Carbon 99 (2016) 222e228

Contents lists available at ScienceDirect

Carbon
journal homepage: www.elsevier.com/locate/carbon

Super-elastic graphene/carbon nanotube aerogel: A novel thermal

interface material with highly thermal transport properties
Peng Lv, Xiao-Wen Tan, Ke-Han Yu, Rui-Lin Zheng, Jia-Jin Zheng, Wei Wei*
School of Optoelectronic Engineering, Nanjing University of Posts & Telecommunications, Nanjing 210023, PR China

a r t i c l e i n f o

a b s t r a c t

Article history:
Received 23 April 2015
Received in revised form
9 December 2015
Accepted 10 December 2015
Available online 13 December 2015

Three-dimensional (3D) graphene structure exhibits promising potential in thermal interface materials
(TIMs) due to the continuous network structure and the high thermal conductivity of graphene.
Nevertheless, the very low density and the high porosity of the 3D graphene monoliths usually lead to
poor thermal transport performance. To overcome these problems, we fabricated the graphene/carbon
nanotube (Gr/CNT) aerogels by a synergistic assembly strategy. The entangled CNTs bond the graphene
sheets together to avoid the sliding of them under compression and greatly enhance the elastic stiffness
of cell walls, which brings the aerogels super-elasticity. Bearing a high compression strain of 80%, the
continuous thermal transport paths in Gr/CNT aerogels are still preserved. Signicantly increased thermal conductivity of Gr/CNT aerogels can be obtained by directly mechanical compression. Meanwhile,
the thermal transport properties of Gr/CNT aerogels can be further improved by elevating their initial
density. With an initial density of 85 mg cm
3, a thermal conductivity up to 88.5 W m
1K
1 and a
thermal interface resistance as low as 13.6 m m2KW
1 were obtained, which outperforms other carbonbased TIMs reported previously.
2015 Elsevier Ltd. All rights reserved.

1. Introduction
Development of high-power density electronics made efcient
thermal energy dissipation a critical issue for device lifetime and
speed [1,2]. But gaps between the contact solid surfaces usually
cause high interfacial thermal resistance [3]. Thermal interface
materials (TIMs) inserted between the mating surfaces can conform
well to surface asperities and reduce the temperature across the
interface [4]. In the past decades, signicant attentions have been
focused on developing carbon-based TIMs due to the extraordinarily high theory thermal conductivity of carbon nano-materials
[5e9]. Normally, for achieving high thermal transport properties,
carbon-based TIMs should have the interconnected structure to
ensure the continuous thermal transport, meanwhile own high
exibility for good contact with the mating surface.
Three-dimensional (3D) graphene monoliths have been widely
studied because it can assemble the individual graphene sheets
with dramatic properties into a macroscopic functional architecture. In 3D graphene monoliths with interconnected structure, the

* Corresponding author.
E-mail address: weiwei@njupt.edu.cn (W. Wei).
http://dx.doi.org/10.1016/j.carbon.2015.12.026
0008-6223/ 2015 Elsevier Ltd. All rights reserved.

heat uxes conduct along the graphene sheets and come together
at their junctions, then continue to transport to adjacent graphene
sheets, which brings 3D graphene monoliths continuous thermal
transport paths. And, the ultrahigh exibility of graphene sheets in
3D graphene monoliths is benecial to its matching to the mating
surface [10]. Thus, 3D graphene monoliths show great promise in
developing high performance TIMs.
There are several literature reported the thermal transport
properties of 3D graphene monoliths [10e14]. The measured
thermal conductivities of graphene foam grown by chemical
vapour deposition (CVD) were 1.7 W m
1K
1 (grown on nickel
foam) [12] and 8.28 W m
1K
1 (grown on porous Al2O3) [11]. And
some phase change materials were also introduced into graphene
aerogel [10] and CVD-graphene foam [13], obtaining the thermal
conductivities of 2.635 W m
1K
1 [10] and 0.44 W m
1K
1 [13],
respectively. It is noteworthy that the thermal conductivity of these
3D graphene monoliths mentioned above is lower than that of
other carbon-based TIMs [5e9] and far below that of single layer
graphene [15]. The major reason is attributed to the very low graphene volume fraction and the ultrahigh porosity of 3D graphene
monoliths [12]. Unfortunately, the most straightforward way, mechanical compression, is unable to decrease their porosity, since
these 3D graphene monoliths easily collapse under pressure.

P. Lv et al. / Carbon 99 (2016) 222e228

Recently, some studies about 3D graphene monoliths with

super-elasticity have attracted intense interests. The super-elastic
graphene foams, aerogels and monoliths prepared by CVD
method [16], freeze-casting strategy [17,18], 3D printing technique
[19] and hydrothermal process [20] show excellent mechanical
properties, especially the high compressibility (compressive strain
up to 60%~90%). These progresses provide new insight and strategy
for developing high performance TIMs: fabricating a novel superelastic graphene monolith with continuous thermal transport
path even under high compressive deformation; then signicantly
improving the thermal conductivity of 3D graphene monoliths by
simply mechanical compression.
In this study, we fabricated the super-elastic graphene/carbon
nanotube (Gr/CNT) aerogels by hydrothermal method and subsequent freeze-drying process. The aerogels with a 3D framework are
constructed with cell walls of graphene sheets and entangled CNTs
coating on them (Fig. 1). The entangled CNTs bond the graphene
sheets together to avoid the sliding of them under compression and
enhance the elastic stiffness of cell walls, which offers the asprepared aerogels super-elasticity. Resulting from the excellent
mechanical properties, Gr/CNT aerogels can afford high compression while maintain the continuously thermal transport paths. The
maximum thermal conductivity of Gr/CNT aerogel TIMs reaches up
to 88.5 W m
1K
1 and the thermal interface resistance is as low as
13.6 mm2 KW
1, which outperforms other carbon-based TIMs in
literature.

2. Experimental details
2.1. Preparation of 3D Gr/CNT aerogel
Graphene oxide (GO) was prepared by the modied Hummers
method from natural graphite and got exfoliated GO sheets in their
aqueous dispersions according to the previous process [21]. CNTs
(diameter of 30e50 nm, length of 50e100 um) were functionalized
by reuxing in the mixture of concentrated H2SO4 and HNO3 (3:1
by volume) for about 80 min, and then collected by repeated
centrifuging and washing with deionized water. After gentle stirring, we obtained aqueous functionalized CNTs (fCNTs) dispersions.
Typically, fCNT aqueous dispersion was added into GO aqueous
dispersion with a mass ratio of GO:fCNTs 3:1. Gr/CNT hydrogel
assembled with GO sheets and fCNTs was prepared using a hydrothermal reaction maintained at 180  C for 12 h in a Teon-lined
autoclave. After washing the as-obtained hydrogel with distilled
water following with freeze-drying, the Gr/CNT aerogel was

223

produced. A neat graphene aerogel without CNTs was also prepared

in the same way for comparison. In addition, Gr/CNT aerogels with
various initial densities were also prepared by controlling GO/fCNT
concentrations. The as-prepared aerogels were dened as Gr/CNT-n
(n 2, 3, 4, 5) based on the GO/fCNT concentration of 2, 3, 4 and
5 mg mL
1, respectively.
2.2. Characterizations
Scanning electron microscope (SEM) imaging was conducted on
a Hitachi S4800 eld-emission SEM system with a 5 kV accelerating
voltage. Mechanical tests were done by a single-column system
(Instron 5843) equipped with two at-surface compression stages
and 1 kN load cells. The initial density (ri) and the compression
density (rc) of the samples were calculated as the mass of the
samples divided by their corresponding volumes without and with
compression, respectively.
2.3. Measurement of thermal transport properties
The samples were prepared in cylindrical shape (~12 mm in
diameter and 1.5 mm in height) for the measurement of thermal
transport properties. The thermal resistance measurement system
designed in accordance with the standard of American Society for
Testing and Materials (ASTM) D5470. In a typical testing procedure,
a sample was inserted into two parallel Cu blocks and compressed
into a thin lm with the affordable compressive strain. The thermal
interface resistance of TIMs (RTIM) was measured by employing Eq.
(1). And thermal conductivity (k) of TIMs and thermal contact
resistance (Rc) across TIM/Cu interface were calculated by the
simultaneous linear equations of Eq. (2) by varying the TIM thickness (l):

RTIM

DT$ASample
Q

RTIM 2RC

l
k

(1)

(2)

Where ASample is the cross-sectional area of the samples, Q is the

thermal ux through the sample, and DT is the temperature
gradient across the sample, respectively.
3. Results and discussion
The micro-morphologies of a neat graphene aerogel with initial

Fig. 1. Schematic illustration for the micro-structure of Gr/CNT aerogels and cartoon models of entangled CNTs preventing the sliding of overlapping graphene sheets and avoiding
splitting of the wrapping graphene sheets. (A colour version of this gure can be viewed online).

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P. Lv et al. / Carbon 99 (2016) 222e228

density of 25 mg cm
3 (Fig. 2 aec) and the Gr/CNT-2 aerogel with

initial density of 23 mg cm
3 (Fig. 2 def) were observed under SEM.
As shown in Fig. 2a, the neat graphene aerogel exhibits a 3D
interconnected porous structure with the cell dimension in range of
2e10 mm, similar to those of previously reported graphene aerogels
[22,23]. Each cell possesses stretched ligaments in the walls that are
joined at the nodes or junctions. The zoom-in SEM images indicate
that the cellar walls consist of partially overlapping (Fig. 2b) and
wrapping graphene sheets (Fig. 2c). However, the p-p interactions
between the adjacent graphene sheets are too weak to construct
the macroscopically graphene aerogels with good mechanical
strength. The graphene sheets easily move past each other when
the graphene aerogels are under external force.
After introducing CNTs into 3D graphene monoliths, the interconnected structure and the cell dimension remain nearly unchanged for Gr/CNT-2 aerogel (Fig. 2d). The CNTs are evenly
distributed in the aerogel (Fig. 2e), which is attributed to CNTs well
dispersed by acid-treatment and well combined with GO sheets
during the hydrothermal process. The structural change of GO
sheets and fCNTs before and after hydrothermal process is reected
by the X-ray diffraction spectra and Raman spectra (Fig. S1). It indicates that the hydrothermal process removes partial oxygen
containing functional groups of GO and fCNTs, which would provide strong p-p interaction between graphene sheets and CNTs.
Closer views (Fig. 2e and f) reveal the highly entangled CNTs
covering the ligaments and junctions of cellar walls, which can
avoid the sliding and splitting of graphene sheets and further
enhance the stiffness of cell walls (The corresponding cartoons of
the interconnections between CNTs and graphene sheets are displayed in Fig. 1). As shown in SEM images of the cross section
(Fig. 2d) and the vertical section (Fig. S2) of Gr/CNT-2, the aerogels
prepared by the hydrothermal process present an isotropic structure. This phenomenon is different from the anisotropy of the
graphene monoliths prepared by freeze-casting process [17,18] but
consistent with the isotropic graphene aerogels fabricated using
hydrothermal strategy [20,24]. Thus, the Gr/CNT aerogels would
present similar mechanical properties and thermal transport
properties in the cross-plane direction and the in-plane direction.
As aforementioned, the compressibility is of particular interest
for the thermal transport properties of a 3D graphene structure.
The compression experiments were performed to evaluate the
mechanical performances of the neat graphene aerogel and the Gr/
CNT aerogel. As shown in Fig. 3a, both neat graphene aerogel and
Gr/CNT aerogel with similar initial density can be squeezed into

pellet under certain pressure. Once the external pressure is

removed, the neat graphene aerogel deforms permanently indicating a structural collapse. In contrast, the Gr/CNT aerogel is able to
almost completely recover to its original shape rapidly.
The compressive curves of the graphene aerogel and Gr/CNT-2
aerogel are shown in Fig. 3b. We could not measure during
unloading of the graphene aerogel because they permanently
deformed during loading to strain of 25%. SEM images of a neat
graphene aerogel after compression shows that the cell walls are
densely packed and are almost parallel from one to another
(Fig. S3). The plastic deformation of the graphene aerogel prepared
by the hydrothermal method is due to the lack of a restorative force
to act on the graphene frameworks. Previous studies [17] suggest
that when 3D graphene monoliths made of few layers of graphene
is severely compressed, the intersheet van der Waals adhesion
would overwhelm the elastic energy stored, preventing elastic
recovery.
In contrast, Gr/CNT-2 aerogel shows super-compressibility and
can bear a compression strain as high as 80%, which close to the
highest value (up to 90%) of 3D graphene monoliths reported
previously [19,25,26]. Fig. S4 also shows its stressestrain curves at
various maximum strains. Similar to other open-cell elastomeric
foams [27e29], the loading process shows three distinct regions:
strain<10%, nearly linear elastic regime, corresponding to bending
of cell walls; 10% < strain<70%, relatively at stress plateau, corresponding to elastic buckling of cell walls; and strain>70%, abrupt
stress increasing regime, corresponding to densication of cells.
Hysteresis loops appear due to dissipation of mechanical energy.
And the stress keeps above zero until strain 0 suggesting the Gr/
CNT-2 aerogel can completely recover to its original volume. The
super-elasticity is also reected from the in situ observation of the
full recovery of cell structure under large strain (insert of Fig. 3b).
The super-elasticity of Gr/CNT aerogel is attributed to its unique
hierarchical structure and the interaction between CNTs and graphene sheets. Firstly, the entangled CNTs attach on the graphene
sheets and tightly bond them together, which ensure the deformation of cell walls rather than the sliding between them during
the compression. It is similar to the exible safety net used for
preventing rock falling and landslip (Fig. S5). Secondly, the coating
of CNTs reinforces the relatively exible graphene substrate and
endows their intrinsic elasticity [30] to the co-organized aerogel.
When the aerogels are subjected to external stress, the load can
effectively transfer from the loosely connected graphene sheets to
the entangled CNT nets, which can greatly enhance the strength

Fig. 2. SEM images of 3D porous structure of (aec) neat graphene aerogel and (def) Gr/CNT-2 aerogel with similar initial density. Microscopic cellar wall architecture consisting of
partially (b) overlapping graphene sheets and (c) wrapping graphene sheets for neat graphene aerogel, and entangled CNTs covering (e) overlapping graphene sheets and (f)
wrapping graphene sheets for Gr/CNT-2 aerogel.

P. Lv et al. / Carbon 99 (2016) 222e228

225

Fig. 3. (a) Digital photographs show that the neat graphene aerogel collapses and the Gr/CNT aerogel recovers its original shape after compression. (b) Compressive stressestrain
curves for neat graphene aerogel along the loading direction and for Gr/CNT-2 aerogel during loadingeunloading cycle. Inserts: SEM images showing the deformation process of Gr/
CNT-2 aerogel at 70% and back to 40%. Scale bars, 5 mm (c) stressestrain curves of several selected cycles on Gr/CNT-2 aerogel during repeated compression (the 1st, 2nd, 10th, 100th,
1000th cycle). (d) The corresponding maximum stress and energy loss coefcient for different cycles derived from (c). (A colour version of this gure can be viewed online).

and elastic stiffness of cell walls, allowing the van der Waals
adhesion to be overcome by the elastic energy.
Furthermore, the cyclic strain-stress curves of Gr/CNT-2 aerogel
at strain up to 60% are shown in Fig. 3c. The stressestrain curves of
the 1000th cycle are similar to that of the rst cycle, with the
exception that the maximum compressive stress decreases slightly
to 76.3% of the original value. The ratio of energy dissipated during
compression was calculated and presented in Fig. 3d. The rst cycle
yields an energy loss coefcient of 78% and this coefcient remains
constant at 71% since the 10th cycle, indicating excellent mechanical robustness of the Gr/CNT aerogel.
Thermal transport properties of the neat graphene aerogel and
the Gr/CNT aerogel were also compared. The values of thermal
interface resistance, thermal conductivity, and thermal contact
resistance of the neat graphene aerogel (initial thickness of 1.5 mm)
at the highest affordable strain (25%) are 379.4 mm2 kW
1,
3.2 W m
1K
1, and 14.2 mm2 KW
1, respectively. In comparison,
the Gr/CNT-2 aerogel (initial thickness of 1.5 mm) at strain of 25%
shows slightly higher thermal conductivity of 5.7 W m
1K
1, which
may be attributed to the conductive bridging effect of CNTs between the graphene sheets. As being pointed out in previous
studies, CNTs between adjacent graphitic layers can act as the
additional heat ux paths and thus improve the thermal conductivity [3,31]. When the strain of Gr/CNT aerogel reached 80%, the
thermal conductivity is as high as 42.3 W m
1K
1, and the thermal
interface resistance and the thermal contact resistance are only
19.5 and 6.2 mm2 KW
1, respectively. The signicant improvement
of thermal transport properties is mainly due to the increased
density (increased from 23 to 159 mg cm
3) of the Gr/CNT-2 aerogel under mechanical compression. Meanwhile, the continuous
thermal transport paths of the Gr/CNT aerogel can be saved even
under high compression, which is also very important for the high

thermal transport properties.

As mentioned above, the thermal conductivity of 3D graphene
monoliths is limited by the very low density [10e12,14]. To further
improve the thermal transport properties of the super-elastic Gr/
CNT aerogels, it is feasible to prepare denser aerogels by increasing
the initial density. Gr/CNT-2~5 aerogels with GO/fCNT concentration of 2e5 mg mL
1 were prepared to investigate the effect of
initial density on the thermal transport properties. The initial
densities of Gr/CNT aerogels increase from 23 to 85 mg cm
3 corresponding to GO/fCNT concentrations from 2 to 5 mg mL
1
(Table 1). As shown in Fig. 4aec, with increasing GO/fCNT concentration, the porous structure becomes denser and the average
pore size is smaller. And the 3D interconnected structure keeps
well, even when GO/fCNT concentration is as high as 5 mg mL
1.
The stressestrain curves of Gr/CNT-3, -4 and -5 aerogels present the
similar shapes with Gr/CNT-2 at strain of 80% (Fig. 4d). The
maximum stress at 80% strain increases from 60.1 KPa for Gr/CNT-2
aerogel to 153.2 KPa for Gr/CNT-5 aerogel. The increase of stress is
due to the smaller pore size of the aerogel providing higher stiffness
and compressive strength. Fig. 4e presents the dependence of the
compressive stress (corresponding to the maximum strains) on the
aerogel initial density. At the low maximum strain (30%), the stress
increases almost linearly with initial density; while for the high
maximum strain (80%), the stress increases abruptly with the initial
density. Such an abrupt rise can be attributed to cell wall densication, which is inuenced by both the aerogel density and the
applied strain.
Table 1 shows the density change and the thermal transport
properties of Gr/CNT aerogels at compressive strain of 80%. The
compression densities of Gr/CNT aerogels are ~5 times higher than
the initial densities, reaching 159e424 mg cm
3. It is found that the
thermal conductivity of Gr/CNT aerogels increases signicantly

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P. Lv et al. / Carbon 99 (2016) 222e228

Table 1
The initial density (ri) of various Gr/CNT aerogels, and their corresponding compression density (rc), thermal conductivity (k), thermal contact resistance (Rc) and thermal
interface resistance (RTIM) at compressive strain of 80%.
Samples

ri (mg cm
3)

rc (mg cm
3)

k (Wm
1 K
1)

Rc(mm2 KW
1)

RTIM(mm2 KW
1)

Gr/CNT-2
Gr/CNT-3
Gr/CNT-4
Gr/CNT-5

23
46
61
85

129
231
305
424

42.3
63.9
77.5
88.5

6.2
5.7
5.5
5.1

19.5
16.1
14.8
13.6

Fig. 4. SEM images of (a) Gr/CNT-3, (b) Gr/CNT-4 and (c) Gr/CNT-5 aerogels, respectively. (d) Stress-strain curves of Gr/CNT-3, -4 and -5 aerogels, respectively. (e) Density
dependence of compressive stress. (A colour version of this gure can be viewed online).

with the initial density. Gr/CNT-5 aerogel with initial density of

121 mg cm
3 presents maximum value of 88.5 W m
1K
1. It means
that the robust structure of Gr/CNT aerogels can keep the 3D
continuous thermal transport paths well at high initial density. But
the thermal transport properties of Gr/CNT aerogel with higher
initial density (>85 mg cm
3) are not considered in the present
work. Because it requires too large pressure to compress denser
aerogels to strain of 80% (Fig. 4e). The increase of initial density of
Gr/CNT aerogels also leads to the slight decrease of thermal contact
resistance across the sample/Cu interface (from 6.2 mm2 KW
1 to
5.1 mm2 KW
1), because the higher pressure favours the better
contact. The thermal interface resistance, as the major parameter
for comparing TIM thermal transport performances, is as low as
13.6 mm2 KW
1 for the Gr/CNT-5 aerogel. Although there are
several super-elastic 3D graphene monoliths have been reported
previously, the densities of these 3D graphene monoliths
(0.161 mg cm
3 [32], 0.5e0.6 mg cm
3 [17], 0.3e14 mg cm
3 [25])
are not high enough to obtain high thermal transport properties
even at the high compressive strain of 90%.
The thermographic image of the Gr/CNT-5 aerogel inserted into
two parallel Cu blocks and pressed under 153 kPa according to the
one dimensional reference bar method (Fig. 5a) was photographed
to directly characterize the thermal transport performance. Fig. 5b
shows the comparison of thermographic images with and without
Gr/CNT-5 aerogel under the same heat ow of 130 KWm
2. The
temperature difference is obvious at the CueCu dry contact interface as shown in the left of Fig. 5b, indicating poor thermal transport across the interface without TIMs. In comparison, the

temperature gradient almost disappears with the presence of Gr/

CNT-5 aerogel (right of Fig. 5b). Fig. 5c presents the plot of the
temperature drop across the interface with and without Gr/CNT-5
aerogel. And the aerogel signicantly decreases the interfacial
temperature drop from 15  C (under dry contact) to only 3.2  C,
indicating the effectiveness of Gr/CNT aerogel in the reduction of
thermal interface resistance.
The super-elastic Gr/CNT aerogels show excellent thermal
transport properties than other carbon-based TIMs. It overcomes
the drawbacks of brittle 3D graphene monoliths and provides much
higher thermal conductivity than the reported value of the brittle
3D graphene monoliths [10e12]. Although the graphite-based TIMs
own high thermal conductivity along the in-plane direction
(>200 W m
1K
1), the thermal conductivity across the thickness
direction of graphite-based TIMs (5e24.3 W m
1K
1) [31,33,34] is
much lower than that of our Gr/CNT aerogels. By comparing the
thermal transport properties of our Gr/CNT aerogels with the
commercial available TIMs, the thermal interface resistance of the
Gr/CNT-5 aerogel with compression thickness of 0.3 mm is much
lower than that of graphite foil with the thickness of 0.115 mm
(52 m m2KW
1) [35] and silicon grease with thickness of 0.02 mm
(27 m m2KW
1) [35].
The thermal transport properties of the Gr/CNT-5 aerogel are
even better than that of some best carbon-based TIMs reported
previously, such as VACNT array, CNT buckypaper, and vertical
graphene (Fig. 6). The relatively high thermal conductivity value of
Gr/CNT-5 aerogel is attributed to that the density of the compressed
aerogels (up to 424 mg cm
3) is much larger than that of VACNT

P. Lv et al. / Carbon 99 (2016) 222e228

227

Fig. 5. (a) Thermal interface testing of Gr/CNT aerogel. (b) Thermographic images of the copper blocks under steady state cooling without and with Gr/CNT-5 aerogel. (c) Plots of the
temperature drop across the interface without and with Gr/CNT-5 aerogel. (A colour version of this gure can be viewed online).

cell walls rather than sliding between them and enhance the elastic
stiffness of the cell walls. The compression experiment results show
that Gr/CNT aerogels can be compressed to 80% strain and are able
to almost completely recover to its original shape. And the thermal
conductivity of Gr/CNT-2 aerogel is much higher than that of neat
graphene aerogel with similar initial density, which is attributed to
the signicantly increased density of the aerogels under compression. In addition, the thermal transport properties of Gr/CNT aerogels are improved by increases their initial density. A maximum
thermal conductivity of 88.5 W m
1K
1 and a minimum thermal
interface resistance of 13.6 mm2 KW
1 of the Gr/CNT-5 aerogel
with initial density of 85 mg cm
3 are obtained. The comparison of
thermal transport properties between Gr/CNT aerogels and other
carbon-based TIMs indicates the advantages of Gr/CNT aerogel
TIMs and suggested the prospective applications in advanced
thermal management.
Acknowledgement
We acknowledge nancial support by the National Natural Science Foundation of China (grant nos. 51503102 and 61274054), the
Natural Science Foundation of Jiangsu Province, China (grant no.
BK20140869) and NUPTSF (grant nos. NY214055 and NY213082).
Fig. 6. Comparison of thermal transport properties of carbon-based TIMs reported
previously (refs [8,32,35,37e39]) with the results in this work. (A colour version of this
gure can be viewed online).

3

3

array (60 mg cm [36]) and CNT buckypaper (260 mg cm [35]),

meaning more carbon nano-materials in unit volume participating
in thermal transport. The relatively low thermal interface resistance of Gr/CNT aerogels results from ultrahigh exibility of graphene sheets and CNTs benecial to its matching to mating surface
under pressure. As described in Eq. (2), TIMs with larger thickness
should present higher thermal interface resistance. But the thermal
interface resistance of the Gr/CNT-5 aerogel with compression
thickness of 300 mm is even lower than that of CNT buckypaper
with thickness of 56 mm [35] and that of CNT epoxy with thickness
of 6 mm [36], and is similar with that of CNT array with thickness of
7 mm [37]. These excellent performances suggest the promising
potentials of Gr/CNT aerogels in current demanding thermal management for electronic and photonics devices.

4. Conclusions
Gr/CNT aerogels with super-elasticity were prepared by a synergistic assembly strategy. The highly entangled CNTs were introduced into 3D graphene monoliths to make sure the deformation of

Appendix A. Supplementary data

Supplementary data related to this article can be found at http://
dx.doi.org/10.1016/j.carbon.2015.12.026.
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