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Computational Materials Science 48 (2010) 576–581

Contents lists available at ScienceDirect

Computational Materials Science


journal homepage: www.elsevier.com/locate/commatsci

A computational and experimental investigation on thermal conductivity


of particle reinforced epoxy composites
Rajlakshmi Nayak a,*, Tarkes Dora P. b, Alok Satapathy a
a
National Institute of Technology, Rourkela 769 008, India
b
National Institute of Technology, Tiruchirappalli 620 015, India

a r t i c l e i n f o a b s t r a c t

Article history: The finite element method (FEM) is a powerful computational technique for approximate solutions to a
Received 25 December 2009 variety of ‘‘real-world” engineering problems having complex domains subjected to general boundary
Received in revised form 10 February 2010 conditions. In this paper FEM is implemented to determine the effective thermal conductivity of partic-
Accepted 16 February 2010
ulate filled polymer composites and is validated by experimentation. A commercially available finite-ele-
Available online 12 March 2010
ment package ANSYS is used to for this numerical analysis. Three-dimensional spheres-in-cube lattice
array models are constructed to simulate the microstructure of composite materials for various filler con-
Keywords:
centrations ranging from about 6 to 36 vol.%. Composites with similar filler contents are fabricated by
Polymer composite
Pine wood dust reinforcement
hand layup technique by reinforcing micro-sized pine wood dust in epoxy resin. Guarded heat flow meter
Thermal conductivity test method is used to measure the thermal conductivity of these composites using the instrument Uni-
Finite-element analysis therm™ Model 2022 as per ASTM-E1530. This study shows that the incorporation of pine wood dust
results in reduction of conductivity of epoxy resin and thereby improves its thermal insulation capability.
With addition of 6.5 vol.% of filler, the thermal conductivity of epoxy is found to decrease by about 19.8%
and with about 36 vol.% of filler addition, a 57.3% reduction in thermal conductivity of neat epoxy is
achieved. The experimentally measured conductivity values are compared with the numerically calcu-
lated ones and also with the existing theoretical and empirical models. The values obtained using
finite-element analysis (FEA) are found to be in reasonable agreement with the experimental values.
Ó 2010 Elsevier B.V. All rights reserved.

1. Introduction play an important role in improving electrical, mechanical and


thermal properties of the composites [9,10]. Currently, particle size
Hard particulate fillers consisting of ceramic or metal particles is being reduced rapidly and many studies have focused on how
and fiber fillers made of glass are being used these days to dramat- single-particle size affects mechanical properties [11–17]. The
ically improve the mechanical properties such as wear resistance, shape, size, volume fraction, and specific surface area of such
even up to three orders of magnitude [1]. Various kinds of poly- added particles have been found to affect mechanical properties
mers and polymer matrix composites reinforced with metal parti- of the composites greatly. In this regard, Yamamoto et al. [18] re-
cles have a wide range of industrial applications such as heaters, ported that the structure and shape of silica particle have signifi-
electrodes [2], composites with thermal durability at high temper- cant effects on the mechanical properties such as fatigue
ature [3], etc. These engineering composites are desired due to resistance, tensile and fracture properties. Nakamura et al. [19–
their low density, high corrosion resistance, ease of fabrication 21] discussed the effects of size and shape of silica particle on
and low cost [4–6]. Similarly, ceramic filled polymer composites the strength and fracture toughness based on particle–matrix
have been the subject of extensive research in last two decades. adhesion and also found an increase of the flexural and tensile
The inclusion of inorganic fillers into polymers for commercial strength as specific surface area of particles increased.
applications is primarily aimed at the cost reduction and stiffness Considerable work has been reported on the subject of heat
improvement [7,8]. Along with fiber-reinforced composites, the conductivity in polymers by Hansen and Ho [22], Peng and Landel
composites made with particulate fillers have been found to per- [23], Choy and Young [24], Tavman [25], etc. It is well known that
form well in many real operational conditions. When silica parti- thermal transport increases significantly in the direction of orien-
cles are added into a polymer matrix to form a composite, they tation and decreases slightly in the direction perpendicular to the
orientation. But most of these studies were confined to the thermal
behaviour of neat polymers only and not to their composites.
* Corresponding author.
Reports are available in the existing literature on experimental as
E-mail address: jhilli02@gmail.com (R. Nayak).

0927-0256/$ - see front matter Ó 2010 Elsevier B.V. All rights reserved.
doi:10.1016/j.commatsci.2010.02.025
R. Nayak et al. / Computational Materials Science 48 (2010) 576–581 577

well as numerical and analytical studies on thermal conductivity of which describe the spatial distribution of the two phases. By
some filled polymer composites [26–38]. The fillers most fre- assuming a parabolic distribution of the discontinuous phase in
quently used are aluminum particles, copper particles, brass parti- the continuous phase, Cheng and Vachon [48] obtained a solution
cles, short carbon fiber, carbon particles, graphite, aluminum to Tsao’s [47] model that did not require knowledge of additional
nitrides and magnetite particles. Progelhof et al. [26] was the first parameters. Agari and Uno [49] propose a new model for filled
to present an exhaustive overview on models and methods for pre- polymers, which takes into account parallel and series conduction
dicting the thermal conductivity of composite systems. Procter and mechanisms. According to this model, the expression that governs
Solc [39] used Nielsen model as a prediction to investigate the the thermal conductivity of the composite is:
thermal conductivity of several types of polymer composites filled
with different fillers and confirmed its applicability. Nagai and Lai
log kc ¼ ØC 2 log kf þ ð1  ØÞ logðC 1 km Þ ð3Þ
[40] found that Bruggeman model for Al2O3/epoxy system and a
modified form of Bruggeman model for AlN/epoxy system are both
good prediction theories for thermal conductivity. Griesinger et al. where C1, C2 are experimentally determined constants of order
[41] reported that thermal conductivity of low-density PE in- unity. C1 is a measure of the effect of the particles on the secondary
creased from 0.35 for an isotropic sample, to the value of 50 W/ structure of the polymer, like crystallinity and the crystal size of the
m K for a sample with an orientation ratio of 50. The thermal polymer. C2 measures the ease of the particles to form conductive
and mechanical properties of copper powder filled poly-ethylene chains. The more easily particles are gathered to form conductive
composites are found by Tavman [25] while Sofian et al. [37] inves- chains, the more thermal conductivity of the particles contributes
tigated experimentally on thermal properties such as thermal con- to change in thermal conductivity of the composite and C2 becomes
ductivity, thermal diffusivity and specific heat of metal (copper, closer to 1. Later, they modified the model to take into account the
zinc, iron, and bronze) powder filled HDPE composites in the range shape of the particles [50]. Generally, this semi-empirical model
of filler content 0–24% by volume. They observed a moderate in- seems to fit the experimental data well. However, adequate exper-
crease in thermal conductivity up to 16% of metal powder filler imental data is needed for each type of composite in order to deter-
content. Mamunya et al. [42] also reported the improvement in mine the necessary constants.
electrical and thermal conductivity of polymers filled with metal For an infinitely dilute composite of spherical particles, the ex-
powders. In a recent research Weidenfeller et al. [43] studied the act expression for the effective thermal conductivity is given as:
effect of the interconnectivity of the filler particles and its impor-
tant role in the thermal conductivity of the composites. They pre-  
k kd  kc
pared PP samples with different commercially available fillers by ¼1þ3 ð4Þ
kc kd þ 2kc
extrusion and injection molding using various volume fractions
of filler content to systematically vary density and thermal trans-
port properties of these composites. Surprisingly, they measured where k, kc and kd are thermal conductivities of composite, contin-
that the thermal conductivity of the PP has increased from 0.27 uous-phase (matrix), and dispersed-phase (filler), respectively, and
up to 2.5 W/m K with 30 vol.% talc in the PP matrix, while the same Ø is the volume fraction of the dispersed-phase. Eq. (4) is the well-
matrix material containing the same volume fraction of copper known Maxwell equation [51] for dilute composites.
particles had a thermal conductivity of only 1.25 W/m K despite An exhaustive review of the published literature reveals that
the fact that copper particles have a thermal conductivity approx- most of the investigations are aimed at enhancing the thermal con-
imately 40 times greater than that of talc particles. Tekce et al. [38] ductivity of the polymer rather than attempting to improve its
noticed the strong influence of the shape factor of fillers on thermal insulation capabilities. Although a large number of particulates
conductivity of the composite. While Kumlutas and Tavman [44] have been used as fillers in the past, there is no report available
carried out a numerical and experimental study on thermal con- on bio-based materials like any kind of wood dust being used for
ductivity of particle filled polymer composites, Amar et al. reported composite making. Investigation on thermal conductivity of partic-
the existence of a possible correlation between thermal conductiv- ulate filled fiber-reinforced composites is rare and the understand-
ity and wear resistance of particulate filled composites [45]. ing of the relationship between the effective thermal conductivity
Many theoretical and empirical models have been proposed to of a composite material and the micro-structural properties (vol-
predict the effective thermal conductivity of two-phase mixtures. ume fractions, distribution of particles, aggregation of particles,
Comprehensive review articles have discussed the applicability of properties of individual components, etc.) is far from satisfactory.
many of these models [46,26]. For a two-component composite, Besides, though it becomes clear that improved thermal conductiv-
the simplest alternatives would be with the materials arranged ity in polymers may be achieved either by molecular orientation or
in either parallel or series with respect to heat flow, which gives by the addition of conductive fillers, it is yet to be seen how the
the upper or lower bounds of effective thermal conductivity. For incorporation of bio-based particulates with poor heat conductiv-
the parallel conduction model: ity affects the overall conductivity of any polymer composite.
In view of the above, the present work is undertaken to investi-
kc ¼ ð1  ØÞkm þ Økf ð1Þ gate numerically and experimentally the thermal conductivity of
epoxy matrix composites filled with pine wood dust. The objec-
where kc, km, kf are the thermal conductivities of the composite, the
tives of this work include fabrication of a new class of low cost
matrix and the filler respectively and Ø is the volume fraction of
composites using pine wood dust as the reinforcing filler with an
filler.
objective to improve the insulating properties of epoxy resin.
For series conduction model:
Epoxy is already a known thermal barrier. Since this work aims
1 1Ø Ø at developing some kind of a light, cheap and insulating material,
¼ þ ð2Þ epoxy emerged as the first choice for the matrix material. Epoxy
kc km kf
is chosen primarily because it happens to be the most commonly
The correlations presented by Eqs. (1) and (2) are derived on the used polymer and because of its insulating nature (low value of
basis of the rules-of-mixture. Tsao [47] derived an equation relat- thermal conductivity, about 0.363 W/m K). It also reports the esti-
ing the two-phase solid mixture thermal conductivity to the con- mation of the equivalent thermal conductivity of particulate–poly-
ductivity of the individual components and to two parameters mer composite system using finite element method.
578 R. Nayak et al. / Computational Materials Science 48 (2010) 576–581

2. Experimental details sample is required. Non-solids, such as pastes or liquids, can be


tested using special containers. Thin films can also be tested accu-
2.1. Matrix material rately using a multi-layer technique. The tests are in accordance
with ASTM E-1530 Standard.
Epoxy LY 556 resin, chemically belonging to the ‘epoxide’ family
is used as the matrix material. Its common name is Bisphenol A 2.5. Operating principle of Unitherm™ 2022
Diglycidyl Ether. The low temperature curing epoxy resin (Araldite
LY 556) and corresponding hardener (HY951) are mixed in a ratio A sample of the material is held under a uniform compressive
of 10:1 by weight as recommended. The epoxy resin and the hard- load between two polished surfaces, each controlled at a different
ener are supplied by Ciba Geigy India Ltd. Epoxy is chosen primar- temperature. The lower surface is part of a calibrated heat flow
ily because it happens to be the most commonly used polymer and transducer. The heat flows from the upper surface, through the
because of its insulating nature (low value of thermal conductivity, sample, to the lower surface, establishing an axial temperature gra-
about 0.363 W/m K). dient in the stack. After reaching thermal equilibrium, the temper-
ature difference across the sample is measured along with the
2.2. Filler material (pine wood dust) output from the heat flow transducer. These values and the sample
thickness are then used to calculate the thermal conductivity. The
Pine wood dust (PWD) is generated during the cutting of pine temperature drop through the sample is measured with tempera-
tree wood. Pine trees are found in the Himalayan subtropical re- ture sensors in the highly conductive metal surface layers on either
gion and this natural resource can be gainfully converted to value side of the sample.
added products. Various types of pine trees are found in this re- By definition thermal conductivity means ‘‘The material prop-
gion; especially in HP, wide ranging tracts of Chir Pine are seen. erty that describes the rate at which heat flows with in a body
The scientific name of Chir Pine is Pinus roxburghii. Main organic for a given temperature change.” For one-dimensional heat con-
constituents of pine wood are: cellulose, glucomannan, xylan, lig- duction the formula can be given as Eq. (5).
nin and some extractives. Its dust particles appear as cream or dark T1  T2
brown fibrous powder. It is chosen as the filler material in this Q ¼ KA ð5Þ
x
work mostly for its very low thermal conductivity (0.068 W/m K)
where Q is the heat flux (W), K is the thermal conductivity (W/m K),
and low density (0.52 gm/cc). Moreover, it is renewable, eco-
A is the cross-sectional area (m2), T1  T2 is the difference in tem-
friendly, available at low cost, non-toxic and basically the wood
perature (K), x is the thickness of the sample (m). The thermal resis-
dust is considered as a waste product.
tance of a sample can be given as

2.3. Composite fabrication T1  T2


R¼ ð6Þ
Q =A
The low temperature curing epoxy resin (LY 556) and corre-
where R is the resistance of the sample between hot and cold sur-
sponding hardener (HY951) are mixed in a ratio of 10:1 by weight
faces (m2 K/W). From Eqs. (3) and (4) we can derive that
as recommended. Pine wood dust (PWD) particles (collected from
HP) are reinforced in epoxy resin (density 1.1 gm/cc) to prepare the x
K¼ ð7Þ
composites. The dough (epoxy filled with PWD) is then slowly dec- R
anted into the glass tubes, coated beforehand with wax and uni- In Unitherm™ 2022 the heat flux transducer measures the Q va-
form thin film of silicone-releasing agent. The composites are lue and the temperature difference can be obtained between the
cast by conventional hand-lay-up technique in glass tubes so as upper plate and lower plate. Thus the thermal resistance can be
to get cylindrical specimens (dia. 9 mm, length 120 mm). Compos- calculated between the upper and lower surfaces. Giving the input
ite samples of four different compositions, as listed in Table 1 are value of thickness and taking the known cross-sectional area, the
made. The mean particle size of pine wood dust used in samples thermal conductivity of the samples can be calculated using Eq. (7).
1 (6.5 vol.%), 2 (11.3 vol.%), 3 (26.8 vol.%) is 100 micron and in sam-
ple 4 (35.9 vol.%) it is 700 lm. The castings are left to cure at room 3. Numerical analysis: concept of finite element method and
temperature for about 24 h after which the tubes are broken and ANSYS
samples are released. Specimens of suitable dimension are cut
using a diamond cutter for further physical characterization and The finite element method (FEM), originally introduced by
thermal conductivity test. Turner et al. [52], is a powerful computational technique for
approximate solutions to a variety of ‘‘real-world” engineering
2.4. Experimental determination of thermal conductivity problems having complex domains subjected to general boundary
conditions. FEA has become an essential step in the design or mod-
Unitherm™ Model 2022 is used to measure thermal conductiv- eling of a physical phenomenon in various engineering disciplines.
ity of a variety of materials. These include polymers, ceramics, A physical phenomenon usually occurs in a continuum of matter
composites, glasses, rubbers, some metals, and other materials of (solid, liquid, or gas) involving several field variables. The field
low to medium thermal conductivity. Only a relatively small test variables vary from point to point, thus possessing an infinite num-
ber of solutions in the domain.
The basis of FEM relies on the decomposition of the domain into
Table 1
a finite number of sub-domains (elements) for which the system-
List of composites fabricated by hand-lay-up technique.
atic approximate solution is constructed by applying the varia-
Samples Composition tional or weighted residual methods. In effect, FEM reduces the
1 Epoxy + 6.5 vol.% (3.2 wt.%) filler problem to that of a finite number of unknowns by dividing the
2 Epoxy + 11.3 vol.% (5.7 wt.%) filler domain into elements and by expressing the unknown field vari-
3 Epoxy + 26.8 vol.% (14.8 wt.%) filler
able in terms of the assumed approximating functions within each
4 Epoxy + 35.9 vol.% (20.9 wt.%) filler
element. These functions (also called interpolation functions) are
R. Nayak et al. / Computational Materials Science 48 (2010) 576–581 579

defined in terms of the values of the field variables at specific typical three-dimensional sphere-in-cube model with a body
points, referred to as nodes. Nodes are usually located along the centered cubic (BCC) structural arrangement for the composite
element boundaries, and they connect adjacent elements. The abil- with pine wood dust concentration of 35.9 vol.% is illustrated
ity to discretize the irregular domains with finite elements makes in Fig. 2. The temperature profiles obtained from FEM analysis
the method a valuable and practical analysis tool for the solution of for the composites with particulate concentrations of 6.5, 11.3,
boundary, initial, and eigenvalue problems arising in various engi- 26.8 and 35.9 vol.% are presented in Fig. 3a–d respectively.
neering disciplines. The values of effective thermal conductivities of the particulate
The FEM is a numerical procedure that can be used to obtain filled epoxy composites with varied proportions of pine wood dust
solutions to a large class of engineering problems involving stress obtained using Maxwell’s correlation, rules-of-mixture model and
analysis, heat transfer, fluid flow etc. ANSYS is general-purpose fi- those obtained from FEM analysis are presented in Table 2. It pre-
nite-element modeling package for numerically solving a wide sents a comparison among the results obtained using these models
variety of mechanical problems that include static/dynamic, struc- with regard to the values of effective conductivity obtained
tural analysis (both linear and nonlinear), heat transfer, and fluid experimentally.
problems, as well as acoustic and electromagnetic problems. Fig. 4 presents comparative picture of the thermal conductiv-
ity values obtained from different methods. It is noticed that the
results obtained from the finite-element analysis using ANSYS
4. Results and discussion
are closer to the measured values of effective thermal conduc-
tivity for composites of different filler content. On comparison,
4.1. Numerical analysis
it is found that while the errors associated with the FEM values
with respect to the experimental ones lie in the range of 3–13%,
Using the finite-element program ANSYS, thermal analysis is
the same for results from rules-of-mixture and Maxwell’s corre-
carried out for the conductive heat transfer through the composite
lation lie in the ranges of 2–44% and 4–28% respectively. The
body. In order to make a thermal analysis, three-dimensional phys-
percentage errors associated with each method for individual
ical models with spheres-in-a-cube lattice array have been used to
composites are given as Table 3. It is further noted that while
simulate the microstructure of composite materials for four differ-
the FEM and Maxwell’s model overestimate the value of thermal
ent filler concentrations. Furthermore, the effective thermal con-
conductivity the rules-of-mixture model underestimates the
ductivities of these epoxy composites filled with pine wood dust
up to about 36% by volume is numerically determined using
ANSYS.

4.2. Description of the problem

The determination of effective properties of composite materi-


als is of paramount importance for functional design and applica-
tion of composite materials. One of the important factors that
influence the effective properties and can be controlled to an
appreciable extent is the microstructure of the composite. Here,
microstructure means the shape, size distribution, spatial distribu-
tion and orientation distribution of the reinforcing inclusion in the
matrix. Although most composite possess inclusion of random dis-
tributions, great insight of the effect of microstructure on the effec-
tive properties can be gained from the investigation of composites
Fig. 1. Boundary conditions.
with periodic structure. System with periodic structures can be
more easily analyzed because of the high degree of symmetry
embedded in the system.
In the numerical analysis of the heat conduction problem, the
temperatures at the nodes along the surfaces ABCD is prescribed
as T1 (=100 °C) and the convective heat transfer coefficient of ambi-
ent is prescribed as 2.5 W/m2 K at ambient temperature of 27 °C.
The heat flow direction and the boundary conditions are shown
in Fig. 1. The other surfaces parallel to the direction of the heat flow
are all assumed adiabatic. The temperatures at the nodes in the
interior region and on the adiabatic boundaries are unknown.
These temperatures are obtained with the help of finite-element
program package ANSYS. In the analysis of the ideal case it will
be assumed that the composites are macroscopically homoge-
neous, locally both the matrix and filler are homogeneous and iso-
tropic, the thermal contact resistance between the filler and the
matrix is negligible, the composite lamina is free of voids and the
filler are arranged in a square periodic array/uniformly distributed
in matrix.
Thermal conductivities of epoxy composites filled with pine
wood dust particles to 36% by volume are numerically esti-
mated by using the spheres-in-cube model and the numerical
results are compared with the experimental results and also Fig. 2. Three-dimensional sphere-in-cube model with particle concentration of
with some of the existing theoretical and empirical models. A 35.9 vol.%.
580 R. Nayak et al. / Computational Materials Science 48 (2010) 576–581

Fig. 3. Temperature profiles for composite with particle concentration of: (a) 6.5 vol.%, (b) 11.3 vol.%, (c) 26.8 vol.%, (d) 35.9 vol.%.

Table 2
Thermal conductivity values for composites obtained from different methods.

Sample Particulate content (vol.%) Effective thermal conductivity of the composites (W/m K)
Rule of mixture model Maxwell’s model FEM model Experimental value
1 6.5 0.2831 0.336 0.300 0.291
2 11.3 0.2436 0.317 0.315 0.273
3 26.8 0.1678 0.254 0.270 0.242
4 35.9 0.1317 0.217 0.170 0.155

value with respect to the experimental ones. It leads to a con-


clusion that for a particulate filled composite of this kind the
FEM model can very well be used for predictive purpose in
determining the effective thermal conductivity for a wide range
of particle concentration.
Fig. 5 compares the results of FEM with those found from exper-
iments. The difference between the calculated values and the mea-
sured value of conductivity for any particular composite sample
may be attributed to the fact that some of the assumptions taken
for the FEM analysis are not real. The shape of PWD is assumed
to be spherical, while in actual practice they are irregular shaped.
Although the distribution of pine wood dust in the matrix body
is assumed to be in an arranged manner, it is actually dispersed
in the resin almost randomly. It is also interesting to note that
the incorporation of PWD results in reduction of thermal conduc-
tivity of epoxy resin and there by improves its thermal insulation
capability with addition of 6.5 vol.% of PWD, the thermal conduc-
tivity drops by about 19.8% and with addition of 35.9% of PWD
Fig. 4. Comparison of thermal conductivity values obtained from different the thermal conductivity drops by about 57.3% in neat epoxy is
methods. achieved.
R. Nayak et al. / Computational Materials Science 48 (2010) 576–581 581

Table 3
Percentage errors with respected to the measured value.

Model Particulate content (vol.%) Percentage errors with respected to the measured value
Rule of mixture model (%) Maxwell’s model (%) FEM model (%)
1 6.5 2.79 13.3929 3.0000
2 11.3 12.06 13.8801 13.3333
3 26.8 44.21 4.7244 10.3704
4 35.9 17.69 28.5714 8.8235

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