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Journal of Reinforced Plastics and Composites OnlineFirst, published on September 8, 2009 as

doi:10.1177/0731684409343325

A Comparative Study between Gamma and


UV Radiation of Jute fabrics/Polypropylene
Composites: Effect of Starch

HAYDAR U. ZAMAN, MUBARAK A. KHAN,* RUHUL A. KHAN


M. Z. I. MOLLAH, SHAMIM PERVIN AND MD. AL-MAMUN
Radiation and Polymer Chemistry Laboratory, Institute of Nuclear
Science and Technology, Bangladesh Atomic Energy Commission
Dhaka, Bangladesh

ABSTRACT: Jute fabrics (hessian cloth) reinforced polypropylene (PP) matrix composites were
fabricated by compression molding. Jute fabrics and matrices were irradiated with gamma and
UV radiation at different doses. Mechanical properties of irradiated jute fabrics and matrices
based composites were found to increase significantly. Optimized jute fabrics were treated with
starch solution of different concentrations for different soaking time and composite made of
0.5% (for UV) and 0.3% (for gamma) starch treated jute fabrics (5 min soaking time) showed
the best mechanical properties. Scanning electron microscopic analysis of untreated and treated
composites was also performed.

KEY WORDS: Jute fabrics, polypropylene, composite, starch and mechanical properties.

INTRODUCTION

PRE-REQUISITE OF most engineering materials is that they have good stiffness and
A strength along with adequate toughness. Man-made composites usually fill this
requirement, especially since they exhibit crack-stopping capacity, which makes them
very attractive for structural or semi-structural applications. On the other hand, over
the recent years there is an increasing interest in natural fibers as a substitute for glass
fibers mainly because of their low specific gravity, low cost, as well as their renewable and
biodegradable nature [1]. However, natural fiber-reinforced materials have substantially
inferior mechanical and water resistance properties than conventional glass-fiber-
reinforced composites. Jute is a vegetal fiber made up of mainly cellulose, polyols, and
lignin. In the plant, the jute fiber has the function of phloem; that is, it carries sap
elaborated by the plant. It is located between the medulla and the bark [2—5].
Therefore, the jute fiber represents a small portion of the plant, about 5—6% of the
total weight of the green plant. There is a large group of composites prepared from poly-
meric matrices reinforced with vegetal fibers [6,7]. These composites constitute a unique

*Author to whom correspondence should be addressed. E-mail: makhan.inst@gmail.com

Journal of REINFORCED PLASTICS AND COMPOSITES, Vol. 0, No. 00/2009 1


0731-6844/09/00 0001—10 $10.00/0 DOI: 10.1177/0731684409343325
ß The Author(s), 2009. Reprints and permissions:
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2 H.U. ZAMAN ET AL.

combination of materials, which may result in the improvement of properties such as


strength and impact. To enhance the use of jute and vegetal fibers, a broader system of
investigations is necessary to search for chemical modifiers and physical treatments that
would alter these undesirable characteristics. The most important chemical modification
involves coupling methods. The coupling agent used contains chemical groups, which can
react with the fiber and the polymer. The bonds formed are covalent and hydrogen bonds,
which improve the interfacial adhesion. Khan et al. [8] has produced degradable jute-
reinforced polymer composites using vinyl and silicon monomers as coupling agents.
Also several reports have documented where the jute fibers are used as reinforcement in
thermoplastics like polyethylene (PE) and polypropylene (PP) and thermosets like unsat-
urated polyester and epoxy resin [9,10]. Khan et al. also prepared and characterized jute-
polycarbonate and jute-bipol composites and reported probable alternative of synthetic
composites [11,12]. The treatment of jute fibers with high-energy radiation (gamma) and
nonionizing radiation (UV) have been employed successfully for significant physical and
chemical changes as well as changes in surface structure and surface energy of the fibers.
There has been increasing significant growth in the development and application of radi-
ation (UV, electron beam and gamma) curable materials in various industrial areas [13].
Gassan and Gutowski [14] studied the effect of corona discharge and UV radiation on the
properties of jute fiber epoxy composites. Some jute-reinforced composites with urethane
oligomer under gamma radiation were prepared and characterized [15]. The influence of
ionizing radiation on polymers has been studied quite extensively over the past few dec-
ades. Gamma radiation known to deposit energy in solid cellulose by Compton scattering,
and the rapid localization of energy with in molecules produced trapped macrocellulosic
radicals. The radicals thus generated are responsible for changing the physical, chemical,
and biological properties of cellulose fibers [16]. Starch is the most abundant naturally
occurring polymers, a truly renewable resource, and it is a biodegradable polymer because
it can readily be metabolized by a wide range of microorganisms. Unlike other synthetic
thermoplastic polymers, starch can be processed into a thermoplastic material in the pres-
ence of plasticizers and under the influence of heat. The most important sources of starch
are wheat, potato, rice, tapioca, and corn. Starch is a polysaccharide produced by many
plants as a storage polymer. It is composed of glucose monomers joined by 2-(1—4)
linkages. The use of granular starch as filler in plastics would be advantageous because
(1) Starch is an abundant, low cost, and easily available renewable resource and (2) Starch
is biodegradable and is useful in applications in which recovery or recycling would be
different. Many researchers are already improved the mechanical properties of biodegrad-
able composites based on starch and natural fibers [17—21]. In this work we compare the
effects of 60Co g-radiation and UV radiation on the jute fabrics/PP composites and the
effect of starch as a method of surface treatment was investigated. Scanning electron
microscopy of the composites was studied here for diversified industrial applications.

EXPERIMENTAL

Materials

Bleached jute fabrics (Tossa jute) were collected from Bangladesh Jute Research Institute,
Dhaka, Bangladesh. PP (trade name; Cosmoplene) was collected from the Polyolefin
Company Limited, Singapore. Starch was purchased from Lova Chemicals, India.
A Comparative Study between Gamma and UV Radiation of Jute fabrics 3

METHODS

Composites Preparation

PP sheets of 0.20—0.35 mm were prepared from granules of PP by compression molding


at 180 C for 5 min between two steel plates under a pressure of 4 tons. For preparing the
composites, PP sheets and jute fabrics were cut into small pieces (15 cm  12 cm). Jute
fabrics were dried in an oven at 100 C for about 2 h to remove moisture and weighed by
means of electronic balances. Dried jute fabrics and also PP sheets were treated with
gamma radiation for different doses (250—1000 krad) at 350 krad/h using Co-60 gamma
source (Bangladesh Atomic Energy Commission). In gamma source, a Co-60 (25 kCi)
source with loaded GBS-98 that comprises 36 double encapsulated capsules. Irradiated
jute fabrics and irradiated PP sheets were used for the preparation of composites. Now
another dried jute fabrics and PP sheets were subjected to irradiation with UV radiation
(254—313 nm) using a minicure (UV Minicure Me-200, IST Technik, Germany), which
delivers 2-kW power strength. The speed of the conveyor of the Minicure was 4 m/min for
each pass of the substrate under the lamp by maintaining different UV radiation (50—200
UV pass) intensities. The irradiated samples (jute fabrics and PP sheets) after 24 h of
radiation were subjected to use for the preparation of composite materials. Composites
were prepared by sandwiching four layers of jute fabrics between five layers of pre-
weighted PP sheets. Composites were made by pressing this sandwich at 180 C for
5 min under a pressure of 4 tons using Carver Laboratory press (model 2518). Then
composites were cooled to room temperature using another press, then cut to the desired
size and kept in the polythene bag. The fiber weight fraction of the composites was
calculated to be 45%. Mechanical properties of the pretreated composite samples were
also measured. In order to improve the surface modification of jute fabrics by different
concentrations of starch along with hot water. Starch solutions were prepared with a
mixed of different concentrations (1—5%) of starch in hot water. Gamma and UV pre-
treated jute fabrics were soaked in these solutions for different time periods (2—10 min).
After soaking, jute fabrics were dried in an oven at 100 C and the amount of starch was
determined from the mass gain.

Determination of the Mechanical Properties

Tensile properties such as tensile strength (TS), tensile modulus (TM) and bending
properties like bending strength (BS) and bending modulus (BM) were determined for
both PP sheets and composites according to DIN 53455 and DIN 53452 standard methods
by a universal testing machine (model H50KS-0404, Hounsfield series S, UK). Impact
strength (IS) was measured by an impact tester (MT-3016) according to DIN EN IS0 179
standard in the flat wise, un-notched mode. Test samples were conditioned at 25 C and
50% relative humidity for several days before testing and all the tests were performed
under the same conditions. All the results were taken as the average values of five samples.

Scanning Electron Microscopy

The non-conducting surface of the composites can be coated with gold in agar auto
sputter coater (model 108A, England) before subjected to Scanning Electron Microscope
(SEM). The fiber matrix adhesion of the tensile fracture surface of the composites can be
4 H.U. ZAMAN ET AL.

examined by SEM (model XL 30, Philips, Netherlands). The gold coated composites
samples were kept in an aluminum disk plate. A computer is integrated with the machine
with relevant software. Scanning electron micrographs of the sample is obtained from
computer.

RESULTS AND DISCUSSION

Comparative Studies of the Mechanical Properties of the Composites

The effect of gamma radiation on the mechanical properties such as strength, modulus,
and impact properties of the PP sheet and jute fabrics/PP composites were evaluated and
are given in Table 1. It was found from the Table 1 that with the increase of gamma dose,
TS, and TM of the PP sheet increased from 25.88 MPa (indicated as 0 krad, i.e., untreated)
to 32.12 MPa (500 krad) and 0.49—0.55 GPa (500 krad) and then decreased to 28.93 MPa
and 0.52 GPa at 1000 krad, respectively. Thus by using 500 krad of gamma dose on the PP
sheet, the TS and TM values increased 24 and 6% compared to that of untreated PP
sheet. For irradiated jute/irradiated PP composite, TS and TM values increased up to
500 krad then decreased. The maximum TS and TM values were found to be 57.95 MPa
and 1.24 Gpa, respectively. This is 21% enhancement of TS and 31% enhancement of
TM compared to the untreated composite. Investigation showed that BS, BM, and IS of
the composites were increased significantly compared to the nontreated one. Maximum
BS, BM, and IS for irradiated jute/irradiated PP composites were found to be 62.45 MPa,
1.58 Gpa, and 24.25 kJ/m2 at 500 krad gamma dose, respectively. The polymer (PP and
cellulose) may under cleavage or scission (i.e., the polymer molecules may be broken into
smaller fragment). Subsequently rupture of chemical bonds yields fragments of the large
polymer molecules. The free radicals thus produced may react to change structure of the
polymer and after the physical properties of the materials. It also may undergo cross-
linking (i.e., the molecules may be linked together into large molecules) [22—24]. Gamma
irradiation also affects the polymeric structure of the fiber and produces active site.
Gamma irradiation of PP resulted with increased cross-linked density, which produces
higher mechanical properties up to certain dose. Active sites inside matrix might be pro-
duced by the application of gamma radiation. As a result, better bonding between jute and
PP matrix may occur. This may be the reason behind the increased mechanical properties

Table 1. Mechanical properties of gamma treated jute fabrics/PP composite.

Gamma
Materials radiation TS (MPa) BS (MPa) TM (GPa) BM (GPa) IS (kJ/m2)

PP sheets 0 25.8  1.1 34.1  1.2 0.49  0.02 0.53  0.02 5.1  0.67
250 28.1  0.6 36.6  2.1 0.51  0.07 0.59  0.09 7.2  0.71
500 32.1  1.0 40.3  1.5 0.55  0.04 0.63  0.06 10.2  0.84
750 30.7  1.3 37.8  2.1 0.53  0.06 0.61  0.06 9.5  1.10
1000 28.9  0.8 35.5  2.4 0.52  0.49 0.58  0.07 8.8  0.63
Composit 0 48.0  1.2 51.2  0.8 0.95  0.06 1.12  0.09 17.1  0.45
250 51.1  0.9 56.2  1.4 0.99  0.07 1.35  0.08 20.2  1.55
500 57.9  1.1 62.4  0.9 1.24  0.08 1.58  0.08 24.2  0.82
750 54.2  1.7 59.7  1.6 1.14  0.09 1.51  0.10 23.1  1.11
1000 51.8  0.9 57.1  1.2 1.1  0.10 1.42  0.07 21.9  1.58
A Comparative Study between Gamma and UV Radiation of Jute fabrics 5

of pre-irradiated jute fabrics/pre-irradiated PP composites. At higher radiation dose,


mechanical properties decrease notably because at higher dose only bond scission of PP
occurred.
Jute fabrics and PP sheets were irradiated using UV radiation of different intensities
(50—200 UV radiations dose). The effect of UV radiation on TS and TM of the composites
(and PP sheet) are shown in Table 2. It is clear that with the increase of UV radiation dose,
the TS and TM of the PP sheet increased from 25.88 MPa (indicated as 0 UV dose, i.e.,
untreated) to 36.64 MPa (100 UV dose) and 0.32—0.41 GPa (100 UV dose) and then
decreased to 33.91 MPa and 0.35 GPa at 200 UV dose, respectively. Thus by using 100
UV pass on the PP sheet, the TS and TM values increased 31% and 28% compared to
that of untreated PP sheet. For irradiated jute/irradiated PP composite, TS and TM values
increased up to 100 UV radiation dose then decreased. The maximum TS and TM values
were found 59.69 MPa and 1.32 Gpa, respectively. This is increased 24% of TS and 39%
of TM compared to untreated composite. The effect of UV radiation on BS, BM, and IS of
the composites are given in Table 2. Investigation showed that BS, BM, and IS of the
composites were increased significantly compared to the non-treated one. Maximum BS,
BM, and IS for irradiated jute/irradiated PP composites were found to be 65.37 MPa,
1.62 Gpa, and 26.14 kJ/m2 at 100 UV dose, respectively. UV treated jute fabrics/PP com-
posites showed significantly higher TS, TM, BS, BM, and IS over the gamma treated jute
fabrics/PP composites. It was revealed that UV treated jute fabrics/PP composites found
to be 3% and 7% improvement of TS and TM over the gamma treated jute fabrics/PP
composites. It was also reported that BS, BM, and IS also improved 5%, 3%, and 8%
higher than that of gamma treated jute fabrics/PP composites. The increase of mechanical
properties of composites with increasing UV radiation dose may be due to the intercross-
linking between the neighboring cellulose molecules, which resulted in the strength of
natural/synthetic fiber. It is observed that tensile properties increase with UV pretreatment
up to a certain limit and then decrease due to the two opposing phenomena, namely, photo
cross-linking and photo degradation that take place simultaneously under UV radiation
[25]. At lower doses, free radicals are stabilized by a combination reaction and, as a result,
photo cross-linking occurs. The higher the number of active sites generated on the poly-
meric substrate, the greater the grafting efficiency. But at higher radiation, the main chain
may be broken down and polymer may degrade into fragments and, as a result, tensile

Table 2. Mechanical properties of UV treated jute fabrics/PP composite.

Materials UV pass TS (MPa) BS (MPa) TM (GPa) BM (GPa) IS (kJ/m2)

PP sheets 0 25.8  1.1 28.1  1.2 0.32  0.02 0.54  0.02 4.4  0.67
25 28.1  0.6 30.1  2.1 0.35  0.05 0.58  0.08 6.3  0.98
50 31.6  1.1 32.6  1.5 0.38  0.03 0.62  0.05 7.1  1.30
100 33.9  1.3 36.6  2.1 0.41  0.04 0.65  0.06 8.9  0.89
150 30.6  0.8 32.2  2.4 0.39  0.07 0.63  0.04 6.3  0.91
200 28.4  0.8 31.1  2.4 0.35  0.03 0.62  0.08 5.9  1.24
Composite 0 48.1  2.5 51.2  2.7 0.95  0.07 1.12  0.07 17.1  0.60
25 52.1  1.3 56.6  2.2 0.98  0.04 1.25  0.06 20.1  1.23
50 56.2  2.5 59.1  1.5 1.25  0.05 1.47  0.08 24.2  0.88
100 59.6  2.1 65.3  2.7 1.32  0.06 1.62  0.05 26.1  1.30
150 56.6  1.1 63.2  2.5 1.29  0.07 1.58  0.04 23.4  0.96
200 54.2  2.2 60.4  1.1 1.26  0.06 1.52  0.07 21.6  1.21
6 H.U. ZAMAN ET AL.

properties will decrease after certain UV doses. An intense radiation results in a loss of
tensile strength, and a reduced degree of polymerization is observed [26].

Effect of Starch and their Mechanical Properties of the Composites

Starch solution of different concentrations (1—10 wt%) was prepared by dissolving the
required amount of starch in hot water (w/w) and then stirred for 10 min. The formu-
lation is given in the Table 3. Optimized jute fabrics (500 krad and 100 UV pass) were
soaked individually in the prepared formulations for 2—10 min. After soaking, jute fabrics
were dried in an oven at 105 C for 6 h and then kept in the PE bag.
The results of starch loading (SL) of the composite with respect to different starch
concentrations (formulations) against different soaking times are presented in Figure 1.
It was observed from Figure 1 that SL increased with soaking time as a function of
different starch concentrations (formulations) up to a maximum value, and then begins
to decrease with the increase of soaking time. The maximum SL value for UV and gamma
treated jute fabrics/PP composites were found to be 39% for S3 formulation (5% starch)
at 5 min soaking time and 35% for S3 formulation (3% starch) at 5 min soaking time,
respectively.

Table 3. Formulation of starch solution (w/w) used to treat the jute


fabrics for composite fabrication.

Compositions of formulations (w/w%)

UV treated jute fabrics Gamma treated jute fabrics

Formulations Starch Water Starch Water

S1 2 98 1 99
S2 3 97 2 98
S3 5 95 3 97
S4 7 93 4 96
S5 10 90 5 95

(a) 48
2% 3% 5% (b) 48 1% 2% 3%
7% 10% 4% 5%
40
Starch loading (%)

Starch loading (%)

35
32
26
24

17
16

8 8
0 2 4 6 8 10 12 0 2 4 6 8 10 12
Soaking time (min) Soaking time (min)

Figure 1. Starch loading of: (a) UV treated jute fabrics/PP and; (b) gamma treated jute fabrics/PP composites
against soaking time as a function of different concentrations.
A Comparative Study between Gamma and UV Radiation of Jute fabrics 7

The SL values were increased because starch diffused into the sites of reaction and
caused a greater amount of starch loading when fiber swelled in starch solution. At low
concentration and soaking time the SL values is less, because soaking increases the cross-
sectional area of the fiber at the same time the fiber surface become lustrous. As a result,
starch can easily diffuse in the fiber and react with cellulose in low soaking time.
The decrease in starch loading value at higher concentration and soaking time could be
associated with the fact that the swelling of the cellulose backbone with water is insuffi-
cient due to low water concentration. As a result starch molecules are incapable of pen-
etrating the cellulose molecules in the presence of low solvent concentration. This may
cause a smaller number of reacting sites at the cellulose backbone and thus continue to
reduce the active sites as water concentration decrease with higher starch concentration.
In higher soaking time, the fiber become twisted, shrinks and changes its outer fibrillar
layers. The TS, BS, and IS of the untreated jute fabrics/PP composites were found to be
48.08, 51.27 Mpa, and 17.13 kJ/m2, respectively. But all starch treated (1—10 wt%) jute-
based composites showed higher TS, BS, and IS values. Figure 2 shows TS, BS, and IS of
the starch treated composites against different soaking times (2—10 min).
From Figure 2(a), it is seen that for 5% starch treated composites, the soaking time for
TS, BS, and IS was gradually increased up to 5 min and then decreased. The maximum TS,
BS, and IS were found to be 66.15, 72.65 Mpa, and 28.19 kJ/m2, respectively, which is 38,
42, and 65% higher than that of the untreated composites. It was observed from
Figure 2(b) that for 3% starch treated composites, the TS, BS, and IS was increased up
to 5 min soaking time and after that decreased. The maximum TS, BS, and IS were found
to be 63.15, 72.16 Mpa, and 31.46 kJ/m2, respectively, which is 31, 41, and 84% higher
than that of the untreated composites. When jute fabrics were treated with starch solution,
the cause of increase of TS, BS, and IS values, may be that starch was working here as a
good stiffening agent. It is well known that starch is widely using as stiffening agent for
fabrics. As a result, stress transfer from the fibers to matrix is higher, so higher TS, BS, and
IS values found from the starch-based composites. At higher starch concentration (10%),
the jute fibers become too sticky and as a result the adhesion between the fibers and matrix
may not be so good. Probably this is the cause of low TS, BS, and IS of the10% starch
treated composites as found in the experiment. The TM and BM of the untreated

(a) 85 (b) 90
TS BS IS TS BS IS

70 74
Mechanical properties

Mechanical properties

55 58

40 42

25 26

10 10
0 2 4 6 8 10 12 0 2 4 6 8 10 12
Soaking time (min) Soaking time (min)

Figure 2. Mechanical properties of: (a) UV treated jute fabrics/PP and; (b) gamma treated jute fabrics/PP
composites against soaking time.
8 H.U. ZAMAN ET AL.

(a) (b) 1.9


TM BM TM BM
1.7
1.7

Modulus (GPa)
Modulus (GPa)
1.5
1.5

1.3
1.3

1.1 1.1

0.9 0.9
0 2 4 6 8 10 12 0 2 4 6 8 10 12
Soaking time (min) Soaking time (min)

Figure 3. Modulus of: (a) UV treated jute fabrics/PP and; (b) gamma treated jute fabrics/PP composites
against soaking time.

(a) (b)

(c)

Figure 4. SEM image of the fracture surface of the untreated (a); gamma + 3% starch (b); and UV + 5%
starch treated composites (c).

composites were found to be 0.95 and 1.12 Gpa, respectively, which are much lower than
that of treated composites. TM and BM of the starch treated (1—10 wt%) composites were
evaluated and is shown in Figure 3. It is clear that the TM and BM values were found the
highest at 5% starch composites for 5 min soaking time and the values are 1.52 and
A Comparative Study between Gamma and UV Radiation of Jute fabrics 9

1.6 Gpa, respectively. This is almost 29 and 43% increase of TM and BM over the
untreated composite. On the other hand, gamma treated jute fabrics/PP composites
were found the highest values 1.35 GPa for TM and 1.64 GPa for BM at 3% starch
composites for 5 min soaking time. This is 42% and 46% increase of TM and BM
over the untreated composite. The improvement of the modulus properties may be the
similar as explained for strength properties of the composites.

Scanning Electron Microscopic Analysis

Scanning electron microscopy (SEM) was used to study the interfacial properties of the
composites based on untreated and treated (gamma + 3% starch and UV + 5% starch)
jute fabrics/PP composites. Figure 4(a)—(c) shows the tensile fracture surfaces of the
untreated, gamma and UV treated jute fabrics/PP composites, respectively. It revealed
that the untreated fiber partly adhered to the PP matrix, demonstrating a week
fiber—matrix adhesion. On the contrary, gamma + 3% starch and UV + 5% starch trea-
ted jute fiber was completely surrounded with the PP matrix proving a better fiber—matrix
adhesion. These micrographs also revealed that the fiber—matrix adhesion of treated fiber
composite was superior after chemical (5% starch) treatments.

CONCLUSION

Jute fabrics (hessian cloth) reinforced PP-based composites (50 wt% fiber) were fabri-
cated by compression molding and the mechanical properties were evaluated. For UV
treated jute fabrics/PP composites, TS, TM, BS, BM, and IS of the composites were found
to be 59.69 MPa, 1.32 GPa, 65.37 MPa, 1.62 Gpa, and 26.14 kJ/m2, respectively. On the
other hand, for gamma treated jute fabrics/PP composites, TS, TM, BS, BM, and IS of the
composites were found to be 57.95 MPa, 1.24 GPa, 62.45 MPa, 1.58 Gpa, and 24.25 kJ/m2,
respectively. From this investigation it was found that the mechanical properties of UV
treated jute fabrics/PP composites had increased TS, TM, BS, BM, and IS compared to
that of the gamma treated jute fabrics/PP composites. SEM images of the fracture sides of
the composites were supported that gamma treated jute fabrics/PP composites had poor
fiber matrix adhesion than that of the UV treated jute fabrics/PP composites.

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