COMPOSITES

SCIENCE AND
TECHNOLOGY
Composites Science and Technology 66 (2006) 2719–2725
www.elsevier.com/locate/compscitech

Thermophysical properties of natural fibre reinforced

polyester composites
Maries Idicula a, Abderrahim Boudenne b,*, L. Umadevi c, Laurent Ibos b,
Yves Candau b, Sabu Thomas d
a
Department of Chemistry, Mar Thoma College, Tiruvalla 689 103, Kerala, India
b
Centre d’Etude et de Recherche en Thermique, Environnement et Systèmes, Université Paris 12 Val de Marne, 61 Avenue du Général de Gaulle,
94010 Créteil cedex, France
c
Department of Chemistry, St.Thomas College, Kozhencherry, Kerala, India
d
School of Chemical Sciences, Mahatma Gandhi University, Priyadarshini Hills P.O., Kottayam 686 560, Kerala, India

Received 26 January 2006; received in revised form 13 March 2006; accepted 14 March 2006
Available online 5 May 2006

Abstract

Thermal conductivity, diffusivity and specific heat of polyester/natural fibre (banana/sisal) composites were investigated as function of
filler concentration and for several fibre surface treatments. The thermophysical behaviour of hybrid pineapple leaf fibre (PALF) and
glass fibre reinforced polyester composites has been also evaluated for a constant total fibre loading of 0.40 Vf by varying the ratio
of PALF and glass. The results show that chemical treatment of the fibres reduces the composite thermal contact resistance. Hybridisa-
tion of natural fibre with glass allows a significantly better heat transport ability of the composite. The thermal conductivity measured in
the direction transverse to the plane of composite plate could be well represented by a series prediction model.
 2006 Elsevier Ltd. All rights reserved.

Keywords: B. Thermal properties; A. Glass fibres; A. Polymer–matrix composites; Natural fibres

1. Introduction mechanical properties of short fibre reinforced polymer

Fibre reinforced polymer composites have many appli-
cations as a class of structural materials because of their
ease of fabrication, relatively low cost and superior
mechanical properties compared to polymer resins. These
composites are considered as replacements for metal mate-
rials where the association of metallic fibre with polymeric
matrix is attractive material for electronic packaging appli-
cations. The combination of reinforcement with high ther-
mal conductivity embedded in a resin matrix with low
thermal conductivity is desirable to dissipating the heat flux
for electronic packaging components. Studies on the
*
Corresponding author. Fax +33 1 45176551.
E-mail address: boudenne@univ-paris12.fr (A. Boudenne).
composites have shown that both fibre length distribution
and fibre orientation distribution play very important role
in determining the mechanical properties [1–4]. A number
of analytical models have been proposed to predict the
thermal conductivity of short fibre composites [5–8]. Ther-
mal conductivity is a bulk property analogous to mechan-
ical modulus. Moreover, it is well accepted that a
mathematical analogy exists between thermal conduction
and elasticity of fibre composites. Mai and Fu [9] studied
the effects of fibre length and fibre orientation angle on
the thermal conductivity of short (carbon) fibre reinforced
polymer composites. It is observed that the thermal con-
ductivity of the composite increases with mean fibre length
but decreases with mean fibre orientation angle with
respect to the measured direction. Saxena et al. [10] ana-
lyzed the variation of thermal conductivity and thermal

0266-3538/$ - see front matter  2006 Elsevier Ltd. All rights reserved.
doi:10.1016/j.compscitech.2006.03.007
2720 M. Idicula et al. / Composites Science and Technology 66 (2006) 2719–2725

Table 1
Mechanical properties of banana, sisal, pineapple leaf and glass fibre
Fibre Diameter Density Tensile strength Tensile modulus Elongation Flexural modulus Lumen size Micro fibrillar
(lm) (kg m3) (MPa) (GPa) at break ( %) (GPa) (lm) angle
Banana fibre 120 ± 5.8 1350 550 ± 6.7 20 5–6 2–5 5 11
Sisal fibre 205 ± 4.3 1450 350 ± 7 12.8 6–7 12.5–17.5 11 20
Pineapple leaf fibre 50 ± 6 1526 413 ± 8 4.2 3–4 – – 14
Glass fibre 15 ± 5.8 2540 2500 ± 8 56–72 3 – – –

diffusivity of banana-fibre reinforced polyester composites
caused by the addition of glass fibre. They observed that
the thermal conductivity of composites increased when
compared to the matrix. However, the thermal conductiv-
ity of the composites with increased percentage of glass
fibre decreases in comparison to composite of pure banana
fibre.
Composites having two or more fillers contained in the
same matrix are called hybrid composites [11,12]. The rein-
forcement of glass fibre in polyester matrix produces com-
posites with impact strength comparable to reinforced
thermoplastics [13]. Recently there is a growing interest
in hybridizing different natural fibres in order to produce
high performance composite materials. Paiva et al. [14]
used plain weave hybrid ramie-cotton fabrics as reinforce-
ment in polyester matrix and showed the high potential of
ramie fibre and weak contribution of cotton fibre as rein-
forcement in lignocellulosic fibre composites. Thomas
et al. [15] studied the mechanical properties and cure char-
acteristics of sisal and oil palm hybrid fibre reinforced nat-
ural rubber composites.
In a previous work, we have studied the static and
dynamic mechanical properties of banana/sisal hybrid fibre
as well as PALF/glass hybrid fibre reinforced polyester
composites. The mechanical properties and composition
of banana, sisal, pineapple leaf fibre (PALF) and glass
fibres are given in Tables 1 and 2, respectively. A synergis-
tic strengthening of fibres was observed in the case of
banana/sisal hybrid fibre composites, where tensile and
flexural properties showed a positive hybrid effect [16,17].
In this paper, the thermophysical properties of banana/
sisal hybrid fibre reinforced composites were studied as a
function of fibre volume fraction and fibre surface modifi-
cation. The thermal behaviour of PALF/glass hybrid fibre
composites were also evaluated for a constant total fibre
loading of 0.40 Vf by varying the ratio of PALF and glass.
The results will be like an indication for the improvement
of the process and the utilisation of natural fibre composite
materials for their low or high thermal properties. The
thermal conductivity measurement values are compared
to models based on an electrical analogy.
2. Experimental
2.1. Materials
Banana, sisal and pineapple leaf fibre were obtained from
Sheeba Fibre and Handicraft, Poovancode, Tamilnadu,
India. Glass fibre was supplied by Ceat Ltd., Hyderabad,
India. Unsaturated isopthalic polyester HSR 8131 obtained
from M/S Bakelite, Hylam, Hyderabad, India, was used as
the matrix. The important characteristics of the polyester
resin are given in Table 3. Polystyrene maleic anhydride
(PSMA), sodium hydroxide, cobalt naphthenate and methyl
ethyl ketone peroxide were of commercial grade.
2.1.1. PSMA treatment
A fixed amount of cut fibres was kept in 5% solution of
PSMA in toluene and refluxed for half an hour. The fibre
was then filtered and dried at 70 C in an oven.
2.1.2. NaOH treatment
Cut fibres were treated with 10% sodium hydroxide
solution for 1 h and then washed with very dilute acid to
remove any particles of alkali. Washing was continued till
the fibres were alkali free. The washed fibres were dried in
an oven at 70 C.
2.2. Preparation of composites
Neatly separated banana and sisal fibre, cut at an uni-
form length of 30 mm were evenly arranged in a mould
measuring 150 mm · 150 mm · 2.5 mm. Composite sheets
Table 3
Typical properties of liquid resin
Appearance A clear pale
yellow liquid

Table 2 Viscosity at 25 C (cps) Brookefield viscometer 650

Composition of banana, sisal and pineapple leaf fibre Specific gravity at 25 C 1.11

Banana Sisal Pineapple Typical properties of cured unreinforced resin (specimens cured for 24 h
at room temperature followed by post-curing for 4 h at 80 C)
Cellulose % 63–64 65 81
Hemicellulose % 19 12 – Tensile strength 33 MPa
Lignin % 5 9.9 12.7 Flexural strength 70 MPa
Moisture content % 10–11 10 13.5 Impact strength 9 kJ m2
 M. Idicula et al. / Composites Science and Technology 66 (2006) 2719–2725
were prepared by keeping the volume ratio of banana and
sisal 1:1 and impregnating the fibre with the polyester resin
to which 1 volume per cent cobalt naphthenate and 1 vol-
ume per cent methyl ethyl ketone peroxide were added. The
resin was degassed before pouring and air bubbles were
removed carefully with a roller. The closed mould was kept
under pressure for 12 h, samples were allowed to post-cure
at 30 C for 48 h and test specimens of the required size
were cut. Different volume fractions of fibre were used
for the preparation of samples. Two other composites were
prepared by using PSMA and sodium hydroxide treated
fibre, for a fixed volume fraction (0.40 Vf).
Finally, PALF and glass fibre composites were also pre-
pared as mentioned above. Several hybrid composites were
prepared by varying the relative volume fraction of PALF
and glass. The fibre loading was kept constant to 0.40 Vf
for all PALF/glass fibre composites.
3. Thermal measurements
3.1. Experimental set-up
A periodical method was used to estimate simulta-
neously thermal conductivity, diffusivity and specific heat
of polymer composite materials at room temperature
(Fig. 1). This method is based on the use of a small temper-
ature modulation in a parallelepiped-shape sample
(44 mm · 44 mm · 2.5 mm) and allows obtaining all of
these thermophysical parameters in only one measurement
with their corresponding statistical confidence bounds [18].
The composite sample is fixed between two metallic plates.
Using conductive grease ensures a good thermal exchange
between the different plates and the sample. The front side
of the first metallic plate is heated periodically using a sum
of five sinusoidal signals and the temperature is measured
with thermocouples placed inside both front and rear
Fig. 1. Thermophysical measurements set up.
2721
metallic plates [18,19]. The thermophysical parameters of
the sample are identified by comparison of the experimen-
tal and theoretical heat transfer functions [18]. The system
under study is modelled with one-dimensional quadrupoles
theory. The experimental heat transfer function H is calcu-
lated at each excitation frequency as the ratio between the
Fourier-transform temperatures of the front and rear
plates [18]. A parameter estimation technique is then
applied to estimate simultaneously both thermal conductiv-
ity (k) and diffusivity (a). The identification of the set of
thermophysical parameters is a non-linear optimisation
problem that is solved iteratively: starting with sufficiently
accurate initial guesses for the unknown parameters, we
successively refine the estimates by using the Levenberg–
Marquardt method.
3.2. Example of measurement
The measurements of composite samples were achieved
for a large frequency range (0.5 mHz < f < 32 mHz). The
choice of the excitation frequencies is largely empirical
but remains limited by the heating source, the thermal
resistance of sample and the temperature variation gener-
ated inside the sample. The thermophysical properties of
the sample can be considered as constants during the exper-
iment because the total amplitude of the temperature vari-
ation is lower than 6 C.
Fig. 2 shows an example of the identification result for a
composite sample prepared with 0.60 Vf of polyester and
0.40 Vf of banana/sisal fibre. The experimental transfer
function modulus and phase angle is calculated using ther-
mal conductivity and diffusivity identified values and com-
pared to the experimental ones. A good agreement between
theoretical and experimental heat transfer functions is
observed. A study of the sensitivity of the heat transfer
function to the identified parameters was performed in
Fig. 2. Theoretical and experimental heat transfer functions (modulus and
phase) for the composite sample prepared with 0.60 Vf of polyester and
0.40 Vf of banana/sisal fibre.
2722 M. Idicula et al. / Composites Science and Technology 66 (2006) 2719–2725
Fig. 3. Sensitivity to identified parameter of heat transfer function
modulus and phase for the composite sample prepared with 0.6 Vf of
polyester and 0.4 Vf of banana/sisal fibre.
order to determine the optimal frequency domain of excita-
tion. We show in Fig. 3 that for the low frequency range,
the heat transfer function modulus is very sensitive to the
thermal conductivity of the sample and little sensitive to
the thermal diffusivity. The heat transfer function phase
is sensitive to the thermal conductivity at low frequencies
and to the thermal diffusivity only at high frequencies.
We note that for the frequency range used during experi-
ments, the variation of the sensitivity curves are not the
same but the thermal model remains sensitive to both k
and a. Thus, we can estimate correctly these two thermo-
physical properties in the frequency range chosen.
3.3. Specific heat determination
The specific heat capacity (Cp) values of the composite
samples were determined using thermal conductivity and
diffusivity values and knowing the density q
k untreated fibre composite. The NaOH treatment removes
Cp ¼
qa
The density measurements were achieved using the square
plates samples used for thermal measurements. A Met-
tler-ToledoTM AT61 delta range balance was used to mea-
sure samples weight. The sample sizes were measured using
a caliper square.
Table 4
Thermal conductivity, thermal diffusivity, specific heat and density of banana/sisal composites
k (W m1 K1)
Polyester only 0.181 ± 0.003
Polyester + 0.20 Vf 0.153 ± 0.002
Polyester + 0.40 Vf 0.140 ± 0.002
Polyester + 0.40 Vf treated with NaOH 0.201 ± 0.003
Polyester + 0.40 Vf treated with PSMA 0.213 ± 0.002
4. Results and discussion
4.1. Effect of fibre volume fraction
In order to explain the behaviour of the effective thermal
conductivity of the composite, we need thermal conductiv-
ity values of its constituents, i.e., fibre and matrix. Accord-
ing to the literature, the effective thermal conductivity of a
composite or a blend depends upon the conductivity of the
individual components [10]. Fibre length, fibre aspect ratio,
relative modulus of the fibre and matrix, thermal expansion
mismatch are all-important variables that control the per-
formance of a composite [11,12]. The thermal conductivity
and diffusivity measurements are presented in Table 4 with
their associated uncertainties for the polyester and the
composite samples loaded with banana/sisal fibres. The
specific heat and the density measurements are also given
in the same table.
The results show that the addition of banana and sisal
fibre in the polyester matrix induces a decrease of the effec-
tive thermal conductivity of the composite: i.e., from
0.181 W m1 K1 for polyester matrix to 0.153 W m1 K1
and 0.140 W m1 K1 for 0.20 and 0.40 Vf, respectively.
Nevertheless, the specific heat and thermal diffusivity val-
ues given in Table 4 have not a significant variation. This
is mainly due to high uncertainty bounds obtained for these
two thermal parameters. However, we notice that the den-
sity of the composite decreases when the fibre volume frac-
tion increases.
4.2. Effect of fibre treatment
The results of the thermophysical and density measure-
ments of the composites prepared with chemically treated
fibres are given in Table 4 with their uncertainties. We
notice that the variation of Cp and a are not significant,
as their uncertainties remain important.
Nevertheless, the thermal conductivity of sodium
hydroxide treated fibre composite is 43% higher than the
ð1Þ practically all non-cellulose components except waxes. By
the dissolution of lignin by alkali, some pores are formed
on the fibre surface, which improves the contact area
between the fibre and the matrix. Fig. 4 shows the scanning
electron micrographs of the fracture surfaces of untreated
(a) and NaOH treated (b) fibre composites. Compared to
the fracture surface of the untreated composite, more brit-
a (m2 s1) · 107 Cp (J kg1 K1) q (kg m3)
1.08 ± 0.09 1408 ± 123 1190 ± 123
1.25 ± 0.09 1199 ± 88 1021 ± 88
1.14 ± 0.09 1246 ± 103 986 ± 103
1.37 ± 0.10 1270 ± 98 1155 ± 98
1.43 ± 0.25 1194 ± 120 1248 ± 77
 M. Idicula et al. / Composites Science and Technology 66 (2006) 2719–2725
Fig. 4. Scanning electron micrographs of the fracture surfaces of
untreated (a) and NaOH treated (b) fibre composites.
tle failure can be observed and matrix particles are found to
adhere on the surface of the NaOH treated fibre composite.
In the case of PSMA treated fibre composite, thermal
conductivity is increased by 52% compared to untreated
composite. In the case of PSMA coating, maleic anhydride
group of PSMA form hydrogen bonding with the hydroxyl
group of the fibre and the polystyrene segments present in
the PSMA improves the compatibility between the fibre
and the polyester matrix. As a result of this, the interfacial
interaction between the fibre and matrix increases. A hypo-
thetical model of interface of polyester-PSMA treated fibre
is shown in Fig. 5. The hydrophilic fibre –OH groups are
replaced by the hydrophobic moieties by the hydrogen
bonding between the PSMA and –OH groups of the fibre.
This increases the strength of the chemical interlocking of
Fig. 5. A hypothetical model of interface of polyester-PSMA treated fibre.
2723
the hydrophobic centres of the polyester resin and the
fibres. Fig. 6 shows a scanning electron micrograph of frac-
ture surface of PSMA treated fibre composite. Fibrillation
can be observed in the fracture plane due to strong fibre-
matrix adhesion. Surface coating can be seen on the fibre
due to the possible reaction between the cellulose fibre
and PSMA.
4.3. Effect of hybridisation with glass fibre
In order to show the effect of the hybridisation on ther-
mophysical properties of the polymer composites, several
samples were prepared for the same filler volume fraction
(0.40 Vf) and using different ratio between PALF and glass
fibre. For that, we took PALF fibre instead of sisal or
banana one. Indeed, banana, sisal and PALF are natural
fibres and there is not much difference in their thermophys-
ical properties.
Table 5 shows the thermophysical and density measure-
ments of PALF/glass fibre hybrid composites. We note an
increasing of thermal diffusivity and density values with the
glass fibre volume fraction. In the same way, the thermal
conductivity of polyester/glass composite is 50% more
important than the polyester/PALF one. The opposite
effect is noted for the specific heat values. In fact, the glass
fibre have a high value of thermal conductivity, diffusivity
and density compared to the PALF fibre as well as the
polyester resin. These results show that the glass fibre
allows better ability to the heat transport in the composite
and that PALF can not be completely substituted to glass
fibre in order to insure the same heat transfer.
4.4. Thermal conductivity and the first order model
Many theoretical and empirical thermal models have
been developed to predict the effective thermal conductivity
of polymer composite materials [20]. The simplest alterna-
tives would be with the materials arranged in either parallel
or series with respect to heat flow (see Fig. 7), which gives
Fig. 6. Scanning electron micrograph of fracture surface of PSMA treated
fibre composite.
2724 M. Idicula et al. / Composites Science and Technology 66 (2006) 2719–2725

Table 5
Thermal conductivity, thermal diffusivity, specific heat and density of PALF/glass fibre hybrid composites (fibre loading was fixed to 0.40 Vf)
k (W m1 K1) a (m2 s1) · 107 Cp (J kg1 K1) q (kg m3)
0.40 Vf PALF 0.184 ± 0.003 1.60 ± 0.25 979 ± 155 1175 ± 155
0.36 Vf PALF + 0.04 Vf glass fibre 0.198 ± 0.002 1.64 ± 0.20 972 ± 121 1243 ± 121
0.20 Vf PALF + 0.20 Vf glass fibre 0.216 ± 0.003 1.68 ± 0.20 925 ± 113 1390 ± 113
0.40 Vf glass fibre 0.277 ± 0.003 2.14 ± 0.24 798 ± 92 1622 ± 92

compared to the experimental data. We note that the

Fig. 7. Thermal conductivity first-order models of fibre composites.
the upper or lower bounds of effective
conductivity.
Parallel model
k sup ¼ k 1 /1 þ k 2 /2 þ    k n /n
Series model
1 / / /
¼ 1 þ 2 þ  n
k inf k1 k2 kn
where ki and /i are the thermal conductivity and volume
fraction of the ith material, respectively.
The arrangement of the fibres in our composite sam-
ples can be modeled with parallel or series model. The
thermal conductivity of PALF was calculated using Eqs.
(2) and (3), the experimental values of the polyester
matrix and the composite prepared with 0.40 Vf of PALF
and 0.60 Vf of polyester. In fact, in this case these two
experimental values are close; thus, the use of the series
or parallel model leads to the same value of the PALF
thermal conductivity: kPALF = 0.188 W m1 K1. As the
ratio between the thermal conductivity values of the
matrix and the fibres is close to 1, a first-order model
can be used to estimate the effective thermal conductivity
of the composite.
Then, the thermal conductivity of hybrid PALF/glass
fibre composites are calculated using the thermal conduc-
tivity value of the glass given in the literature
(kglass = 1.2 W m1 K1) [21] and considering that the
material is composed of three components: polyester
matrix, PALF and glass fibres. The curves corresponding
to the series and parallel models are plotted in Fig. 8 and
experimental values are in agreement with kinf (Series
model). This result is foreseeable because the thermal con-
ductivity was measured in the transverse direction to the
plane of the composite plate. So, in this case, the composite
can be seen as a stacking of several fibre layers separated by
polymeric matrix. It would be interesting in future works to
study thermophysical measurements in a parallel direction
to the plane of the sample in order to check the existence of
anisotropic thermophysical properties in this kind of
material.
Fig. 9 shows the variation of the thermal conductivity
kC as function of density qC for all composites studied.
These two parameters are normalised to the corresponding
polyester measured values (kMatrix and qMatrix). We clearly
notice a correlation between these two physical properties
for the untreated composites. So, a simple relationship
thermal between these two physical properties can be deduced
 
kC qC
1¼a 1 ð4Þ
k Matrix qMatrix
ð2Þ
The value of the a coefficient obtained from a linear regres-
sion is a = 1.254 ± 0.073, with a correlation coefficient
r = 0.993. Nevertheless, the fibre treatment with NaOH
ð3Þ and PSMA allows a higher thermal conductivity for a given
concentration and leads to an increase of the interfacial
interaction between fibre and matrix.
Fig. 8. Effect of PALF and glass fibre volume fraction on experimental
and theoretical thermal conductivity of PALF/glass hybrid fibre
composites.
 M. Idicula et al. / Composites Science and Technology 66 (2006) 2719–2725 2725

have shown that a good agreement was obtained between

thermal conductivity measurement values and series model
predictions in the case of PALF/glass fibre hybrid compos-
ites. This last appears sufficient for the effective thermal
conductivity estimation of his kind of composites.

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