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Effect of water absorption on pultruded jute/glass fiber-reinforced unsaturated polyester hybrid


composites
Mohd Hafiz Zamri, Hazizan Md Akil, Azhar Abu Bakar, Zainal Arifin Mohd Ishak and Leong Wei Cheng
Journal of Composite Materials 2012 46: 51 originally published online 21 September 2011
DOI: 10.1177/0021998311410488
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JOURNAL OF
COMPOSITE
M AT E R I A L S

Article

Effect of water absorption on pultruded


jute/glass fiber-reinforced unsaturated
polyester hybrid composites

Journal of Composite Materials


46(1) 5161
! The Author(s) 2011
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DOI: 10.1177/0021998311410488
jcm.sagepub.com

Mohd Hafiz Zamri, Hazizan Md Akil, Azhar Abu Bakar,


Zainal Arifin Mohd Ishak and Leong Wei Cheng

Abstract
The use of natural fibers in polymer composites has given renewed interest to the development of green composites
today. However, the moisture absorption of natural fibers gives serious concern, especially for their potential outdoor
applications. This article reports the study results on the water absorption of pultruded jute/glass fiber-reinforced
unsaturated polyester hybrid composites, which was subjected to various water conditions and their effects on its
mechanical properties. Water absorption tests were performed by immersing composite specimens into three different
water conditions, namely: distilled water, sea water, and acidic water, which were at room temperature, for a period of
3 weeks. The characteristic parameter of diffusion coefficient (D) and maximum moisture content (Mm) were determined
from the obtained water absorption curves. The water absorption behavior of the glass/jute fiber-reinforced unsaturated
polyester hybrid composite was found to follow a non-Fickian behavior. The effects of the various aqueous environments
on the flexural and compression characteristics were investigated in this study. The flexural and compression properties
were found to decrease with an increasing percentage of water uptakes.

Keywords
Fibers, hybrid composites, environmental degradation, mechanical property, pultrusion

Introduction
With an increasing environmental awareness by the
general public, there are active research interests on
the studies of natural ber-reinforced polymer matrix
composites. This is largely due to their eco-friendliness
and cost eectiveness.1 The advantages of natural ber
composites are, reasonable strength, lightweight, free
from health hazards, biodegradable, and therefore,
their potential to be used as building materials.24 The
natural bers also promise sustainability, cheaper, and
lighter in weight, which provides better stiness per
weight than glass.5
Despite the advantages listed above, their limitations
include, a lower modulus, low strength and poor moisture resistance, and especially their absorption when
compared with synthetic bers, such as glass.6
Natural bers also have poor wettability by non-polar
plastics, and insucient adhesion between untreated
bers and the polymer matrix, which can lead to debonding with age.7,8 The moisture absorption, by

composites containing natural bers, has several


adverse eects on their properties and thus, aects
their long-term performance. For example, increased
moisture causes the bers to swell, decreases their
mechanical properties, provides the necessary conditions for biodegradation, and changes their
dimensions.9
Several research works have been reported on eect
of water absorption in natural ber-reinforced composites, such as bambooglass ber, sisal, ax pineapple
leaf ber, jute, short roselle and sisal ber, and
bamboo ber, which shows the relevancy of the subject.
Presence of moisture in the natural composites would
School of Materials and Mineral Resources Engineering, Engineering
Campus, Universiti Sains Malaysia, Penang, Malaysia
Corresponding author:
Hazizan Md Akil, School of Materials and Mineral Resources Engineering,
Engineering Campus, Universiti Sains Malaysia, 14300 Nibong Tebal,
Penang, Malaysia
Email: hazizan@eng.usm.my

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52

Journal of Composite Materials 46(1)

lower the exural strength, tensile strength, and other


mechanical properties of the composites system.912
All polymers and composites absorb moisture in
humid atmospheres when immersed in water. In general, moisture diusion in composites, depends on factors, such as the volume fraction of ber, void volume,
additives, humidity, and temperature.13,14 Moisture diffusion in polymer composites has been shown to be
governed by three dierent mechanisms. The rst
involves the diusion of water molecules inside the
micro gaps between the polymer chains. The second
involves capillary transportation into the gaps and
aws at the interfaces between the ber and the
matrix. The third involves transportation of micro
cracks in the matrix, arising from the swelling of
bers, particularly in the case of natural ber
composites.9,12
One possibility, to obtain a composite with better
mechanical performance, is reinforcement by two or
more ber-types in a single matrix, leading to hybrid
composites with a greater diversity of material properties. The advantage of using a hybrid composite; is that
one type of ber could complement what is lacking in
the other. Besides that, hybridization signicantly
enhances the mechanical properties of composites.12,15
In this research, glass bers, which have higher mechanical properties, were combined with the jute bers to
give biodegradable properties to the composite samples.16 Hybridization of natural ber, with stronger
and more corrosion-resistance synthetic ber (e.g.,
glass ber), can improve the stiness, strength, as well
as the moisture resistance of the composites, and therefore, a balance between environmental impact and performance may be achieved. Besides the increase in the
mechanical properties of the composites, hybridization
also reduces the weight of composites and their production costs.
Importantly, hybridization between natural bers
and glass bers is expected to improve the properties
of the materials and decrease their water uptake, and
subsequently reducing the water absorption problem.
By improving the water absorption resistance, the composite will maintain its properties, even though it is
being used in humid environment. It is really important
to consider the water absorption into composites, since
the presence of moisture in the composite sample,
reduces its mechanical properties.
The inuence of the moisture absorption eect, on
the mechanical properties of a hybrid sandwich composite, formed by polyester resin-reinforced woven fabrics of glass and jute ber, has been discussed in
previous studies.10 The objective of this study was to
investigate the eect of moisture absorption on the
hybrid jute/glass ber-reinforced unsaturated polyester,
after exposure to dierent types of solution.

Samples of pultruded jute/glass ber-reinforced


unsaturated polyester hybrid composites, have been
successfully produced, using the pultrusion method.
The pultrusion process was selected, because of its
unique processing technique of composite manufacture.
Pultruded composite is always associated with high
strength and stiness, which is particularly due to its
high ber content i.e., 70%. So, pultrusion is one of
several composite processing techniques that could process composites with up to 70% ber content, in a unidirectional ber conguration.5,17
In this study, the hybrid-pultruded composite was
manufactured with a higher ratio of matrix to ber
loading i.e., 30:70, with a ratio of glass to jute of
50:50, by volume. A maximum ber loading was
selected to observe maximum moisture absorption
and will be used as a reference or standard, for the
next study (the results from another study will be published soon). Water immersion tests in various water
conditions have been successfully performed. Hybrid
jute/glass ber-reinforced polyester-pultruded composites, were immersed in three dierent solutions of distilled water, seawater, and an acidic solution at room
temperature. The data collected were used to compare
the maximum water absorption (Mm) with the diusion
coecient (D), of composites made using 100% natural
and synthetic bers. Finally, the eect of water absorption on the properties of jute/glass ber-reinforced
hybrid composites were evaluated, based on exural
and compression testing. Compression properties,
before and after immersion, were analyzed and
discussed.

Materials
Jute bers were supplied by Alam Fiber Impex Ltd,
Bangladesh, in a twisted roving form. Glass bers
were in a direct roving form and were supplied by
MMFG Composites Sdn. Bhd. Unsaturated polyester
resin (Crystic P9901) was purchased from the Revertex
Company, Malaysia. Table 1 gives an overview of the
jute bers properties. The properties of the glass ber
and unsaturated polyester resin can be found in
Tables 2 and 3.

Preparation of pultruded composites


The hybrid composite used in this study was a unidirectional jute ber/glass ber-reinforced composite rod,
measuring 12.7 mm in diameter, and produced using a
thermoset pultrusion machine. The parameters used for
pultrusion processing, are shown in Table 4.
This machine is equipped with a creel, guidance
devices, resin bath, preforming guide, heated die,

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Zamri et al.

53

pulling device, and cut-o saw, as shown in Figure 1.


The continuous jute and glass bers were rst impregnated with an unsaturated polyester resin in a resin
impregnation tank. A pulling device was used to pull
the impregnated jute and glass ber through a steel die,
to achieve the desired shape, and also establish the correct resin/ber ratio. A curing process was carried out
using a curing die, which is precision machined to
impart the nal shape. A pulling device draws the
stock though a die and also determines the production
speed. Finally, a cut-o mechanism was used to cut the
continuous pultruded composites into the desired

Table 1. Properties of the jute fiber

lengths.17,18 The average diameter, of all composite


rods, is 12.7 mm.

Material characterization
Water absorption investigation. Specimens were
immersed into three dierent aqueous environments,
which were distilled water, sea water, and an acidic
solution. For the water absorption measurements, the
specimens were withdrawn from the solution, wiped dry
to remove surface moisture, and then weighted using an
electronic balance (accurate to 104 g) to monitor the

Table 3. Properties of unsaturated polyester resin1

Properties

Unit

Value

Tex
Density
Diameter
Tensile strength
Specific strength
E-modulus
Specific modulus
Elongation

g/km
g/cm3
mm
MPa
UTS/density
GPa
E/density
%

828
1.3
25.2
393773
302595
26.5
20.4
1.51.8

Properties
Viscosity at 23 C
Brookfield RVT 2/10 rpm
Density
Reticulation at 23 C
Operational time
Youngs modulus
Tensile stress at break
Tensile strain at break

Unit

Value

Standard

MPas
kg/dm3

1200
1.2

ISO 2555
ISO 2811

min
MPa
MPa
%

20
4000
61
2.5

ISO 527
ISO 527
ISO 527

Table 2. Properties of the glass fiber


Properties

Unit

Value

Tex
Density14
Diameter15
Tensile strength14
Specific strength
E-modulus14
Specific modulus
Elongation14

g/km
g/cm3
mm
MPa
UTS/density
GPa
E/density
%

4400
2.5
525
25003500
10001400
70.0
28
2.5

Table 4. Details of pultrusion parameter

Jute fiber-pultruded composites


Glass fiber-pultruded composites

Figure 1. The schematic of pultrusion machine.

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Pulling
speed
(mm/min)

Temperature
( C)

195
350

135
135

54

Journal of Composite Materials 46(1)

Table 5. Effect of immersion environments on the diffusion


coefficient, D and the maximum moisture content, Mm of jute
glass fiber reinforced unsaturated polyester hybrid composite
Flexural specimen
Distilled water
D (m2/s)
Mm (%)
Sea water
D (m2/s)
Mm (%)
Acidic solution
D (m2/s)
Mm (%)

Compression specimen

7.14  1012
4.46

2.68  1011
5.16

12

11

5.98  10
3.55

6.17  1012
4.30

2.23  10
4.72

2.30  1011
4.92

mass during the aging process. The moisture content


M (%), absorbed by each specimen was calculated
from its weight before, wo and after, wt absorption, as
follows:


M1  M0
M% 100
M0

where M (%), is the moisture content in percentage; M1


(g) the weight of the wet sample at a given time, and M0
(g) the initial weight of the sample. Further analysis of
water absorption characteristics of pultruded samples
in various solutions, was performed by measuring the
diusion coecient (D). The diusion coecient (D),

Figure 2. Weight gain as a function of time for (a) flexural specimen and (b) compression specimen of juteglass reinforced
unsaturated polyester hybrid composite materials exposed to distilled water, sea water, and acidic solution at room temperature.

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RT
45
4.84  1012 (504)a
n/a
6.54  1012 (504)a
2.87  1013 (4700)a
10.25
n/a
10.71 (504)a
1.20 (4700)a
Duration of immersion (hours).
a

70:30
70:30 Where
50:50 of glass
and jute
70:30
66:34
Kenaf/polyester
Glass and
jute/polyester

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Jute/polyester
Graphite/epoxy

68:32
55:45

10.34
n/a

21.27
4.72
25.30 (6240)a
4.46 (504)a

5.93  1012 (504)a


n/a

RT
RT
17.91  103 (6240)a
2.23  1011 (504)a
19.85  103 (6240)a
2.68  1011 (504)a

1.33  10 8 (8760)a
8.56  106 (1440)
n/a
n/a
0.55 (8760)a
0.23

n/a
n/a

Distilled
Acidic

D (mm2 s1) (hours)a

Glass/vinylester
Glass/polyester

In this study, hybrid composite samples were immersed


into three types of aqueous environments, which were
distilled water (pH 7), sea water (pH 8), and an
acidic solution (pH 3). These three types of solution
were selected because they represent real-life conditions, where these samples can be applied. These solutions have also been used in previous studies.5,7 Water
absorption curves, for exural and compression specimens of jute/glass ber-reinforced unsaturated polyester hybrid composites, are shown in Figure 1(a) and (b),

Mm (%) (hours)a

Results and discussions


Water absorption behavior of pultruded jute/glass
hybrid composites

Matrix:fibers
ratio

out using Instron 3367 according to the standard


ASTM D 695-02 a. The diameter and length of the
specimen were 12.7 and 25.4 mm, respectively. The
crosshead speed for compression test was set at 5 mm/
min. Three specimens for each condition were used to
minimize errors.

Composites
system

Compression testing. A compression test was carried

Table 6. Comparison of moisture content (Mm) and diffusion coefficient (D) for various composites system

Flexural testing. A exural test was carried out using


Instron 8802 according to the standard ASTM D4476
03. Specimens (pultruded rods with diameters of
12.7 mm) were cut into two parts, where the cross-section of each part is smaller than a half-round section.
The total specimen length was 125 mm with an overhang length of 12.5 mm, at both supports. The crosshead speed for the exural test was set at 5 mm/min.
Three specimens for each condition were used to obtain
a satisfactory result.

Sea

The times were chosen at a very early stage of


the moisture process, so that the weight change could
still be taken to vary linearly with the square root
of time.

n/a
n/a

19.22  103 (6240)a


2.30  1011 (504)a

2

n/a
n/a

M2  M1
k p p
T2  T1

Sea

Temperature
( C)

where Mm (%) is the maximum weight gain (%); h


(mm) the thickness of the composites; and k the initial
slope from a plot of M (%) vs. T (h), as shown in
Equation (3).9

25.10
4.92

40
40

2

Distilled

kh
4Mm

Acidic


D

References

for the composite specimen was calculated using


Equation (2):

Nosbi et al.5
Jarukumjorn,
and Suppakarn6

55
Mishra et al.2
Velmurugan
and Manikandan3
Wambua et al.4

Zamri et al.

56

Journal of Composite Materials 46(1)

Figure 3. (a) Flexural strength, (b) maximum flexural strain, and (c) flexural modulus for juteglass fiber-reinforced unsaturated
polyester hybrid composite after exposed to environmental conditions.

respectively. Each curve represents the average data of


all three specimens. From the water absorption curves,
it is clear that the absorbed water content increased
with an increasing immersion time. This nding has
been reported previously concerning the natural berreinforced composites.57,19
In general, the water absorption behavior of hybridpultruded composites in all three solutions can be considered as a non-Fickian process, where it shows an
increasing trend and the moisture uptake never reaches
equilibrium after the initial take-o. Similar observations have been reported previously.5,7 In principle, the
diusion process of water in polymers and polymeric
composites may depart from the idealizations inherent
in the classical formulation of Ficks law.9,20,21 Since
the moisture uptake does not reach equilibrium, a
non-Fickian moisture absorption process may have signicant eects for long-term applications in humid
environments.
Further analysis of the water absorption characteristics of hybrid-pultruded composites in various solutions was done by measuring the diusion coecient
(D). The diusion coecient (D), for the composite
specimens, was calculated using Equation (2).
Diusion coecient, D and the maximum of moisture content, Mm for exural specimens and

compression specimens of jute/glass ber-reinforced


unsaturated polyester hybrid composite are represented
in Table 5. From the values shown in Table 5, the highest diusion coecient was recorded for jute/glass
hybrid-pultruded composites, immersed in distilled
water, followed by an acidic solution, and seawater.
Based on the diusion coecient Ds value in
Table 5, diusion of water into jute/glass hybrid-pultruded composite was more favorable in distilled water,
compared to the acidic solution and seawater. This was
due to the presence of large salt molecules in the sea
water (notably sodium chloride), which slows the diusion process into the matrix of the composite materials,
resulting in lower absorption kinetic parameters.22 This
trend can be related to the hydrolysis mechanism of the
cellulose within natural ber. The hydrolysis of cellulose is expected to be more pronounced in seawater
(alkaline) and acidic solution, compared to distilled
water. In seawater (alkaline), it is expected that the
electro negativity of the solution has a strong inuence
on the diusion process, which can make the jute
bers swell with a highly positive charge. In terms
of electro negativity, seawater has the highest, compared to the acidic water, and then the distilled water.
This nding is in agreement with previously reported
work (Figure 2).23

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Zamri et al.

57
(b) 900

(a) 900
Standard
1st Day
1st Week
2nd Week
3rd Week

700
Stress, MPa

600
500

800

600

400

500
400

300

300

200

200

100

100

0
0

10

20

30

Standard
1st Day
1st Week
2nd Week
3rd Week

700
Stress, MPa

800

40

50

Strain,

x103

60

70

80

90

10

20

30

40

50

Strain,

x103

60

70

80

90

(c) 900
Standard
1st Day
1st Week
2nd Week
3rd Week

800
700
Stress, MPa

600
500
400
300
200
100
0

10

20

30

40

50

60

70

80

Strain, x103

Figure 4. Stressstrain curves for flexural specimen of juteglass fiber-reinforced unsaturated polyester hybrid composite after
exposed to (a) distilled water, (b) sea water, and (c) acidic solution.

The most common glass, used in ber reinforcement,


consists of 54% SiO2, 17.2% CaO, 15.2% Al2O3, 8.0%
B2O3, 4.7% MgO, and 0.6% Na2O, by weight. Weak
acidic solutions, such as acetic acid solutions, buered
at pH values of 35, do not cause signicantly more
extensive corrosion than distilled water. However,
during immersion, there was an ion exchange of protons for metal ions on the glass surfaces and thus, acid
would catalyze depolymerization of the polymer matrix
and hydrolysis of the siloxy bonds, in the interphase
region, causing a degradation of the glass bers.24
The maximum water absorption (Mm) and diusion
coecient (D) for various composites systems are summarized in Table 6. In comparison, the maximum moisture absorption (Mm) for jute/polyester and kenaf/
polyester composites system, show higher values compared to the other composites. The maximum moisture

absorption for jute/polyester composites, immersed in


distilled water is reported at 10.71%.7 For kenaf/polyester composites system immersed in distilled water, the
maximum moisture absorption is higher i.e., 25.30%.5
The addition of natural bers to the composites system
causes a higher moisture uptake compared to synthetic
bers. This is due, in particular, to the hydrophilic
nature of natural bers, that are more sensitive
toward water absorption than synthetic bers, which
cause instability in the properties of the composites.5,7
The synthetic ber composites system shows minimum moisture absorption, compared to others. For
composites reinforced by glass bers immersed in distilled water, it shows that moisture absorption is less
than 1.00%. For graphite/epoxy composites system
immersed in distilled water, the moisture absorption is
only 1.20%.2527 The incorporation of glass ber with

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58

Journal of Composite Materials 46(1)

Figure 5. (a) Compression strength, (b) maximum compression strain, and (c) compression modulus for juteglass fiber-reinforced
unsaturated polyester hybrid composite after exposed to environmental conditions.

jute ber in polyester decreases the water absorption of


the composites. As shown in Table 6, due to the hybridization of jute and glass bers, the maximum absorption decrease to 4.46%, which lies between the 100%
natural ber composites systems and the 100% of synthetic bers. It is expected that the hybridization not
only reduces the moisture uptake, but also increases the
physical and mechanical properties of the polymer
composites.

Effect of water absorption on flexural properties


Flexural strength, maximum exural strain, and exural modulus, for jute/glass ber-reinforced unsaturated polyester hybrid composite, after exposure to
various environmental conditions, are shown in
Figure 3(a)(c), respectively. Each value represents the
average data of three specimens. Consequently, the
exural stressstrain curves, corresponding to the samples immersed in distilled water, sea water, and the
acidic solution, are depicted in Figure 4(a)(c), respectively. Figure 3 shows that for all environmental conditions, as the immersion time increases, both exural
strength and exural modulus decrease. Jute ber is a
natural ber, which tends to absorb high amounts of
moisture after exposure to aqueous environments and
this may lead to a higher degradation rate. This can

also be related to the weak bermatrix interface, due


to water absorption after exposure to the aqueous environments.9 From the gure, it was found that there are
some extraordinary increases in strength and modulus,
during the immersion. This is due to the presence of
glass ber in the hybrid composite. During immersion
in the aqueous environments, all the voids and cracks
within the composite would be lled with water, and
the absorbed water molecules act as a plasticizer, to
improve its bending strength and stiness.28 However,
excessive water absorbed may weaken the bermatrix
interface. On the other hand, the maximum exural
strain changes unpredictably. Jute ber tends to be ductile once the loss of cellulose in its structure after water
is absorbed into its structure and integrity has taken
place.9 Glass ber showed one of its natural properties,
which is a high resistance to water absorption.
For comparison purposes, the exural properties for
glass ber-reinforced unsaturated polyester-reinforced
pultruded composite and jute ber-reinforced unsaturated polyester-pultruded composite, are shown in
Figure 3(a)(c). The exural strength for polyester
resin is shown in Figure 3(a).29 Both of the unsaturated
polyester (UP)/glass and UP/jute samples are made of
the same ber:matrix ratio i.e., 70:30, respectively. For
UP/glass-pultruded composite exural properties, the
data is obtained from standard samples i.e., without

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Zamri et al.

59

Figure 6. Stressstrain curves for compression specimen of juteglass fiber-reinforced unsaturated polyester hybrid composite after
exposed to (a) distilled water, (b) sea water, and (c) acidic solution.

any immersion process. This is because unsaturated


polyester and glass ber are hydrophobic to moisture,
and thus, do not absorb water. The 21-day period of
immersion is too short for any signicant changes to
the composites and its properties. On other hand, the
UP/jute-pultruded composite exural properties are
obtained after 21 days of immersion for each solution.
By referring to Figure 3(a) the polyester resin show
lower exural, compared to the UP/jute-pultruded
composite and the hybrid-pultruded composites. The
UP/glass-pultruded composite shows a higher exural
strength. This statement is clearly proved and demonstrates that hybridization of jute ber with glass ber
insignicantly enhanced the exural properties of the
pultruded composites.

Effect of water absorption on compression properties


Figures 5(a)(c) show the variations of compression
strength, maximum compression strain, and compression modulus for jute ber-reinforced unsaturated polyester composite, after exposure to distilled water, sea
water, and acidic solutions, respectively. Each value
represents the average data of three specimens. On

the other hand, Figure 6(a)(c), show the corresponding stressstrain curves for each environmental condition investigated (i.e., distilled water, sea water, and the
acidic solution). Figure 5 indicates a trend of decrease
in compression strength and compression modulus with
an increasing immersion time. However, it was found
that there are some extraordinary increases in strength
and modulus, during the immersion. These compression results show a similar trend with the exural testing discussed in the above section. There are
uctuations, as indicated by the error bars, causing variations in the results, which could be attributed to the
uneven surfaces of the compression specimen. As a
result, a slightly eccentric applied load will cause premature buckling in the composite materials, rather than
the intrinsic compressive failure. This produced similar
results to those discussed in exural testing.
The compression properties for glass ber-reinforced
unsaturated polyester-reinforced pultruded composite
and jute ber-reinforced unsaturated polyester-pultruded composite are shown in Figure 5(a)(c), for
comparison purposes. On the other hand, the compression strength for polyester resin is shown in Figure 5(a).
Both of the UP/glass and UP/jute samples are made of

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60

Journal of Composite Materials 46(1)

the same ber:matrix ratio i.e., 70:30, respectively. For


UP/Glass-pultruded composite compression properties,
the data is obtained from the standard samples i.e.,
without any immersion process. The reason why this
sample has been taken into account was discussed earlier. By referring to Figure 5(a), the polyester resin
shows lower compression strength compared to the
UP/jute-pultruded composite and hybrid-pultruded
composites. Once again, the UP/glass-pultruded composite shows a higher compression strength compared
to the other pultruded composites. This also clearly
proves that hybridization of jute ber with glass ber
insignicantly enhanced the mechanical properties of
the pultruded composites.

Conclusion
The study of water absorption eects, on the mechanical properties of jute/glass ber-reinforced unsaturated
polyester hybrid composite, has been performed under
dierent water conditions, which were distilled water,
sea water, and acidic solutions at room temperature.
From the results obtained, the following conclusions
can be drawn:
. The water absorption pattern is found to follow nonFickian behavior. The highest values of diusion
coecient (D) and maximum moisture content
value (Mm) were recorded for specimens immersed
in distilled water, then followed by the acidic solution, and nally seawater.
. Hybridization of natural bers with synthetic bers
decreases the maximum moisture absorption and
increases the mechanical properties of the
composites.

Acknowledgment
The authors are grateful to Universiti Sains Malaysia (USM814023) for their assistance and contribution that has resulted
in this article.

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