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Energy Procedia 34 (2013) 664 – 672

10th Eco-Energy and Materials Science and Engineering

(EMSES2012)
Mechanical property of surface modified natural fiber
reinforced PLA biocomposites
Wassamon Sujaritjuna, Putinun Uawongsuwanb*, Weraporn Pivsa-Arta,
Hiroyuki Hamadab
a
Department of Chemical Engineering, Rajamangala University of Technology Thanyaburi, Pathumthani, 12110, Thailand
b
Department of Advanced Fibro-Science, Kyoto Institute of Technology, Matsugasaki, Sakyo-ku, Kyoto, 606-8585, Japan

Abstract

Natural fibers have recently become attractive to researchers, engineers and scientists as an alternative reinforcement
for fiber reinforced polymer composites. This paper is focused on the tensile properties of natural fiber reinforced
polylactic acid composites. The untreated and flexible epoxy treated bamboo fiber, vetiver grass fiber and coconut
fiber were used as reinforcement for PLA biocomposites. The stiffness of untreated biocomposites increased
significantly with increasing of fiber content. However, the tensile strength decreased with increasing of fiber
content. The flexible epoxy surface treatment reduced the stiffness of all composites while it considerably increased
tensile strength when compared against the untreated composites. In addition, it can be seen that the effects of
flexible epoxy treated on the tensile strength improvement were dependent upon the type of natural fiber. The tensile
strength of bamboo fiber and coconut fiber reinforced PLA composites were significantly improved by the flexible
epoxy surface treatment. Unlike the other combinations, vetiver grass fiber reinforced PLA composite showed less
improvement in tensile strength when comparing with other natural fibers. Bamboo fiber proved to be the most
effective reinforcement compared to other reinforcements.

©©2013
2013The Authors.
The Published
Authors. by Elsevier
Published B.V. Open
by Elsevier B.V.
access under CC BY-NC-ND license.
Selection
Selectionandand/or
peer-review under responsibility
peer-review of COE of Sustainalble
under responsibility of COE ofEnergy System,Energy
Sustainable Rajamangala University
System, of Technology
Rajamangala
Thanyaburi (RMUTT)
University of Technology Thanyaburi(RMUTT)
Keywords: Polylactic acid; Bamboo fiber; Coconut fiber; Vetiver grass fiber; Flexible epoxy; Biocomposite

1. Introduction

As a result of the increasing environmental awareness, the concern for environmental sustainability and
the growing global wasted problem is increased year by year. The production of fuel-derived plastics is
often harmful to the environment. As far as synthetic polymer composites are concerned, waste disposal

* Corresponding author. Tel.: +81-75-724-7844; fax: +81-75-724-7844.

E-mail address: putinunu@kmutnb.ac.th.

1876-6102 © 2013 The Authors. Published by Elsevier B.V. Open access under CC BY-NC-ND license.
Selection and peer-review under responsibility of COE of Sustainalble Energy System, Rajamangala University of Technology
Thanyaburi (RMUTT)
doi:10.1016/j.egypro.2013.06.798
 Wassamon Sujaritjun et al. / Energy Procedia 34 (2013) 664 – 672 665

and recycling are major issues worldwide. In addition, concern about the preservation of natural resources
and recycling has led to renewed interest in biomaterials with the focus on renewable raw materials. Eco-
friendly biocomposites from plant-derived fiber and crop-derived polymer are novel materials and would
be of great importance to the composite materials world [1-2].
Polylactic acid (PLA) is a rigid thermoplastic that has a special interest as a matrix in composite
materials. PLA is a highly versatile biopolymer and is highlighted because it is derived from a renewable
resource such as corn. PLA can be processed by injection molding, blow molding, and film forming [3].
Although the mechanical properties of PLA suited for some industrial applications, it is considered too
brittle for many commercial applications. It is possible to overcome the brittleness by combining it with
other materials. Natural fiber as a replacement to synthetic fiber in polymer matrix offers a good
mechanical performance and eco-friendliness. The application of natural fiber based composites is
increasing rapidly. The combination of interesting mechanical and physical properties together with their
environmentally friendly character has aroused interest in a number of industrial applications [4-6].
The quality of the fiber-matrix interface is significant for the application of natural fibers as
reinforcement for polymer matrices. In order to improve the compatibility between hydrophobic
thermoplastics and hydrophilic cellulosic fibers, many chemical and physical surface treatments have
been applied to achieve high performance natural fiber reinforce composites. A variety of silanes have
been applied as coupling agents in the natural fiber composites to promote interfacial adhesion and
improve the mechanical properties of composite [7-9]. However, natural fibers require low processing
temperatures due to possibility of their thermal degradation. Research study on application of
thermosetting resin as the surface treatment of natural fiber to enhance the thermal stability during high
temperature process has been reported [10]. Therefore, the effect of fiber content and processing
parameters on the properties of natural fiber reinforced composites are particularly significance. The
suitable fiber content and processing parameters must be carefully selected in order to get the optimum
property of composite. Many research works have been studied the utilization of natural renewable
resources as the reinforcement in polymer composites [11-14]. In this study, bamboo fiber, vetiver grass
fiber and coconut fiber were selected as the reinforcement for PLA composites. The effects of flexible
epoxy surface treatment on tensile property of different natural fiber reinforced PLA biocomposites were
investigated.

2. Experimental

2.1. Materials

Polylactic acid (PLA: TE-2000C) with a density of 1.25 g/cm3 was obtained from Unitika plastics
division. The natural fiber consisting of bamboo fiber (BF), vetiver grass fiber (VF) and coconut fiber
(CCF) (all materials obtained from Thailand without any pre-sizing treatment) were selected as the
reinforcement for PLA. The composition and characteristic of selected natural fibers were listed in Table
1. Flexible epoxy resin (Epoxidized polybutadiene, EPOLEAD PB 3600, Daicel chemical Co. Ltd., Japan)
was used as surface treatment for the natural fibers.

2.2. Specimen preparation

The flexible epoxy resin (1 wt.% of reinforcement) was dissolved in acetone (1 g resin : 200 ml
acetone) for reducing the viscosity prior the surface treatment process. The treated natural fibers were first
dried at room temperature for 24 hours. Then the treated natural fibers were second dried in vacuum oven
at 80oC for 24 hours. The content of natural fibers were varied from 10, 20, 30 and 40 % by weight,
666 Wassamon Sujaritjun et al. / Energy Procedia 34 (2013) 664 – 672

respectively. The untreated and treated natural fibers were compounded with PLA matrix by twin screw
extruder (JSW TEX30HSS) at 200oC. The dumbbell-shaped testing specimens of untreated and treated
natural fibers were fabricated by injection molding (TOYO TI-30F6) at an injection temperature 200oC.

2.3. Testing

Tensile test (ASTM D638) was conducted on an universal testing machine (Instron 4206) with a
testing speed 1 mm/min. The strain was measured by using strain gauge extensometer. At least five
specimens were repeated.

2.4. Scanning electron microscopy (SEM)

Scanning electron microscope (JEOL JSM 5200) was conducted on the fracture surface of the tested
specimens to examine the failure surface and failure behavior. Samples were mounted on aluminium
holders and gold sputtered for 6 minutes prior observation.

Table 1. Physical, mechanical properties and composition of selected natural fibers [3-5]

Natural fiber Density Modulus Strength Microfibril Cellulose Lignin (%) Average
(g/cm3) (GPa) (MPa) angle (deg) (%) fiber aspect
ratio
Bamboo fiber (BF) 0.80 35.9 441 2-10 60.8 32.2 9.5
Vetiver grass fiber 1.50 12.0-49.8 247-723 N/A 72.6 17.0 3.8
(VF)
Coconut fiber (CCF) 1.10 4.0-6.0 131-175 30-49 43.0 45.0 26.0

Results and discussion

The tensile modulus of biocomposites at different natural fiber content was shown in Fig. 1(a). The
stiffness of composites significantly increased with increasing of fiber content as the results of addition of
high stiffness materials. It can be seen that tensile modulus of untreated bamboo fiber composite was
higher than vetiver grass fiber and coconut fiber composites. This effect was due to the better mechanical
properties of bamboo fiber which related to the composition of natural fiber as shown in Table 1.

12.00 60.00

10.00 50.00
Tensile modulus (GPa)

Tensile strength (MPa)

8.00 40.00
PLA PLA
6.00 Bamboo fiber 30.00 Bamboo fiber
Vetiver fiber Vetiver fiber
4.00 20.00
Coconut fiber Coconut fiber
2.00 10.00

0.00 0.00
0 10 20 30 40 50 0 10 20 30 40 50
Reinforcement content (wt.%) Reinforcement content (wt.%)
(a) (b)

Fig. 1. (a) Tensile modulus; (b) Tensile strength of different natural fiber reinforced PLA composites
 Wassamon Sujaritjun et al. / Energy Procedia 34 (2013) 664 – 672 667

Fig. 2. SEM micrograph of the fracture surface of untreated composites (a) bamboo fiber/PLA;(b) coconut fiber/PLA;(c) vetiver
grass fiber/PLA

The tensile strength of natural fiber reinforced PLA composites did not show the improvement when
compared with neat PLA. Tensile strength of coconut fiber and vetiver grass fiber reinforced PLA
composite decreased with the increasing of natural fiber content as shown in Fig. 1(b). On the other hand,
tensile strength of bamboo fiber reinforced PLA composite almost remained constant and only slightly
decreased when bamboo fiber content reached 40 wt.%. This was due to that bamboo fiber has higher
fiber strength than other natural fibers. Moreover, the bonding between different natural fiber and PLA
matrix were different. As observed from SEM micrograph of fracture surfaces as shown in Fig. 2. The
fiber-matrix interface in bamboo fiber/PLA composite from the Fig. 2(a) which showed better adhesion
bonding than other reinforcement resulted in better tensile strength. The reduction of strength at high
bamboo fiber content may possible due to the increasing of the probability of fiber agglomeration.
Fig. 3 showed how the influence of the flexible epoxy surface treatment affected the stiffness of
biocomposites. It was found that the flexible epoxy surface treatment reduced the tensile modulus of
bamboo fiber/PLA and vetiver grass fiber/PLA composites. The reduction of tensile modulus may due to
the coating of natural fiber surfaces with the flexible material, which reduced the stiffness of the natural
fibers. However the tensile modulus of untreated and treated coconut fiber/PLA composite behaved
differently.
668 Wassamon Sujaritjun et al. / Energy Procedia 34 (2013) 664 – 672

12.00 12.00

10.00 10.00

Tensile modulus (GPa)

Tensile modulus (GPa)

8.00 8.00

6.00 6.00

4.00 4.00
PLA PLA
2.00 Untreated bamboo fiber 2.00 Untreated coconut fiber
Treated bamboo fiber Treated coconut fiber
0.00 0.00
0 10 20 30 40 50 0 10 20 30 40 50
Reinforcement content (wt.%) Reinforcement content (wt.%)
(a) (b)
12.00

10.00
Tensile modulus (GPa)

8.00

6.00

4.00
PLA
2.00 Untreated vetiver fiber
Treated vetiver fiber
0.00
0 10 20 30 40 50
Reinforcement content (wt.%)

(c)

Fig. 3. Tensile modulus of untreated and treated natural fiber reinforced PLA composites (a) bamboo fiber;(b) coconut fiber;(c)
vetiver grass fiber

The effects of flexible epoxy surface treatment on tensile strength of biocomposites were shown in Fig.
4. The tensile strength of treated bamboo fiber and coconut fiber reinforced PLA composites were higher
than the untreated composites. The improvement in tensile strength was believed to be due to the better
interfacial adhesion with the flexible epoxy treatment. However, it can be seen that the effects of flexible
epoxy on tensile strength of vetiver grass fiber/PLA combination was different when compared with other
natural fibers. The flexible epoxy treated vetiver grass fiber reinforced PLA composite showed less
improvement in tensile strength compared with bamboo fiber and coconut fiber.

70.00 70.00

60.00 60.00
Tensile strength (MPa)
Tensile strength (MPa)

50.00 50.00

40.00 40.00

30.00 30.00

20.00 20.00 PLA

PLA
Untreated bamboo fiber Untreated coconut fiber
10.00 10.00
Treated bamboo fiber Treated coconut fiber
0.00 0.00
0 10 20 30 40 50 0 10 20 30 40 50
Reinforcement content (wt.%) Reinforcement content (wt.%)
(a) (b)
 Wassamon Sujaritjun et al. / Energy Procedia 34 (2013) 664 – 672 669

70.00

60.00

Tensile strength (MPa)

50.00

40.00

30.00

20.00 PLA
Untreated vetiver fiber
10.00
Treated vetiver fiber
0.00
0 10 20 30 40 50
Reinforcement content (wt.%)

(c)

Fig. 4. Tensile strength of untreated and treated natural fiber reinforced PLA composites (a) bamboo fiber;(b) coconut fiber;(c)
vetiver grass fiber

The interfacial bonding between fiber and matrix played an important role for the mechanical property
of fiber reinforced composite. The SEM micrographs of fracture surface compared between untreated and
flexible epoxy treated composites of three different natural fibers are shown in Fig. 5. The layer of
flexible epoxy resin formed on the surfaces between natural fiber and matrix after treatment as the
flexible interphase is illustrated in Fig. 6. The interfacial structure to be formed on fiber surface was not

matrix were formed and can

interrupted the debonding and cracks propagation between fiber/matrix interfaces, which was reported by
Yoshikawa et al. [15]. However, in this study the gradient interface between PLA matrix and flexible
epoxy interphase was not clearly observed.
The interfacial adhesion between fiber/interphase and interphase/matrix were the important factors for
the effectiveness of flexible interphase on mechanical property improvement. It can be seen that at the
surface of treated bamboo ffiber and coconut fiber in Fig. 5a -5b, small amount of flexible epoxy resin can
be observed on the surfaces of the fibers. Good adhesion between reinforcing fiber and flexible epoxy
interphase resulted in tensile strength improvement of bamboo fiber and coconut fiber reinforced PLA
composites. However, in case of treated vetiver grass fiber in Fig. 5c, no flexible epoxy resin appeared on
the fiber surfaces. It can be assumed that the interfacial bonding between flexible resin and PLA was
constant with different natural fibers. These two different interfacial adhesions resulted in the different
fracture mechanism when comparing treated vetiver grass fiber reinforced PLA composite with other
reinforcements. It is possible to note that the interfacial adhesion between vetiver grass fiber and flexible
interphase was weaker than the interfacial bonding between flexible interphase and PLA matrix. The
weak bonding of vetiver grass fiber and flexible epoxy resin resulted in slightly different tensile strength
improvement versus other natural fibers.
The tensile modulus and tensile strength improvement performance of untreated composites were
compared with flexible epoxy resin treated composites in Fig. 7. The comparison was obtained from the
differential ratio in percentage of the tensile properties at 40 % by weight natural fiber content and in
reference to the properties of PLA matrix. The tensile modulus of bamboo fiber and vetiver grass fiber
were strongly affected by flexible epoxy surface treatment. On the other hand, the modulus of coconut
fiber was unaltered by the coating of flexible epoxy interphase as shown in Fig. 7(a). Among all
reinforcement bamboo fiber was the most effective reinforcement to enhance the tensile strength of PLA
670 Wassamon Sujaritjun et al. / Energy Procedia 34 (2013) 664 – 672

as shown in Fig. 7(b). Moreover, by using the flexible epoxy resin as the surface treatment for bamboo
fiber the tensile strength of PLA can be improved significantly.

Fig. 5. SEM micrograph of the fracture surface of flexible epoxy treated composites (a) bamboo fiber/PLA;(b) coconut
fiber/PLA;(c) vetiver grass fiber/PLA

Fig. 6.

4. Conclusion

In this study, tensile properties of bamboo fiber, vetiver grass fiber and coconut fiber reinforced PLA
composites were prepared by extrusion and injection molding processes. The tensile modulus of untreated
 Wassamon Sujaritjun et al. / Energy Procedia 34 (2013) 664 – 672 671

natural fiber reinforced PLA composites were increased by the addition of natural fibers. Tensile strength
of untreated vetiver grass fiber and coconut fiber composites were lower than neat PLA and decreased
with increasing of fiber content. However, the tensile strength of untreated bamboo fiber/PLA composites
remained constant and decreased when fiber content reached 40 wt.%. The effects of flexible epoxy
surface treatment on tensile properties were dependent on the type of natural fiber. Tensile strength of
biocomposites decreased with the applied of flexible epoxy surface treatment. The flexible epoxy surface
treatment improved the tensile strength of bamboo fiber and coconut fiber reinforced PLA composites
when compared with untreated composites. However, it can be seen that the flexible epoxy surface
treatment was ineffective with the vetiver grass fiber combination. Bamboo fiber proved to be the most
effective reinforcement for the tensileproperties improvement of natural fiber reinforced PLA composite.

Vetiver grass fiber

Vetiver grass fiber 10.00
200.00
0.00
0
150.00
00 -10.00
.00
-20.00
20.00
100.00
00.00
-30.00
0
50.00
0 -40.00
0.0

0.0
0.00
00 -50.00
5 0

Coconut fiber Bamboo fiber Coconut fiber Bamboo fiber

B
untreated fiber untreated fiber
flexible epoxy treated flexible epoxy treated

(a) Tensile modulus (b) Tensile strength

Fig. 7. Performance improvement comparison between untreated and flexible epoxy treated composites (a) tensile modulus;(b)
tensile strength
672 Wassamon Sujaritjun et al. / Energy Procedia 34 (2013) 664 – 672

References

[1] Rowell RM, Young RA, Rowell J. Paper and Composites from Agro-based Resources. CRC Press; 1996.
[2] Mohanty AK, Misra M., Drzal LT. Sustainable Bio-Composites from Renewable Resources: Opportunities and Challenges
in the Green Materials World. J Polym Envi 2002;10:19-26.
[3] Ajmass W, Amass A, Tighe B. A Review of Biodegradable Polymers: Uses, Current Developments in the Synthesis and
Characterization of Biodegradable Polyesters, Blends of Biodegradable Polymers and Recent Advances in Biodegradation Studies.
Polym Inter 1998;47:89-144.
[4] Mohanty AK, Misra M, Drzal LT. Natural Fibers, Biopolymers, and Biocomposites. CRC Press; 2005.
[5] Pickering KL. Properties and performance of natural-fibre composites. Woodhead Publishing & CRC Press; 2008.
[6] Graupner N, Herrmann AS, Mussig J. Natural and man-made cellulose fibre-reinforced poly(lactic acid) (PLA) composites:
An overview about mechanical characteristics and application areas. Compos Part A 2009;40:810-21.
[7] Valadez-Gonzalez A, Cervantes-Uc JM, Olaya R, Herrera-Franco PJ. Effect of fier surface treatment on the fiber-matrix
bond strength of natural fiber reinforced composites. Compos Part B 1999;30:309-20.
[8] Keener TJ, Stuart RK, Brown TK. Maleated coupling agents for natural fibre composites. Compos Part A 2004;35:357-62.
[9] Xie Y, Hill CAS, Xiao Z, Militz H, Mai C. Silane coupling agents used for natural fiber/polymer composites: A review.
Compos Part A 2010;41:806-19.
[10] Thitithanasarn S, Yamada K, Ishiaku U, Hamada H. The Effect of Curative Concentration on Thermal and Mechanical
Properties of Flexible Epoxy Coated Jute Fabric Reinforced Polyamide 6 Composites. O J of Compo Mater2012;2:133-38.
[11] Chen X, Guo Q, Mi Y. Bamboo fiber-reinforced polypropylene composites: A study of the mechanical properties. J Appl
Polym Sci 1998;69:1891-9.
[12] Huda MS, Drzal LT, Misra M, Mohanty AK. Wood-fiber-reinforced poly(lactic acid) composites: Evaluation of the
physicaomechanical and morphological properties. J Appl Polym Sci 2006;69:4856-69.
[13] Ruksakulpiwat Y, Suppakarn N, Sutapun W, Thomthong W. Vetiver-polypropylene composites: Physical and mechanical
properties. Compos Part A 2007;38:590-601.
[14] Ku H, Wang H, Pattarachaiyakoop N, Trada M. A review on the tensile properties of natural fiber reinforced polymer
composites. Compos Part B 2011;42:856-73.
[15] Nakai A, Ohtani A, Ohki T, Osada T, Iwamoto M, Hamada H, Takeda N. Mechanical Properties of FlatBraided Composite
with Flexible Interphase. Proceeding of 18th International Conference on Composite Materials 2011.