Composites Part A 135 (2020) 105912

Contents lists available at ScienceDirect

Composites Part A
journal homepage: www.elsevier.com/locate/compositesa

Highly thermally conductive polypropylene/graphene composites for T

thermal management
⁎,1 ⁎
Na Songa, , Donglei Caoa,1, Xian Luob, Qi Wanga, Peng Dinga, , Liyi Shia
a
Research Center of Nanoscience and Nanotechnology, Shanghai University, 99 Shangda Road, Shanghai 200444, PR China
b
State Key Laboratory of Solidification Processing, Northwestern Polytechnical University, Xi’ an, Shaanxi 710072, PR China

A R T I C LE I N FO A B S T R A C T

Keywords: As an indispensable part of electronic devices, efficient thermal management materials can promote heat dis-
PP composites sipation of electronic products quickly, thereby greatly improving their reliability, stability and service life.
Interfacial thermal resistance Here, a simple “in-situ building” approach was developed to fabricate highly thermally conductive poly-
3D graphene network propylene (PP)/graphene composites with three-dimensional graphene framework. Different from conventional
Thermal conductivity
filler modification, a unique matrix functionalization method, inspired by mussel, was carried out to form the
interaction (hydrogen bonding and π-π conjugate) between PP and graphene, which greatly reduced interfacial
thermal resistance. The obtained composite exhibits a quite high through-plane thermal conductivity
(10.93 W·m−1·K−1, almost 55 times higher than that of pure PP), and shows excellent heat dissipation when
used as a thermal management material in LED integration. The composite has the potential application in heat
dissipation of high power and highly integrated electronic devices.

1. Introduction problems: constructing a continuous two-dimensional (2D) or three-

Heat diffusion is important for the efficiency, service life and
credibility of electronic devices. The rapid development of miniatur-
ized, powerful densified electronic devices makes thermal dissipation a
bigger challenge [1]. Highly thermally conductive polymer-based
composites are desired to meet heat dissipation requirement due to
their good processability, lightweight, design flexibility, corrosion re-
sistance, lower processing cost, etc. [2]. However, according to the
Debye equation, thermal conductivity (TC) of polymers is too low
(0.1–0.5 W·m−1·K−1) to meet the application in thermal management
because of their quite small phonon mean free path [3]. Adding ther-
mally conductive fillers to polymers is an efficient way to improve their
TC by constructing additional phonon transmission paths [3,4]. Mixing
is one common method for preparing highly thermally conductive
polymer composites, including melt blending [5], solution blending [6]
or in-situ polymerization [7], etc. Before blended with polymers, fillers
are often chemically functionalized to promote the uniform dispersion
and construct thermally conductive pathways. Paradoxically, in some
cases, TC of modifiers may be low [8]. What’s more, sometimes che-
mical functionalization of fillers does not work well owing to the in-
troduction of more defects and decreased intrinsic TC [3].
Therefore, researchers raised another way to solve the above
dimensional (3D) thermally conductive network using ice-template
method [2], chemical vapor deposition (CVD) method [9], hot-pressing
method [10], electrospinning technology [11], layer-by-layer assembly
[12] and so on. High-thermal-conductive fillers networks are like the
“highway” for phonon transmission. Consequently, composites with
enhanced TC several times or even dozens of times were obtained. Yang
et al. [13] and Lin et al. [10] raised a coating graphite/graphene on PP
and hot pressing method to construct interconnected graphene frame-
works in PP-based composites. TC of obtained composites increased
2600% and 665%, respectively. Yet, as is known to all, phonon trans-
mits not only along thermally conductive skeletons, but also through
the matrix and interface between the filler and the matrix. The weak
interaction at the interface leads to phonon scattering, which limits the
further improvement of TC. For non-polarity polymers (such as poly-
propylene (PP) and polyethylene (PE)), improving the interaction with
fillers is a bigger challenge [10].
The frequently-used fillers are metal materials (copper, aluminum,
silver, etc.), inorganic non-metallic materials (boron nitride, alumina,
silica, etc.), carbon materials (graphite, graphene, carbon nanotubes,
etc.) and so on [14–17]. Graphene is a two-dimensional carbon nano-
material composed of sp2-hybridized carbon atoms, appearing honey-
comb-like hexagonal lattice structure [18]. Using graphene as the

⁎
Corresponding authors.
E-mail addresses: snlxf@shu.edu.cn (N. Song), dingpeng@shu.edu.cn (P. Ding).
1
These authors contributed equally to this work.

https://doi.org/10.1016/j.compositesa.2020.105912
Received 19 February 2020; Received in revised form 16 April 2020; Accepted 18 April 2020
Available online 20 April 2020
1359-835X/ © 2020 Elsevier Ltd. All rights reserved.
N. Song, et al.
thermally conductive filler is a hot research topic and has great appli-
cation prospects because of its excellent mechanical properties, high TC
(2000–5300 W·m−1·K−1), super electrical conductivity, etc. [19]
Polypropylene (PP), one of the most widely used polymers, is chosen as
the matrix for its advantages, such as excellent mechanical properties,
chemical resistance, ease of processing, light weight, low cost and so
on. However, TC of PP is only 0.2 W·m−1·K−1. In addition, non-polar
nature of PP, caused by low electronegativity of methyl and hydrogen
atoms on molecular chains, makes it more difficult to prepare highly
thermally conductive PP-based composites [10].
Dopamine (DA) attracts our attention because it can self-polymerize
on almost all types of surfaces and form polydopamine (PDA) layer with
assorted oxygen, nitrogen functional groups and aromatic rings. It is
reported that PDA was used as a modifier for thermally conductive
fillers (graphene, boron nitride, etc.) [20–24]. However, thermal con-
ductivity enhancement is limited. Yuan et al. reported epoxy nano-
composites incorporating a polydopamine-coated thermally conductive
filler – copper nanowires (CuMWs). The authors pointed out a thicker
PDA layer coated on CuMWs leads to lower thermal conductivity [23].
Different from traditional filler modification, we proposed a new stra-
tegy–modifying PP matrix by PDA to avoid disadvantages of fillers'
functionalization mentioned above. There are two main advantages to
append an additional PDA layer on PP surface. On one hand, The PDA
layer on PP surface is rich in oxygen, nitrogen functional groups and
aromatic rings, which can interact with graphene through hydrogen
bonding and π-π conjugate. On the other hand, surface-functionalized
PP matrix, instead of graphene, can fully exert the excellent intrinsic
properties of graphene.
In this work, PP/PDA/graphene composite with enhanced inter-
facial interaction and three-dimensional (3D) thermally conductive
graphene network was fabricated via a simple “in-situ building”
method. PP particles were coated by PDA layer, which endowed
abundant polar functional groups of PP surface. Then graphene coated
on the surface of PP/PDA particles through hydrogen bonding and π-π
conjugate between PDA layer and graphene. Enhanced interface inter-
action reduces phonon scattering at the interface between PP and
graphene. The constructed interconnected graphene skeleton is con-
ductive to phonon transmission. As a result, the through-plane TC of
PP/PDA/graphene composite could reach 10.93 W·m−1·K−1, almost 55
times higher than that of pure PP and 4 times higher than that of PP/
graphene composite. It was also demonstrated that the PP/PDA/gra-
phene composite works as a thermal management material. It greatly
reduced the surface temperature of the LED lamp. Furthermore, flexural
strength and Young’s modulus of PP/PDA/G composites, tested by
three-point bending method, are much higher than that of PP/G com-
posites owing to the enhanced interaction by PDA. The facilely pro-
duced composites have a huge application prospect in the heat dis-
sipation of electronic devices.
2. Experimental
2.1. Materials
Oil-soluble graphene (G) with 5–10 layers, a particle size of
10–30 µm (Fig. S1, SI) and few surface defects (Fig. S2, SI) was pur-
chased by China Carbon Valley Technology Group Co., Ltd. (China).
Polypropylene particles, particles size varying from dozens of microns
to 1.1 mm shown in Fig. S3 (SI), were provided from Renqiu North
China Oilfield Jiujiu Industry and Trade Co. Ltd. (China). N-N di-
methylformamide (DMF) and hydrochloric acid was obtained from Si-
nopharm Chemical Reagent Co.,Ltd. (Shanghai, China). Dopamine (DA)
and 2-Amino-2(hydroxymethyl)-1,3propanediol (tris) hydrochloride
were prepared by Sigma Aldrich.
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Composites Part A 135 (2020) 105912
2.2. Functionalization of PP particles
A certain amount of PP particles and dopamine hydrochloride were
added into Tris-HCl (10 mM, pH 8.5) buffer solution and stirred for 24 h
at 60 °C. The Mass to volume ratio of dopamine hydrochloride and Tris-
HCl buffer solution is 1:200 (g:ml). Then PP particles coated by PDA
were washed with deionized water and ethanol several times. The PP
functionalized by PDA (PP/PDA) was dried in the oven at 70 °C for 2 h.
2.3. Fabrication of PP/PDA/G composites with 3D network
A certain amount of G was dispersed in DMF and sonicated for 4 h,
then PP/PDA particles were added to the above dispersion. The mixture
was stirred for 4 h for better dispersion and contact. The mixture should
be put into the oven at 70 °C for 24 h to remove DMF and PP/PDA
particles coated by G (PP/PDA/G) were obtained. At last, the prepared
PP/PDA/G particles were hot pressed for 30 min at 200 °C, 15 MPa in a
mold with the diameter of 12.7 mm and the thickness of 1.5 mm.
Composites with different G content were named PP/PDA/G-n, in
which n means volume content of G. As a comparison, PP coated G
directly with different G content (PP/G) were also prepared. For an-
other contrast, M-PP/G composites were obtained using melt mixing
method by twin screw mixer.
2.4. Characterization
Fourier transform infrared (FTIR) spectra were acquired on a
Nicolet380 Fourier infrared spectrometer with potassium bromide
powders. Before tested, samples were dried at 50 °C for 6 h. Field
emission scanning electron microscope (SEM, HITACHI-S4800) was
used to observe the morphology of the samples. Internal cross sections
were observed by Micro-CT (skysCan2211, Germany). Precision LCR
Meter (TH2829A, Tonghui) was used to get electrical resistance. The
resistivity (ρ, Ω·m) can be calculated using the formula.
ρ = RS/L (1)
where R is electrical resistance, S and L are area and thickness of
samples, respectively. The three-point bending stress–strain curves
were performed at a temperature of 21.7 °C and a humidity of 43.4% on
a universal tensile tester (Instron 5569A), and the samples were hot-
pressed into strips with a thickness of 1.5 mm. Density (ρ, g·cm−1) was
obtained by a density balance (SARTORIUS, China). Thermal diffusivity
(α, mm2·s−1) of fabricated composites was performed on a Netzsch LFA
447 Nanoflash at 25 °C. More detail information concerning TC test can
be seen in Supporting Information. Every sample was tested six times to
eliminate test errors. The specific heat (Cp, J·g−1·K−1) was got by DSC
(TA 250, America). Thermal conductivity (K) was got using the formula
below:
K= α·Cp ·ρ (2)
Infrared thermal imaging was performed to characterize the thermal
transfer performance of the fabricated composite when it worked as a
thermal management material. Thermal conductivity enhancement
(TCE) is calculated using the formula below:
TCE = (K c − K 0)/K 0 ×100% (3)
where Kc is TC of the obtained composites, K0 is TC of pure PP
(0.2 W·m−1·K−1).
3. Results and discussion
3.1. Fabrication process and morphology
In this study, PP/PDA/G composites were fabricated via a simple
“in-situ building” approach, including two steps: (1) PP particles were
functionalized by DA and coated by graphene; (2) hot-pressing.
N. Song, et al. Composites Part A 135 (2020) 105912

Fig. 1. (a) Schematic illustration of the fabrication process of PP/PDA/G composites. SEM images of surfaces of pure PP (b), PP/PDA (c) and PP/PDA/G (d) particles
and (e) cross section of PP/PDA/G-27.

Fig. 2. SEM images of pure PP (a), PP/PDA (b) and PP/PDA/G (c) particles. The inset schematic (b-c) shows core–shell structure of pure PP and PP/PDA and
particles. (d) Micro-CT image of PP/PDA/G composite. The inset schematic (d) shows segregated structure of the PP/PDA/G composite. Sectional morphology of PP/
PDA/G-27 (e) at 1000 °C in argon atmosphere and partial enlargement (e′). FTIR spectra (g) of comparison of hydroxyl peak positions of PP/PDA/G composites and
PP/G composites and (h) schematic diagram of interaction between PDA and graphene. (For interpretation of the references to colour in this figure legend, the reader
is referred to the web version of this article.)

Detailed preparation procedure could be seen at Experimental section
and Fig. 1(a). After coated by PDA, PP particles’ surface becomes
smooth (Fig. 1(c) and Fig. 2(b)). The crack on PP/PDA surface is caused
by drying in an oven. Polymerization process and polymerization pro-
duct of DA have been studied in many literatures [25,26]. Firstly, 5,6-
dihydroxyindole and 5,6-indolequinone are formed after a series of
oxidation, cyclization and rearrangement in tris-HCl buffer (pH = 8.5).
Then DA, intermediate products and their tautomers polymerized into
PDA by covalent bonding, π-stacking and electrostatic interaction.
Possible molecular structures of PDA can be seen in Fig. S4 (SI). The
PDA layer coated on PP particles’ surface contains a lot of oxygen-
containing groups, nitrogen-containing groups, and six-membered ring
of carbon [26] (Fig. S4, SI). After functionalized by PDA, PP particles
were then coated by graphene through π-π conjugate and hydrogen
bonding during DMF evaporation process. Hydrogen bonding originates
from oxygen-containing groups on graphene and PDA. The aromatic
ring on PDA could interact with the six-membered carbon ring on
graphene. Layer-stacked G can be seen in Fig. 1(d).
At last, PP/PDA/G composites were obtained after hot-press. Some
humps and hollows can be seen on the cross-section image of PP/PDA/
G-27 (blue arrows in Fig. 1(e)). These are exposed PP particles or traces
after the PP particles are peeled off by brittle fracture. Continuous
graphene skeleton is among them (yellow arrows in Fig. 1(e)). To fur-
ther observe the graphene network, we heated PP/PDA/G-27 at 1000 °C
in argon atmosphere. Fig. 2(e) shows its sectional morphology. PP
particles were completely pyrolyzed after heat treatment, leaving some

3
N. Song, et al. Composites Part A 135 (2020) 105912

Fig. 3. (a) Thermal conductivity of PP/PDA/G, PP/G and M-PP/G composites with different graphene content. (b) Thermal conductivity enhancement of PP/PDA/G
composites with different graphene content. (c) Schematic illustration of thermally conductive path. (d) Comparison on through-plane TC with reported literatures.
(For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.)

Fig. 4. (a) The tangent process of the experimental data for PP/PDA/G and PP/G composites to obtain Vc. (b) The fitting process of interface thermal resistance using
Foygel nonlinear models. (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.)

holes. Layered graphene sheets can be seen at the edge of the hole
(Fig. 2(e′)). Micro-CT equipment was employed for further proving the
existence of the graphene network, shown in Fig. 2(d). PP particles, the
dark color parts with irregular shape, were segregated by graphene,
light color parts. These evidences indicate the continuous 3D graphene
network was constructed successfully.
3.2. Interaction between PDA and graphene
Most researchers are committed to the modification of fillers to form
thermally conductive pathway. However, this method is double-edged.
On one hand, it can strengthen the interaction between the filler and
the matrix, as well as promote dispersion. On the other hand, it may
introduce more surface defects to the filler, thereby decreasing intrinsic
TC. Herein, we proposed a new strategy–modifying PP matrix through
the self-polymerization characteristics of dopamine. Abundant
functional groups on PDA chains provide the possibility to enhance the
interaction between PP and graphene, such as hydrogen bonding, π-π
conjugate and electrostatic attraction [27]. Fourier transform infrared
(FTIR) spectra was carried out to prove the existence of hydrogen
bonding between PDA and grapheme [12,28], shown in Fig. 2(g) and
Fig. S6 (SI). The peak at approximately 3400 cm−1 is assigned to the
characteristic stretching vibration of hydroxyl groups (eOH). The peak
of eOH shows a blueshift tendency after the addition of PDA. Fur-
thermore, the strength of the hydrogen bond depends on the content of
the PDA because PDA’s quantity is the least in this system. Thence,
hydrogen bonding interaction weakened as PP/PDA particles decrease
and graphene content increase. As a result, the blueshift tendency of
eOH peak is weakened, shown in Fig. S6(b). The shift of eOH to lower
frequencies is due to the formation of eOH···OH and eOH···N hydrogen
bonding between graphene and PDA. There is also π-π conjugation
between the six-membered carbon ring on graphene and polydopamine

4
N. Song, et al.
Fig. 5. Mechanical properties comparation of pure PP, PP/PDA/G and PP/G composites with different graphene content: (a) flexural stress–strain curves; (b) flexural
strength; (c) young’s modulus. (d) Volume resistivity of PP/PDA/G. (For interpretation of the references to colour in this figure legend, the reader is referred to the
web version of this article.)
[29]. Schematic diagram of hydrogen bonding and π-π interaction is
shown in Fig. 2(h). The enhanced interactions can be expected to
greatly decrease phonons scattering on the interface.
3.3. Thermal conductivity
Fig. 3(a) shows TC variation of PP/PDA/G composites as a function
of graphene volume fraction. With the increase of G content, TC has
been obviously improved. The through-plane TC can reach
10.93 W·m−1·K−1 when graphene content is 27 vol%, almost 55 times
higher than that of pure PP (0.2 W·m−1·K−1) and 4 times higher than
that of PP/G composites (2.73 W·m−1·K−1) (Fig. 3(a, b)). The enhanced
TC is caused by the strengthened interfacial interaction (π-π conjuga-
tion and hydrogen bonding). TC of PP/G-27 (PP particles without PDA
modification) is 3.70 times higher than that of M-PP/G-27 (randomly
dispersed graphene). The high TC of PP/PDA/G is due to successful
construction of the three-dimensional graphene network. The schematic
illustration of thermally conductive path for phonon transmission is
shown in Fig. 3(c). We found both PP/PDA/G and PP/G composites
revealed thermal percolation threshold (Vf) at 10.9 vol% and 11.8 vol
%, respectively (Fig. 4 and SI), consistent with the reported literature
[30]. Below the percolation threshold, PP mediates adjacent graphene
and graphene sheets are not fully attached to each other. Too many
interfaces between PP and graphene lead to phonons scattering and
high interfacial thermal resistance (ITR, R′). Even though above the
percolation threshold, interfaces between PP and graphene still exist. R′
between graphene and PP is much higher than R′ between graphene,
even several orders of magnitude difference [31]. Foygel nonlinear
models [32] gives quantitative descriptions of thermal conductivity
through R′ based on the percolation theory. Some reported papers also
used this model to understand intrinsic factors of improved TC [33,34].
According to Foygel nonlinear models, R′ between graphene and PP
(R′1) was calculated, 3.8 · 10−8 m2·K·W−1. R′ between graphene and
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Composites Part A 135 (2020) 105912
PP/PDA (R′2) decreased to 7.5 · 10−9 m2·K·W−1. Detailed calculation
process can be seen in Fig. 4 and SI. Enhanced interface reduces in-
terface thermal resistance by an order of magnitude. Therefore, TC of
PP/PDA/G composites is much higher than that of PP/G composites.
Especially at 27 vol% graphene content, TC of PP/PDA/G composites is
4 times higher than that of PP/G composites. The above evidence shows
strong interactions (hydrogen bonding and π-π interaction) can reduce
interfacial scattering of phonon because of the improved adhesion be-
tween PP and graphene. The results are consistent with the experi-
mental [33] and simulation results in published literatures. It is inter-
esting that the enhanced interaction makes thermal percolation
threshold at a lower loading fraction (10.9 vol% vs 11.8 vol%). This
phenomenon may be worth further exploring.
TC of the composites rises sharply as the graphene content in-
creases, especially above the TC percolation threshold, because 3D
graphene network becomes more complete and interfaces between PP
and graphene reduce. The efficiency of phonon transmission on the
filler and interfaces between fillers is much higher than that of on in-
terfaces between matrix and filler. In addition, PP particles with dif-
ferent particle sizes as the matrix (Fig. S3, SI) are beneficial to achieve
dense packing of composite materials and obtain highly thermally
conductive composites.
Most reported through-plane TC of polymer matrix composites is
below 10 W·m−1·K−1 (Fig. 3(d) and Table S1, SI), whether the substrate
is polar or non-polar [5,6,8,10,13,35–45]. For non-polar polymer sub-
strates, it is more difficult to prepare highly thermally conductive
composites (< 5.5 W·m−1·K−1). To further evaluate the TC, PP/PDA/G
composites was compared with previously reported polymeric compo-
sites with similar filler contents. The detailed compositions and TC data
shown in Fig. 3(d) are listed in Table S1 (SI). Through-plane TC in this
paper (10.93 W·m−1·K−1) is at a quite high level among reported
polymeric composites. Some literatures reported higher through-plane
TC values than that of ours. For example, Yu et al. [46] developed
N. Song, et al.
Fig. 6. (a) Demonstration of PP/PDA/G composite as a thermal management material for heat dissipation of a LED lamp; (b) The surface temperature variations of
LED versus time; (c) Comparison of infrared thermal images of LED integrated with PP/PDA/G and pure PP as thermal management materials. (For interpretation of
the references to colour in this figure legend, the reader is referred to the web version of this article.)
vertically aligned high-quality graphene hybrid forms through graphi-
tization at 2800 °C and followed impregnated in epoxy. TC of the fab-
ricated composite could reach 35.5 W·m−1·K−1 at 19 vol%. However,
energy consumption is large in the preparation process. Here, we are
devoted to reducing ITR between the filler and the matrix through a
simple PP modification to achieve highly thermally conductive non-
polar matrix composites. Experimental results showed the matrix-
functionalization method for improving thermal conductivity is quite
obvious. In conclusion, construction of the 3D network and enhanced
interfacial interaction simultaneously is a more effective way of pre-
paring high TC composite.
3.4. Mechanical properties and volume resistivity
Mechanical properties are the basic properties of composites, which
is important for the application of thermal management materials.
Flexural stress–strain curves of pure PP, PP/PDA/G and PP/G compo-
sites with different G content can be seen in Fig. 5 and Fig. S7 (SI). The
flexural strength of PP/PDA/G composite can reach 11.34 MPa, which
is almost twice higher than that of PP/G composite at 27 vol% G con-
tent. The flexural strength of PP/G-27 is only 5.64 MPa, which is half of
that of PP/PDA/G-27. It is suggested that PDA enhances the interaction
between PP and graphene by hydrogen bonding and π-π interaction,
resulting in more energy consumed in the fracture between graphene
sheets and PP particles. Young's modulus of PP/G composites increases
from 1.70 GPa to 2.29 GPa after the integration of G into the PP matrix.
Young's modulus of PP/PDA/G composites is higher than that of PP/G
composites. Especially at 27 vol%, Young's modulus of PP/PDA/G
composites (5.07 GPa) is 2.2 times higher than that of PP/G composites,
shown in Fig. 5(b). The flexural strength and elongation at break of
composites decreases (Fig. 5a and b). This may be due to the fact that
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Composites Part A 135 (2020) 105912
the stiffness of 3D graphene network is greater than that of PP. PP
particles are separated by 3D graphene network, leading to adjacent PP
particles failing to lap together through the winding of the chain. More
complete graphene framework formed with the increase of graphene.
Conductivity property was also noticed. Fig. 5(d) shows a pot of
volume resistance (VR) versus graphene content for PP/PDA/G com-
posites. As is known to all, the volume resistivity of PP is 1.6·1014 Ω·m,
an electrically insulating polymer. In this paper, the volume resistivity
of PP composites is significantly decreased even only at 2 vol%. The
great improvement in electrical conductivity is attributed to the suc-
cessful construction of the 3D graphene skeleton. VR of PP/PDA/G
composites is less than 106 Ω·m, far below the critical resistance for
electrical insulation (< 1011 Ω·m) as well as having the antistatic
function (< 109 Ω·m). Good electrical conductivity not only expands
the application of PP in the electrical conduction field, but also avoids
the danger of static electricity.
3.5. Demonstration of PP/PDA/G composites’ application
Application in heat diffusion field of the obtained composite was
investigated. Much heat is generated during the operation of electronic
devices. Efficient thermal diffusion not only enables efficient operation
of electronic devices, but also protects them and extends their service
life. High through-plane TC endows PP/PDA/G composites potential
application for thermal management. Here, the PP/PDA/G composite is
used as a thermal management material for LED’s heat diffusion to
show its excellent thermal management performance. It also can be
used for a thermal management material in other electric devices.
Meanwhile, it is not limited in the part of LED components shown
below. Fig. 6(a) shows the schematic diagram of a LED lamp integrated
with the PP/PDA/G composite and copper block. The three elements
N. Song, et al.
are bonded together with thermally conductive silicone grease. Infrared
thermal images (Fig. 6(c)) vividly demonstrates the heat dissipation
capability of the PP/PDA/G composite. At the same running time,
temperature of LED lamp with the PP/PDA/G composite is much lower
than that of pure PP. After operating for 300 s, the temperature dif-
ference can reach 20 °C, shown in Fig. 6(b). The temperature difference
has not practically changed after LED lamp runs for another 100 s. The
result indicates that the highly thermally conductive PP/PDA/G com-
posite with 3D interconnected graphene network and enhanced inter-
facial interaction is a great potentially valued thermal management
material.
4. Conclusions
In summary, highly thermally conductive PP/PDA/G composites
with 3D graphene network and enhanced interfacial interaction were
prepared via a simple “in-situ building” method. Dopamine was used as
a modifier for the matrix to improve the polarity of PP, enriched with
oxygen-containing groups, nitrogen-containing groups, and six-mem-
bered ring of carbon on its surface. Then graphene coated on the surface
of PP particles through hydrogen bonding and π-π conjugate. Thermal
conductivity of the composite reaches 10.93 W·m−1·K−1 at 27 vol%,
which is at a relatively high level compared with reported literatures,
especially for non-polar substrates. High thermal conductivity is at-
tributed to 3D graphene thermal network and enhanced interface in-
teraction between PP and graphene. In addition, the composite exhibits
certain mechanical properties and good electrical conductivity. At last,
the PP/PDA/G composite shows good heat dissipation when used in
LED lamp as a thermal management material. The composite can meet
the application in high-integration and high-power electronic devices.
CRediT authorship contribution statement
Na Song: Conceptualization, Supervision, Writing - review &
editing. Donglei Cao: Methodology, Software, Validation,
Investigation, Data curation. Xian Luo: Writing - review & editing. Qi
Wang: Methodology, Investigation. Peng Ding: Project administration,
Writing - review & editing. Liyi Shi: Project administration.
Declaration of Competing Interest
Authors have no conflict of interest to declare.
Acknowledgements
The authors gratefully acknowledge the financial support from the
National Science Foundation of China (No. 51703122), the PetroChina
Innovation Foundation (No. 2016D-5007-0508), the Natural Science
Foundation of Shanghai (No. 17ZR1440700), the Development Fund for
Shanghai Talents (No. 2017014), State Key Laboratory of Solidification
Processing in NWPU (No. SKLSP201837).
Appendix A. Supplementary material
Supplementary data to this article can be found online at https://
doi.org/10.1016/j.compositesa.2020.105912.
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