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Results in Physics
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A R T I C LE I N FO A B S T R A C T
Keywords: Graphene nanoplatelets have emerged as an efficient filler in matrices due to their remarkable thermal con-
Composite materials ductivity and electrical conductivity. What is not entirely clear, however, is how the physical properties of the
Thermal properties derived composite materials are directionally dependent. The primary focus of this study was on determining
Electrical properties this dependence. The electrical and thermal properties of the composite materials were studied to understand
Graphene-nanoplatelets
what causes anisotropy and how to control this phenomenon effectively. The results indicated that graphene-
Anisotropy
Thermal interface materials
nanoplatelet-based composite materials can possess a high degree of anisotropy with respect to electrical and
thermal conductivity. Electrical and thermal anisotropy in the derived composite materials arise due to the
alignment of graphene nanoplatelets in the matrices resulting from very high compression. This allows a thermal
management system to be designed to preferentially transfer energy in selected directions. The physical prop-
erties are very different, by up to three orders of magnitude with respect to electrical conductivity and five times
with respect to thermal conductivity, in different directions. The degree of anisotropy increases with decreasing
the viscosity of the matrix. Implications of the results on thermal management applications were discussed, and
recommendations were also presented on the development of graphene-nanoplatelet-based thermal interface
materials.
Introduction materials have fallen short of predicted thermal conductivity values due
to their high thermal interface resistance [15,16].
Thermal interface materials are typically used to facilitate the dis- Graphites [17,18], in particular graphene nanoplatelets [19,20],
sipation of thermal energy from a heat source, more particularly from have many unique physical properties, making it potentially suitable
an electronic package [1,2]. This has become an increasingly important for use in the dissipation of thermal energy from microelectronic de-
problem due to the rapid growth of the electronics industry [3,4]. vices. These materials are readily applicable to thermal management
Commercial thermal interface materials are typically based on com- applications [21,22] due to its ability to conform to any surface aspe-
posites filled with thermally conductive particles such as silver, alu- rities and particularly its extraordinary thermal conductivity. For in-
mina, aluminium, or silica [5,6]. However, these composite materials stance, the thermal conductivity of pyrolytic graphite has been found to
typically require a filler volume fraction of about 70% in order to be approximately 2000 W/m·K at room temperature [23,24]. These
achieve thermal conductivity values in the range of approximately characteristics are of importance to the optimum design of thermal
2.0–5.0 W/m·K [7,8]. Several forms of carbon materials have been used management systems [25,26]. With consideration of the material cost,
as fillers in composite materials [9,10]. In particular, carbon nanotubes the thermal contact conductance, the chemical reactivity, and the
have emerged as an efficient filler in polymer matrices owing to their processing complexity, carbon black is a much more attractive choice
superior mechanical strength, extraordinary electrical conductivity, than graphene nanoplatelets as a filler for thermal interface materials
high thermal conductivity, moderate chemical stability, and high aspect [27,28]. However, the thermal properties of graphene-nanoplatelet-
ratio [11,12]. For example, the thermal conductivity of an individual based composite materials can be directionally dependent, thus al-
single-walled carbon nanotube has been found to be approximately lowing thermal management systems to be designed to preferentially
3500 W/m·K in the longitudinal direction at room temperature [13,14]. transfer energy in selected directions [29,30]. Graphites are made up of
Despite significant recent progress, carbon nanotube based composite layer planes of hexagonal arrays of carbon atoms [31,32], which are
⁎
Corresponding author at: Department of Energy and Power Engineering, School of Mechanical and Power Engineering, Henan Polytechnic University, 2000
Century Avenue, Jiaozuo, Henan 454000, PR China.
E-mail address: cjj@hpu.edu.cn (J. Chen).
https://doi.org/10.1016/j.rinp.2019.102608
Received 11 July 2019; Received in revised form 19 August 2019; Accepted 20 August 2019
Available online 23 August 2019
2211-3797/ © 2019 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/BY-NC-ND/4.0/).
J. Chen and X. Gao Results in Physics 15 (2019) 102608
usually referred to as graphene layers or basal planes [33,34]. Highly and base oil are also typical matrix materials for use in thermal man-
ordered graphites typically possess a high degree of anisotropy due to agement applications. The combination of oil and graphene nanopla-
the preferred orientation of crystallites [35,36]. Arguably, the most telets can improve conformability and, therefore lower the thermal
fundamental aspect of anisotropy is the relationship between structure resistance at contacting surfaces [55,56].
and properties [37,38].
Exfoliated graphene nanoplatelets are new types of nanoparticles Preparation of composite materials
made from graphite. This sheet material has attracted increasing in-
terest as a new form of thermally conducting filler due to their ex- To focus primarily on the influence of the type of matrices, all
tremely high level of the intrinsic thermal conductivity in the directions thermal interface materials were prepared in a similar way. The ma-
parallel to the carbon layers [39,40]. For instance, the thermal con- terial preparation process described herein is provided for the epoxy
ductivity of suspended single layer graphene has been found to be in the resin only. On the other hand, only the epoxy resin was used to prepare
range from 1500 to 2500 W/m·K at room temperature [41,42]. This a series of cured composite materials in accordance with the method
feature facilitates the formation of an efficient conductive network described below.
within a matrix material [43,44]. Graphene nanoplatelets also possess a Shear mixing (Fisherbrand™ 850 Homogenizer, Fisher Scientific
high degree of anisotropy caused by the orientation structure of gra- International, Inc., Pittsburgh, Pennsylvania, United States) of graphene
phite layers [45,46]. Knowledge of electrical and thermal anisotropy is nanoplatelets in acetone was performed at 2000 rpm for one hour at
important in identifying effective energy transport processes in thermal room temperature. Subsequent application of ultrasonic irradiation for
interface materials. It is therefore of great significance to understand eight hours resulted in stable suspensions of graphene nanoplatelets.
what causes anisotropy and how to control this phenomenon effectively The epoxy resin was added to the dispersion of the filler, and shear
for thermal interface materials. Nanometer-scale structures often dic- mixing was performed on the mixture at 2000 rpm for one hour. The
tate the flow of energy in graphene-nanoplatelet-based composite ma- solvent was then removed by heat treatment at approximately 50° C in a
terials [47,48]. For thermal management applications, a high degree of vacuum oven for 20 h. The mixture was subsequently used to prepare a
anisotropy would be particularly advantageous, since it causes the series of epoxy matrix composite materials, including thermal interface
transport of energy to remain fixed, for example, in thermal interface materials and cured composite materials.
materials in some desired direction. However, in spite of the increasing To prepare epoxy matrix thermal interface materials, the mixture
importance of thermal management in thermal interface materials, was processed utilizing a dual asymmetric centrifugal mixing system
there does not exist a unified fundamental understanding of the nan- DAC 1100.1 VAC-P (FlackTek Inc., Landrum, South Carolina, United
ometer-scale structural features contributing to the transport of energy States) at 3200 rpm for 2 min to produce thermally conductive greases.
in graphene-nanoplatelet-based composite materials [49,50]. It is Thermal grease is commonly used as a main kind of thermal interface
therefore necessary to determine how their physical properties are di- materials in the electronics industry. The prepared thermal interface
rectionally dependent. materials did not cure, without adding any curing agent, and their
Graphene-nanoplatelet-based composites are regarded as a poten- viscosity would allow them to stay in position during use. It is worth
tially fruitful area for the development of fundamentally new thermal noting that the prepared thermal interface materials were mainly in the
interface materials. A fundamental understanding of the relationships form of pastes. All the prepared thermal interface materials were
between processing, structure, and anisotropic properties is a major compressed and rolled into thin films so as to obtain roll-induced ani-
goal of this area of research [51,52], which may lead to optimum sotropy. The alignment of graphene nanoplatelets in the matrices re-
performance of thermal interface materials reinforced with graphene sults from high compression, for example, roll pressing. More specifi-
nanoplatelets. However, further investigations into the anisotropic cally, high compression treatment was performed at a pressure of
properties of such materials are needed to understand the reinforcing 0.2 MPa and a temperature of about 60° C for about 2 h.
mechanism at work in different directions. The objective of this study is To prepare cured composite materials, the amine curing agent was
to determine the directional dependence of electrical and thermal added to the prepared thermal interface materials while continuously
properties for graphene-nanoplatelet-based composite materials. The stirring. The mixture containing the curing agent was processed uti-
importance of matrix viscosity in the degree of anisotropy was high- lizing the dual asymmetric centrifugal mixing system to produce a
lighted with respect to electrical and thermal conductivity. Particular thermally conductive grease. The prepared grease was compressed and
emphasis was placed on understanding what causes anisotropy and how rolled into a thin film so as to obtain roll-induced anisotropy. The thin
to control this physical phenomenon effectively, as it is crucial to the film was subsequently loaded into a stainless steel mold, degassed, and
development of nearly all graphene-nanoplatelet-based composite ma- heated in vacuum. Heat treatment and high compression treatment
terials, especially for thermal management applications. were performed simultaneously at a pressure of 0.4 MPa and a tem-
perature of about 100° C for about 2 h, followed by additional heat
Methods treatment and high compression treatment at a pressure of 0.2 MPa and
a temperature of about 150° C for about 2 h to complete the curing
Materials cycle.
2
J. Chen and X. Gao Results in Physics 15 (2019) 102608
Results
3
J. Chen and X. Gao Results in Physics 15 (2019) 102608
Fig. 4. Effect of the type of matrices on the ratio of anisotropy of the electrical
conductivity of thermal interface materials and cured composite materials.
4
J. Chen and X. Gao Results in Physics 15 (2019) 102608
5
J. Chen and X. Gao Results in Physics 15 (2019) 102608
Fig. 7. (a) Schematic illustration of a real thermal interface material and associated temperature distribution. (b) Preferred orientation of graphene nanoplatelets in
the thermal interface material.
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