Effect of MAPP Addition on Impact Strength, Water Absorption, and Filler Volume Fraction of the Waste Polypropylene Modified Coconut Wood Flour Glass Fiber Hybrid Composite

Journal of Polymer Materials : An International
Journal
ISSN: 0973-8622
e-ISSN: 0976-3449
Subject: Chemistry
Periodicity: Quarterly
Month(s) of Publication: Mar., Jun., Sept. & Dec.
Current Volume: 33 (2016)

Chief Editor


Prof. Sukumar Maiti , Subarnarekha, J-23 Bidhannagar, Midnapore 721101,
West Bengal

Editor


Prof. S. K. Dolui, Department of Chemical Sciences, Tezpur University,
Tezpur


Co-Editor


Dr. Dibyendu S. Bag, Polymer Science Division, DMSRDE, Kanpur

Editorial Board




Charles E. Carraher, Florida Atlantic University, USA
Ben Zhong Tang, Hongkong University of Science & Technology
Tamaki Nakano, Hokkaido University, Japan

Advisory Board











A. Kumar, Tezpur University
A. K. Saxena, DMSRDE, Kanpur
Akhil Sen, BIT, Mesra
Amitabha De, SINP , Kolkata
Asim K. Ghosh, BARC, Mumbai
C. P . Reghunandhan Nair , VSSC, Thruvanthapuram
C.V. Avadhani, NCL, Pune
Cedric Gaillard, NIAR, France
Debabrata Chakrabarty, Calcutta University

















Dilip Kumar Kakati, Gauhati University
H. B. Bohidar, JNU, New Delhi
Jude O. Iroh, University of Chincinnati, USA
K. C. Gupta, IIT Roorkee
L. Lapcik, T omas Bata University, Czech Republic
Manoranjan Patri, NMRL, Ambernath
Mariatti Jaafar, Universiti Sains Malaysia
P. H. Parsania, Saurastra University , Rajkot
P. P. Wadgaonkar NCL Pune
Pradip Kumar Dutta, MNNIT, Allahabad

Pranesh Chowdhury, Visva Bharati University
Sabu Thomas, Mahatma Gandhi University, Kottayam
Susanta Banerjee, IIT Kharagpur
V . K. Gupta, Reliance Industries Ltd, Mumbai

List of Content
Volume 33 (2016) Issue 4 , (October-2016 to December-2016)
Oct-Dec
Tribological Behavior of Phenolic Nanocomposites Reinforced by 2D Atomic
Crystal of Boron Nitride (CHINA)by BINGLI PAN, JINLONG TAN, HAINING JIA,
JUN CHEN, YUPING TAI, JICHUN LIU, YONGZHEN ZHANG AND QINGSHAN NIU
Page: 567-577

Experimental Investigation on Bearing Response of Carbon Reinforced
Aluminium laminates - Influence of natural fibre and specimen geometry
(INDIA)by M.VASUMATHI, AND VELA MURALI
Page: 579-588

Curing Characteristics and Tear Properties of Calcium Carbonate/Bentonite
Filled Ethylene Propylene Diene Monomer (EPDM) Rubber Composites

(MALAYSIA)by NURUS SAKINAH CHE MAT, NADRAS OTHMAN AND HANAFI
ISMAIL
Page: 589-595

Isothermal Crystallization Kinetics of Polylactic Acid Toughened with an
Impact Modifier (MALAYSIA)
by RAZAINA MAT TAIB, AND THAM CHO YIN
Page: 597-604

Effect of Hybrid Fillers in PP/EPDM Nanocomposites for Electrical Insulator
Application (MALAYSIA)by M.S. HAMZAH, M. MARIATTI AND M. KAMAROL
Page: 605-613

Comparison of Mechanical Properties of Graphene Oxide and Reduced
Graphene Oxide Based Polymer Composites (MALAYSIA)by N.M.S HIDAYAH,

WEI-WEN LIU, C.W. LAI, N.Z. NORIMAN, S.T. SAM, U. HASHIM, AND HONCHEUN LEE
Page: 615-628

Rigid Polyurethane Foam from Palm Oil Polyol–Polyethylene Glycol Blend

(MALAYSIA)by IZZAH ATHIRAH AHMAD NASIR, ADILAH ALIS, ZURINA
MOHAMAD, SITI HAJJAR CHE MAN, AND ROHAH A. MAJID
Page: 629-637

Recycled Polypropylene/Peanut Shell Powder Composites: Effect of Filler
Loading and Compatibilizer (MALAYSIA)by N.F. ZAABA, M. MARIATTI AND H.
ISMAIL
Page: 639-645

Properties of Recycled Natural Latex Gloves Filled NBR: Effects of Sawdust
and trans Polyoctylene Rubber (MALAYSIA)by OMAR S. DAHHAM, NORIMAN
N.Z., SAM S.T., H. ISMAIL, S. RAGUNATHAN, ROSNIZA H., AND MARWA N. ALSAMARRAI
Page: 647-655

Miscibility and Migration Ability of Triacetin as an Alternative Plasticizer in
Polyvinyl chloride Compounds (MALAYSIA)by ARJULIZAN RUSLI, MOHAMMAD
ZAKWAN MOHAMAD AND AZURA ABDUL RASHID
Page: 657-665

Effect of MAPP Addition on Impact Strength, Water Absorption, and Filler

Volume Fraction of
the Waste Polypropylene/Modified Coconut Wood Flour/Glass Fiber Hybrid
Composite (INDONESIA)
by HALIMATUDDAHLIANA NASUTION, SILVIA, CASTIQLIANA AND NUIM HAYAT
Page: 667-676

The Potential of Donax Grandis Hypodermal Fiber as a reinforcement in
Starch-based Composite (MALAYSIA)by SOFIYAH MOHD RAZALI, MAHANI
YUSOFF, SITTI FATIMAH MHD RAMLE, IRSHAD UL HAQ BHAT, ABD HAMID
MAR IMAN, AND MOHD HASMIZAM RAZALI
Page: 677-684

Preparation of Cross-linked and Fluorine-silicon Modified Acrylate Emulsion
by Using Mixed Green Surfactants (CHINA)by XIUMING WANG, ZHONGBIN
BAO, AND LIJUN CHEN
Page: 685-696

Effect of MAPP Addition on Impact Strength, Water
Absorption, and Filler Volume Fraction of the Waste
Polypropylene/Modified Coconut Wood Flour/Glass

Fiber Hybrid Composite
HALIMATUDDAHLIANA NASUTION1, SILVIA2, CASTIQLIANA3 AND NUIM HAYAT4
Department of Chemical Engineering, Faculty of Engineering,
University of Sumatera Utara, North Sumatra,
20155 Medan, Indonesia
ABSTRACT
In this study, hybrid composite materials were prepared from combination of modified coconut
wood flour (MCWF) and glass fiber (GF) as fillers, and waste polypropylene (WPP) as
matrix. The coconut wood flour (CWF) was modified by 18% sodium hydroxyde solution to
reduce its hydroxyl group.The interfacial adhesion between the non-polar waste
polypropylene matrix and the polar fillers could be enhanced by using maleic anhydride-gpolypropylene (MAPP) which was synthesized from the refluxed reaction of maleic
anhydride, polypropylene, xylene and benzoyl peroxide at 135°C. MAPP and GF composition
were made constant at 2 wt. % and 10 wt. %, respectively and MCWF composition was
varied from 10 – 40 wt.%. Mixing process was carried out in an extruder at 180oC and the
samples were then molded in a hot press machine. The impact strength, water absorption,
and filler volume fraction analysis were investigated. The results showed that addition 30
wt.% of MCWF and 10 wt.% of MAPP can elevate the impact strength of the composite.
The study also revealed that water absorption of the composite has reduced with the
utilization of MAPP. As comparison, composite without MAPP, no fillers and using one type
of filler were also prepared. These results were also supported by Fourier Transform Infra

- Red (FTIR) and Scanning Electron Microscopy (SEM) analysis.
KEYWORDS: Coconut Wood Flour, Hybrid Composite, Waste Polypropylene.
INTRODUCTION
Hybrid composite is a system constituted by
two different reinforcements incorporated into
J. Polym. Mater. Vol. 33, No. 4, 2016, 667-676
© Prints Publications Pvt. Ltd.
Correspondence author e-mail: h_dahliana@yahoo.com

a single matrix or establishment of a single
reinforcement into two different matrices. The
properties exhibited by the hybrid composite
is generally the combination of the individual

668

Nasution et al.

constituents which would give convenience
in balancing each of their superior and inferior

properties. Introduction of extra reinforcement
or matrix are conducted to overwhelm the
weakness of the other reinforcement or
matrix, and this will eventually lead to cost
and performance balance through an
appropriate material design. Using a hybrid
composite that contains two or more types of
different fibers, the advantages of one type
of fiber could complement deficiencies in the
other [1,2]. Environmental issues which has
become major concern is the main reason to
develop replacement of synthetic fibers with
natural fibers. However, the fact if the natural
fibers reinforced composites provide lower
mechanical properties and poorer water
resistance when compared to synthetic fibers
(such as glass fibers) cannot be neglected.
Therefore, in order to overcome these
weaknesses, glass fiber (GF) and natural fiber
can be integrated in a matrix to formulate a

hybrid composite that demonstrates best
properties of its constituents, and thereby, an
superior, economical and environmentfriendly composite could be generated.
Coconut wood flour (CWF) was selected as
the natural fibers in this research due to its
abundant supply (397 thousand m 3 per
annum all over the world) [3]. CWF is also
inexpensive, has a low density [4] ,
biodegradable and is not abrasive during the
process [1,4]. CWF also have high content of
cellulose (40,99%) which shows a good
indication to be used in polymeric composites,
as a material that has high content of cellulose
would exhibit stiff and strong material [5]. The
dispersion and adhesion between the non
polar PP matrix and the polar CWF might be
difficult. Therefore, chemical modification to
JJournal of Polymer Materials, December 2016

CWF is needed to reduce its polarity [6] .
Compatabilizer, such as maleic anhydride-gpolypropylene (MAPP) could also be applied
to improve the compatibility of the matrix with
the reinforcement [7] . In Indonesia, the
production of plastic waste was second
ranked as domestic waste producer at 5,4
million tons per annum (14% of total waste
production in Indonesia). As a matrix,
polypropylene has good physical,
mechanical, and thermal properties at room
temperature. Its stiffness, low density, high
impact strength and lower cost make it widely
use in many applications [8]. Lee et al. [9] have
studied hybrid composite polypropylene/wood
flour/clay with MAPP with improved tensile
strength and stiffness. In this study, the effect
of MAPP addition on impact strength, water
absorption and filler volume fraction of waste
polypropylene (WPP) / Modified coconut
wood flour (MCWF) / Glass Fiber (GF) Hybrid
Composite were investigated. Fourier
Transform Infra - Red (FTIR) characterization
and Scanning Electron Microscopy (SEM)
analysis were used to show the morphology
of the fractured samples and structural
changes after modification.
EXPERIMENTAL CONDITION
Materials Preparation
Wasted Polypropylene (WPP) was collected from wasted
mineral water plastic cup disposal. The WPP were cut
into smaller pieces (±5 mm x 5 mm). Coconut wood flour
(CWF) was supplied from furniture store waste. CWF
was dried under the sunlight and milled in a ball mill into
100 mesh particles. Chopped strand E-type glass fibers
(GF) were supplied by PT. Justus Kimiaraya (Medan,
Indonesia). The GF were milled in a ball mill into 100
mesh particles. Commercial xylene supplied by CV.
Rudang Jaya (Medan, Indonesia) was used as received.

Effect of MAPP Addition on Impact Strength, Water Absorption, and Filler Volume Fraction of
the Waste Polypropylene/Modified Coconut Wood Flour/Glass Fiber Hybrid Composite

669

milled in a ball mill into 100 mesh particles and
characterized by FTIR spectroscopy.

To produce MAPP, isotactic polypropylene (melt flow
index 14 g/10 min) supplied by Titan PP Polymers
(TitanPro 6331 grade) (Johor, Malaysia), maleic
anhydride, acetone and benzoyl peroxide (supplied by
Merck Indonesia) were used as received.

Sample Preparation
Composites were manufactured in a two-stage process.
In the first stage, WPP, MCWF, GF and MAPP were
premixed mechanically at certain formulations. The
mixtures were then fed into a single-screwed extruder
at a screw speed of 50 rpm and temperature profile of
180 oC. In the second stage, the stranded extrudates
were granulated manually and cooled in a water bath.
The procured granules of extrudates were then dried at
105 oC for 24 hours before being molded in a hot press
machine at 180 o C. The hybrid composites were
produced with various contents of MCWF from 10 to 40
wt.%. The GF loadings and MAPP addition were
remained constant at 10 wt.% and 2% respectively. All
formulations of the composite components and
abbreviations used for the respective formulations were
given based on the codes in Table 1.

The coconut wood flour was immersed in 18% solution
of NaOH, heated at 90oC for half an hour. Followed by
washing with distilled water to remove all traces of alkali
until neutral, and then dried in tray dryer to diminish
water absorption.
1 g of maleic anhydride, 10 g of polypropylene and 90
ml xylene were refluxed at 135 oC for 20 minutes. 0,1 g
of benzoyl peroxide which had been dissolved in 10 ml
xylene were added into the solution and reacted for 10
minutes. The product were immersed in acetone to
precipitate the MAPP. The filtered MAPP were then
rinsed with distilled water until neutral pH was obtained.
Finally, the MAPP were dried in a tray dryer for 24 hours,

TABLE 1. Formulation of hybrid composite constituent
Sample
Code

WPP
(%)

MCWF
(%)

GF
(%)

MAPP
(%)

1
2

100

0

0

0

88

10

0

2

3

88

0

10

2

4

80

10

10

0

5

78

10

10

2

6

70

20

10

0

7

68

20

10

2

8

60

30

10

0

9

58

30

10

2

10

50

40

10

0

11

48

40

10

2

Impact Strength

Water Absorption Analysis

Izod impact strength for the specimens was determined
having dimensions 60 x10 x 3 mm as per ASTM D-4812
- 11, with ‘‘V’’ notch depth of 2,54 mm and notch angle of
45o, using Impact Testing Machine. The conventional V
notched specimens were according to ASTM D-256.

The specimens of dimension 25 x 25 mm (ASTM D 570)
were tested. The samples were dried in an oven at 50±
5oC for 24 hour, cooled in desiccators for 24 hours.
Then, all the samples were immersed in a container of
distilled water. At the end of 24 hour, the specimen

Journal of Polymer Materials, December 2016

670

Nasution et al.

were removed from water one at a time, all surface
water was wiped off with a dry cloth, and they were
immediately weighed to the nearest 0,01 g. The
percentage of composite mass accretion during water
absorption was determined. The water absorption of
the test was determined with the following equation:
(1)
where w is the composite mass after t immersion days,
wo is the composite mass before immersion.
Filler Volume Fraction
Consider a composite material that consists of fibers and
matrix material. The volume of the composite material is
equal to the sum of the volume of the fillers and the
matrix.

Vc = Vf + Vm

(2)

where Vc is the composite volume, Vf is the filler volume
and Vm is the matrix volume.
The matrix volume fraction (Mvf) was measured with
the formula:
(3)

The filler volume fraction (Fvf) can be calculated by
this equation:

Fvf = 1 – Mvf

Fourier Transform Infra - Red (FTIR) characterization
and Scanning Electron Microscopy (SEM) analysis were
considered to identify to show structural changes and
morphology of fractured samples, respectively.

RESULTS AND DISCUSSION
Fourier Transform Infra-Red (FTIR)
Analysis
Figure 1. shows the FTIR spectra of the
synthesized compatabilizer, maleic anhydride
- g - polypropylene (MAPP). It revealed the
presence of absorbance in the wavelength
number of 2955 cm -1 which indicated the
existence of alkanes groups (C–H). Ketones
groups (C=O) and C–O from anhydrides were
also observed at 1712 cm-1 and 1165 cm-1
respectively. Moreover the appearance of C–
H from –CH2 (methylene) and C–H from –CH3
(methyl) were also determined in the peak

Fig. 1. FTIR Spectra of maleic anhydride-g-polypropylene (MAPP)

JJournal of Polymer Materials, December 2016

(4)

Effect of MAPP Addition on Impact Strength, Water Absorption, and Filler Volume Fraction of
the Waste Polypropylene/Modified Coconut Wood Flour/Glass Fiber Hybrid Composite

absorbance at 1454 cm-1 and 1369 cm-1. All of
these peak absorbances numbers strongly
supported the chemical structure of maleic

671

anhydride-g-polypropylene which was
presented in Figure 2.

Fig. 2. Chemical structure of maleic anhydride-g-polypropylene (MAPP)

From Figure 3, it is observed that alkaly
modification had successfully decreasing the
polarity of MCWF by strongly reduced the

peak absorbance in the wavelength number of
3444 cm-1 and 2357 cm-1 (for –OH) and 1593
cm-1 (for N–H). It is also indicated the presence

Fig. 3. FTIR Spectra of Hybrid Composite, Unmodified and Modified Coconut Wood Flour

Journal of Polymer Materials, December 2016

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Nasution et al.

of absorbance in the wavelength number of 2878
cm -1 and 2357 cm -1 which indicated the
presence of –OH and N–H (the main functional
group of cellulose) had been dispersed well into
the matrix (WPP).
Impact Strength
Figure 4 shows the variation of impact properties
of the hybrid composites. The impact strength
is a parameter that shows the maximum
number of pressure caused by the high speed
could be received by a material before it
undergoes cracking. Results of this testing

indicate the toughness, it is strongly influenced
by the strength of the bond interphase and the
characteristic of the matrix and fillers [10].
From Figure 4, the drop of impact properties is
occurred to composites without MAPP (sample
code 4, 6, 8, 10). It might be due to poor
interfacial adhesion between the matrix and the
fillers, which is a general phenomenon in
incompatible composites with different
characteristics, such as non polar of the PP
and GF and the polar of CWF [6].

Fig. 4. Impact strength properties of hybrid composites as functions of the fiber loadings

However, addition of GF gave a significant
effect in raising the impact strength of the
composite, from 37.9 J/cm2 to 40.5 J/cm2 (for
sample codes 2 to 5). Abdul Khalil et al. [11]
also reported a similar trend. This result is

JJournal of Polymer Materials, December 2016

due to the high energy absorption capability
of the glass fiber. Conversely, declining
impact strength was observed when MCWF
was added into composite from 49.5 J/cm2
to 40.5 J/cm2 (sample code 3 to 5). This 21%

Effect of MAPP Addition on Impact Strength, Water Absorption, and Filler Volume Fraction of
the Waste Polypropylene/Modified Coconut Wood Flour/Glass Fiber Hybrid Composite

reduction was stimulated by the lower ability
to absorb energy.
Otherwise, the improvement of impact
properties is occurred to composites with
MAPP (sample code 5, 7, 9) with the
increased of MCWF loadings up to 30 wt.%.
Further increment of MCWF resulted to
weaker impact properties. The increased
impact strength were caused by improved
interfacial adhesion between the matrix and
the fibers [12]. However as the fiber loadings
content were extended, fibers to fibers contact
were increased and this eventually lead to
lower ability of fibers to support stresses
transferred from matrix. This observation was
also in approval of previous study reported
by Ashori et al. [13].

673

Water Absorption
The rate of water absorption depends on the
internal material status, nature of
reinforcements, fiber–matrix interface, as well
as environmental factors such as temperature
and applied stress[12]. The material shrinks or
swells when the incorporated wood is dried or
absorbs water; this lack of dimensional stability
is a major drawback of such materials [14]. In
this study, after the test period, the samples
were removed from the water, dried with a cotton
cloth, and reweighed.
Figure 5 shows the water absorption of hybrid
composites. With the increased of MCWF
loadings, the water absorption increased
from 9.7% to 13.5% (sample codes 8 to 10).
Sample code 2 (with formulation of 88/10/0/2)

Fig. 5. Water absorption of hybrid composites

Journal of Polymer Materials, December 2016

674

Nasution et al.

and sample code 5 (with formulation of 78/10/
10/2) resulted the same amount of water
absorption due to negligible water absorption
capacity of water impermeable glass fiber [12].
However, addition of MAPP had significantly
reduced the water absorption by 11.3%
(sample codes 10 to 11) since there is more
compatibility and better adherence to the
polymer matrix which covers more wood’s
surface and reduces the direct contact woodwater. It also increases the ester linkages
between the hydroxyl groups of MCWF and
the anhydride part of MAPP. Therefore, the

amount of free OH– in the wood cellulose is
reduced because some of them are interacting
with succinic anhydride, so this change
generates less water absorption, compared to
the composite without MAPP [14].
Fiber Volume Fraction
Table 2 shows that the fiber volume fraction
increased with the increasing amount of fillers
in the composite. The increasing amount of
MCWF which has lower density than the WPP
and GF, resulting in a lower density of the
composite. It is also indicated that the

TABLE 2. Filler Volume Fraction of Hybrid Composite
Sample code

Composite ratio (WP/MCWF/GF/MAPP)

Filler Volume

Filler Volume Fraction

1

100/0/0/0

0

0

2

88/10/0/2

12

0,125

3

88/0/10/2

12

0,126

4

80/10/10/0

20

0,224

5

78/10/10/2

22

0,203

6

70/20/10/0

30

0,318

7

68/20/10/2

32

0,303

8

60/30/10/0

40

0,421

9

58/30/10/2

42

0,413

10

50/40/10/0

50

0,522

11

48/40/10/2

52

0,502

composite with MAPP has lower fiber volume
fraction. This was due to the improved
interfacial adhesion between the matrix and
the fillers that causes the composite to have
less void and higher density.

JJournal of Polymer Materials, December 2016

Fracture Sample Analysis
Figure 6 displays SEM micrographs of the
fractured composite which had the highest
impact strength property. In addition, the
sample without MAPP, but similar filler

Effect of MAPP Addition on Impact Strength, Water Absorption, and Filler Volume Fraction of
the Waste Polypropylene/Modified Coconut Wood Flour/Glass Fiber Hybrid Composite

675

Fig. 6. Fractured sample morphology of composites (a) sample code 9 (b) sample code 8

composition is also presented. It was clearly
showed the uniform distribution of filler in
WPP matrix. This was due to the improved
interfacial adhesion created by the MAPP.
Without MAPP, fillers pull-out was observed.
It is caused by the weak interfacial adhesion
that makes the stress transfer from the fillers
to the matrix and consequently failed.
Adding MAPP had significantly helped in
enhance the interfacial adhesion of the
composite.
CONCLUSION
The utilization of MAPP as compatibilizer
improved the impact properties and reduced
water absorption of the composite. The
highest impact strength was achieved in
WPP/MCWF/GF/MAPP ratio of 58/30/10/2.
Moreover, SEM micrographs showed that
MAPP had significantly enhanced the
interfacial adhesion between the matrix and
the fillers.
Acknowledgment
The authors would like to thank to University
of Sumatera Utara.

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