GRAPHICAL ABSTRACT
In this research, cocoa pod husk (by-product from cocoa industrial) has been utilized as filler
in polypropylene (PP) matrix biocomposites. The CPH filler was modified with different
contents of methacrylic acid (MAA) and its effect on tensile properties of PP/CPH
biocomposites was investigated. The result showed that 3% of MAA gave the optimum
improvement on tensile strength and tensile modulus of PP/CPH biocomposites. However,
the MAA modification reduced the elongation at break of PP/CPH biocomposites. The
improvement of tensile properties is attributed by the presence of MAA enhancing the
filler-matrix interfacial bonding. The scanning electron microscope results indicated that
the modified CPH exhibited less filler pull-out and was well wetted by the PP matrix,
which indicated better interfacial bonding. Fourier transmission infrared (FTIR) confirm
that the MAA was covalently bonded to the CPH filler surface.
Keywords Biocomposites; Cocoa pod husk; Methacrylic acid; Polypropylene
Address correspondence to Salmah Husseinsyah, Division of Polymer Engineering, School of Materials Engineering, Universiti Malaysia
Perlis 02600, Jejawi, Perlis, Malaysia. E-mail: irsalmah@unimap.edu.my
Color versions of one or more of the figures in the article can be found online at www.tandfonline.com/lpte.
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INTRODUCTION
Cocoa (Theobroma Cacao) is one of the important
agricultural crops in Malaysia. Cocoa pod husk (CPH) is a
nonfood part of the cocoa pod, usually accounting for 52 to
76% of the cocoa pod wet weight[1,2]. In the cocoa industry,
the CPH is a by-product of the process of obtaining cocoa bean
from cocoa pod. Usually, the CPH is abundant but does not
have economic value. Therefore, the utilization of CPH as
natural filler in thermoplastic materials will provide a new
application route for CPH and a useful resource for
thermoplastic industry.
Nowadays, natural filler has become a popular choice of the
plastic industry. This is because natural fillers show some
excellent benefits compared to mineral fillers (such as lower
cost), are obtained from renewable resources, present
a minimal health hazard, have low density, are less abrasive
to processing machinery, and are eco-friendly[3-5]. In our previous research, an eco-packaging product and eco-tableware
were developed from coconut shell, corn cob and polylactic
acid[5,6]. The new development of CPH-filled polypropylene
biocomposites is applicable to wooden fittings, fixtures, deck
and furniture as well.
Generally, poor adhesion between the hydrophilic natural
filler and the hydrophobic thermoplastic is the main drawback
to producing biocomposites. However, filler modification
can be used to modify the hydrophilic natural filler, which
can improve filler dispersion, wettability, and filler-matrix
adhesion. In previous work, it was found that filler modification with acrylic acid[3,7], silane coupling agent[4,8], maleic
acid[5], modified fatty acid[6], sodium dodecyl sulphate[9,10],
and cross-linking agent[11] enhanced the properties of biocomposites. In our current work, methacrylic acid (MAA) was
used as a modifying agent for PP/CPH biocomposites. The
influence of various MAA contents on the tensile properties
of PP/CPH biocomposites was studied.
EXPERIMENTAL
Materials
Polypropylene (PP) type co-polymer, grade SM 340 was
supplied by Titan Petchem (M) Sdn. Bhd. Cocoa pod husk
(CPH) was obtained from cocoa plantation at Perak region.
The collected CPH was dried in an oven at 80C for 24 h.
Then, the dried CPH was crushed into small pieces and further
ground into fine powder. The CPH powder was sieved, and the
average particle size of the CPH powder was 22 m, measured
using a Malvern Particle Size Analyzer Instrument. The
ethanol and methacrylic acid (MAA) used for filler modification
were obtained from Sigma Aldrich, Penang.
Filler Modification
First, the MAA solution was prepared by dissolving MAA
into ethanol according to the formulation in Table 1. Then, the
CPH powder was added slowly to MAA solution and stirred
TABLE 1
Formulation of PP/CPH biocomposites
Materials
PP/CPH Biocomposites
PP (phr)
CPH (phr)
MAA (%)
100
20
0, 1, 3, 5*
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K. S. CHUN ET AL.
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Morphology
Figures 6a and 6b display the SEM micrographs of the
tensile fracture surface of PP/CPH biocomposites without
and with 3% MAA. The SEM micrographs show that the
unmodified CPH has poor filler dispersion in the PP matrix.
CONCLUSION
Modified CPH with MAA increased in tensile strength and
modulus, but decreased in elongation at break of PP/CPH biocomposites. The 3% of MAA was the optimum content for filler modification of CPH giving the greatest improvement of
tensile properties. The FTIR results showed that the MAA
was covalently bonded with CPH via ester bonding. The
SEM micrograph also demonstrated that the filler modification
with 3% MAA improved interfacial bonding between CPH
and the PP matrix.
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K. S. CHUN ET AL.
ACKNOWLEDGMENTS
The authors are thankful to Dr. Alias from Cocoa Research
& Development Center (Hilir Perak), Malaysian Cocoa Board
for supplying the cocoa pod husk for this research.
ORCID
Koay Seong Chun
http://orcid.org/0000-0003-2884-6027
REFERENCES
Chun, K.S.; Husseinsyah, S.; Osman, H. Tensile properties of polypropylene/
cocoa pod husk biocomposites: effect of maleated polypropylene. Adv.
Mater. Res. 2013, 747, 645648.
Chun, K.S.; Husseinsyah, S.; Osman, H. Modified cocoa pod husk-filled polypropylene composites by using methacrylic acid. BioResour. 2013, 8,
32603275.
Salmah, H.; Koay, S.C.; Hakimah, O. Surface modification of coconut shell
powder filled polylactic acid biocomposites. J. Thermoplast. Compos.
Mater. 2013, 26, 809819.
Chun, K.S.; Husseinsyah, S.; Osman, H.; (2012). Mechanical and thermal properties of coconut shell powder filled polylactic acid biocomposites: effect of the
filler content and silane coupling agent. J. Polym. Res. 2012, 19, 18.
Chun, K.S.; Husseinsyah, S.; Osman, H. Properties of coconut shell powderfilled polylactic acid ecocomposites: effect of maleic acid. Polym. Eng. Sci.
2013, 53, 11091116.