International Journal of Thermal Sciences 171 (2022) 107209

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International Journal of Thermal Sciences

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

Influence of graphene nano-platelets on thermal transport performance of

carbon fiber-polymer hybrid composites: Overall assessment of
microstructural aspects
Mohammad Kazem Hassanzadeh-Aghdam a, *, Reza Ansari b, Hamed Mohaddes Deylami a
a
Faculty of Technology and Engineering, East of Guilan, University of Guilan, Rudsar, Iran
b
Faculty of Mechanical Engineering, University of Guilan, Rasht, Iran

A R T I C L E I N F O A B S T R A C T

Keywords: This study comprehensively investigates the thermal transport behavior of unidirectional hybrid composites
Hybrid composite (UHCs) by means of a micromechanical methodology. The constructional feature of the UHC is that the
Thermal transport performance continuous carbon fibers are embedded in the graphene nano-platelets (GNPs)-modified epoxy resin. The in­
Nano-graphene
fluences of volume fraction, length, thickness, and alignment of GNPs, the interfacial thermal resistance (ITR)
Agglomeration
Micromechanics
between the nano-graphene and polymer matrix, as well as the volume fraction, arrangement type, and off-axis
angle of carbon fibers on the thermal conductivities of UHCs are extensively analyzed. Further, the micro­
mechanical model is extended to account the effect of GNP agglomeration on the UHC thermal conductivities.
The results show that uniformly dispersed GNPs play a dominant role in improving the UHC thermal conductivity
along the transverse direction, while the axial thermal conductivity is insignificantly influenced by the nano-
graphene particles. Besides, using the GNPs with a higher aspect ratio (length/thickness) is an efficient
manner to obtain much better thermal transport performance for the UHCs. It is observed that the formation of
GNP agglomeration within the epoxy resin severely decreases the transverse thermal conductivity. The presence
of GNP/epoxy ITR is a lowering factor of the thermal conductivity. As compared to the hexagonal and random
arrays, the square array of carbon fibers within the GNP-modified epoxy produces the largest transverse thermal
conductivity. On the basis of comparative studies, the model predictions agree very well with the experimental
data available in the literature.

1. Introduction fiber fracture, matrix yielding, fiber/matrix interfacial debonding, as

Carbon fiber reinforced polymer composites (CFRPCs) have been
extensively used as primary structures in aerospace, automotive, and
renewable energy industries because of their high specific strength and
stiffness, remarkable fatigue characteristics and good corrosion resis­
tance [1–3]. The CFRPCs have excellent in-plane properties dominated
by the high-performance carbon fibers. But, the out-of-plane properties
of CFRPCs governed by the matrix are very low which can limit their
structural applications [4]. For instance, the low out-of-plane thermal
conductivity of CFRPCs is due to the poor thermal conductivity of the
polymer matrixes [5,6]. Generally, the directional conduction can be an
advantage of fibrous composite materials that can be conducting in one
direction and insulating in the other. Consequently, heat is not effi­
ciently conducted away which may lead to several damage types, such as
well as the delamination in the laminated composites. Since the local­
ized damages can result in catastrophic failure of the CFRPC structures
[7], the accumulated heat must be dissipated. Therefore, development
of CFRPCs with high thermal transport performance to hinder incipient
thermal-induced structural damage is of great interest to numerous in­
dustrial sectors.
Tremendous efforts have been devoted to improve the out-of-plane
thermal conductivities of fiber/polymer composites. It was stated that
the out-of-plane heat transfer mechanisms in CFRPCs are intensely
affected by the thermal conductivity of the matrix. It seems that adding
thermally conductive nano-sized carbon particles into the polymer
matrix to be a practical method to achieve suitable out-of-plane heat
dissipation performance [7–9]. The main reason is that carbonaceous
nanomaterials efficiently improve the matrix thermal transport

* Corresponding author.
E-mail address: Mk.hassanzadeh@gmail.com (M.K. Hassanzadeh-Aghdam).

https://doi.org/10.1016/j.ijthermalsci.2021.107209
Received 29 September 2020; Received in revised form 30 June 2021; Accepted 2 August 2021
Available online 10 August 2021
1290-0729/© 2021 Elsevier Masson SAS. All rights reserved.
M.K. Hassanzadeh-Aghdam et al.
Fig. 1. Schematic sketch of the GNP/fiber-reinforced UHCs.
coefficient [10,11]. Among carbon-based particles, graphene consisting
of a sheet of carbon atoms arranged in a honeycomb structure [11,12]
offers the potential to enhance the thermal properties of polymer com­
posites [11,13]. It is due to the ultrahigh thermal conductivity of gra­
phene (~5300 W/mK) [14]. Graphene nano-platelets (GNPs) are unique
nanoparticles composed of several layers of graphene. Due to the low
cost, the mass production of GNPs is suitable [15]. The addition of GNPs
into the fiber/polymer composites promises an efficient and economical
route to create a new class of hybrid composites for thermal manage­
ment in high-tech industries such as aircraft structural applications. As
compared to the conventional fiber/polymer composites, the fiber/­
GNP/polymer hybrid composites combine the properties of all the
constituents and display improved performance.
A number of research works have been devoted to analyze the
thermal conductivity of carbon fiber/polymer hybrid composites con­
taining graphene particles [7,16–18]. For instance, Kandare et al. [7]
found that the inclusion of 1 vol% GNPs into the carbon fiber/epoxy
composites results in 9 % enhancement in the out-of-plane thermal
conductivity of the hybrid composites at room temperature. Wang and
Cai [9] experimentally investigated the effect of GNP weight fraction on
the thermal conductivity of the carbon fiber/epoxy hybrid composites.
The out-of-plane thermal conductivity of the hybrid composite con­
taining 0.5 wt% GNPs indicated a 55.6 % enhancement as compared to
the base carbon/epoxy composite [9]. Zhang et al. [18] produced the
epoxy nanocomposites modified with 0.5, 1, 2, and 4 wt% graphene
nanoflakes. These nanocomposite materials were used as the matrix
phase for carbon fibers to manufacture the hybrid composites. The
hybrid composite thermal properties were improved with increasing the
graphene content. The thermal conductivity of the carbon fiber/epoxy
hybrid composites with 4 % nano-graphene was improved 45 % as
compared to the base carbon fiber/epoxy composites [18]. By ball
milling and hot-press processing, Liu et al. [19] produced carbon
fiber-reinforced poly(ether ether ketone) (PEEK) hybrid composites with
different weight fractions of graphene. The thermal conductivity of the
carbon fiber/PEEK hybrid composite containing 1 wt% graphene
Fig. 2. Schematic representation of (a) GNP as an equivalent oblate spheroid and (b) GNP coated with a thin interfacial thermal barrier layer.
2
International Journal of Thermal Sciences 171 (2022) 107209
additive was 53.7 % greater than that of the carbon fiber/PEEK com­
posite [19]. According to the test results of Noh and Kim [20], the
isotropic thermal conductivity of the 5 wt% carbon fiber/15 wt%
GNP-reinforced hybrid composite attained improvement of 82 % as
compared to the 20 wt% GNP-reinforced composite, and improvement
of 65 % as compared to the 20 wt% carbon fiber-reinforced composite.
Heat transfer mechanism of fiber/GNP/polymer hybrid composites is
largely influenced by the amount, size, and dispersion degree of GNPs,
volume fraction, and orientation of carbon fibers and most importantly
the nanofiller/polymer interfacial thermal resistance (ITR) [7,9,11,13].
Up to now, no systematic study concerning the overall thermal con­
ductivities of unidirectional hybrid composites (UHCs) consisting of the
carbon fiber, GNP and epoxy resin has been performed. It is imperative
to develop innovative strategies for predicting the thermal conductiv­
ities of UHCs and investigate the effects of critical microstructural as­
pects on heat transfer performance.
In addition to experimental methods, a lot of simulation tools have
been designed to predict the effective thermal conductivities of com­
posite materials [13,21–23]. The main advantages of the theoretical
methods are their simplicity and low cost. In this work, a hierarchical
micromechanical method is proposed to analyze the thermal conduc­
tivity of carbon fiber/GNP/epoxy UHCs. The organizations of the pre­
sent research paper are as follows. The micromechanical models and
procedures of predicting the UHC thermal conductivities are established
in Section 2. Section 3 presents the numerical results to investigate the
effects of volume fraction, length, thickness, agglomeration degree, and
alignment of GNPs, the ITR between the nano-graphene and polymer
matrix, volume fraction, arrangement type, and off-axis angle of carbon
fibers on the UHC thermal transport properties. Besides, the simulation
results are validated by comparing them with the experimental data
mainly to confirm the ability of micromechanical methodology in pre­
dicting the thermal conductivities.
M.K. Hassanzadeh-Aghdam et al. International Journal of Thermal Sciences 171 (2022) 107209

2. Theoretical approach

The thermal conductivity of GNP-modified polymer matrix nano­

composites (PMNCs) is obtained within the framework of the micro­
mechanics first. The important microstructural aspects of PMNCs,
particularly the nanoparticle/polymer ITR and the GNP agglomeration
are taken into account. Then, a unit cell-based micromechanical model
is developed to estimate the thermal conductivities of unidirectional
fiber-reinforced composites. Finally, the detailed procedures of the
prediction of UHC thermal transport coefficients are presented. Fig. 1
shows a schematic sketch of the GNP/fiber-reinforced UHCs.

2.1. GNP-modified PMNCs

The GNPs are assumed to be uniformly distributed and randomly

oriented in the polymer matrix. The GNP is modeled as an equivalent
oblate spheroid with a specified aspect ratio p (length/thickness)
[24–26]. The review of literature confirms that the ITR (RK ) between the
nanoparticles and polymer matrix has a high influence on the thermal
transport behavior of composite materials [27–30]. The nano­
particle/polymer ITR denotes all combined effects which contribute to
an interfacial thermal barrier [24,31]. To take the ITR influence into Fig. 3. Schematic sketch of the PMNC containing GNP agglomeration.
account, the nano-graphene particle is seen as a nanoscale plate coated
with a very thin interfacial thermal barrier layer [24,26,32], as shown in GNP-reinforced nanocomposites are extracted. In Eq. (3), H reflects the
Fig. 2. In this figure l and t are the length and thickness of GNP. The geometrical factors and is expressed as [24].
equivalent thermal conductivities of GNP along the in-plane (Kx ) and ⎡ √̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅ ⎤
through-thickness (Kz ) directions are given by [24]. ( )2
ln⎣tl + l
t
− 1 ⎦ tl
Kg Kg
Kx = 2RK Kg , Kz = 2RK Kg (1) H= √̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅
1
(4)
l
+ 1 t
+1 [( )2 ]3̅ − ( )2 .
l
l
− 1 t
− 1
t
where Kg is the GNP thermal conductivity. The thickness of GNP
robustly affects its thermal conductivity [33,34]. The thickness depen­ It has been previously mentioned that the agglomeration of nano-
dence of Kg can be expressed as follows [34]. graphene particles is one of the most significant problems decreasing
( )− 1/2 the graphene capability in improving the effective properties of PMNCs
t
Kg = 4058 × 10
. (2) [36–39]. Herein, a micromechanics-based technique is offered in a
3.4 × 10−
nested modeling procedure to capture the GNP agglomeration. Such
Thus, the magnitude of Kg can be determined from the thickness of method has been already used to investigate the role of nanotube
GNP. Micromechanical methods are able to predict the thermal con­ agglomeration in the elastic properties of polymer composite materials
ductivity of the GNP-filled composites. Several assumptions and limi­ [40–42]. In this approach, a number of GNPs are uniformly dispersed
tations exist in these methods. For example, the micromechanical inside the polymer matrix making the equivalent matrix, and other GNPs
models have been fundamentally developed for the continuum rein­ appear in the agglomeration form, as presented in Fig. 3. It is assumed
forcing agent, while graphene has a lattice structure. Furthermore, a that the regions with the agglomerated GNPs have spherical shapes, and
perfect structure without any defects is assumed for GNPs. In the are incorporated as “inclusions”. The whole volume of GNPs in the
micromechanical modeling, a similar size is supposed for all GNPs PMNC, signified by VGNP , can be divided into two parts as
dispersed within the composites. The interfacial area between nano- SI
VGNP = VGNP EM
+ VGNP (5)
graphene and polymer is governed by the molecular interactions,
while an equivalent solid continuum interphase between the nano­ SI EM
where VGNP is the GNP volume in the spherical inclusions, and VGNP is
particle and polymer is frequently assumed in the micromechanical
the GNP volume in the effective matrix. Two parameters to describe the
rules. Besides, formation of voids is not considered in the micro­
GNP agglomeration are presented as
mechanical modeling of the thermal conductivity of the GNP-reinforced
composites. On the basis of micromechanics approach [24,34,35], the VSI V SI
ξ= , ζ = GNP 0 ≤ ξ, ζ ≤ 1 (6)
effective thermal conductivity of the PMNCs with randomly oriented V VGNP
GNPs (KPMNC ) can be predicted by the following relation
⎡ ⎤ ⎡ ⎤ where V and VSI are the PMNC volume and the spherical inclusion
volume in the PMNCs, respectively. ξ specifies the volume fraction of
2⎢ fGNP KM ⎥ 1⎢ fGNP KM ⎥
KPMNC = KM + ⎢ ( )− 1 ⎥ ⎢
⎦ +3⎣ ( )− 1 ⎥ (3) inclusions with respect to the PMNC volume, and ζ denotes the volume
3⎣ ⎦
H + KKMx − 1 1− H
+ KKMz − 1 ratio of GNPs inside the spherical inclusions over the whole GNP inside
the PMNC. A uniform dispersion of GNPs throughout the PMNCs
2

without agglomeration occurs when ξ = 1. By the reduction of ξ, the

where KM denotes the thermal conductivity of the polymer matrix, and
fGNP signifies the GNP volume fraction. The corresponding formulas for
the axial and transverse thermal conductivities of the aligned GNP-
reinforced composites can be derived by means of Eq. (3) as intro­
duced in Ref. [35]. Thus, the results about the orientation of GNPs can be
investigated. In other words, the thermal conductivities of the aligned
degree of GNP agglomeration becomes more severe. Once ζ = 1, all the
GNPs are located in the sphere zones. The case ξ = ζ means that all the
GNPs are dispersed evenly without agglomeration. By the consideration
of fGNP ( = VGNP /V) along with Eqs. (5) and (6), following relations can
be derived as

3
M.K. Hassanzadeh-Aghdam et al. International Journal of Thermal Sciences 171 (2022) 107209

Fig. 4. Schematic representation of an RVE with a square array packing of fibers.

Fig. 5. Extension of the RVE of the SUCM

SI
VGNP ζ V EM (1 − ζ) Several assumptions are imposed in developing Eq. (8). For example,
SI
fGNP = EM
= fGNP , fGNP = GNP = fGNP (7)
VSI ξ V − VSI (1 − ξ) the spherical inclusion in the representative volume element (RVE) is
replaced by a cubic inclusion of the same volume so as to keep the same
SI
where fGNP EM
and fGNP signify the GNP volume fractions in the spherical volume fraction. Furthermore, spherical inclusions with similar shapes
inclusions and in the equivalent matrix, respectively. Therefore, the and sizes are dispersed uniformly in the matrix. Both phases (inclusion
total GNP-modified PMNC is a composite material consisted of the and matrix) behave as isotropic materials. Additionally, a perfectly
spherical inclusions embedded in the equivalent matrix. The micro­ bonded interface between the inclusion and the matrix is assumed, and
mechanical modeling starts from the prediction of the thermal con­ no interfacial resistance between these two phases is considered.
ductivities of spherical inclusion (KSI ) and equivalent matrix (KEM ) using
Agg
Eq. (3). Then, we calculate KPMNC , the effective thermal conductivity of 2.2. Unidirectional composites
the whole PMNC with the GNP agglomeration by capturing the spherical
inclusion as the reinforcement and the equivalent matrix as the new The micromechanical method based on the simplified unit cell model
matrix, as follows [43]. (SUCM) is presented to evaluate the thermal transport behavior of
unidirectional fiber-reinforced composites. The SUCM has been exten­
ξ0.67 KEM ( )
Agg
KPMNC = ( ) + 1 − ξ0.67 KEM . (8) sively used to predict the mechanical properties of unidirectional com­
1 − ξ0.33 1 − posites [44,45]. The SUCM with an RVE consisted of four sub-cells has
KEM
KSI
been developed to estimate the thermal conductivities of unidirectional

4
M.K. Hassanzadeh-Aghdam et al. International Journal of Thermal Sciences 171 (2022) 107209

composites [46]. The cross-section of composite was idealized with a

square regular array of fibers [46], as shown in Fig. 4. However, the real
arrangement of the fibers within the cross-section of the unidirectional
composite is random. Therefore, the micromechanical formulations of
the SUCM should be modified to simulate the random array of fibers
embedded in the matrix [8]. The geometry of the RVE of the SUCM is
extended to r × c sub-cells, as can be seen in Fig. 5. The size of each
sub-cell and whole RVE can be seen in this figure. The perfect bonding
conditions are applied between the RVE sub-cells.
Introducing the global heat flow Ql (l = x, y, z) over the RVE leads to
the following equilibrium equations for the heat flux within the sub-cells
as [46].
∑
r ∑
c r ∑
∑ c
bj q1j
x = Qx L r , ai qi1
y = Qy Lc , bj ai qijz = Qz Lr Lc . (9)
j=1 i=1 j=1 i=1

ij
where ql is the local heat flux in the sub-cell ij in direction l. According to
the equivalence of the local heat flux components at the sub-cell in­
terfaces, following relations are extracted as [8,46,47].

q1j ij i1 ij
x = qx (i > 1), qy = qy (j > 1). (10)

In the unit cell approaches, the temperature gradient inside the sub-
cells of the RVE is supposed to be linear [46,47]. The temperature
compatibility on the basis of RVE description leads to
⎧
⎪
⎪ ∑ c ∑c
⎪
⎪ ai T,xi1 = ai T,xij = Lc T ,x (j > 1),
⎪
⎪
⎪
⎪ i=1 i=1
⎨
∑ ∑ (11)
r r
⎪
⎪ bj T,y1j = bj T,yij = Lr T ,y (i > 1) Fig. 6. Multi-step modeling of the thermal conductivities of UHCs.
⎪
⎪ j=1
⎪
⎪ j=1
⎪
⎪
⎩ T ij = T (i > 1, j > 1) 2.3. Thermal conductivities of UHCs
,z ,z

ij
in which T,l is the local temperature gradient inside the sub-cell ij, and T,l Fig. 6 shows the various steps involved in the micromechanical
prediction of the UHC thermal conductivities. First, the thermal con­
is the global temperature gradient in direction l. On the basis of Fourier’s
ductivities of the spherical inclusion and equivalent matrix are needed.
law, the relation between the heat flow vector q and temperature
By considering ξ, ζ, fGNP , and the properties of GNP and polymer, Eq. (3)
gradient for the sub-cell ij is expressed as
is employed to calculate the values of KSI and KEM . These results are used
Tij, = Kij
− 1
: qij (12) as an input to the micromechanical model in Eq. (8) to estimate the
thermal conductivity of GNP-modified PMNCs. In this step, the spherical
where Kij stands for the thermal conductivity tensor of the sub-cell ij. A inclusion plays the role of reinforcing phase and the equivalent matrix is
system of cr + c + r equations with the identical number of unknowns considered as the new matrix phase. The combination of the fibers and
will be obtained by substituting Eq. (12) in Eq. (11) along with Eqs. (9) the PMNC is viewed as a UHC containing GNPs that its thermal con­
and (10), as follows ductivity is estimated by the SUCM. In the RVE of UHCs, the rein­
forcement is the unidirectional fiber and the matrix phase is the GNP-
Am×m qm×1 = Fm×1 where m = cr + c + r (13) modified PMNCs.

in which q and F denote the heat flux vector inside each sub-cell and the
3. Results and discussion
external heat flux vector, respectively. Moreover, A specifies the coef­
ficient tensor made of the geometrical and material characteristics of the
To verify the validity of the micromechanical model in estimating the
sub-cells. Solving Eq. (13) gives the components of local heat flux for all
thermal conductivity of the GNP-modified PMNCs, the calculations are
sub-cells. Then, the components of local temperature gradient for all
compared with the experimental data [48]. Fig. 7 shows the comparison
sub-cells are calculated by Eq. (12). The components of global temper­
between two sets of results. The thermal conductivity of the GNP-epoxy
ature gradient are determined by Eq. (11). Finally, the thermal con­
nanocomposite is plotted as a function of GNP volume fraction. Two
ductivities in directions z, y and x are estimated, respectively, as
types of GNPs, including (i) multi-layered GNP with l = 1.7 μm and t =
Qz 60 nm, and (ii) few-layered GNP with l = 0.35 μm and t = 1.7 nm are
(14)
considered [34,48]. The value of RK is 3.5 × 10− 9 m2K/W [34,49]. The
Kz = when Qz ∕
= 0 and Qx = Qy = 0,
T ,z
micromechanical modeling is performed for two conditions of nano­
Qy particle dispersion, including (i) uniformly dispersed GNPs, and (ii)
Ky = when Qy ∕
= 0 and Qx = Qz = 0, (15)
T ,y agglomerated GNPs with ξ = 0.5 and ζ = 0.85. It is found from Fig. 7 a
and b that a substantial discrepancy exists between the experimental
Qx outcomes [48] and the predicted values by the model with uniformly
Kx = when Qx ∕
= 0 and Qy = Qz = 0. (16)
T ,x dispersed GNPs and ignoring the GNP/epoxy ITR. This is more obvious
at higher GNP volume fraction. Considering only the ITR in the micro­
It is noticed that for a transversely isotropic composite, we have Kx =
mechanical modeling leads to the predictions to be close to the experi­
Ky =
∕ Kz .
mental measurements at the low graphene content. Nevertheless, the

5
M.K. Hassanzadeh-Aghdam et al. International Journal of Thermal Sciences 171 (2022) 107209

Fig. 7. Comparison of the model predictions and experimental measurements [48] of the thermal conductivity of the GNP-modified epoxy nanocomposites, (a) l =
1.7 μm and t = 60 nm, and (b) l = 0.35 μm and t = 1.7 nm.

Fig. 8. Effect of agglomeration parameter on the thermal conductivity of the GNP-modified epoxy nanocomposites, (a) l = 1.7 μm and t = 60 nm, and (b) l = 0.35
μm and t = 1.7 nm.

6
M.K. Hassanzadeh-Aghdam et al.
Fig. 9. Effect of ITR value on the thermal conductivity of the GNP-modified
epoxy nanocomposites.
thermal conductivities achieved by the model considering the ITR and
uniform dispersion of GNPs are still far from the experiments at the
higher GNP content. Excellent agreement between two sets of results
occurs when both the agglomeration of GNPs and graphene/polymer
ITR are taken into account in the micromechanical analysis. As expected
from the properties of graphene, the thermal conductivity of the epoxy
nanocomposites increases with the increase of nanoparticle volume
fraction. Based on the micromechanical results, the ITR between the
GNP and epoxy matrix significantly decreases the thermal properties of
the PMNCs. Because of the discrepancy in the phonon density of state,
phonons are scattered at the GNP/epoxy interface and thus, the thermal
transport is seriously hindered. The PMNCs filled with uniformly
dispersed GNPs have a higher thermal conductivity than those filled
with non-uniformly dispersed GNPs; i.e. agglomerated state. Thus, GNPs
with a homogenous dispersion are really beneficial to the heat transfer
ability of the PMNCs.
The micromechanical predictions of the thermal conductivity of the
GNP/epoxy nanocomposite with different values of agglomeration
parameter are provided in Fig. 8. Both nanocomposite systems with
different dimensional characteristics of GNPs are analyzed. The values
of ξ and RK are 0.85 and 3.5 × 10− 9 m2K/W, respectively. Also, the
experimental measurements [48] are given in this figure. The results
indicate that to have the best agreement between the model predictions
Fig. 10. Variation of the thermal conductivity of the GNP-modified epoxy nanocomposites with (a) GNP length, t = 1.7 nm, (b) GNP thickness, l = 0.35 μm.
7
International Journal of Thermal Sciences 171 (2022) 107209
and experimental measurements, the values of ξ and ζ should be about
0.5 and 0.85, respectively.
The effect of ITR values on the thermal conductivity of GNP/epoxy
nanocomposites is investigated as shown in Fig. 9. When the value of ITR
is 3.5 × 10− 9 m2K/W, a good agreement exists between the predictions
and experiments [48]. The thermal conductivity of the polymer nano­
composites decreases as the value of ITR increases. A great amount of
phonon scattering can be occurred at the filler/matrix interface because
of the unbalanced density of phonon states. This causes high thermal
resistance during the interfacial thermal transport process [7].
The effects of geometrical characteristics and dispersion type of
GNPs on the thermal conductivity of the epoxy nanocomposites are
investigated. Both uniform (or perfect) dispersion and alignment of
GNPs are considered. This case may be an examination about the role of
GNP orientation in the nanocomposite thermal conductivity. To analyze
in more detail, the micromechanical modeling is accomplished under
two conditions; (i) with ITR, and (ii) without ITR. The variation of the
nanocomposite thermal conductivity with the GNP length is depicted in
Fig. 10a. It is found that the thermal conductivity of the epoxy nano­
composites in the presence of ITR is nonlinearly enhanced by increasing
the GNP length. More thermal conductive paths can be constructed by
the increase of GNP length which facilitates the heat transfer. The results
show that the thermal conductivity of the aligned GNP-reinforced
nanocomposites is higher than that of the randomly dispersed GNP-
reinforced nanocomposites. Thus, a better thermal transport can be
conducted by the alignment of GNPs along the thermal loading. When
the ITR is not taken into account in the modeling, the thermal conduc­
tivity of the epoxy nanocomposite suddenly increases by the increase of
GNP length up to 0.75 μm and then, its value saturates. In other words,
when l > 0.75 μm, further increase of GNP length does not affect the
nanocomposite thermal conductivity. Furthermore, in the absence of
ITR, the alignment of GNPs leads to higher thermal conductivities for the
polymer nanocomposites as compared to the random dispersion. The
thermal conductivity of GNP-epoxy nanocomposites as a function of
GNP thickness is shown in Fig. 10b. With increasing the thickness of
GNP up to about 40 nm, the thermal conductivity decreases. In the
absence of ITR, the thermal conductivity drop is very notable. When t >
40 nm, variation of GNP thickness insignificantly affects the nano­
composite thermal conductivity. The thermal conductivity is further
enhanced by aligning the GNPs in the polymer matrix. It can be
concluded from Fig. 10 that the variations of GNP orientation and shape
change the thermal conductivity of the polymer nanocomposites
without (or with) the ITR.
Fig. 11 shows the role of GNP thermal conductivity on the thermal
conductivity of the GNP-modified epoxy nanocomposites. The theoret­
ical results are provided under two conditions for GNP thermal con­
ductivity; (i) Kg = 5300 W/mK, and (ii) Kg based on Eq. (2) which is a
M.K. Hassanzadeh-Aghdam et al.
Fig. 11. Effect of GNP thermal conductivity on the thermal conductivity of the
GNP-modified epoxy nanocomposites.
thickness-dependent variable. It has been reported in the available
literature that the thermal conductivity of the graphene may be up to
5300 W/mK [14,34]. On the other hand, the thermal conductivity of the
GNP remarkably depends on its thickness [33,34]. The value of Kg de­
creases as the GNP thickness increases. The experimental measurements
[48] are included in Fig. 11. When the thermal conductivity of GNP is
derived from Eq. (2), a good agreement is observed between the results
of the micromechanical modeling and experiment [48].
McIvor et al. [50] measured both the axial and transverse
temperature-dependent thermal conductivities of carbon
fiber-reinforced epoxy composites. As another verification of the model,
the calculations are compared with the experimental data [50], as
shown in Fig. 12. The effective thermal conductivities of the carbon
fiber/epoxy composites are plotted as a function of temperature (T).
Based on Ref. [50], the temperature-dependent thermal conductivity of
the constituents is
for carbon fiber: KFA = 173.3 + 0.488 T − 0.00178 T2 W/m◦ C and
KFT = 30 W/m◦ C
for epoxy: KM = 0.5655 + 0.00124 T W/m◦ C.
where kFA and kFT stand for the axial and transverse thermal conduc­
tivities of carbon fiber. The model predictions are seen to be in good
agreement with the test results [50].
To further validate the presented model, the thermal conductivities
of the carbon fiber/epoxy composites predicted by the SUCM are
compared with the predictions of the composite cylinder assemblage
(CCA) approach. Fig. 13 shows this comparison. The longitudinal (KL )
and transverse (KT ) thermal conductivities of the fiber-reinforced com­
posites are estimated by the CCA as [28].
KL = fF KF + (1 − fF )KM
/ tivities as a function of GNP length are presented in Fig. 16. The UHC
g1 (1 + fF ) + 1 − fF
KT = KM , g 1 = KF KM .
g1 (1 − fF ) + 1 + fF
where fF and KF are the volume fraction and thermal conductivity of the
fiber. Moreover, the results of the upper and lower bounds are included
in Fig. 13. The thermal conductivities of the unidirectional composites
can be predicted by the upper and lower bounds [51], respectively, as
Kub = fF KF + (1 − fF )KM
International Journal of Thermal Sciences 171 (2022) 107209
1 1 − fF fF
= + . (20)
Klb KM KF
As can be seen in Fig. 13a, three sets of results predicted by the
SUCM, CCA, upper bond are in excellent agreement. It is found from
Fig. 13b that a good agreement exists between the results of the SUCM
and CCA for the transverse thermal conductivity. The lower bound gives
lowest transverse thermal conductivity as compared to other models.
The effective thermal conductivities of carbon fiber/GNP/epoxy
UHCs are estimated by the micromechanical method developed in Sec­
tion 2. To generate the numerical results following values are used in the
micromechanical modeling: KM = 0.2 W/mK, KFA = 183 W/mK, KFT = 30
W/mK, l = 1.7 μm, t = 60 nm, RK = 3.5 × 10− 9 m2K/W, fGNP = 5 %,
unless otherwise stated. The dispersion of GNPs is assumed to be uni­
form and random inside the epoxy resin.
First, to explore the reinforcement effect of GNPs on the thermal
transport behavior of UHCs, micromechanical analysis is carried out.
The thermal conductivities along the axial and transverse directions as a
functions of carbon fiber volume fraction are shown in Fig. 14 a and b,
respectively. The results of the upper and lower bounds as well as the
CCA approach are included in the figure. The addition of GNPs is
thought to have an insignificant effect on the axial thermal conductivity
of the UHCs as depicted Fig. 14a. It is attributed to the fact that the axial
heat conduction in unidirectional fiber-reinforced composite materials
is dominated by the fiber properties. The thermal conductivity of the
UHCs along the axial direction linearly increases with the increase of
carbon fiber volume fraction. As can be observed in Fig. 14b, the
transverse thermal conductivity displays a significant enhancement with
the addition of GNPs. For instance, at 50 vol% carbon fiber, the trans­
verse thermal conductivity of the UHCs filled by 5 vol% GNPs increases
by 930 % in comparison with the carbon fiber/epoxy composites. The
reason is that the transverse heat conduction in unidirectional fiber-
reinforced composites is dominated by the matrix properties. As ex­
pected from the properties of graphene, since a small amount of GNPs
significantly enhances the thermal conductivity of the enriched epoxy
matrix therefore, the transverse thermal conductivity of the UHCs can be
increased. The presence of nano-graphene particles in the polymer
matrix can serve to promote the formation of effective heat transfer
pathways between adjacent micron-sized carbon fibers embedded in the
hybrid composite system. Thus, the carbon fiber/graphene/polymer
UHCs can transfer heat in higher efficiency to the surrounding envi­
ronment compared to the traditional CFRPCs which is a crucial issue for
industrial applications. The transverse thermal conductivity of the UHCs
is nonlinearly increased with the increase of carbon fiber volume
fraction.
The variation of carbon fiber/GNP/epoxy UHC thermal conductiv­
ities with the GNP volume fraction along the axial and transverse di­
rections can be observed in Fig. 15 a and b, respectively. The GNP
content varies from 0 to 10 % by volume. The thermal transport per­
formance of UHCs in transverse direction is improved by increasing the
GNPs, as expected from the properties of graphene. The increase of GNP
content contributes to the increase in GNP distribution density in the
polymer matrix, and more thermal conductive paths can be created to
bridge adjacent fibers, which finally results in a higher transverse
thermal conductivity of the UHCs.
The geometrical characteristics of the GNP on the thermal properties
(17)
of carbon fiber/GNP/epoxy UHCs are examined. The thermal conduc­
(18) thermal conductivities asymptotically increase with increasing the GNP
length up to l = 10 μm. It is much noticeable in the case of transverse
thermal conductivities as shown in Fig. 16b. The improvement in the
thermal conductivities may be attributable to the reduced effect of ITR
between the graphene and polymer matrix which leads to an increase in
the thermal conductivity of the enriched epoxy matrix. Furthermore, the
formation of thermal conductive paths between adjacent carbon fibers
(19) becomes easier by the increase of GNP length. At 50 vol% carbon fiber,
8
M.K. Hassanzadeh-Aghdam et al. International Journal of Thermal Sciences 171 (2022) 107209

Fig. 12. Comparison of the model predictions and experimental measurements [50] of the (a) axial and (b) transverse thermal conductivities of the unidirectional
carbon fiber-reinforced epoxy composites.

Fig. 13. Comparison between the results of the SUCM, CCA, upper and lower bounds for the (a) axial and (b) transverse thermal conductivities of the unidirectional
carbon fiber-reinforced epoxy composites.

9
M.K. Hassanzadeh-Aghdam et al. International Journal of Thermal Sciences 171 (2022) 107209

Fig. 14. Effect of GNPs on the (a) axial and (b) transverse thermal conductivities of UHCs.

Fig. 15. Variation of (a) axial and (b) transverse thermal conductivities of UHCs with the GNP volume fraction.

Fig. 16. Variation of (a) axial and (b) transverse thermal conductivities of UHCs with the GNP length.

the value of transverse thermal conductivity increases from 6.2 W/mK
for l = 1.7 μm to 19.98 W/mK for l = 10 μm, i.e., an increase of 222 %.
Accordingly, the ultimate heat transfer ability of UHCs can be hugely
enhanced by the use of higher lengths of GNPs. Fig. 17 a and b show the
axial and transverse thermal conductivities of the carbon fiber/GNP/
epoxy UHCs, respectively, versus the GNP thickness. The thermal con­
ductivity of the hybrid composites, especially in transverse direction,
increases as the GNP thickness decreases. It may be due to the increase in
the GNP thermal conductivity by the decrease of GNP thickness as
shown in Eq. (2). In general, the results prove that GNPs with high aspect
ratio allow heat to transfer rapidly and have a better thermal
performance for the composite structures.
To assess the role of ITR between the GNP and epoxy matrix in the
thermal transport performance of UHCs, the micromechanical analysis
is carried out in the absence and the presence of ITR as revealed in
Fig. 18. The high surface area-to-volume ratio of GNPs causes a large
interfacial region between the nano-graphene and matrix. The phonons
are scattered at the GNP/epoxy interface due to the discrepancy in the
phonon density of state. This leads to that the thermal transport is
extremely hindered. The axial thermal conductivity is not influenced by
the ITR according to the results of Fig. 18a. This may be explained by the
dominant role of carbon fiber properties in axial thermal conductivity of

10
M.K. Hassanzadeh-Aghdam et al. International Journal of Thermal Sciences 171 (2022) 107209

Fig. 17. Variation of (a) axial and (b) transverse thermal conductivities of UHCs with the GNP thickness.

Fig. 18. Effect of ITR on the (a) axial and (b) transverse thermal conductivities of UHCs.

Fig. 19. Variation of (a) axial and (b) transverse thermal conductivities of UHCs with the ITR.

the UHCs. On the basis of the results shown in Fig. 18b, the UHCs in the
presence of ITR exhibit lower thermal conductivity in transverse direc­
tion as compared to the UHCs in the absence of ITR. The presence of the
interface thermal resistance across the GNP/polymer interface leads to a
substantial reduction in the thermal conductivity of the enriched poly­
mer matrix which finally decreases the transverse thermal conductivity
of the UHCs. Note that matrix properties play the dominant role in
effective properties of the fibrous composite systems. The relationship
between the thermal conductivities of the UHCs along the axial and
transverse directions according to the value of GNP/epoxy ITR is shown
in Fig. 19 a and b, respectively. In general, a low resistance to heat
transfer at the GNP/polymer interfacial region becomes technologically
significant for applications for which the UHCs with very high heat
dissipation ability are needed.
In order to illustrate the role of dispersion of GNPs predicted by our
approach in the UHC thermal properties, a comparative study is per­
formed. For two conditions of nano-graphene dispersion, including
uniformly dispersed GNPs, and agglomerated state of GNPs with ξ = 0.5
and ζ = 0.85, the UHC thermal conductivities are predicted and the
numerical results are given in Fig. 20. The UHCs containing uniformly
dispersed GNPs have much higher transverse thermal conductivity than
those containing agglomerated GNPs. From the physical point of view,

11
M.K. Hassanzadeh-Aghdam et al. International Journal of Thermal Sciences 171 (2022) 107209

Fig. 20. Effect of GNP agglomeration on the (a) axial and (b) transverse thermal conductivities of UHCs.

Fig. 21. Variation of (a) axial and (b) transverse thermal conductivities of UHCs with parameter ζ

Fig. 22. Effect of GNP alignment on the (a) axial and (b) transverse thermal conductivities of UHCs.

the UHCs containing uniformly dispersed GNPs are much more efficient
in constructing thermal conductive paths between adjacent carbon fi­
bers. However, the agglomeration of GNPs in the polymer matrix is not
beneficial to form thermal conductive paths. In other words, graphene
agglomeration is found to destroy the heat transfer pathways between
adjacent carbon fibers. The uniform dispersion of GNPs provides higher
thermal conductivity enhancement for the epoxy matrix as compared to
the agglomerated state. As a result, producing the hybrid composites
with homogeneous dispersion of nanoparticles would offer significant
advantages over hybrid composites with non-uniform dispersion of
nanoparticles in terms of the thermal transport performance. Fig. 21
shows the relation between the effective thermal conductivities and
agglomeration parameters (ξ, ζ). The transverse thermal conductivity of
the UHCs is found to rise with increasing ζ up to ξ = ζ and then, it
sharply decreases. The highest thermal conductivity in the transverse
direction is observed when ξ = ζ; i.e. GNPs are uniformly dispersed in
the epoxy matrix. Under such condition, the graphene nanoparticles
within the polymer matrix would likely touch each other or link the
adjacent carbon fibers.
Fig. 22 compares the effects of the GNP alignment on the thermal
transport performance of the carbon fiber/GNP/epoxy UHCs. The nu­
merical results for the uniformly (or perfectly) dispersed GNPs in the

12
M.K. Hassanzadeh-Aghdam et al.
Fig. 23. Variation of thermal conductivity of UHCs with the off-axis angle of
carbon fiber.
polymer matrix are included in this figure. Also, the micromechanical
analysis is performed in the presence and absence of ITR. The axial
thermal conductivity is very negligibly influenced by the variation of
GNP orientation and ITR, as can be seen in Fig. 22a. In contrast, the GNP
orientation significantly contributes to the UHC thermal conductivity in
transverse direction as shown in Fig. 22b. The improvement in the
transverse thermal conductivity of the UHC is maximized when GNPs
are perpendicular to the carbon fibers. The aligned GNPs significantly
enhance the matrix thermal conductivity along the perpendicular to the
carbon fiber.
Fig. 23 displays the predictions of the thermal conductivity of carbon
fiber/GNP/epoxy UHCs as a function of off-axis angle of carbon fibers.
Also, the micromechanical results without GNPs are presented in this
figure. The rate of improvement in thermal conductivity with respect to
the off-axis angle of carbon fibers is increased after the addition of GNPs
within the epoxy resin. In other words, when the fiber orientation varies
from 0◦ to 90◦ , the improvement in the thermal conductivity becomes
more prominent. When the thermal loading is varied from directly in
line with the fiber axis to normal to the fiber axis so-called off-axis
loading, the thermal conductivities of the composite systems vary from
fiber-dominated to matrix-dominated. The material properties of carbon
fiber play the dominant role in the UHC thermal conductivity when the
Fig. 24. Effect of carbon fiber array on the (a) axial and (b) transverse thermal conductivities of UHCs.
13
International Journal of Thermal Sciences 171 (2022) 107209
fiber axis is oriented at the thermal loading direction. The dominate role
belongs to the matrix properties when the thermal loading is normal to
the carbon fiber axis.
The effect of carbon fiber arrangement within the GNP-modified
epoxy nanocomposite matrix on the thermal conductivity of UHCs is
investigated, as shown in Fig. 24. The comparison is made with random
and regular arrangements of the carbon fibers. Both square and hexag­
onal packing arrays are reflected as the regular arrangement. Also, the
fiber random arrangement is assumed to be under uniform statistical
distribution. For this case, the RVE is extended to 50 × 50 sub-cells. It is
observed from Fig. 24a that the axial thermal properties are not affected
by different types of fiber arrangement. But, the outcomes of Fig. 24b
reveal that the square array provides higher thermal conductivity
enhancement along the transverse direction as compared to the random
and hexagonal arrays. The random and the hexagonal arrangements
yield almost the same results for the transverse thermal conductivities.
Generally, the axial properties of fibrous composites are not affected by
the fiber arrangement. But, regular arrangement of fiber with square
array can provide better material properties for the fiber-reinforced
composites [52]. Thus, the highly heat-dissipating UHCs can be fabri­
cated by a square array of continuous fibers.
On the basis of available literature, one can expect an anisotropic
conductivity of GNPs [34]. Using the micromechanical model, an
analysis is performed to investigate the effect of anisotropy of graphene
on the thermal conductivity of the GNP-filled epoxy nanocomposites as
shown in Fig. 25. The results indicate that the transverse thermal con­
ductivity of the graphene has negligibly influence on the nanocomposite
thermal conductivity. However, the axial thermal conductivity of the
GNPs significantly affects the final thermal conductivity of the epoxy
Fig. 25. Effect of GNP anisotropy on the thermal conductivity of the GNP-filled
epoxy nanocomposites.
M.K. Hassanzadeh-Aghdam et al.
Fig. 26. Axial thermal conductivity of the UHC versus carbon fiber vol­
ume fraction.
nanocomposites.
Carbon fibers used in structural applications generally can have
thermal conductivities about 10 W/mK [53]. By the proposed micro­
mechanical method, a sensitive study is performed to investigate the
effect of carbon fiber thermal conductivity on the final thermal con­
ductivities of the UHCs along the axial direction. The micromechanical
results are shown in Fig. 26. It is found that adding GNPs in the polymer
matrix can enhance the axial thermal conductivity of the UHCs as the
fiber thermal conductivity is low about 10 W/mK. For example, when
the carbon fiber volume fraction is 50 %, the incorporation of GNPs at a
loading of 5 vol% results in approximately 26 % enhancement in the
axial thermal conductivity of UHCs. According to the results shown in
Fig. 14a, addition of GNPs does not affect the axial thermal conductivity
of the UHCs when the carbon fiber thermal conductivity is high.
4. Conclusions
A hierarchical micromechanics technique was developed to analyze
the effect of adding the GNPs within the polymer matrix on the thermal
transport performance of the carbon fiber/GNP/epoxy UHCs. The GNPs
improved the transverse thermal conductivity of the UHCs. A high
content, high length, and low thickness of the GNPs led to the
improvement in the thermal conductivity along the transverse direction.
Adding the GNPs in the polymer matrix enhanced the axial thermal
conductivity of the UHCs when the fiber thermal conductivity is low.
The agglomeration of GNPs within the epoxy matrix decreased the ca­
pacity of heat dissipation. Besides, the ITR between the GNP and epoxy
matrix led to the reduction of thermal transport properties. A uniform
dispersion of GNPs and low ITR were effective routs to obtain the
thermally conductive UHCs with the higher performance. It was
observed that GNPs can be perpendicular to the carbon fibers with the
objective of further enhancing the transverse thermal conductivity. The
influences of several critical microstructure aspects related to the carbon
fibers, including the volume fraction, orientation and arrangement type
on the UHC thermal transport properties were examined. Heat can be
more efficiently dissipated by the square array of carbon fibers
embedded in the GNP-epoxy matrix thereby reducing thermal damage.
According to some comparisons, there was a good agreement between
the model predictions and experimental measurements. The developed
micromechanics technique gives a more accurate insight into the ther­
mal transport mechanisms of the general UHC systems which can be
utilized as structural materials in the next-generation.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
14
International Journal of Thermal Sciences 171 (2022) 107209
the work reported in this paper.
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