International Journal of Heat and Mass Transfer 102 (2016) 713–722

Contents lists available at ScienceDirect

International Journal of Heat and Mass Transfer

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

Effects of thermal contact resistance on the thermal conductivity

of core–shell nanoparticle polymer composites
Ich-Long Ngo, S.V. Prabhakar Vattikuti, Chan Byon ⇑
School of Mechanical Engineering, Yeungnam University, Gyeongsan 712-749, South Korea

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

Article history: This paper describes a numerical study on the thermal conductivity (TC) of core–shell nanoparticle poly-
Received 2 February 2016 mer composites under the effects of thermal contact resistance (TCR), in addition to other parameters.
Received in revised form 10 June 2016 Finite element method is used for both numerical simulation and solving the related nonlinear equations.
Accepted 20 June 2016
Consequently, the effective thermal conductivity (ETC) depends significantly on the TCR, and it decreases
Available online 7 July 2016
sharply for larger volume fractions (VF) and larger TC of core–shell. The ETC from the present study
matches well with that obtained by Felske model only if the TCR is negligible. Core VF of 0.516 times
Keywords:
greater than that of shell is a necessary condition for an existence of the maximum ETC regardless of
Core–shell nanoparticles
Finite element method
the presence of the TCR. In addition, the ETC is independent on the TCR at core–shell interface when
Polymer composites either the TCR at shell-matrix interface is large or the TC of shell approaches a critical value. Many other
Thermal conductivity good guidance are provided for enhancing the TC of core–shell nanoparticle polymer composites, and it
Thermal contact resistance plays an important role in producing advanced polymer composites.
Ó 2016 Elsevier Ltd. All rights reserved.

1. Introduction only one or some of composites, and it depends on the character-

Enhancing the thermal conductivity (TC, hereafter) of polymers
by adding organic or inorganic micro-/nanoparticles with higher
TC is becoming increasingly important in producing advanced
polymer composites. Potential applications of such composites
include electronic packaging and encapsulations, satellite devices,
and areas where good heat dissipation, low thermal expansion,
and light weight are required [1,2]. The TC of polymers is known
to be commonly very low, and it has traditionally been enhanced
by adding fillers (dispersed phase) such as graphite, carbon black,
carbon fibers, and ceramic or metal particles with high TC, into
matrix materials (continuous phase). It is evident that polymer
composites containing highly conductive fillers have advantages
due to their easy processability, low cost, and durability against
corrosion. More reasons for the use of fillers can be found in [3].
In order to predict the TC of particle-filled composite materials,
a variety of theoretical and empirical models have been provided
for a number of years [4]. For example, Maxwell model [5], Lewis
and Nielsen model [6,7], Agari and Uno model [8], or Bruggeman
model [9] are some well-known models which have been widely
used in literature. However, each TC model shows to be valid for
⇑ Corresponding author. Fax: +82 53 810 4627.
E-mail address: cbyon@ynu.ac.kr (C. Byon).
istic quantities, for example the volume fraction (VF) of filler, the
TC ratio between filler and the matrix, the filler shape and orienta-
tion. Tavman [10] indicated that the Agari and Uno model effec-
tively estimates the TC of aluminum powder-filled high-density
polyethylene composites at high filler content. He et al. [11]
reported that both the effective medium theory (EMT) and Nielsen
models can predict well the TC at a low filler VF. Most of these
models were considered to predict the TC of composites containing
a single filler (also called mono-particle filler) [12], thus other
types of filler should be considered extensively for enhancing the
TC of polymers.
Indeed, the TC of polymers can be enhanced using various types
of filler such as mono-particle filler, two or more components in
combination. For example, single fillers are being used, and the
TC of such polymer composites can be predicted using theoretical
and empirical models mentioned above. The synergic effect of
hybrid filler (two particles with the same or different properties
and sizes) in improving the TC was also investigated in [13–16].
Furthermore, Gao and Zhao [17] considered the effects of nano-
fillers on the TC of epoxy, and suggesting that the TC can be effec-
tively improved using different fillers, single fillers, hybrid fillers,
and particularly the combination of three fillers. The TC of compos-
ite was shown to not only depend on filler properties, but it also
depends on other effects like the formation of conductive chains
and heat transfer networks.

http://dx.doi.org/10.1016/j.ijheatmasstransfer.2016.06.064
0017-9310/Ó 2016 Elsevier Ltd. All rights reserved.
714 I.-L. Ngo et al. / International Journal of Heat and Mass Transfer 102 (2016) 713–722

Recently, a new type of filler, core–shell nanoparticle has been the nanoparticles are isolated, thus total VF of core–shell consid-
regarded as a promising candidate for enhancing the TC of polymer ered is less than about 0.52 and 0.74 for single core–shell and
composites. Zhou et al. [18] indicated that the TC was remarkably face-centered cubic (FCC) arrangement shown in Fig. 2, respec-
improved by adding core–shell Ag/SiO2 nanoparticles into poly- tively. In addition, the TCs are assumed to be constant for all core
imide matrix. Kim et al. [19] reported the significant enhancement nanoparticles (kc), shell layer (ks), and the matrix materials (km).
of the TC using FeCr metal core–aluminum oxide shell particles The thermal flow through a composite structure is considered
with a highly mesoporous shell layer compared to the use of to be homogeneous with no heat source. Laplace equations can
uni-modal particles. In addition, Thiele et al. [20] investigated be therefore used to describe the heat transfer, which are given
numerically and discussed about some effects of specific parame- by
ters, the VF and TC of core and shell on the TC of composites con-



@ @T i @ @T i @ @T i
taining spherical core–shell capsules. More recently, Ngo and Byon þ þ ¼ 0 i ¼ c; s; m ð1Þ
@x @x @y @y @z @z
[21] have performed an extensive study on the TC of core–shell
nanoparticle polymer composites, and provided optimum condi- The subscripts ‘‘c”, ‘‘s” and ‘‘m” denote for the spherical-core
tions for enhancing and achieving the maximum TC. While these nanoparticle, shell layer and matrix material, respectively. The fol-
studies have examined the effectiveness of core–shell particles to lowing non-dimensional variables are introduced:
the TC, very limited number of them considers the effects of
x y z T i  T cw
thermal contact resistance (TCR) on the TC of such polymer com- x ¼ ; y ¼ ; z ¼ ; T i ¼ ð2Þ
posites. These effects were demonstrated to play an importance L L L T hw  T cw
role in the TC enhancement of advanced polymer composites used where the characteristic length in this problem is L, the dimension
in potential applications [22–25]. of a unit cell, as shown in Fig. 1. Consequently, Eq. (1) can be rewrit-
The purpose of this study is to describe and examine the effec- ten in non-dimensional form as:
tive thermal conductivity (ETC) of core–shell nanoparticle polymer



@ @T i @ @T i @ @T i
composites under the effects of the TCR, in addition to other þ þ ¼ 0 i ¼ c; s; m ð3Þ
parameters, the TC ratios between spherical core nanoparticles, @x @x @y @y @z @z
shell layer and the matrix material, and the VFs of core and shell. The boundary conditions are also shown in Fig. 1. All side walls
A numerical method is used for both simulating the thermal flow are considered as adiabatic walls, and isothermal conditions are
through such composite structure and solving a nonlinear Ordinary applied at the top and bottom walls. As a result, the temperature
Differential Equation (ODE) originated from Felske model. The difference between the inlet (top) and outlet (bottom) is control-
thermal behaviors of core–shell nanoparticle polymer composites lable and the thermal flow mainly moves along z direction. The
under the effects of TCR at shell-matrix and core–shell interfaces effect of the TCR is considered extensively in the present study.
are discussed in detail. The contact interface between the particles and the matrix is mod-
eled as a thin-virtual shell with uniform thickness dint and TC kint
2. Numerical method [22]. In simulation, the following boundary conditions are imposed
at the interface between two different materials:
8  
2.1. Mathematical formula < na :rT a ¼  T b T a
R c
ð4Þ
Fig. 1 shows a numerical model as well as boundary conditions. : n :ðjrT  Þ ¼  T a T 
b
b b R c
In this figure, a unit cell can be utilized as a control volume since
the number of spherical-core–shell nanoparticles dispersed In Eq. (4) above, the TCR (Rc) is defined in a non-dimensional
throughout the matrix material is very large. It is assumed that form:

km dint
Rc ¼ Rc ¼  ð5Þ
L kint
where kint is considered as the harmonic mean TCs of two materials.
According to this definition, the TC of the interface is slightly higher
than that of a material with lower TC, which is in good agreement
with the assumptions by Tsekmes et al. [26]. In addition, the inter-
face thickness is normalized by the characteristic length of the unit
cell. Consequently, the non-dimensional forms of dint and kint shown
in Eq. (5) are represented by Eq. (6). Notably, there are two

Fig. 2. Unit cells used for simulation. (a) Single core–shell filler, and (b) Face-
Fig. 1. Numerical model and boundary conditions. centered cubic (FCC) arrangement of core–shell filler.
 I.-L. Ngo et al. / International Journal of Heat and Mass Transfer 102 (2016) 713–722 715

interfaces, one is between shell layer and the matrix (denoted by a  dint  kint;s-m 2js  kint;c-s 2jc js
dint ¼ ; kint;s-m ¼ ¼ ; kint;c-s ¼ ¼
subscript ‘‘s-m”), and another is between core nanoparticle and L km js þ 1 km jc þ js
shell layer (denoted by a subscript ‘‘c-s”). ð6Þ

3.0 Other important parameters that must be considered, are TC

ratios between a spherical core nanoparticle, shell layer and matrix
material jc, js, the core VF /c, and the shell VF /s. These parame-
2.5
ters are defined as follows:

kc ks Vc Vs
2.0 jc ¼ ; js ¼ ; /c ¼ ; and /s ¼ ð7Þ
km km V cell V cell
where V is denoted for the spatial volume. Based on the thermal
keff / km

1.5
present work, FCC flow field, the ETC is determined by the following equation:
present work, single core-shell
1.0 Q
Thiele et al. (2014) keff ¼  ð8Þ
Lichtnecker (1926), Eq. (10) LðT hw  T cw Þ
0.5 Brailsford & Major (1964), Eq. (11)
Felske (2004), Eq. (13) where Q is the overall heat flux obtained by integrating the heat
fluxes across the outlet face of the unit cell. It should be noted that
0.0 the heat fluxes across the inlet face or outlet face are constant, since
this is a steady-state thermal conduction problem. Eq. (8) can be
0 20 40 60 80 100 rewritten by:
κc Z Z 
 keff 0:5 0:5
@T    
keff ¼ ¼ 
dx dy ð9Þ
Fig. 3. Comparing the ETC from present simulation with that obtained from km 0:5 0:5 @z z ¼0:5
literature [20,28–30], js = 3, /s = 0.145, and /c = 0.2.

Fig. 4. ETC as a function of TCR at shell-matrix interface for various VFs of core–shell nanoparticles, js = 100jc = 500.
716 I.-L. Ngo et al. / International Journal of Heat and Mass Transfer 102 (2016) 713–722

2.2. Literature review and model validation non-linear variation of the ETC in terms of specific parameters.
However, it may contain the interesting phenomena and
Several existing models for predicting the TC of core–shell poly- particular-thermal behaviors underlying [21].
mer composites are collected here. Woodside and Messmer [27]
 ð2  2/c  2/s Þw þ b2 hN
applied the Lichtenecker model [28] to predict the ETC of three- keff ¼ ð12Þ
component composites, as shown in Eq. (10). This model is
ð2 þ /c þ /s Þw þ b2 hD
well-known as a geometric mean model. Brailsford and Major 8  
>
> /s jc 2/s
[29] developed another model for predicting the ETC of three- > w ¼ 3 þ /c js þ /c
>
>
>  
component composites based on two-component model for homo- >
>
>
> hN ¼ ð2  2/c  2/s Þ 3 þ 2 //cs þ //cs jjcs
geneous particles randomly distributed in the matrix material. This >
>
>
>
model is given by Eq. (11). Notably, both Eqs. (10) and (11) are >
> h  i
>
> þð1 þ 2/c þ 2/s Þ 3 þ /s jc þ 2/s js
expressed in non-dimensional form for more convenience in < /c /c
comparison. where  
>
>
>
> hD ¼ ð2 þ /c þ /s Þ 3 þ 2 //cs þ //cs jjcs
keff ¼ j/c c j/s s

ð10Þ >
>
>
> h  i
>
>
>
> þð1  /c  /s Þ 3 þ //cs jc þ 2/ s
j
3j c 3js >
> / c
s
1  /c  /s þ /c 2þ jc þ /s 2þjs
>
> qffiffiffiffiffiffiffiffiffiffiffiffiffiffi

keff ¼ ð11Þ >
>
1  /c  /s þ /c 2þ3jc þ /s 2þ3js : b ¼ 1 rs ; R ¼ Rc km ; Rc ¼ 1 ; r  ¼ 3 3ð/c þ/s Þ
2 R jsc c L hc s 4p

Particularly, another well-known model are Felske model [30],
which has been widely used in literature for predicting the ETC
of core–shell composites. The self-consistent field approximation
method was used to gain this model. By careful transformation,
the Felske’s model can be represented in non-dimensional form,
as shown in Eq. (12). It can be found from this equation that the
Felske model is very cumbersome and complicated with the
In Eq. (12), the b2 is as a function of TCR (Rc) that is a reciprocal
of thermal contact conductance (hc). When the TCR between shell
layer and continuous matrix material is negligible, Rc = 0, then b2
approaches infinity, hence Eq. (12) reduces to a more simple equa-
tion shown in Eq. (13). This equation has been used to predict the
maximum ETC of core–shell nanoparticle polymer composites
accurately and effectively, as discussed in [21].

Fig. 5. Isothermal lines on yz-plane in terms of TCR at shell-matrix interface for various core VFs, js = 100jc = 500 and /s = /c.
 I.-L. Ngo et al. / International Journal of Heat and Mass Transfer 102 (2016) 713–722
  h  i
hN ð2  2/c  2/s Þ 3 þ 2 /c þ /c js þ ð1 þ 2/c þ 2/s Þ 3 þ /c jc þ /c js
/s /s j c /s 2/s

keff ¼ ¼   h  i
hD ð2 þ /c þ /s Þ 3 þ 2 //cs þ //cs jjcs þ ð1  /c  /s Þ 3 þ //cs jc þ 2/ s
js
/c
ð13Þ
Two configurations of core–shell polymer composite are
examined to be single core–shell filler with only one core–shell
nanoparticle and FCC arrangement with 14 ones, as shown in
Fig. 2. The aim is to either consider the configuration effects of
core–shell fillers distributed in the matrix or study extensively
from previous ones, particularly a study of Thiele et al. [20]. The
computational code mentioned above has been thoroughly
validated by comparing the present results with those from
Eqs. (10), (11) and (13), and Thiele’s study, as shown in Fig. 3. It
was found that the present results match very well with those
obtained by Thiele et al. [20] and Felske model [30] for both config-
urations mentioned. However, comparing to single core–shell
filler, the ETC for FCC arrangement is shown to be more close to
that obtained from Thiele’s study and Felske model. Furthermore,
FCC arrangement of core–shell filler was demonstrated to be
suitable for this thermal problem [20]. Therefore, this packing
arrangement is used for further computations in the present study.
Grid model should be considered to ensure that the final results
are independent on the number of grid elements. Indeed, the test-
ing results for the ETC of core–shell nanoparticle composites are
Fig. 6. ETC as a function of TCR at shell-matrix interface for various TC ratios of core–shell particles. /s = 0.5/c = 0.1 used for all cases.
717
shown to be independent on the number of grid elements since
it is a pure conduction problem in a solid structure. This is in line
with the results obtained in previous studies [13,22]. The relative
error is less than 0.1% compared to the finer grid model in COMSOL.
Consequently, a grid model with more than 17  104 elements was
used, which depends on the VF of core and shell fillers.
3. Results and discussions
3.1. Effects of TCR at shell-matrix interface
Interfacial properties, particularly the TCR, play an important
act on heat transfer characteristics of polymer composites
[22–24]. The TCR is due to the roughness of contact surfaces
between the particles and the surrounding medium, or between
different phases, resulting from fabrication process in general. In
this section, the TCR is assumed to exist only at shell-matrix inter-
face while the TCR at core–shell interface is set to zero. This
assumption was also discussed by Felske [30] and Lee et al. [31].
Fig. 4 shows the variation of the ETC (k⁄eff) with respect to the
TCR for various VFs of core and shell. Core VF is kept constant
through all parts of Fig. 4 while the shell VF is set for three particular
cases, /s < /c (Fig. 4a), /s = /c (Fig. 4b), and /s > /c (Fig. 4c). Notably,
the TCR (R⁄c ) in this section specified at the shell-matrix interface, is
718 I.-L. Ngo et al. / International Journal of Heat and Mass Transfer 102 (2016) 713–722

Fig. 7. Isothermal lines on yz-plane in terms of TCR at shell-matrix interface for various core TC ratios, js = 0.5jc and /s = 0.5/c = 0.1.

Table 1
Comparing the ETC from present simulation with that obtained from Felske model for various TCRs at two specific cases.

/c = /s = 0.2; jc = 0.01js = 5 /c = 2/s = 0.2; jc = 0.5js = 103

R⁄c k⁄eff (Felske) k⁄eff (present) Relative error (%) k⁄eff (Felske) k⁄eff (present) Relative error (%)
103 2.93096 2.93368 0.09 2.26837 2.25643 0.53
0.01 2.75803 2.66454 3.39 2.15911 2.09031 3.19
0.05 2.21561 1.95665 11.69 1.80816 1.63327 9.67
0.07 2.03164 1.75307 13.71 1.68621 1.49671 11.24
0.10 1.81942 1.53636 15.56 1.54363 1.34895 12.61
0.15 1.57189 1.30489 16.99 1.37469 1.18848 13.55
0.20 1.40256 1.15815 17.43 1.25746 1.08537 13.69
0.25 1.27943 1.05675 17.4 1.17135 1.01351 13.48
0.3 1.18587 0.98249 17.15 1.10542 0.96056 13.10
0.4 1.05308 0.88096 16.34 1.01112 0.88776 12.20
0.5 0.96337 0.8148 15.42 0.9469 0.84006 11.28
0.7 0.84987 0.73375 13.66 0.86508 0.78135 9.68
1 0.75586 0.66875 11.52 0.79682 0.73405 7.88

R⁄c,s-m used in Section 3.2. As shown in all parts of Fig. 4, the ETC
depends significantly on the TCR, it decreases with the increase of
TCR, and it decreases sharply for larger VFs of core–shell. This is also
illustrated in Fig. 5 for all values of core–shell VF. It is due to the fact
that the core–shell nanoparticle acts as an obstacle to the thermal
flow under the effects of TCR, then the larger core–shell VF means
the obstacle size is larger, resulting in larger thermal resistance,
hence the ETC is reduced. This thermal behavior is similar to that
in a single-filler composite structure with the presence of TCR [22].
Fig. 4 also indicates that the ETC increases with increasing VF
when the TCR is low and less than a critical value, but this trend
changes for the larger TCR. This behavior is also illustrated in
 I.-L. Ngo et al. / International Journal of Heat and Mass Transfer 102 (2016) 713–722 719

Fig. 8. Deviation between the ETC from the present simulation and that obtained from Felske model. (a) jc = 0.01js = 5; (b) /c = 2/s = 0.2.

Fig. 5 for very small TCR (R⁄c = 109) and large one (R⁄c = 1). The crit- example R⁄c = 0.2 shown in Table 1; and then it gradually decreases
ical value increase for larger shell VFs, R⁄c  0.26 (/c = 2/s in with increasing the TCR. This behavior is also explicitly seen in
Fig. 4a), R⁄c  0.3 (/c = /s in Fig. 4b), and R⁄c  0.35 (/c = 0.5/s in Fig. 8 for various VFs and TC ratios of core and shell. This figure also
Fig. 4c). It implies that the TC of composite cannot be enhanced indicates that the relative error increases with the increase of both
regardless of VFs of core–shell and their TC ratios. This effect of VF and TC ratio of core–shell nanoparticle in general. This deviation
TCR should be considered and prevented during synthesizing the may arises from two methods for predicting the ETC, finite element
core–shell nanoparticle composites. method in present work and self-consistent approximation by
The effects of TCR is also examined for variation of TC ratios Felske [30]. Based on an extensive parametric study, it is concluded
while keeping the VFs constant, as shown in Figs. 6 and 7. The TC that the maximum relative error is less than 10% when /c, /s 6 0.1
ratios of core-matrix are kept constant through all parts of Fig. 6 and jc, js 6 108 which cover the entire range typically found in
while that of shell-matrix are set for three particular cases, jc = practical applications [22]. In addition, it is less than 18% when
10js (Fig. 6a), jc = js (Fig. 6b), and jc = 0.1js (Fig. 6c). These two /c, /s 6 0.2 and jc, js 6 108.
figures indicate that the ETC decreases with the increase of TCR, It is worth noting from Table 1 and Fig. 8 that the relative error
and it decreases sharply for larger TC ratios of core–shell. This is is approximate zero when the TCR is negligible, thus the ETC from
also illustrated in Fig. 7 for all values of TC ratio. The isothermal the present simulation becomes matching well with that obtained
lines cover along the surfaces of core–shell nanoparticles at low by Felske model. This is in line with the statement in previous
TCR, particularly with high TC ratios. Therefore, the external flow studies [20,21]. However, when the TCR is not negligible, the max-
is able to conduct into the nanoparticles. However, all isothermal imum relative error specifies at larger TCR for higher VFs (Fig. 8a),
lines move toward the interfaces at high TCR, or the thermal flow whereas it specifies at smaller TCR for higher TC ratios (Fig. 8b). It
is forced away from the nanoparticles, resulting in much less heat is suggested that further studies, particularly experimental ones,
transferred between the particles and surrounding medium. It should be performed to find out the most appropriate and accurate
implies that the high TCR not only confines the conductive heat model for predicting the ETC of core–shell nanoparticle polymer
transfer into the core–shell nanoparticles, but it also reduces the composites.
rate of heat transferred through the whole composite structure. Since the deviation between the ETC from present simulation
Theses two figures also show that the ETC always increases and that obtained by Felske model is not very large mentioned
with the increase of TC ratios of core–shell for a given value of above, the Felske model can be initially used to analyze and reveal
TCR. It is different from the behavior mentioned above for varying an optimum conditions for achieving the maximum ETC under the
core–shell VF, and suggesting that the ETC can be improved using effects of TCR. In addition, this analysis also provides a quantitative
core–shell filler with higher TC ratio regardless of the prersence of understanding on the thermal behaviors inside these polymer
the TCR. In addition, there exists a threshold value of TC ratios composites. By applying the same procedure proposed by Ngo
(j  103) over which the ETC is nearly unaffected by variation of et al. [21], the results obtained are shown in Table 2. It should be
j. The ETC curves on Fig. 6a through c is lifted up by the increase
of js, particularly at low TCR. It is due to the dominant role of shell
layer in contributing to the ETC of core–shell nanoparticle polymer Table 2
composites. Therefore, the ETC can be enhanced by mainly increas- Optimal jc/s for achieving the maximum ETC at various TCRs and /c/s values.
ing the TC ratio of shell. This is why the core–shell nanoparticle is R⁄c /c/s = 10 /c/s = 0.523 /c/s = 0.5023
being considered as a promising candidate for the TC enhancement
jc/s,opt k⁄eff,max jc/s,opt k⁄eff,max jc/s,opt k⁄eff,max
of a polymer composite.
106 5.4013 1.2385 0.0076 1.6422 0.0577 1.6706
Table 1 shows the ETC from the present simulation compared
0.01 5.4013 1.2162 0.0076 1.5936 0.0577 1.6199
with that of Felske model for two particular cases, high VFs and 0.05 5.4013 1.1477 0.0076 1.4380 0.0577 1.4577
high TC ratio of shell layer. It was found that the ETC from simula- 0.1 5.4013 1.0908 0.0076 1.3017 0.0577 1.3160
tion is generally low than that obtained from Felske model, and the 0.3 5.4013 0.9850 0.0076 1.0288 0.0577 1.0330
relative error (also called as deviation) between them varies with 0.5 5.4013 0.9426 0.0076 0.9117 0.0577 0.9119
0.7 5.4013 0.9198 0.0076 0.8466 0.0577 0.8447
the TCR. At first, the relative error increases rapidly with increasing
1 5.4013 0.9002 0.0076 0.7897 0.0577 0.7859
the TCR; then it reaches a maximum value at a given TCR, for
720 I.-L. Ngo et al. / International Journal of Heat and Mass Transfer 102 (2016) 713–722

Fig. 9. ETC as a function of TCR at shell-matrix interface for various TCR at core–shell interface, the effect of VF, (a) /s = 0.5/c = 0.05; (b) /s = /c = 0.1; (c) /s = 2/c = 0.2, and
js = 2jc = 10 used for all cases.

noted that Eq. (12) with the effect of TCR is applied in the present
study instead of Eq. (13) used in previous one. As a result of this
analysis, the optimal jc/s (=jc/js) is shown to be independent on
the TCR and only depends on /c/s (=/c//s), while the maximum
ETC is still affected significantly by the TCR and other parameters.
In addition, the maximum ETC specifying at the same jc/s,opt
regardless of the jc+s (=jc+js) value, is also observed, but is not
shown here. This is in good agreement with results obtained in
[21], thus Eq. (14) proposed for determining the jc/s,opt as a func-
tion of /c/s is still valid and can be utilized regardless of the
presence of the TCR. Furthermore, /c/s > 0.516 is a necessary condi-
tion for an existence of the maximum ETC, and other guidelines for
enhancing the TC of composites can be found in [21].



/c=s /c=s
jc=s;opt ¼ 7:3619  6:6764 exp  2:8145 exp
8:1551 0:5417
3.2. Effects of TCR at both core–shell and shell-matrix interfaces
Unlike the previous section that the TCR at the core–shell inter-
face is neglected, the effects of TCR at both core–shell (R⁄c,c-s) and
shell-matrix (R⁄c,s-m) interfaces are examined here. This is due to the
fact that the roughness of surfaces between different materials
always exists and arises from many unexpected factors in fabrication
[19,32]. Therefore, the ETC varying with the TCR at shell-matrix inter-
face for various TCR at core–shell interface is shown in Fig. 9 for three
particular cases, /s > /c (Fig. 9a), /s = /c (Fig. 9b), and /s < /c (Fig. 9c).
This figure indicates that the ETC is affected by both R⁄c,c-s and R⁄c,s-m
when R⁄c,s-m is small, it decreases as the R⁄c,c-s and R⁄c,s-m increase.
However, the ETC only depends on R⁄c,s-m when R⁄c,s-m is large enough.
This confirms the dominant role of shell-matrix interface in con-
tributing to the ETC. Then, the thermal flow is restricted and stopped
at this interface prior to penetrating into the core nanoparticle even
with very high TC. The interfaces acts as a thermal barrier to resist
the heat transfer between core–shell nanoparticles and the
surrounding medium. This result suggests that the TCR, particularly
: at shell-matrix interface, should be concerned in the TC enhancement
of core–shell nanoparticle polymer composites.
ð14Þ Fig. 10 shows the effects of TCR at both core–shell and shell-
matrix interfaces for four particular cases, js = 0.1 (Fig. 10a),
js = 10 (Fig. 10b), js = 600 (Fig. 10c), and js = 103 (Fig. 10d) while
keeping jc = 10 and VFs of core–shell. It was found that the ETC
is affected significantly by R⁄c,c-s and R⁄c,s-m only if js is small
(Fig. 10a and b), but it only depends on R⁄c,s-m when js is large and
approaches a critical value, js = 600 (Fig. 10c compared to Fig. 10d).
This critical value is found to also depend on the shell VF. It implies
 I.-L. Ngo et al. / International Journal of Heat and Mass Transfer 102 (2016) 713–722
Fig. 10. ETC as a function of TCR at shell-matrix interface for various TCR at core–shell interface, the effect of TC ratio, (a) js = 0.01jc = 0.1; (b) js = jc = 10; (c) js = 60jc = 600;
(d) js = 100jc = 103, and /c = 2/s = 0.2 used for all cases.
that the ETC of core–shell nanoparticle polymer composites can be
improved significantly by only controlling the shell thickness and
its critical TC. This is a good guidance for the thermal design in appli-
cations which require higher TC.
4. Conclusions
An investigation on the TC of composite materials containing
core–shell nanoparticles has been performed by a numerical
approach. The effects of the TCRs, in addition to other parameters,
the TC ratios between spherical core, shell and the matrix material,
and the VFs of core and shell, has been studied extensively. Based
on the numerical results, the thermal behaviors related to the ETC
of such polymer composites are found and discussed in detail. Con-
sequently, the major results are drawn as:
(1) The ETC depends significantly on the TCR, it decreases with
the increase of TCR, and it decreases sharply for both larger
VFs and larger TC of core–shell. The TC of composite cannot
be enhanced regardless of VFs of core–shell when the TCR is
greater than a critical value that depends on the shell VF. On
the other hand, the ETC can be improved by mainly increas-
ing the TC ratio of shell regardless of the TCR.
(2) The ETC from present simulation matches well with that
obtained by Felske model only if the TCR is negligible. How-
ever, the further studies, particularly experimental ones,
should be performed to find out the most appropriate and
721
accurate model for predicting the ETC of core–shell nanopar-
ticle polymer composites.
(3) The optimal jc/s is shown be independent of the TCR and
only depends on /c/s, while the maximum ETC is still
affected significantly by the TCR and other parameters.
/c/s > 0.516 is a necessary condition for an existence of the
maximum ETC regardless of the presence of the TCR.
(4) The ETC is affected significantly by R⁄c,c-s and R⁄c,s-m when js
and R⁄c,s-m are small, but it is independent on R⁄c,c-s when
R⁄c,s-m is large and js approaches a critical value, js = 600. This
result provides a good guidance for enhancing the TC of core–
shell nanoparticle polymer composites.
Acknowledgments
This research was supported by Basic Science Research Program
through the National Research Foundation of Korea (NRF)
funded by the Ministry of Science, ICT and Future Planning
(2014R1A2A2A01007081).
References
[1] I.H. Tavman, In Nanoengineered Nanofibrous Materials, NATO Science Series II,
Mathematics, Physics and Chemistry, Dordrecht, Netherlands, 2004.
[2] C. Liu, T. Mather, ANTEC 2004, Society of Plastic Engineers, 2004.
[3] I.H. Tavman, Thermal and mechanical properties of copper powder filled poly
(ethylene) composites, Powder Technol. 91 (1) (1997) 63–67.
722 I.-L. Ngo et al. / International Journal of Heat and Mass Transfer 102 (2016) 713–722
[4] I.-L. Ngo, S. Jeon, C. Byon, Thermal conductivity of transparent and flexible
polymers containing fillers: a literature review, Int. J. Heat Mass Transfer 98
(July) (2016) 219–226.
[5] J.C. Maxwell, A Treatise on Electricity and Magnetism Unabridged, Dover,
1954.
[6] T.B. Lewis, L.E. Nielsen, Dynamic mechanical properties of particulate-filled
composites, J. Appl. Polym. Sci. 14 (6) (1970) 1449–1471.
[7] L.E. Nielsen, Thermal conductivity of particulate-filled polymers, J. Appl.
Polym. Sci. 17 (12) (1973) 3819–3820.
[8] Y. Agari, T. Uno, Estimation on thermal conductivities of filled polymers, J.
Appl. Polym. Sci. 32 (7) (1986) 5705–5712.
[9] D. Bruggeman, Dielectric constant and conductivity of mixtures of isotropic
materials, Ann. Phys. (Leipzig) 24 (1935) 636–679.
[10] I.H. Tavman, Thermal and mechanical properties of aluminum powder-filled
high-density polyethylene composites, J. Appl. Polym. Sci. 62 (12) (1996)
2161–2167.
[11] H. He, R.L. Fu, Y.H. Han, Y. Shen, X.F. Song, Thermal conductivity of ceramic
particle filled polymer composites and theoretical predictions, J. Mater. Sci. 42
(16) (2007) 6749–6754.
[12] I.-L. Ngo, C. Byon, A review on enhancing thermal conductivity of transparent
and flexible polymer composites, Sci. Adv. Mater. 8 (2) (2016) 257–266.
[13] I.-L. Ngo, C. Byon, A generalized correlation for predicting the thermal
conductivity of composites with heterogeneous nanofillers, Int. J. Heat Mass
Tranfer 90 (2015) 894–899.
[14] G.W. Lee, M. Park, J. Kim, J.I. Lee, H.G. Yoon, Enhanced thermal conductivity of
polymer composites filled with hybrid filler, Compos. Part A: Appl. Sci. 37 (5)
(2006) 727–734.
[15] K. Sanada, Y. Tada, Y. Shindo, Thermal conductivity of polymer composites
with close-packed structure of nano and micro fillers, Compos. Part A: Appl.
Sci. 40 (6–7) (2009) 724–730.
[16] Y.C. Zhou, Y.Y. Bai, K. Yu, Y. Kang, H. Wang, Excellent thermal conductivity and
dielectric properties of polyimide composites filled with silica coated self-
passivated aluminum fibers and nanoparticles, Appl. Phys. Lett. 102 (25)
(2013).
[17] Z. Gao, L. Zhao, Effect of nano-fillers on the thermal conductivity of epoxy
composites with micro-Al2O3 particles, Mater. Des. 66 (Part A(0)) (2015) 176–
182.
[18] Y.C. Zhou, L. Wang, H. Zhang, Y.Y. Bai, Y.J. Niu, H. Wang, Enhanced high thermal
conductivity and low permittivity of polyimide based composites by core–
shell Ag@SiO2 nanoparticle fillers, Appl. Phys. Lett. 101 (1) (2012).
[19] S.W. Kim, H.-S. Choi, K.-S. Lee, Thermal conductivity of thermally conductive
composites consisting of core–shell particles with nanostructured shell layers,
Mater. Res. Bull. 60 (2014) 843–848.
[20] A.M. Thiele, A. Kumar, G. Sant, L. Pilon, Effective thermal conductivity of three-
component composites containing spherical capsules, Int. J. Heat Mass
Transfer 73 (2014) 177–185.
[21] I.-L. Ngo, C. Byon, An extensive study on enhancing the thermal conductivity of
core–shell nanoparticle composites using finite element method, Int. J. Heat
Mass Transfer 101 (2016) 147–155.
[22] I.-L. Ngo, C. Byon, A generalized correlation for predicting the thermal
conductivity of composite materials, Int. J. Heat Mass Transfer 83 (2015)
408–415.
[23] F. Zhou, G. Cheng, Lattice Boltzmann model for predicting effective thermal
conductivity of composite with randomly distributed particles: considering
effect of interactions between particles and matrix, Comput. Mater. Sci. 92
(2014) 157–165.
[24] B. Mortazavi, J. Bardon, S. Ahzi, Interphase effect on the elastic and thermal
conductivity response of polymer nanocomposite materials: 3D finite element
study, Comput. Mater. Sci. 69 (2013) 100–106.
[25] C.L. Yeh, C.T. Lin, Thermal contact resistance correlation for metals across
bolted joints, Int. Commun. Heat Mass Transfer 30 (7) (2003) 987–996.
[26] I.A. Tsekmes, R. Kochetov, P.H.F. Morshuis, J.J. Smit, Modeling the thermal
conductivity of polymeric composites based on experimental observations,
IEEE Trans. Dielectr. Electr. Insul. 21 (2) (2014) 412–423.
[27] W. Woodside, J.H. Messmer, Thermal conductivity of porous media. I.
Unconsolidated sands, J. Appl. Phys. 32 (9) (1961) 1688–1699.
[28] K. Lichtenecker, Dielectric constant of natural and synthetic mixtures, Phys. Z
27 (1926) 115–158.
[29] A.D. Brailsford, K.G. Major, The thermal conductivity of aggregates of several
phases, including porous materials, Br. J. Appl. Phys. 15 (3) (1964) 313.
[30] J.D. Felske, Effective thermal conductivity of composite spheres in a
continuous medium with contact resistance, Int. J. Heat Mass Transfer 47
(14–16) (2004) 3453–3461.
[31] Y.-M. Lee, R.-B. Yang, S.-S. Gau, A generalized self-consistent method for
calculation of effective thermal conductivity of composites with interfacial
contact conductance, Int. Commun. Heat Mass Transfer 33 (2) (2006) 142–150.
[32] Y.P. Mamunya, V.V. Davydenko, P. Pissis, E. Lebedev, Electrical and thermal
conductivity of polymers filled with metal powders, Eur. Polym. J. 38 (9)
(2002) 1887–1897.