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The Influence of Adding Polycaprolactone and Polyethylene Grafted Maleic

Anhydride on the Mechanical, Morphological and Biodegradation Properties
of HDPE *Address for Correspondenc...

Article · October 2020

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Indian Journal of Natural Sciences www.tnsroindia.org.in ©IJONS

Vol.10 / Issue 58 / February / 2020 International Bimonthly ISSN: 0976 – 0997

RESEARCH ARTICLE

The Influence of Adding Polycaprolactone and Polyethylene Grafted

Maleic Anhydride on the Mechanical, Morphological and
Biodegradation Properties of HDPE

Tamam M. S. Aljabori1, Salah F. Abdellah Ali1,2 and M. E. El-Rafey1*

1Department of Materials Science, Institute of Graduate Studies and Research, Alexandria University,

Egypt.
2College of Science and Arts, Jouf University, Saudi Arabia.

Received: 19 Nov 2019 Revised: 22 Dec 2019 Accepted: 25 Jan 2020

*Address for Correspondence

M. E. El-Rafey,
Department of Materials Science,
Institute of Graduate Studies and Research,
Alexandria University, Egypt.
E.mail: igsrdean@gmail.com / tamam82.mo@gmail.com

This is an Open Access Journal / article distributed under the terms of the Creative Commons Attribution License
(CC BY-NC-ND 3.0) which permits unrestricted use, distribution, and reproduction in any medium, provided the
original work is properly cited. All rights reserved.

ABSTRACT
This study aims to prepare environment friendlypolymer blends in order to reduce the usage of the non-
biodegradable polymers and contribute to the environment preservation. High density polyethylene
(HDPE) and polycaprolactone (PCL) blends were prepared with different percentages, polyethylene
grafted maleic anhydride (PE-g-MA) was added to the blend as a compatibilizer. The samples were
prepared using the conventional injection molding technique. The mechanical properties were observed
to have remarkable changes with the blend composition as the tensile strength and the elongation
percentage at break increased significantly when compared to the neat HDPE. The morphology imaging
by SEM showed that the addition of PE-g-MA improved the comptability and accordingly aided in
obtaining a synergic blend with better properties. The soil burial test gave a significant biodegradation
results and proved the blend’s ability to biodegrade in soil which would encourage its usage as the main
polymer for manufacturing single use products while preserving the environment.

Keywords: High density polyethylene, polycaprolactone, polyethylene grafted maleic anhydride,

biodegradation, soil burial, mechanical properties.

INTRODUCTION
Nowadays, petroleum-based polymer products are still dominant because of their excellent mechanical, physical and
thermal properties.These polymers are versatile and provide millions of tons of plastic products produced by the end
of each year. These products are threatening the environmental preservation and our whole life. That’s why; the
society has been demanding the elimination of the non-biodegradable plastics usage. The polymer scientists have

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Vol.10 / Issue 58 / February / 2020 International Bimonthly ISSN: 0976 – 0997

Tamam M. S. Aljabori et al.

suggested as using biopolymers and biodegradable polymers as an alternative to the petroleum-based polymers.
Reducing the usage percentage of the petroleum-based polymers or the non-biodegradable polymers would aid the
environmental preservation and decrease the ecological issues that we are facing currently (1-3).Thus, the purpose of
this study is to prepare partially biodegradable blends that can biodegrade naturally over time and decrease the
impact of the petroleum based plastics on the environment.

MATERIALS AND METHODS

The used HDPE grade (HDPE6070) has a melt flow rate of 7.6 g/10min at (190°C, 2.16 Kg) and a density of 0.960
g/cm 3. It was supplied by SidiKerir Petrochemicals Company (SIDPEC), Egypt in the form of powder.
Polycaprolcatone with Mwt = 80,000 and melting temperature of 60°C was used, it was supplied by Sigma Aldrich,
UK.High density polyethylene grafted maleic anhydride grade (Fusabond® E100) with a melt flow rate of 2 g/10min
at (190°C, 2.16 Kg) and a density of 0.954 g/cm3 was purchased from E.I. DuPont De Nemours and Company Inc.

Samples preparation

The different combinations of the blends used in this study are shown in Table 1. Materials were mixed and
processed in a robot coupe Blixer 4 for 6 min with speed of 3000 rpm. The injection molding of the different samples
using was carried out using Arburg allrounder 221k, Germanysingle screw-injection molding machine.

Methods
Mechanical Properties
The tensile properties of HDPE / PCL and PE-g-MA blends were measured using the universal testing machine with
load cell 5 KN (Zwick /z005, Germany) as shown Figure 1. The dumbbell-shaped specimens, in accordance with
ASTM D638 - 08, of all specimens were tested at room temperature. The samples were conditioned prior to testing at
labconditions for 24 h. The tensile test was performed in uniaxial tension at a crosshead speed of 20 mm/min.

Scanning Electron Microscopy (SEM)

The test was used to reveal information on how a compatibilizer plays a role in improving composites properties.
The test was carried out using JEOL, JSM-5300.

Biodegradation test
The samples were cut into circles Radius(r) = 2 mm and a thickness of 4mm and dried in a vacuum oven at 40 ° C till
weight is constant then buried in soil mud which contains different types of Bacillus bacteria of the genus (Bacillus
Spp), Other bacteria belong to the genus (Corynebacterium Spp) fungi such as (Fusarium solani), (Fusarium oxysporum),
and (Rhizoctonia solani) with a pH of 7.41 as listed in the report performed at the faculty of Agriculture Alexandria
University, Egypt. The temperature has never been much higher than room temperature (25 ± 2) ° C with a minimum
airflow rate. Each sample was removed, washed with fresh water and dried again to constant weight. The degree of
degradation was evaluated (referred as the percentage of weight loss). Samples kept wet in the soil by frequent water
spraying. Weight loss percentage was calculated according to the following equation.

% Weight Loss=((Wi-Wf ))/Wi ..................... (1)

The Wi and Wfare weight before soil burial and weight after soil burial, respectively.

RESULTS AND DISCUSSION

Mechanical properties
The tensile test was conducted on all of the blended samples and neat HDPE, yield strength and elongation
percentage at break values were recorded (Table 2). The addition of PCL with different percentages of 1 wt%, 2 wt%,

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Vol.10 / Issue 58 / February / 2020 International Bimonthly ISSN: 0976 – 0997

Tamam M. S. Aljabori et al.

4 wt% and PE-g-MA to the HDPE matrix seemed effective in improving the mechanical properties generally as
shown in Figure 2. Regarding samples S11, S21 and S41, the tensile strength increased gradually from 26 MPa for
neat HDPE to 28 MPa for S41. The elongation percentage at break also increased gradually from 1085% for neat
HDPE to 1199% for S41. This improvement might be attributed to the comptability that was induced by the addition
of PE-g-MA as a compatibilizer which enhanced the miscibility and interfacial adhesion between PCL and HDPE.
The induced comptability can be resulted from thereaction between maleic anhydride with the hydroxyl (OH) end
groups of PCL that may be taken place providing aninterface with higher performance. The neat PCL has high
ductility which might also affect the elongation percentage at break positively and raised it higher than the neat
HDPE (4-9).

Scanning electron microscope (SEM)

Scanning electron microscope (SEM) was used to investigate the cross section area morphology and the possible
interfacial adhesion between the HDPE matrix, PCL and HDPE-g-MA as shown in Figure 3. The morphology of the
blends is controlled by the processing conditions, composition, as well as the nature of the polymers (interfacial
tension and viscosity ratio)[5, 10, 11].HDPE has homogenous, smooth, and uniform surface, unlike the blended
samples which showed less homogeneity. By increasing the PCL content, the homogeneity decreased which hinted
less comptability within the blend. The incorporation of PE-g-MA improved the homogeneity gradually, this might
mean that the PE-g-MA played its role as a compatibilizer and enhanced the comptability between HDPE and PCL. It
is very clear for samples S41, S42 and S44 that the gradual increase of the PE-g-MA percentage improved the
morphology and the interfacial adhesion between the matrix components which would generally affect the other
properties positively (1, 12, 13).

Soil burial test

The biodegradation of plastics proceeds actively under soil conditions according to their properties and the soil
microorganism’s optimal growth conditions[14, 15].It is noteworthy to mention that only biodegradation is measured
without any consideration of UV degradation which also has a major importance in case of HDPE degradation.The
weight loss percentage increased by raising the polycaprolactone content and with the factor of time. In four months,
the weight loss increased gradually from 0.05 wt% for sample S11 that contains 1 wt% PCL to 0.1 wt% for sample S41
which contains 4 wt% PCL as shown in Table 3. The incorporation of PE-g-MA resulted in improving the
performance of the biodegradation and increasing the ability of each PCL content to induce the biodegradability in
the samples. For example, the weight loss percentage increased from 0.1 wt% to 0.13 wt% for samples S41 and S44,
respectively, and that’s when the PE-g-MA percentage was raised from 1 wt% to 4 wt%.

The presence of PCL and PE-g-MA induced the biodegradability within HDPE. PCL is biodegradable polyester
affected by the action of microorganisms in the soil. The enhanced degradation of the blends compared to HDPE can
be explained by the initiation of microbial degradation of PCL chains. Therefore, as the PCL concentration is
increased, the biodegradation increased. Also, the PE-g-MA incorporation into the matrix improved the comptability
between HDPE and PCL and enhanced the PCL biodegradable influence on the blend which raised the weight loss
percentage. By increasing the PE-g-MA concentration, the moisture absorption and the swelling are increased too,
leading to a faster biodegradation as well. This is shown in other studies that have similar results (15-17).

CONCLUSION

The incorporation of small percentages PCL into the HDPE matrix had a positive influence on its properties. The
mechanical properties improved significantly after the addition of PE-g-MA as a compatibilizer which enhanced the
comptability within the blend and influenced the interfacial adhesion. The biodegradation in soil gave remarkable
results after four months with regard to the small PCL percentages used in this study. This study can represent a
beginning to replace the totally non-biodegradable plastics with partially biodegradable products.

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and aliphatic polyester blends. International Polymer Processing 2007; 22: 512-518.
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Materials Science Forum 2008, pp.520-524. Trans Tech Publ.
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dispersed phase morphology of poly (lactic acid)/polycaprolactone blends containing peroxide. Journal of applied
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with diols under mild conditions catalyzed by reusable rare-earth triflate. Macromolecules 2003; 36: 1772-1774.
9. 9.França DC, Morais DD, Bezerra EB, et al. Photodegradation Mechanisms on Poly (ε-caprolactone)(PCL).
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10. 10.Abderrahim B, Abderrahman E, Mohamed A, et al. Kinetic thermal degradation of cellulose, polybutylene
succinate and a green composite: comparative study. World Journal of Environmental Engineering 2015; 3: 95.
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88-91.
12. 12.Kemp RB. Handbook of thermal analysis and calorimetry: from macromolecules to man. Elsevier, 1999.
13. 13.Liu W, Wang YJ and Sun Z. Effects of polyethylene‐grafted maleic anhydride (PE‐g‐MA) on thermal
properties, morphology, and tensile properties of low‐density polyethylene (LDPE) and corn starch blends.
Journal of Applied Polymer Science 2003; 88: 2904-2911.
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properties of hemp/high-density polyethylene green composites. Journal of Thermal Analysis and Calorimetry 2015;
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Table 1. The design of the blended samples

SAMPLE HDPE PCL PE-g-MA
S0 100% 0% 0%
S11 98% 1% 1%
S12 97% 1% 2%
S14 95% 1% 4%
S21 97% 2% 1%
S22 96% 2% 2%
S24 94% 2% 4%
S41 95% 4% 1%
S42 94% 4% 2%
S44 92% 4% 4%
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Table 2.Tensile test results of neat HDPE and its blends

Sample Tensile strength at yield Elongation at break (%)

(MPa)
S0 26 1085
S11 27 1136
S12 26 1145
S14 26 1115
S21 27 1186
S22 26 1049
S24 27 982
S41 28 1199
S42 26 1078
S44 26 1036

Table 3.Weight loss percentage of neat HDPE and its blends in burial soil test over four months

Sample Weight loss% Weight loss% Weight loss%

1 Month 2 Months 4 Months
S0 0 0 0
S11 0 0.02 0.05
S12 0 0.02 0.06
S14 0 0.03 0.07
S21 0 0.03 0.07
S22 0 0.03 0.08
S24 0 0.05 0.09
S41 0 0.07 0.10
S42 0 0.07 0.11
S44 0 0.09 0.13

Figure 1.Sample dimension according to American Standard ASTM D638-08

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S
0
S
1
1
S
2

Figure 2.Stress-Strain curves of samples S0, S11, S21 and S41

Figure 3.SEM micrographs of neat HDPE and its blends

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