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Preparation and Characterization of Durian
Husk Fiber Filled Polylactic Acid Biocomposites
Man Chee Lee1 , Seong Chun Koay1*, , Ming Yeng Chan2 , Ming Meng Pang1 , Pui May
Chou1 , and Kim Yeow Tsai3
1School of Engineering, Faculty of Built Environment, Engineering, Technology and Design,
Taylor’s University Lakeside Campus, 47500 Subang Jaya, Malaysia
2Centre for Engineering Programmes, HELP College of Arts and Technology, 55200 Kuala Lumpur,
Malaysia
3Faculty of Engineering, The University of Nottingham, 43500 Semenyih, Malaysia.
Abstract. Polylactic acid (PLA) is biodegradable thermoplastic that made
from renewable raw material, but its high cost limited the application.
Thus, addition of natural fiber can be effectively reduced the cost of PLA.
This research is utilised natural fiber extracted from durian husk to made
PLA biocomposites. This paper is focus on the effect of fiber content on
tensile and thermal properties of PLA/durian husk fiber (DHF)
biocomposites. The results found that the tensile strength and modulus of
this biocomposites increased with increase of fiber content, but the strength
still lower compared to neat PLA. Then, the elongation at break of
biocomposites was expected decreased at higher fiber content. The
PLA/DHF biocomposites with 60 phr fiber content exhibited tensile
strength of 11 MPa, but it is too brittle yet for any application. The addition
of DHF caused an early thermal degradation on PLA biocomposites. Then,
the thermal stability of PLA biocomposites was decreased with more fiber
content.
1 Introduction
In 2015, researchers found 8.3 billion metric tons of plastics waste were produced
globally and 6.3 billion tons of this plastic products are turning into waste. As well known,
not all the plastic can be recycle, thus only 9% of that waste total was recycled, 12% was
used for energy recover and left were sent to landfills. The amount of plastics waste for
land fill are expected to achieve 12 billion metric tons, if the current trends is keep going on
[1]. Plastic material made from petroleum resources are chemically stable which hardly to
biodegrade in environment. In present, part of the plastic product has replace by bioplastic
that able to biodegradable after disposal. Polylactic acid (PLA) is a type of bioplastic that
synthesized from natural material, such as corn starch, tapioca root and sugarcane [2-3].
Besides, PLA offers a biodegradable properties and also good mechanical strength, non-
toxic and sustainable since it made from renewable resources [4-5]. Nowadays, the
production of bioplastic over the world is about 750,000 tons per year. Unfortunately, this
* Corresponding author: SeongChun.Koay@taylors.edu.my
© The Authors, published by EDP Sciences. This is an open access article distributed under the terms of the Creative Commons
Attribution License 4.0 (http://creativecommons.org/licenses/by/4.0/).
MATEC Web of Conferences 152, 02007 (2018) https://doi.org/10.1051/matecconf/201815202007
Eureca 2017
amount still very small compare to conventional plastic that produced 200 million tons per
year. The main reason why PLA is seldom choose by industrial as their main choice of
material, because the price of PLA resin is more expensive than conventional plastic [5-6].
In order to promote the usage of PLA material, natural filler can be introduced to PLA
and make it into a biocomposites. The natural filler can be easily obtained from any
agricultural crop and waste, for instance, corn cob [7], cocoa pod [8], coconut shell [3] and
palm kernel shell [9]. The main benefit of natural filler very low cost, biodegradable, less
abrasive to machine, and inexhaustible resources [10-11]. Thus, by making the PLA in to
biocomposite, the addition of natural filler can be partially replace the PLA without
influences its biodegradability and highly reduced the cost of final product. Durio
zibethinus Murray, also called as durian, the famous fruit among the Southest Asia
countries especially in Malaysia, Thailand, Indonesia and Philippine [12]. The durian fruit
is made up of 40% of flesh and 60% of husk. Usually, the durian husk was discarded and
end up on landfills or burnt which poses an environmental issues. In Malaysia, about 3,800
metric tons of durian fruits are produced in year 2016. Assuming every 60% of total
amount produced durian fruits is husk, it estimated the durian husks waste produced in year
2016 was achieved 2,280 metric tons. The production of durian fruits are predicted to
achieve 22,000 metric tons at year 2020 [13]. This meaning the amount durian husks waste
will be increased. The durian husk consists 60.45% of cellulose, 15.45% of lignin and
13.09% of hemicellulose, and the content are similar to wood fiber [14]. For this reason,
this research is underway to utilize the fiber obtained from durian husk and combined with
PLA to produce biocomposites.
This present research is focus on the effect of fiber content on the tensile and thermal
properties of durian husk fiber filled polylactic acid biocomposites.
2 Methodology
2.1 Research Materials
PLA used in this experiment was supplied by TT Biotechnologies Sdn. Bhd. (Malaysia)
and durian husk was collected from durian fruit stall at SS2, Petaling Jaya (Selangor).
2.2 Preparation of Durian Husk Fiber
The durian husks obtained from durian fruit stall were washed with tap water and cut
into small pieces. Then, the durian husks were dried using circulated air oven at 70oC until
completely dried. The dried durian husks were ground into short fiber using mechanical
grinder. Next, the short durian husk fiber (DHF) was passed through a sieve with mesh size
of 600 micron to get the homogenous size of fibers. The DHF further dried using oven
before compounding process.
2.3 Preparation of PLA/DHF Biocomposites
The PLA/DHF biocomposites were compounded using Haake Rheomix 600p at SIRIM
Malaysia (Shah Alam). The biocomposites were prepared with fiber various from 15, 30,
45, and 60 phr (part per hundred resin). The processing temperature was fixed at 180 oC and
rotor speed of 80 rpm. The compounding procedures included: i) addition of PLA resin in
2
MATEC Web of Conferences 152, 02007 (2018) https://doi.org/10.1051/matecconf/201815202007
Eureca 2017
amount still very small compare to conventional plastic that produced 200 million tons per
year. The main reason why PLA is seldom choose by industrial as their main choice of
material, because the price of PLA resin is more expensive than conventional plastic [5-6].
In order to promote the usage of PLA material, natural filler can be introduced to PLA
and make it into a biocomposites. The natural filler can be easily obtained from any
agricultural crop and waste, for instance, corn cob [7], cocoa pod [8], coconut shell [3] and
palm kernel shell [9]. The main benefit of natural filler very low cost, biodegradable, less
abrasive to machine, and inexhaustible resources [10-11]. Thus, by making the PLA in to
biocomposite, the addition of natural filler can be partially replace the PLA without
influences its biodegradability and highly reduced the cost of final product. Durio
zibethinus Murray, also called as durian, the famous fruit among the Southest Asia
countries especially in Malaysia, Thailand, Indonesia and Philippine [12]. The durian fruit
is made up of 40% of flesh and 60% of husk. Usually, the durian husk was discarded and
end up on landfills or burnt which poses an environmental issues. In Malaysia, about 3,800
metric tons of durian fruits are produced in year 2016. Assuming every 60% of total
amount produced durian fruits is husk, it estimated the durian husks waste produced in year
2016 was achieved 2,280 metric tons. The production of durian fruits are predicted to
achieve 22,000 metric tons at year 2020 [13]. This meaning the amount durian husks waste
will be increased. The durian husk consists 60.45% of cellulose, 15.45% of lignin and
13.09% of hemicellulose, and the content are similar to wood fiber [14]. For this reason,
this research is underway to utilize the fiber obtained from durian husk and combined with
PLA to produce biocomposites.
This present research is focus on the effect of fiber content on the tensile and thermal
properties of durian husk fiber filled polylactic acid biocomposites.
2 Methodology
2.1 Research Materials
PLA used in this experiment was supplied by TT Biotechnologies Sdn. Bhd. (Malaysia)
and durian husk was collected from durian fruit stall at SS2, Petaling Jaya (Selangor).
2.2 Preparation of Durian Husk Fiber
The durian husks obtained from durian fruit stall were washed with tap water and cut
into small pieces. Then, the durian husks were dried using circulated air oven at 70oC until
completely dried. The dried durian husks were ground into short fiber using mechanical
grinder. Next, the short durian husk fiber (DHF) was passed through a sieve with mesh size
of 600 micron to get the homogenous size of fibers. The DHF further dried using oven
before compounding process.
2.3 Preparation of PLA/DHF Biocomposites
The PLA/DHF biocomposites were compounded using Haake Rheomix 600p at SIRIM
Malaysia (Shah Alam). The biocomposites were prepared with fiber various from 15, 30,
45, and 60 phr (part per hundred resin). The processing temperature was fixed at 180 oC and
rotor speed of 80 rpm. The compounding procedures included: i) addition of PLA resin in
to mixing chamfer for 1 minute to fully melt the PLA resin; ii) Then, the DHF was added
into melted PLA and compounded for 5 minutes; iii) Last, the compound was removed
from mixing chamber.
The PLA/DHF biocomposites were further molded into thin sheet with thickness of 1
mm. The hotpress machine (model Moore) was used in this molding process and
temperature was set at 180oC. The molding procedures included: i) preheated to soften the
compound for 2 min; ii) fully compressed the softened compound under 100 MPa pressure
for 1 min; and iii) Last, cooled specimen under same pressure for 20 minutes. All the
biocomposite sheets were cut into tensile specimen and dimension following ASTM D638.
2.4 Testing and Characterization
Tensile test was performance using Instron Universal Testing Machine (Model 5569).
The tensile test was referring to ASTM D638. The cross-head speed of machine was set at 5
mm/min and a 15kN load cell was used. The tensile strength, modulus and elongation at
break of the samples were recorded by Bluehill 3 software. A minimum of 7 specimens
were tested for every formulated biocomposites.
Thermogravimetric analysis (TGA) was carried out using Pyris Diamond TGA (Perkin -
Elmer). The specimen was prepared in small size with weight from 6 to 8 mg and placed in
a ceramic pan. The specimen was heated from 30oC to 600oC at hearing rate of 10oC/min.
The TGA analysis was run under nitrogen atmosphere with gas flow rate of 20 ml/mm.
3 Results and Discussion
3.1 Tensile Properties
Figure 1 shows the tensile strength of PLA/DHF biocomposites with different DHF
content. The tensile strength of PLA/DHF biocomposite exhibits an increasing trend as the
DHF content increased. Usually, natural fiber displays a higher mechanical strength
compared to most plastic material [15]. Thus, the addition of DHF fiber might share part of
the tensile load which subjected PLA matrix and increased the tensile strength of
biocomposite. From the previous study found that the tensile strength of neat PLA was
about 54 MPa [3]. The biocomposites exhibited lower strength compared to neat PLA. This
is because the DHF used in this experiment was short fiber and the reinforcing ability of the
fiber is highly depending on the fiber orientation. The short fibers usually is randomly
orientated. The presence of fibers that orientated perpendicular to direct of applied load
might unable to share the load which caused the strength of biocomposite to decrease.
However, at higher fiber content, the presence of more fibers that parallel to direction of
load and it will share load that subjected to biocomposite. Thus, the strength of
biocomposite was raised when more fiber content was added. Similar findings have also
been reported by Yu et al. [16].
The effect of different fiber content on PLA/DHF biocomposites is illustrated in Figure
2. As expected, the tensile modulus of the biocomposites gradually increases with
increasing amount of DHF. It is because the modulus of DHF is usually higher than plastic
[12]. Therefore, the presence of higher amount of DHF contributed to higher modulus of
the PLA/DHF biocomposite. For this reason, the tensile modulus of PLA/DHF
biocomposite increases due to addition of DHF. Moreover, Gunti et al. [17] also agreed that
3
MATEC Web of Conferences 152, 02007 (2018) https://doi.org/10.1051/matecconf/201815202007
Eureca 2017
the modulus of biocomposite is highly depending on the amount of filler. Hence, the
biocomposite with higher fiber content showed higher tensile modulus.
Fig. 1. Tensile strength of PLA/DHF biocomposites with different fiber content.
Fig. 2. Tensile modulus of PLA/DHF biocomposites with different fiber content.
Figure 3 displays the elongation at break of the PLA/DHF biocomposite with different
DHF content. The result trend of tensile modulus of biocomposite typically opposite with
elongation at break. The neat PLA is well known brittle material and its elongation at break
was only 4.2% [3]. The addition of DHF had dramatically reduced the elongation at break
of PLA. The result found the fiber content increased, the elongation at break of PLA/DHF
biocomposite decreased. In general, natural fiber is rigid material that not elongate much
[18]. Thus, the addition of DHF would not contribute on the elongation of PLA matrix. In
addition, the friction presents between PLA matrix and DHF fiber will significantly reduce
the mobility of the polymer chains. For this reason, PLA/DHF biocomposite with more
fiber content became more rigid and brittle. This observation is in agreement with findings
of many others researcher [19].
4
MATEC Web of Conferences 152, 02007 (2018) https://doi.org/10.1051/matecconf/201815202007
Eureca 2017
the modulus of biocomposite is highly depending on the amount of filler. Hence, the
biocomposite with higher fiber content showed higher tensile modulus.
Fig. 1. Tensile strength of PLA/DHF biocomposites with different fiber content.
Fig. 2. Tensile modulus of PLA/DHF biocomposites with different fiber content.
Figure 3 displays the elongation at break of the PLA/DHF biocomposite with different
DHF content. The result trend of tensile modulus of biocomposite typically opposite with
elongation at break. The neat PLA is well known brittle material and its elongation at break
was only 4.2% [3]. The addition of DHF had dramatically reduced the elongation at break
of PLA. The result found the fiber content increased, the elongation at break of PLA/DHF
biocomposite decreased. In general, natural fiber is rigid material that not elongate much
[18]. Thus, the addition of DHF would not contribute on the elongation of PLA matrix. In
addition, the friction presents between PLA matrix and DHF fiber will significantly reduce
the mobility of the polymer chains. For this reason, PLA/DHF biocomposite with more
fiber content became more rigid and brittle. This observation is in agreement with findings
of many others researcher [19].
Fig. 3. Elongation at break of PLA/DHF biocomposites with different fiber content.
3.2 Thermal Properties
The TGA curves of DHF, neat PLA, and PLA/DHF biocomposites at selected fiber
content is shown in Figure 4. All the data obtained from TGA curves are tabulated in Table
1. The TGA result shows the DHF was thermal degraded earlier than neat PLA and yielded
high char residue at 600oC. The earlier thermal degradation of DHF was due to the
removing of moisture and volatile compounds that found in DHF. Then, the thermal
degradation of DHF was following by degradation of hemicellulose at temperature above
250oC. Furthermore, the thermal degradation of lignin and cellulose from DHF were found
beyond 350oC [20]. The thermal degradation of lignin and cellulose were contributed to
char formation that caused high amount of char residue. From Table 1, the temperature at
5% (Td5%) and 50 % (Td50%) weight loss of PLA/DHF biocomposites were shifted to lower
temperature when fiber content increased from 30 to 60 phr. The PLA/DHF biocomposites
also exhibited lower Td5% and Td50% compared to neat PLA. This indicated the PLA/DHF
biocomposites have lower thermal stability compared to neat PLA. The biocomposite had
lower thermal stability was due to components in DHF that decomposed when subjected to
high temperature. The char residue of PLA/DHF biocomposites also increased with the
increases of fiber content. As mentioned early, the formation of more char residue was due
to thermal degradation of lignin and cellulose from DHF. The similar observation also
found by other researchers [21-22].
4 Conclusion
The increase of fiber content increased the tensile strength and modulus of PLA/DHF
biocomposites, but decrease in elongation at break. The PLA/DHF biocomposites exhibited
lower strength compared to neat PLA, but the average tensile strength of PLA/DHF
biocomposites with 60 phr of fiber still have 11 MPa. The strength is comparable to low
density polyethylene, but its to brittle to make any application. Besides, the addition of
DHF had caused an early thermal degradation on PLA/DHF biocomposites and also lower
in thermal stability. The TGA results also found the biocomposite with more fiber content
exhibited high char residue after decomposed at temperature 600oC.
5
MATEC Web of Conferences 152, 02007 (2018) https://doi.org/10.1051/matecconf/201815202007
Eureca 2017
Fig. 4. TGA curves of DHF, neat PLA and PLA/DHF biocomposites at selected fiber content.
Table 1. Formatting sections, subsections and subsubsections.
Samples
Temperature at
5% weight loss
(
o
C)
Temperature at
50% weight loss
(
o
C)
Char residue
at 600oC (%)
Neat PLA
313.4
365.1
0.7
DHF
55.5
339.3
22.7
PLA/DHF:
100/30 260.9 331.5 0.8
PLA/DHF:
100/60 232.6 307.7 0.9
5 Acknowledgement
The authors gratefully acknowledge use of services and facilities at Taylor’s University,
funded by Taylor’s Research Grant Scheme (Project code: TRGS/ERFS/1/2017/SOE/033).
References
1. R. Geyer, J.R. Jambeck, K.L. Law, Sci. Adv. 3, 1 (2017).
2. A.A. Yussuf, I. Massoumi, A. Hassan, J. Polym. Envir. 18, 442 (2010)
3. K.S. Chun, S. Husseinsyah, H. Osman, Polym. Eng. Sci. 53, 1109 (2013)
4. K. S. Chun, S. Husseinsyah, J. Thermoplast. Compos. Mater. 27, 1667 (2014)
5. R.E. Drumright, P.R. Gruber, D.E. Henton, Adv. Mater. 12, 1841 (2000)
6. P.A. Fowler, J.M. Hughes, R.M. Elias, J. Sci. Food Agricul. 86, 1781 (2006)
6
MATEC Web of Conferences 152, 02007 (2018) https://doi.org/10.1051/matecconf/201815202007
Eureca 2017
Fig. 4. TGA curves of DHF, neat PLA and PLA/DHF biocomposites at selected fiber content.
Table 1. Formatting sections, subsections and subsubsections.
Samples
Temperature at
5% weight loss
(oC)
Temperature at
50% weight loss
(oC)
Char residue
at 600oC (%)
Neat PLA
313.4
365.1
0.7
DHF
55.5
339.3
22.7
PLA/DHF:
100/30
260.9
331.5
0.8
PLA/DHF:
100/60
232.6
307.7
0.9
5 Acknowledgement
The authors gratefully acknowledge use of services and facilities at Taylor’s University,
funded by Taylor’s Research Grant Scheme (Project code: TRGS/ERFS/1/2017/SOE/033).
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MATEC Web of Conferences 152, 02007 (2018) https://doi.org/10.1051/matecconf/201815202007
Eureca 2017