 144.1 21.4 5.19
10 N. F. ZAABA AND H. ISMAIL
by the minor content of oil component in PNS which is
0.92 wt.%. Notably, the 40PNS exhibits the lowest value
of Tg. This implied that the highest amount of moisture
content in PNS caused hydrolysis of the PLA chains
and generated short chains for example oligomers, lac-
tic acid and other water soluble product [112]. The
short chains performed well as plasticizers to rise the
chain mobility during the heating lead to the decreasing
of Tg. Likewise, the PNS biocomposites also have lower
melting temperature (Tm) and cold crystallization tem-
perature (Tcc) compared to PLA. A comparable results
has also been reported in other PLA biocomposites
[113]. The Tcc of PLA/PNS biocomposites decreased
as PNS loading increases. This indicated that the PNS
facilitates the crystallization process of PLA.
Furthermore, the crystallinity of the PNS biocomposites
improved 5% to 9% in contrasted with that of PLA
which is 4%. The results revealed that PNS was an
effective nucleating agent for PLA. Besides that, when
PNS loading up to 30 wt.%, the crystallinity of the
biocomposites also raised. The addition of 40 wt.%
PNS loading displays a reduction in crystallinity,
owing to the occurrence of several void or pores struc-
tures [47].
While for PSP/thermoset composites, the thermal sta-
bility of the composites was examined with TGA by
Prabakar et. al [46]. on the PSP/epoxy composites.
Figure 5(a) presented the TGA curves of the PSP/epoxy
composites. It was found that, the weight loss from seg-
mental decomposition can be detected from the enhance-
ment in thermal stability for epoxy networks by the
inclusion of the PSP molecules into the systems. During
the first stage, a minor weight loss was spotted, accredited
to the dehydration of moisture and other volatiles [101,
114, 115]. In fact, degradation occured in second stage,
owing to the thermal degradation of cellulose, hemicellu-
loses and lignin together with polymeric matrix.
Figure 5. Thermal properties of PSP/Epoxy composite; (a) TGA and (b) DTA [5].
Subsequently, the rate of decomposition is getting slow.
These outcomes are also proven by differential thermal
analysis (DTA) curves in Figure 5(b) whereas, it can be
detected that most decomposition take place at the tem-
perature of 321 to 420°C (second region). Additionally,
onset thermal degradation temperature, end of degrada-
tion temperature, corresponding weight loss, weight loss
peak temperatures and the char yields are the quantitative
data that can be observed in the second region. Obviously,
from TGA and DTA curves, the lowest initiation tem-
perature of thermal decomposition is for C1 composite
sample (5 wt.% of PSP materials with epoxy resin) while
the highest for C9 composite sample (15 wt.% of PSP
material with epoxy resin).
Degradation studies
Researchers and scientists have through a serious deter-
mination to enhance the stability and properties of
plastic materials by concerning the environmental
impacts ever since the first developments of these mate-
rials. Presently, plastic materials have created a serious
environmental problem mainly caused by waste plastic
packaging. Alternatively, the waste management strate-
gies such as incineration, plastic recycling and land-
filling are not an optimal solution and remain as a
controversy subject among researchers, scientist and
public. Therefore, intensive studies have been carried
out to develop novel plastic materials which have
equivalent performance to the conventional plastic
materials as well as capable to dispose under environ-
mental degradation. Degradation is referred to the
changes in plastic properties including mechanical,
morphological, physical and thermal properties.
Plastic degradation in the environment involves few
mechanisms: photo-oxidative degradation, thermo-oxi-
dative degradation, and biodegradation by
 POLYMER-PLASTICS TECHNOLOGY AND ENGINEERING 11

a b

c d

e f

Figure 6. SEM images of (a) PNS at 0.4 k magnification; (b) PNS at 0.6 k magnification; (c) PLA; (d) 30PNS; (e) 40PNS; (f), 40PNS at 1k
magnification [15].

microorganisms [116, 117]. Conversely, this whole pro-

cess is totally slow, taking 50 or more years to fully
degrade [118]. Scanning electron micrographs (SEM) of
the samples after biodegradation is a convenient
approach to study the extent of biodegradation as well
as to evaluate the level of filler/matrix adhesion.
Specifically, the SEM morphology results for PSP/
thermoplastic composites have been shown in Figure 6.
According to Chamaiporn Yamoum and Rathanawan
Magaraphan [47], the peanut shell (PNS) seen in
Figure 6(a) and (b), is a short fiber which has an
average diameter of 13.44 ± 6.81 µm and an average
length of 66.82 ± 13.24 µm (an average aspect ratio of
4.97). Additionally, PNS displays agglomeration and
irregularity on the surface. While in Figure 6(d) and Figure 7. Weight loss of PLA and the PNS biocomposites [15].
(e), the PNS is well dispersed in the PLA matrix, which
is probably the outcome of processing under high shear
rate. On the contrary, the aggregates and pulled-out of voids happening at the interphase between the PNS
PNS in the PLA matrix were detected in Figure 6(f), and the PLA matrix. The fractured surface of 40PNS
which implied that the adhesion between the PNS and (Figure 6(e)) displays more microvoids than that of
the PLA matrix was poor. Likewise, for 40 wt.% PNS 30PNS (Figure 6(d)). In addition, the PNS agglomera-
loading (Figure 6(e) and (f)), it displays some small tions were increased, yielding poor adhesion at
12 N. F. ZAABA AND H. ISMAIL

interphase (voids displayed at high PNS loading). The
result discovers that the mechanical properties is not
improved at high PNS loading. The biodegradability
(weight loss) of PLA/PNS biocomposites is demon-
strated in Figure 7. The PNS biocomposites have clearly
shown a higher weight loss than that of PLA. After
8 weeks of composting in soil at 60°C, the weight loss
become more intense as PNS loading increases. This
was due to the PNS that could absorb the moisture
during composting. Thus, enhanced the hydrolysis of
PLA chains. The sequence of biodegradation is revealed
as follows: 40PNS>30PNS>20PNS>10PNS>PLA. The
result signifies that the biodegradation of the biocom-
posites increased as the addition of PNS increases.
Analogous finding of biodegradation of other biocom-
posites has been stated [119].
Whereas for PSP/thermoset composites, Figure 8
demonstrates the SEM micrographs of surfaces of the

b c

d e

Figure 8. SEM surface of (a) NR; 10 phr (b) NR-PSP45–90 and (c) NR-APSP45–90; 40 phr (d) NR-PSP45–90 and (e) NR-APSP45–90 of
NR/PSP composites exposed to soil for six months.
NR: natural rubber; APSP: alkali-treated peanut shell powder [17].

rubber, natural rubber/peanut shell powder (NR/PSP)
and natural rubber/alkali-treated peanut shell powder
(NR/APSP) composites exposed to soil burial for six
months. The microbial attack which has occurred on
the sample surface may be supplemented by huge loss
of oligomers, resulted to a corroded surface. As can be
seen in NR matrix (Figure 8(a)), only microvoids have
been founded after the microbial attack. While in NR
composites (Figure 8(b)-(e)), the effect of biodegrada-
tion was more noticeable. Besides, in the Figure 8(b)-
(e), the degradation of PSP filler and the bacterial
action on the surface of the composites are clearly
visible. The finding was beyond verified by the rise in
surface erosion and roughness, together with the crea-
tion of microviods and cracks on the sample surface.
Perhaps another reason is the short oligomers formed
by oxidative degradation may be metabolized by the
microorganisms leading to occurrence of the micro-
voids and corroded surface. Besides that, the degrada-
tion was less detected in alkali-treated PSP (APSP)
composites compared to their untreated composites
(Figure 8(c) and (e)). Owing to the better interaction
between the alkali treated PSP and the matrix, leading
to a formation a smoother appearance of composites’
surface. This is due to the fact that alkali treatment acts
as a protective covering for the fillers, preventing its
degradation. At 40 phr PSP loading (Figure 8(d) and
(e)), the microvoids and surface roughness are more
visible compared to 10 phr loading (Figure 8(b) and
(c)). The results reveal that the extent of biodegradation
increased more as PSP loading increases [73].
Conclusions
Research on peanut shell powder reinforced polymer
composite is creating increased consideration, owing to
its outstanding properties and environmental delibera-
tions. A brief discussion of peanut shell powder rein-
forced composites is revealed along with a review
according to the previous study. The above-mentioned
issues are intended at conveying researchers to consider
the potential of peanut shell powder as another
approach to substitute conservative materials or syn-
thetic fillers as reinforcement in different types of poly-
mer composites. Processing methods for peanut shell
powder reinforced composite are well documented and
their main properties have been considered. Overall,
the use of peanut shell powder reinforced composite
can aid to produce professions in both urban and rural
areas; in addition to help out to lessen waste, as well as
providing to a better circumstance. Nevertheless, by
observing at the future anxieties, further decisive stu-
dies are essential on manufacturing processes and
POLYMER-PLASTICS TECHNOLOGY AND ENGINEERING 13
product commercialization, particularly for bulky scale
finish products.
Developments for the future
Peanut shell powder reinforced polymer composite
proves to have an optimistic prospect amongst other
natural filler reinforced composites for the numerous
explicit purposes that were emphasized in the prior dis-
cussion. The most fascinating innovation of peanut shell
powder reinforced polymer composite is employing its
accessibility and inclination to be processed with different
type of polymer matrices and countless manufacturing
procedures that have never been related with other nat-
ural fillers before. According to this brief review, the
application of peanut shell powder reinforced polymer
composite is potential as an alternative composite mate-
rial, particularly in packaging, household, automotive and
building application, owing to its lightweight and low-
cost properties.
Acknowledgments
The authors wish to thank Universiti Sains Malaysia (USM)
Postdoctoral Fellow Scheme for their assistant and financial
support.
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