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Finite element modeling of polymer curing in

natural fiber reinforced composites
ARTICLE in COMPOSITES SCIENCE AND TECHNOLOGY JUNE 2007
Impact Factor: 3.57 DOI: 10.1016/j.compscitech.2006.06.021

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COMPOSITES
SCIENCE AND
TECHNOLOGY
Composites Science and Technology 67 (2007) 16661673
www.elsevier.com/locate/compscitech

Finite element modeling of polymer curing in natural ber

reinforced composites
T. Behzad a, M. Sain
a

b,*

Department of Chemical Engineering and Applied Chemistry, University of Toronto, 200 College Street, Toronto, Ont., Canada M5S 3E5
b
Faculty of Forestry/Chemical Engineering, 33 Willcocks Street, University of Toronto, Ont., Canada M5S 3B3
Received 22 November 2005; received in revised form 16 June 2006; accepted 29 June 2006
Available online 2 October 2006

Abstract
Plant-based bers have been selected as suitable reinforcements for composites due to their good mechanical performances and environmental advantages. This paper describes the development of a simulation procedure to predict the temperature prole and the curing
behavior of the hemp ber/thermoset composite during the molding process. The governing equations for the non-linear transient heat
transfer and the resin cure kinetics were presented. A general purpose multiphysics nite element package was employed. The procedure
was applied to simulate one-dimensional and three-dimensional models. Experiments were carried out to verify the simulated results.
Experimental data shows that the simulation procedure is numerically valid and stable, and it can provide reasonably accurate predictions. The numerical simulation was performed for a three-dimensional complex geometry of an automotive part to predict the temperature distribution and the curing behavior of the composite during the molding process.
 2006 Elsevier Ltd. All rights reserved.
Keywords: Natural ber composite; B. Curing; B. Modeling; C. Finite element analysis (FEM)

1. Introduction
Natural bers such as hemp, ax, jute, wood, and several waste cellulosic products have been used as suitable
alternatives to synthetic reinforcements for composites in
many applications. These bers oer specic benets such
as low density, low pollutant emissions, biodegradability,
high specic properties, and low cost [1,2].
Many studies have been carried out to develop dierent
manufacturing processes and to study the mechanical performances of natural ber composites [37]. The successful
production of thermoset composite parts depends upon a
proper cure cycle during the molding process that leads
to uniform curing and compaction. A few reports in the literature employed numerical analysis to study curing
behavior and temperature distribution of synthetic ber
composites during autoclave, resin transfer molding
*

Corresponding author. Tel.: +1 416 946 3191; fax: +1 416 978 3834.
E-mail address: m.sain@utoronto.ca (M. Sain).

0266-3538/$ - see front matter  2006 Elsevier Ltd. All rights reserved.
doi:10.1016/j.compscitech.2006.06.021

(RTM), and other manufacturing processes. For instance,

Guo et al. [8] conducted a one-dimensional transient heat
transfer analysis during the autoclave cure cycle for thick
carbon ber/epoxy laminates using a commercial nite element (FE) software. It was found that the conventional
curing cycles should be modied to prevent temperature
overshoot. The temperature proles of a thick unidirectional glass/epoxy laminate during an autoclave vacuum
bag process were predicted by Oh and Lee [9] using
three-dimensional transient heat transfer FE analysis.
Then, the viscosity proles, degree of cure, and resin pressure distribution in the laminate were obtained from the
results of the heat transfer analysis. Joshi et al. [10] performed a transient heat transfer analysis using a general
purpose FE software and two user programs to simulate
resin cure kinetics of a thick graphite/epoxy laminate.
The results showed excellent agreement with the experimental data. The modeling and simulation of resin ow,
heat transfer, and the curing of multilayer thermoset composites during autoclave processing were investigated by

T. Behzad, M. Sain / Composites Science and Technology 67 (2007) 16661673

Blest et al. [11]. The simulation was performed with varying

composite thicknesses and conrmed the approximate
validity of the model. Liu et al. [12] developed a numerical
procedure for the simulation of temperature and cure proles for the pultrusion process. A commercial general purpose FE package was combined with a user program to
solve the convection heat transfer and the resin reaction.
A one-dimensional non-linear cure simulation model was
developed by Pantelelis et al. [13] to track the temperature
evolution in thick composites. Moreover, an optimization
algorithm was coupled to the model to design the cure
cycle. Cheung et al. [14] presented a three-dimensional
thermo-chemical cure simulation employing the Galerkin
FE method. Several numerical examples were depicted
for dierent synthetic bers and resins in at or curve
shaped parts. Park et al. [15] studied modeling for cure simulation of composite structures with an arbitrary geometry
under non-uniform autoclave temperature distribution.
No signicant work has been reported concerning the
simulation of heat transfer and cure kinetics of natural ber
thermoset polymer composites during the molding process.
Rouison et al. [16] presented only a one-dimensional model
using nite dierence (FD) method to predict the temperature distribution and cure behavior of natural ber composites in the RTM process. Most of the commercially used
nite element software are not applicable for temperature
and cure behavior simulation of thermoset composites during the molding process. In this case, either some user programs should be combined with the commercially available
software or a non-linear transient heat transfer nite element model should be coded. In the present study, a nonlinear transient heat transfer nite element model is introduced to simulate the curing behavior of natural ber thermoset polymer composites. The model is dened for one
and three-dimensional analysis using only a commercially
available multiphysics software (COMSOL 3.2) without
utilizing user written programs. It is assumed that no resin

1667

ow or thickness reduction occurs during the curing process. The temperature and degree of cure proles inside
the composite can be evaluated by solving the non-linear
anisotropic heat conduction equation including the internal
heat consumption as a result of the chemical reaction. The
internal heat consumption can be expressed in terms of the
cure rate. The minimum curing time required to completely
solidify the composite can also be predicted. Hemp ber/
acrylic composites were considered and thermo-physical
properties and the equation for the cure rate were studied.
2. Experimental
An environmentally friendly acrylic polymer was
obtained from BASF Company; Ontario, Canada. Hemp
bers were supplied by Hempline Company, Ontario, Canada. In order to prepare prepreg mats, hemp bers were
randomly oriented on a perforated screen and the acrylic
resin solution was circulated to impregnate the bers with
the solution. Vacuum ltration was applied to remove the
excess solution. After circulation of the resin solution, the
wet mat was displaced on a polyester sheet and then kept
in the oven at 50 C for 48 h to remove all the moisture
content and to complete the thickening process [17,18].
Heat compression molding experiments were conducted
to verify the validation of the simulation. A metallic block
mold with dimension of 15 15 1.2 cm3 was sprayed with
the released agent. Total of ten prepreg plies were placed
inside the mold to completely compact the composite. In
order to verify the numerical modeling, temperature proles at ve dierent points inside the composite block were
recorded through the experiment and compared with the
numerical results. Fig. 1 illustrates the schematic diagram
of the experimental set-up used to measure the temperature
evolution during the molding process. The thermocouples
were placed at dierent locations inside the composite
and connected to a data acquisition system to monitor

Fig. 1. Schematic diagram of the experimental set-up.

1668

T. Behzad, M. Sain / Composites Science and Technology 67 (2007) 16661673

the temperature versus time. The mold temperature was

kept at 175 C under the constant pressure for 25 min.
The evolution of the heat capacity with temperature for
hemp bers was measured using a dierential scanning calorimeter (DSC) in a TA instruments DSC Q 1000. The
non-cured resins heat capacity was obtained by a similar
experiment.

where k is the reaction constant and is usually assumed to

be in the Arrhenius form, A is frequency factor, Ea is the
activation energy, R is the universal gas constant, T is
the absolute temperature, and n is order of the reaction.
This expression can be written in the logarithmic form:
 
oa
Ea
ln
n ln1  a
5
ln A 
ot
RT

3. Analysis

A multilinear regression can be performed to calculate

the values of A, Ea, and n. In a previous study, the total
heat of reaction and the kinetic parameters of the resin
have been investigated [22]. The kinetic parameters of the
resin are shown in Table 1.

3.1. Governing equations

In compression molding, the reinforcement was already
saturated with the resin and the resin was uniformly distributed through the mat. Therefore, the convective heat transfer eect caused by the resin ow is negligible. Moreover, it
was assumed that the geometry, the thickness, and the resin
mass remain constant during the molding process. It was
also assumed that the curing reaction takes place after closing the mold. Moreover, the thermo-physical properties of
the resin and composite were considered to be independent
of the degree of cure. With these assumptions, the transient
non-isothermal heat transfer is governed by the following
equation in the Cartesian system [19]:






oT
o
oT
o
oT
o
oT
oQ
qc C pc

Kx
Ky
Kz


ot
ox
ox
oy
oy
oz
oz
ot
1
where qc, Cpc, and Ki (i = x, y, z) are density, specic heat,
and thermal conductivity of the material in three orthogonal directions, respectively.
The endothermic eect of the resin cure reactionrepre
oQ
sents by the internal heat consumption sink term
.
ot
Ignoring the eect of resin ow in the material,
  the term
oa
can be directly related to the rate of cure
by the folot
lowing equation:
oQ
oa
qr V r H R
ot
ot

where, qr is the density of resin, Vr is the resin volume fraction of composite, and HR is the total heat of reaction, and
a is the degree of cure.

One of the most widely accepted methods to study the

cure kinetics of a thermoset resin system is dierential scanning calorimetry (DSC) [20,21]. The reaction rate, ra, and
the degree of cure are related as follows:
oa
ra
ot

The rate of the curing reaction is often described according to the following equation:
n

To predict the curing behavior of the composite accurately, the thermo-physical properties of the composite
have to be well-known. The densities of the non-cured
and cured resin, qr, were measured 1.53 g/cm3 and 1.45
g/cm3, respectively. The density of the hemp ber, qf, was
assumed to be 1.48 g/cm3. The density of the composite,
qc, was calculated using the rule of mixture as follows:
qc tf qf 1  tf qr

where tf is the volume fraction of ber.

The variations of the bers heat capacity, Cpf, could be
tted quite well by a polynomial of the second order as follow in J/g K [22]:
C pf 2  105 T 2  0:0008T 1:0812

where T is the absolute temperature.

The heat capacity of the non-cured resin increased linearly with temperature in the range of 35190 C [22]. These
variations could not be neglected in the model and the following linear relationship was used as the resins heat
capacity, Cpr, in J/g K:
C pr 0:0149T 0:459

To predict the temperature variations in the composite

during the molding process, the heat capacity of the composite materials is required. Therefore, the heat capacity
of the composite, Cpc, was evaluated using the rule of mixture as follows:
C pc T C pf T  tf C pr T  1  tf

3.2. Cure kinetics

ra k1  a AeEa =RT 1  a

3.3. Thermo-physical properties

where tf is the volume fraction of the ber.

The transverse conductivity of the composite, Kt, (zdirection in Fig. 1) was calculated based on the thermalelectrical analogy technique for elliptical laments and a
Table 1
Resin kinetic parameters used in modeling
Total heat
of reaction
(J/kg)

Frequency
factor (1/s)

Activation
energy
(J/mol)

Order of
reaction

491,000

18,033

46,700

1.4

T. Behzad, M. Sain / Composites Science and Technology 67 (2007) 16661673

where
Km is the thermal conductivity of matrix, c
p
pl=tf =2, d = l(1/b  1), and b = Kf/Km. Where l is the
geometry ratio of the ller (l = a/b), where a and b are
the axial lengths of the ellipse along the x-axis and y-axis,
respectively, tf is ber volume fraction of the composite,
and Kf is the conductivity of ber. When l = 1 (i.e.,
a = b), the present model can be simplied as the cylindrical laments in a square packing array unit cell model.
The in-plane longitudinal conductivity of the composite,
Kl (x- and y-directions in Fig. 1) was experimentally measured at dierent volume fractions of ber. Experimental
procedure and results were reported in detail elsewhere
[24]. The longitudinal thermal conductivity of the composite versus the volume fraction of bers can be expressed by
the following linear relationship:
K l 0:724tf 0:4033

11

where tf is the volume fraction of ber.

3.4. Finite element modeling of heat transfer
The temperature distribution in the composite during
the curing process can be obtained using a non-linear transient heat transfer analysis including the internal heat consumption (Eq. (1)). The model is dened based on nite
element method (FEM) using only a commercially available software with multiphysics environment (COMSOL
3.2) and without adding any user written programs. First,
the transient heat transfer model is dened in the heat
transfer module of the software to obtain the temperature.
Then, a general form equation is considered separately in
the partial dierential equation (PDE) module to evaluate
the cure kinetics and degree of cure reached in each element. The above mentioned governing equations can be
solved considering the initial and boundary conditions.
At t = 0, T = T0 and a = a0 (a0 = 0), where T0 and a0 are
the initial temperature and degree of cure of the material,
respectively. For the heat transfer model, the temperature
of boundaries is set to the temperature of mold. The Neumann boundary conditions are considered for the kinetic
model. The rule of mixture is used to calculate the density
and heat capacity of the composite (Eqs. (6) and (9)). The
thermal conductivity of the composite at dierent directions is obtained using dierent models (Eqs. (10) and (11)).
The energy and kinetic equations are coupled where the
rate of cure reaction is a function of temperature which
leads to a non-linear system. The rates of internal heat sink
are calculated from the rates of cure at each time step for
all the nodal elements. These are then applied as heat sinks
at the respective nodal points for the nite element transient heat transfer analysis in the next time step. The execu-

tion of the nite element analysis is repeated until the

completion of the cure cycle.
4. Results and discussion
4.1. One-dimensional cure modeling
The one-dimensional cure modeling of the composite
was carried out considering the transient heat transfer analysis combined with cure kinetics. The eect of number of
elements and time steps on the temperature distribution of
the composite was investigated. Little variation with respect
to the mesh density and time step conrmed the stability
and convergence of the procedure. It means that the results
are not sensitive to either the mesh density or time step.
To validate the present procedure (FEM) it was compared to the one-dimensional result obtained from nite
dierence method (FDM). For the nite dierence method,
a code in MATLAB was developed to simulate the heat
transfer and cure kinetic for a one-dimensional model.
The code employed a nite dierence solution technique
to predict the temperature and degree of cure proles for
thin at composites. Detail descriptions of the FDM procedure and results were published elsewhere [22]. A onedimensional model with 1.2 cm thickness with the same
number of elements for both procedures was considered.
A time step of 1 s was selected to achieve the desired accuracy. The temperature results for the central point of the
composite by FDM and the present procedure (FEM) were
compared; see Fig. 2. A very good agreement was observed
during the rst and the last part of the curing cycle. A few
degree discrepancies in the intermediate stage of the curing
cycle can be observed.
The degree of cure at the center of the composite versus
time is presented in Fig. 3. The FDM technique predicts
the degree of cure with slower rate compared to FEM
which can be due to dierences in the estimated temperatures. In FDM, the CrankNicholson technique was
applied followed by a dichotomy method to obtain the

180
160
Temperature (C)

square packing array unit cell model (ES model) [23]. It

can be expressed as follows:

p
p d d 2  c2 
Kt


2
10
1  1=c p=2d  c=d d  c2 ln 



Km
c

1669

140
120
100
80

FDM
FEM

60
40
20
0
0

100

200

300

400

500

600

Time (second)

Fig. 2. Temperature proles at the center of the composite versus time

obtained by dierent numerical methods.

1670

T. Behzad, M. Sain / Composites Science and Technology 67 (2007) 16661673

180

Temperature (C)

Degree of cure

160
0.8
0.6

FDM
FEM

0.4
0.2
0
0

100

200

300

400

500

600

140
120
100
80
40
20

Time (second)

0
0

Fig. 3. Degree of cure proles at the center of the composite versus time
obtained by dierent numerical methods.

temperature and degree of cure at each time step. Whereas,

in FEM, the NewtonRaphson method was employed
which results in a dierent temperature and degree of cure
at each time step due to dierent numerical errors.
4.2. Three-dimensional cure modeling for a block
In three-dimensional heat transfer analysis, due to
anisotropic nature of the material, it is necessary to provide
thermal conductivity of the material in three orthogonal
directions. For the three-dimensional analysis, a simple
block (15 15 1.2 cm3) was used which composed of
600 solid elements and the time step was selected to be
10 s. The temperature of all outer surfaces was set to the
mold temperature. Fig. 4 represents the meshed nite element model for the analysis.
The model was simulated in both 1D and 3D heat transfer models. Fig. 5 compares one-dimensional and threedimensional temperature simulations at the center of the
block. It shows that there is good agreement between 1D
and 3D temperature proles from heat transfer models.
This result indicates that for the center of block, a 1D heat
transfer model can precisely predict the temperature prole. As one moves from the center to corner of the block,
discrepancies between the temperature obtained in 1D

1D
3D

60

200

400

600

800

1000

Time (second)
Fig. 5. Temperature proles at the center of the composite in 1D and 3D
model.

and 3D heat transfer model will arise due to boundary conditions. Fig. 6 shows the temperature evolution versus time
at the center and corner of the block using the 3D heat
transfer model. As it can be seen, the simple 1D heat transfer model is not applicable and 3D model has to be considered to predict the results accurately.
In order to verify the three-dimensional modeling, the
temperature proles at ve points inside a block of composite with 15 15 1.2 cm3 dimensions were measured
experimentally and compared with the numerical results.
Fig. 7 shows the temperature proles at two dierent locations; center and corner of the block obtained by the simulation and experiment. The predicted temperature
proles were in good agreement with the experimental
results. There are a few degree discrepancies which can
be due to the assumptions considered for the modeling
such as constant thickness, constant density, and ignoring
the eect of degree of cure on heat capacity and thermal
conductivity. In addition, the thermocouples could be displaced from their initial location during the experiment in
compression molding.

200

Temperature (C)

180
160
140
120
100
80

Corner
Center

60
40
20
0
0

200

400

600

800

1000

Time (Second)
Fig. 4. Finite element model of a block of the composite (all units are in
meters).

Fig. 6. Temperature proles at the center and corner of the composite in

3D model.

T. Behzad, M. Sain / Composites Science and Technology 67 (2007) 16661673

Temperature (C)

200
180
160
140
120
100
80
60
40
20
0

1671

Experiment
Model

200

400

600

800

1000

Time (second)

Temperature (C)

200
180
160
140
120
100
80
60
40
20
0

Fig. 8. Finite element mesh for a segment of an automotive mirror case

(all units are in meters).

Experiment
Model

200

400

600

800

1000

Time (second)
Fig. 7. Comparison of experimental and predicted temperature proles of
the hemp ber acrylic composites at two dierent locations (a) center and
(b) corner.

4.3. Three-dimensional cure modeling for an automotive

mirror case
To demonstrate the ability of the three-dimensional
model, the numerical simulation was performed for a complex three-dimensional geometry of an automobile part to
predict the temperature distribution and cure behavior of
the composite during the molding process. A transient heat
transfer three-dimensional simulation was conducted for a
real automotive mirror case geometry. The mold temperature was selected to be 185 C. Due to the symmetry of the
part, to save the computation time only a segment of the
corner of the structure was considered. The thickness of
the part is dierent at the corner, edge, and top sections
of the model. The governing equation is solved subjected
to the mold-wall temperature conditions and the isothermal condition on symmetry boundaries:
T T m on mold surfaces
oT
0 on symmetry surfaces
k
on

12
13

Fig. 8 shows the nite element model of the geometry at

dierent views. The numerical model was performed at different number of tetrahedral meshes (7296, 11,269, 15,112)
and time steps (100, 50, 10). Although there was no signicant dierence in temperature proles, but applying 15,112

Fig. 9. Temperature distributions (C) at dierent curing times in various

slides of the structure: (a) curing time = 50 s and (b) curing time = 500 s
(units of axis are in meters).

elements and 10 s for time step, the model shows more stable and smoother proles. Figs. 9 and 10 show the temperature distribution and degree of cure of the structure at
dierent slides inside the composite after 50 and 500 s.

1672

T. Behzad, M. Sain / Composites Science and Technology 67 (2007) 16661673

an automotive mirror case. The temperature and degree

of cure proles were predicted for the structure. The cure
behavior of a structure with dierent geometries, curvatures, and thicknesses can be simulated using the multiphysics software.
Acknowledgments
The authors would like to thank Network of Centre of
Excellence-Auto 21 Canada for their nancial support.
References

Fig. 10. Degree of cure distributions at dierent curing times in various

slides of the structure: (a) curing time = 50 s and (b) curing time = 500 s
(units of axis are in meters).

As it can be seen, corners are the last sections which

reach to the nal temperature of curing due to their greater
thickness. Consequently, the corners are the last areas to
completely solidied and cured. From the simulation
results it can be estimated that the molding time to achieve
100% cure for the entire structure is approximately 500 s.
Hence, the simulation model is capable to display the cure
behavior of any complex geometry.
5. Conclusion
A non-linear transient heat transfer analysis combined
with a cure kinetic model based on nite element procedures was developed. In order to accurately predict the
result, the thermo-physical properties of the composite
were investigated. The temperature and degree of cure
distribution for hemp ber/acrylic composites during
the molding process were developed for a one-dimensional model and compared with previous results from
a nite dierence method. A three-dimensional model
was developed for a simple block of the composite and
compared with experimental results. Experimental data
shows that the simulation procedure is numerically valid
and stable, and provides reasonably accurate predictions.
To demonstrate the simulation model for a complex
geometry, the model was carried out for a segment of

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