See

discussions, stats, and author profiles for this publication at: https://www.researchgate.net/publication/279530907

Effects of Compatibilizer on Thermal and

Mechanical Properties of PLA/NR Blends

Article in Materials Science Forum · May 2015

DOI: 10.4028/www.scientific.net/MSF.819.241

CITATION READS

1 129

4 authors:

Agus Bin Arsad Abdul Razak Rahmat

Universiti Teknologi Malaysia Universiti Teknologi Malaysia
42 PUBLICATIONS 46 CITATIONS 98 PUBLICATIONS 698 CITATIONS

SEE PROFILE SEE PROFILE

Nur Syazana Abdullah Sani Nor Nisa Balqis Mohammad

5 PUBLICATIONS 4 CITATIONS Universiti Teknologi Malaysia
7 PUBLICATIONS 12 CITATIONS
SEE PROFILE

SEE PROFILE

Some of the authors of this publication are also working on these related projects:

Synthesis and Characterization of Polyaniline/Sago Starch bio-hybrid composite using Ultrasonic

Irradiation. View project

Graphene Reinforced Polymer Nanocomposites for Automotive Application View project

All content following this page was uploaded by Agus Bin Arsad on 02 July 2015.

The user has requested enhancement of the downloaded file.

Materials Science Forum Vol 819 (2015) pp 241-245
© (2015) Trans Tech Publications, Switzerland
doi:10.4028/www.scientific.net/MSF.819.241

Effects of compatibilizer on thermal and mechanical properties of

PLA/NR blends
Nur Syazana Abdullah Sania, Agus Arsadb*, Abdul Razak Rahmatc,
Nor Nisa Balqis Mohammadd
Department of Polymer Engineering. Faculty of Chemical Engineering,

Universiti Teknologi Malaysia.

Skudai, Malaysia.
a
nursyazana29@gmail.com, bagus@cheme.utm.my, ck-razak@cheme.utm.my,
d
nisabalqis89@gmail.com

Keywords: polylactic acid, natural rubber, compatibilizer, melt blending, mechanical properties,
thermal properties

Abstract. The aim of the research is to study the effects of compatibilizer on thermal and
mechanical properties ofbiopolymer poly (lactic acid) (PLA) and natural rubber (NR) blends. PLA
was blended with NR in the composition of 95/5 weight percentage with present of compatibilizer.
The compatibilizers, PLA grafted maleic anhydride (MA) (PLA-g-MA) and NR grafted MA (NR-g-
MA) were synthesized in a composition of 9 phr of MA by using internal mixer in presence of
benzoyl peroxide (BPO). The formulations of PLA/NR blended with the compatibilizer were in the
range of 1, 3, 5 and 10 wt.% of PLA-g-MA and NR-g-MA, respectively. Blending process was
conducted using twin screw extruder then were pelletized and hot pressed before characterized. The
mechanical (tensile, flexural, impact) and thermal properties of the blends was investigated and
from the results, the addition of PLA-g-MA in PLA/NR blendimproved the impact strength and
elongation at break of the blends as compared with neat PLA and PLA/NR blend without
compatibilizer and for thermal stability, it only had a slight influence on the blends. Addition of
NR-g-MA on contrary did not give improvement on mechanical properties but increasing in thermal
stability.

Introduction
Polylactic acid (PLA) is known as a biodegradable thermoplastic polymer with widely
potential application that has attracted a lot of commercial attention because the polymer is made by
a fermentation process from 100% annually renewable resources. As a biodegradablepolymer, PLA
is becoming increasingly popular. PLA advantages and their limitation has been reviewed by Rasal
et al. (2010),which can be highlighted as eco-friendly, biocompatibility, processibility and energy
savings. On the other side, poor toughness, slow degradation rate, hydrophobicity and lack of
reaction side-chain groups were becomes PLA limitations.
Natural rubber (NR) has received a lot of attention from researchers because NR is
recyclable rubber and derivative from renewable resource. Due to its high molecular weight and
very low glass transition temperature about -70˚C, NR is an interesting candidate to use as a
toughening agent for PLA. The statement before was consolidated by Wongsorat et al. (2011)
reported that NR has excellent properties such as high specific strength, high resilience, high
elongation at break and low cost.
Due to low of compatibility between PLA and NR, the compatibilizer will be much needed
to make the blend has a good interfacial adhesion as well as improved their properties. Juntuek et
al. (2011) were able to further improve the compatibility between PLA and NR by using glycidyl
methacrylate-grafted natural rubber (NR-g-GMA) as compatibilizer. The impact strength and

All rights reserved. No part of contents of this paper may be reproduced or transmitted in any form or by any means without the written permission of Trans
Tech Publications, www.ttp.net. (ID: 161.139.126.248-08/06/15,11:25:27)
242 International Conference on Functional Materials and Metallurgy (ICoFM
2014)

elongation at break of PLA/NR blend increased with increasing NR-g-GMA content without
significantly loss in tensile strength and modulus.
In case of PLA/NR blend, the difference in the polarity and molecular weight of PLA and
NR may result in the poor compatibility and may lead to poor impact strength. Thus the
compatibility between PLA and NR need to be improved. In this study, a third component called
compatibilizer would be prepared and it is expected to increase the interaction between immiscible
phases. There are two choices between MA grafted PLA or MA grafted NR. Thus, these two
compatibilizers need to be investigated.

Experimental
Materials. The matrix was polylactic acid (PLA 1323A), purchased from Shenzen Esun Industrial
Co. Ltd. andnatural rubber was denoted by Malaysian Rubber Board. MA used in the study is MA
for synthesis and was supplied from Merck KgaA, Germany.
Blending preparation. PLA were dried for 24 h in a dry hopper at 50ºC, while NR were masticated
for 20 minutes and chopped into small pieces. PLA/NR with compatibilizer were melt blended
using a counter-rotating twin screw extruder (Werner & Pfleiderer) with the mixing temperature
varied between 160 to 190°C. All the extruded samples were pelletized and hot pressed to produce
test specimens for further analysis. The compatibilizers content were varied between 1 to 5 wt%
meanwhile PLA/NR blends were fixed about 100 wt%.
Mechanical testing. The blending were evaluated by tensile and flexural using Instron testing
machine (model 5567) according to ASTM D638 and ASTM D790 respectively. Testing was
conductedat room temperature with a testing speed of 10 and 3 mm/min respectively on at least 5
specimens for each formulation. Impact strength was measured on V-notched specimens with Izod
test methods using Toyoseiki Izod impact tester according to ASTM D256.
Thermal analysis.Thermogravimetric analysis (TGA) was performed using Mettler Toledo
Thermogravimetry Analyzerv (TGA TSO800GC1), to study the thermal stability and degradation.

Results And Discussion

Tensile Properties. The effect of percentage compatibilizer on tensile strength, tensile modulus
and elongation at break of PLA/NR blending were showed in Figure 1(a), (b) and (c). Addition of
PLA-g-MA did not give significant effect on PLA/NR blend and it falls within the acceptable of
value range of PLA/NR without compatibilizer but increased for elongation at break. The increment
of elongation at break indicated that the presence PLA-g-MA has apparently transformed the blends
into more ductile material as it improve the interfacial adhesion of blends. Similar trend were
reported by Wang et al.(2010) and Nainar et al. (2012) which stated that the ability of grafted MA
as a good compatibilizer for PLA. Different with NR-g-MA addition, the tensile properties were
dropped gradually. This indicated that the compatibility between PLA and NR was not improved
when NR-g-MA was used as compatibilizer.
 Materials Science Forum Vol. 819 243

(a) (b)

(c)
Figure 1: Tensile properties of PLA/NR blends: (a) tensile strength, (b) tensile modulus, (c)
elongation at break

Flexural Properties.Figure 2 shows the effects of PLA-g-MA and NR-g-MA on the flexural
strength and modulus of PLA/NR composites. Interesting to note that, the flexural modulus of
PLA/NR composites increased up to 3% of PLA-g-MA compatibilizers with value 2.33% compared
to PLA/NR without compatibilizer which is 1.84%. According to Chow et al.(2012), the increment
may be attributed to the bulkiness and stiffness of the MA group in the PLA composites. The
presence of bulk anhydride moiety group can lead to the improvement in modulus as well as in
interfacial interaction between PLA and NR but it still has limit for the content of MA that can lead
decreasing in properties.However, the flexural strength of PLA/NR with NR-g-MA was lower than
PLA/NR without NR-g-MA. The reduction in these properties was due to the result of the rubbery
nature of NR (Juntueket al., 2011).
244 International Conference on Functional Materials and Metallurgy (ICoFM
2014)

(a) (b)
Figure 2: Flexural properties of PLA/NR blends: (a) flexural strength and (b) flexural modulus

Impact strength. Figure 3 shows the impact strength of PLA/NR and PLA/NR with different
percentage of compatibilizers. The impact strength of PLA/NR blends increased with increasing
PLA-g-MA content but decreased when the addition of NR-g-MA. With increasing PLA-g-MA
content to 5 and 10% (w/w), impact strength of PLA/NR blends was slightly decreased to 35.91 and
35.90 J/m, respectively. However, these values were still higher than PLA/NR without
compatibilizer which is 35.74 J/m. The improvement of impact strength for PLA/NR with PLA-g-
MA was due to the enhancement in compatibility between PLA and NR.For NR-g-MA, the
decreasing of impact strength was due to poor distribution of the blends where it is very much
related to each other.The impact strength of the polymer blends depends on several factors like
dispersed particle size, interfacial adhesion and interparticle distance (Wang et al., 2010). Other
than that, addition NR caused the agglomeration of NR in an one area hence reduced the interfacial
adhesion between matrix and dispersed phase.

Figure 3: Impact strength of PLA/NR blends at various percentage of compatibilizer

Thermogravimetric analysis (TGA). TGA results are summarized in Table 1 and Table 2 for
PLA-g-MA and NR-g-MA, respectively. The 5% decomposition temperature (T5) of PLA/NR
90/10 blends compatibilized by 0, 1, 3, 5 and 10% of PLA-g-MA and NR-g-MA, T5was
investigated and from that thermal degradation of PLA and NR showed single step of weight loss.
From Table 1, it can be seen that the compatibilizer had a slight influence on the thermal stability of
the blends. These results are in agreement with study by Chongprakobkit et al. (2007) on PP/PA6
compatibilized with grafted MA. Besides that, the degradation temperature increased with the
 Materials Science Forum Vol. 819 245

incorporation of NR-g-MA as shown in Table 2. The compatibilizer might be contributed to the

higher interaction and better dispersion of NR in PLA matrix (Juntuek et al., 2011). NR itself has
higher thermal stability that influenced the thermal properties of the blends.
Table 1: TGA results of PLA/NR/PLA-g-MA blends
Composition % of PLA-g-MA T5%weight loss Tmax weight Residue at
(wt%) (°C) loss (°C) 420°C
PLA/NR 0 306.7 345.7 12.52
PLA/NR/PLA-g-MA 1 311.0 345.7 15.76
PLA/NR/PLA-g-MA 3 311.0 345.7 13.72
PLA/NR/PLA-g-MA 5 311.0 345.7 13.28
PLA/NR/PLA-g-MA 10 311.0 345.7 15.68
Table 2: TGA results of PLA/NR/NR-g-MA blends
Composition % of NR-g-MA T5%weight loss Tmax weight Residue at
(wt%) (°C) loss (°C) 420°C
PLA/NR 0 306.67 345.67 12.52
PLA/NR/NR-g-MA 1 315.33 350.00 14.72
PLA/NR/NR-g-MA 3 319.67 350.00 11.22
PLA/NR/NR-g-MA 5 319.67 350.00 10.99
PLA/NR/NR-g-MA 10 328.83 354.33 16.21

Conclusions
PLA and NR blends with compatibilizers were examined in this paper. PLA-g-MA and NR-g-MA
were added as a compatibilizer to improve the properties of the blends. The results showed that
properties of PLA/NR with PLA-g-MA were improved thus improving the compatibility and
interfacial adhesion between the phases. The blends received an enhancement on impact strength
and elongation at break accompanied by maintaining the tensile and flexural strength. In contrary,
addition NR-g-MA shows in decreasing properties but increasing in thermal stability.

References
[1] P. Juntuek, C. Ruksakulpiwat, P. Chumsamrong, Y. Ruksakulpiwat. Mechanical Properties of
Polylactic Acid and Natural Rubber Blend using Calcium Carbonate and Vetier Grass Fiber as
Filler. (2012) 18TH International Conference on Composite Materials.
[2] R.M. Rasal, A. V. Janorkar and D. E. Hirt. Poly(Lactic Acid) Modifications. Progress in
Polymer Science. Vol. 35 (2010) 338-356.
[3] S. Chongprakobkit, M. Opaprakasit and S. Chuayjuljit. Use of PP-g-MA Prepared by Solution
Process as Compatibilizer in Propylene/Polyamide 6 Blends. Journal of Metals, Materias and
Minerals. Vols. 12 (2007) 9-16.
[4] S. M. Nainar, S. Begum, Z. Hasan, M. N. M. Ansari and H. Anuar. Influence of maleic
anhydride on mechanical properties and morphology of hydroxyapatite/poly-(lactic acid)
composites. Regenerative Research. Vols. 1(2) (2012) 32-38.
[5] W. S. Chow, W. L. Tham and P. C. Seow. Effects of maleated-PLA compatibilizer on the
properties of poly(lactic acid)/halloysite clay composites. Journal of Thermoplastic Composite
Materials. Vols. 26(10) (2012) 1349-1363.
[6] W. Wongsorat, N. Suppakarn and K. Jarukumjorn, Mechanical Properties, Morphological
Properties, and Cure Characteristics of Sisal Fiber/Natural Rubber Composites: Effects of Fiber
and Compatibilizer Content. Advanced Meterials Research.Vols. 123-125 (2010) pp 1171-
1174.
[7] Y. –L. Wang, X. Hu, H. Li. X. Ji and Z. –M. Li. Polyamide-6/Poly(lactic acid) Blends
Compatibilized by the Maleic Anhydride Grafted Polyethylene-Octene Elastomer. Polymer-
Plastics Technology and Engineering. Vols. 49 (2010) 1241-1246.