Carbon 170 (2020) 302e326

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

Review article

An overview of graphene and its derivatives reinforced metal matrix

composites: Preparation, properties and applications
Zhanyong Zhao a, Peikang Bai a, b, **, Wenbo Du d, Bin Liu a, Duo Pan c, f, Rajib Das e,
Chuntai Liu c, ***, Zhanhu Guo f, *
a
School of Materials Science and Engineering, North University of China, Taiyuan, 030051, China
b
Shanxi Institute of Technology, Yangquan, 045000, China
c
Key Laboratory of Materials Processing and Mold (Zhengzhou University), Ministry of Education, National Engineering Research Center for Advanced
Polymer Processing Technology, Zhengzhou University, Zhengzhou, China
d
National Key Laboratory for Remanufacturing, Academy of Army Armored Forces, China
e
Oxea Chemical Company (OQ), Bay City, TX, 77414, USA
f
Integrated Composites Laboratory (ICL), Department of Chemical and Biomolecular Engineering, University of Tennessee, Knoxville, TN, 37996, USA

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

Article history: Graphene (Gr) and its derivatives (such as graphene oxide (GO), reduced graphene oxide (RGO), nano-
Received 19 March 2020 particles decorated graphene, etc.) reinforced metal matrix composites (MMC) with good structural
Received in revised form mechanical properties and functional properties have wide applications in aerospace, automotive,
11 August 2020
electronics and military fields. However, some problems exist in preparing high performance MMC
Accepted 14 August 2020
Available online 21 August 2020
including poor wettability between Gr-type fillers and metal matrix, and weak interfacial bonding
strength. Efficient methods for preparing Gr-related nanomaterials filling metal matrix parts with high
performance, especially for complex parts still need be further developed. The engineering application
Keywords:
Metal matrix composites
field of Gr MMC needs to be further expanded. In this paper, methods to prepare high performance MMC
Graphene including surface modification of Gr and its derivatives, properties and applications of these reinforced
Surface modification MMC were reviewed with detailed examples. The main challenges were analyzed and the development
Fabrication trend of Gr-type types reinforced MMC was discussed.
Properties © 2020 Elsevier Ltd. All rights reserved.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 303
2. Interfacial bonding between graphene and metal . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 304
3. Methods to improve the wettability of graphene . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 304
3.1. Surface modification of graphene . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 304
3.2. Micro-alloying . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 306
3.3. Graphene defect engineering . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 306
4. Fabrication of graphene reinforced metal matrix composites (MMC) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 306
4.1. Liquid-state fabrication methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 307
4.1.1. Stirring casting . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 307
4.1.2. Selective laser melting . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 307
4.1.3. Pressure infiltration . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 307
4.2. Solid-state fabrication methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 310
4.2.1. Powder metallurgy . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 310
4.2.2. Friction stir welding . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 310

* Corresponding author.
** Corresponding author. School of Materials Science and Engineering, North University of China, Taiyuan, 030051, China.
*** Corresponding author.
E-mail addresses: baipeikang@nuc.edu.cn (P. Bai), ctliu@zzu.edu.cn (C. Liu), zguo10@utk.edu (Z. Guo).

https://doi.org/10.1016/j.carbon.2020.08.040
0008-6223/© 2020 Elsevier Ltd. All rights reserved.
 Z. Zhao et al. / Carbon 170 (2020) 302e326 303

4.2.3. Severe plastic deformation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 311

4.2.4. Layer-by-layer assembly . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 313
4.2.5. Molecular level mixing . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 313
4.2.6. Template method . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 314
4.3. Deposition processing . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 315
4.3.1. Electrochemical deposition method . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 315
4.3.2. Cold spray forming . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 315
4.3.3. In-situ synthesis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 316
5. Properties of graphene reinforced metal matrix composites . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 317
5.1. Mechanical properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 317
5.2. Thermal conductivity . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 317
5.3. Electrical performance . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 318
5.4. Anticorrosion properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 319
6. Applications . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 320
6.1. Aerospace industry . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 320
6.2. Electronics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 320
6.3. Automotive industry . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 320
7. Conclusion and perspective . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 320
Declaration of competing interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 322
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 322
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 322

1. Introduction (Gr) from the graphite [37e39]. Gr is a two-dimensional crystal in

the form of a single atomic plane of carbon atoms [40], one layer of
Metal (such as pure metals and their alloys) matrix composites atomic thickness is only about 0.35 nm, the carbon atoms are sp2
(MMC) are one kind of materials filled with reinforcing materials hybridized (Fig. 1a). The length of the carbon-carbon bond is
such as fibers, whiskers or particles [1e6]. Based on the types of 0.142 nm, and the 3 s bonds form a stable hexagonal structure in
matrix, MMC are mainly divided into Al matrix, Mg matrix, Zn the lattice, and the carbon atoms contribute to the remaining 1 p
matrix, Cu matrix, Ti matrix, Ni matrix, intermetallic compound orbital electrons and form the large p bonds, in which p electrons
matrix and others [7e9]. In the widely used Al matrix composites can move freely [41]. The modulus of elasticity and intrinsic frac-
[10,11], the Al matrix is face-centered cubic structure, and has good ture strength of monolayer Gr are 1 TPa and 130 GPa. Gr has both
plasticity and toughness. In addition, the advantages of workability, high carrier mobility (about 2
105 cm2/(Vs)) and thermal con-
engineering reliability and low price favor engineering applications ductivity (between 3000 and 5000 W m1 K1) [37,38,42,43]. The
[12,13]. Meanwhile, the ultra-light, high specific stiffness and high functionalized Gr was normally prepared [44,45], for example,
specific strength make Mg matrix composites are preferred for graphene oxide (GO) was formed (Fig. 1b) when the carbon core
aerospace [14,15]. Because of excellent high-temperature proper- structure was oxidized. The GO containing oxygen functional
ties, the Ni matrix composites are mainly used to work in high- groups is more active than Gr [46e51]. The reduced graphene oxide
temperature conditions [16]. Offering high specific strength and (RGO) is the reduced state of GO with vacancy defects (Fig. 1c) and
stiffness compared with steel and nickel-base materials, Ti matrix lacks the oxygen-containing functional groups [52e55]. Gr as a
composites can be used in the aerospace, medical field and other reinforcing phase was added into metal materials and significantly
industrial fields [17]. With excellent electrical conductivity, thermal improved the hardness, wear resistance and electrical conductivity
conductivity and wear resistance, Cu matrix composites are often of metal materials. Compared with traditional reinforcement pha-
used in electricity [18,19]. The low density, high strength and high ses such as carbides, metal oxides, nitrides, borides and so on. Gr
stiffness reinforcers are added to effectively reduce the density of Fe has obvious advantages in enhancing efficiency because of its high
matrix, and to improve its hardness, wear resistance and high specific surface area.
temperature performance, which can be used in industrial appli- Realizing the importance of Gr in metal matrices, the fabrication
cations such as cutting tools and wear-resistance parts [20,21]. methods to prepare Gr MMC can be generally divided into liquid-
Special properties can be achieved in MMC by adding proper state fabrication, solid-state fabrication and deposition process-
reinforcing phases. As an important part of MMC, the reinforcing ing. Gr dispersion and interfacial bonding affect the performance of
phase is required to have not only good mechanical properties and Gr MMC. For example, Ghodrati et al. summarized the effects of Gr
functional properties, but also good chemical stability and dispersion and interfacial bonding on the mechanical properties of
compatibility with the metal matrix. At present, the reinforcing MMC [56]. However, due to poor wettability, large density differ-
phases mainly include carbides, metal oxides, nitrides, borides and ence between Gr and metal, easy aggregation of Gr, and low
so on. Carbides mainly include SiC, B4C and TiC [22e24]. Metal bonding between Gr and metal, thus strong interfacial bonding and
oxides mainly include Al2O3, ZrO2 and MgO [25,26]. Nitrides mainly homogeneous distribution of Gr in the metals are still challenges. In
include Si3N4, AlN and BN [27e29]. Borides mainly include TiB2 and order to improve the wettability between Gr and metal, surface
TiB [30,31]. The reinforcing phase can be added to the metal matrix modification of Gr is normally used and some methods have been
in different sizes (such as micron, submicron or nanometer), reported [56]. Recent progress and developments focusing on
different morphologies (such as particle, whisker or fiber) and mechanical properties, and potential applications of Gr and Gr-
different proportions. These reinforcing phases can improve the based nanocomposites have been reported [57e61]. However, to
performance of metal matrix, and the MMC have been applied in specifically address the surface modification of Gr, fabrication of Gr
the aerospace, automotive, electronics and military fields [32e36]. MMC, properties and applications of Gr reinforced MMC have not
In 2004, Geim and Novoselov successfully prepared graphene been reviewed yet.
304 Z. Zhao et al. / Carbon 170 (2020) 302e326
Fig. 1. Structures of (a) Gr, (b) GO, (c) RGO, with permission from Ref. [46]. Copyright © 2019 Elsevier Ltd. (A colour version of this figure can be viewed online.)
In this paper, surface modifications of Gr, fabrication of Gr
reinforced MMC, properties and applications of Gr reinforced MMC
are critically summarized and discussed with detailed examples.
The main problems are disclosed and the development trend of Gr
reinforced MMC is briefly discussed with detailed examples.
2. Interfacial bonding between graphene and metal
The interfacial bonding between Gr and metal affects the me-
chanical properties of composites. There are two main interface
bonding modes, i.e., physical (mechanical) and chemical bonding.
The weak physical bonding mainly includes van der Waals and
hydrogen bonds, while the chemical bonding is strong, and the
bond energy is one order of magnitude greater than physical bond
[56]. The mechanisms on the interface bonding between Gr and
metal focus on the sorption of transition metals on Gr. The phys-
isorption interface is formed by charge transfer [56,62]. Pauli
exclusion interaction between the p-electrons of Gr and the s-
electrons of the metals is one important physisorption interface
[56,62]. Pauli-exclusion interaction occurs due to the approaching
of metal surface atoms to the Gr, the p-electrons in Gr are over-
lapped by shell occupied by the s-electrons of the metal in outer-
most. Gong et al. reported that the Gr’s p-band structure with a
linear band crossing at Dirac point (K and K0 ) was maintained at the
physisorption interface, but the Dirac point was moved depending
on the doping [56,62]. The chemisorption interface is normally
formed by orbital hybridization. The d-electrons of metal are
overlapped by the p-electrons of Gr, the hybridization interaction
occurs, the electronic structure is much more complicated, and the
hybridization is strong, which causes the strong covalent chemical
bonding. Strong interfacial bonding is one of the most important
factors for preparing high performance Gr reinforced MMC [56,62].
Some problems exist in preparing high performance Gr MMC. Gr
agglomerates easily since it has a large specific surface area, high
surface energy and other factors such as the existence of van der
Waals forces between Gr layers, and non-flat of Gr arising from
nanoscale wrinkles caused by compression (in-plane) or shear on
the surface and edge of Gr monolayer [63]. The wettability between
Gr and metal matrix is poor. Most molten metals are difficult to wet
the Gr, and the contact angle is usually larger than 90 . For example,
when the Al alloy is heated to 660e860  C, the contact angle be-
tween Al alloy and carbon is about 150 , and there is no formation
of carbide at the liquid/solid interface [64]. The contact angle be-
tween Cue1%Ti alloy and graphite is 150 at 1150  C. Because the
wetting tension is small, the wettability is poor.
Some alloy element can react with Gr, and improve the wetting,
such as Ti alloy reacts with Gr to produce TiC. This can improve the
contact angle. For example, Sn improved the contact angle between
Cu-xSn-1%Ti alloy and graphite, when the Sn content was increased
from 0 to 20 wt%, the contact angle between Cu-xSn-1% Ti alloy and
graphite was decreased from 150 to 22 at 1150  C, and the contact
angle between Cu-xSn-3% Ti alloy and graphite was decreased from
140 to 0 at 1150  C [65]. The wettability and dispersion of Gr are
affected by the surface properties of Gr and alloy elements.
Improving the wettability and dispersion between Gr and metal
matrix is the key scientific problem, and it needs be solved urgently.
The methods for improving the wettability and dispersion are
discussed in the following section.
3. Methods to improve the wettability of graphene
In order to improve the wettability of Gr and interface bonding
performance between Gr and metal, the processing methods of Gr
can be divided into three main categories, i.e., surface modification
of Gr, micro-alloying and Gr defect engineering, as shown in Fig. 2.
3.1. Surface modification of graphene
The Gr surface is normally modified by adding the ally element
to improve the wettability between Gr and metal, and to increase
the interfacial bonding strength. The reported methods for Gr
surface modification are summarized as follows.
The chemical reduction method is easy to operate, low cost and
simple in process. It can improve the wettability between Gr and
metal matrix. During the process, metal particles are deposited on
the Gr surface by chemical reduction method, as shown in Fig. 3.
The Ag, Au and Ni are usually synthesized and deposited on the Gr
by chemical reduction method. For different metal particles, the
solution and reaction condition are also different. For example, Hao
et al. prepared Ag-doped Gr using the solution of AgNO3. Ag-doped
Gr were uniformly dispersed in the silver matrix and improved the
mechanical property and conductivity of the composites [66].
Muszynski et al. synthesized gold nanoparticles using chemical
reduction of AuCl4 (Aldrich) with NaBH4 in a Gr-octadecylamine
suspension, the gold nanoparticles were well dispersed on the Gr
[67]. Tang et al. decorated Ni on GNPs using NiSO4$6H2O, N2H4$H2O
and NaOH by an in-situ chemical reduction method, which greatly
improved the dispersion of the GNPs in the Cu matrix [68]. The Gr
coated with metal particles synthesized by chemical reduction
method can be easily dispersed uniformly in the metal matrix,
 Z. Zhao et al. / Carbon 170 (2020) 302e326
Fig. 2. Methods to improve the wettability of Gr. (A colour version of this figure can be viewed online.)
Fig. 3. Schematic of chemical reduction method, with permission from Ref. [66]. Copyright © 2018 Elsevier Ltd. (A colour version of this figure can be viewed online.)
however, during the chemical reduction process, there are certain
dangers, the experimental waste liquid needs be discharged after
the treatment.
Hydrothermal method with a low cost, no sintering and good
controllability is generally used to prepare composites with high
purity. Hydrothermal method involves synthesizing metal particles
via chemical reactions in high-temperature aqueous solutions un-
der high vapor pressure level. For example, Kumar et al. synthe-
sized Ag nanoparticles on Gr by the hydrothermal method, the Gr/
aqueous silver nitrate solution was in Teflon-lined autoclave and
heated at 140  C for 6 h [69]. MoO3 and nickel selenide silver were
also synthesized and dispersed on the Gr through hydrothermal
methods [70,71]. However, hydrothermal synthesis is affected by
temperature, reaction time and the kinds of solvents, the reaction
conditions need to be controlled precisely.
During the electrochemical deposition process, metal nano-
particles are deposited on the Gr surface from ionic solutions. There
are working electrode, counter electrode and reference electrode.
Metal ions near the working electrode are gradually reduced when
enough current is passed through the solution, as shown in Fig. 4.
The types, structures and sizes of the metal particles can be altered
by controlling electrolyte and process parameters. For example,
Zhao et al. prepared GNPs reinforced Cu matrix composites by
electrochemical deposition, the electrolyte was composites of
CuSO4$5H2O and NiSO4$6H2O, the adjusting temperature was
15e35  C, the current was 0.1 A, the pH was 3.5e5.5, and the
duration was 48 h [72]. Dau et al. deposited Fe3O4 nanoparticles
onto few-layered GNPs by the in-situ electrochemical deposition
method, the Gr electrode was scanned between 1.5 and 1.5 V at
50 mVs1 for 20 cycles in KCl solution containing K3[Fe(CN)6] [73].
305
Yu et al. electrodeposited platinum nanoparticles on Gr, the Gr
electrode was in H2PtCl6 solution, the potential was 0.2 V (versus
Ag/AgCl) and continued for 20 s [74]. During electrochemical
deposition process, it does not need to add chemical reagents,
therefore, this method not only is easy to operate, green and
environmentally friendly, but also has a good dispersion of Gr.
However, the thickness of Gr is difficult to be controlled in the
deposition process.
Physical vapor deposition (PVD) can coat thin metal films on Gr.
During the PVD process, the raw material is heated or sputtered to
produce a vapor of material under the low-pressure/vacuum or
gaseous plasma environment, which is condensed and forms a
coating on Gr, as shown in Fig. 5 [75]. The coating thickness is
affected by the surface properties of Gr. The morphology of the
nanoparticles varies markedly for different metals. For example,
Pandey et al. established the model and explained the phenomenon
[76]. In addition to metal nanoparticles, some non-metallic nano-
particles were also deposited on Gr by PVD. For example, Suzuki
et al. prepared the SiO-coated Gr by thermal evaporation [77]. The
advantage of thermal evaporation is that the device is relatively
simple and easy to operate, and the coating has a high quality, high
purity, accurate thickness, low cost, large scale and so on.
Self-assembly is the spontaneous organization of molecules
under thermodynamic equilibrium conditions into structurally
well-defined and rather stable arrangements through a number of
noncovalent interactions. The self-assembly method is highly effi-
cient and simple to coat nanoparticles on Gr. The kinds, shapes and
sizes of the metal particles can be controlled by altering self-
assembly materials and process parameters. Self-assembly
method can be used to prepare various forms of nanomaterials,
306 Z. Zhao et al. / Carbon 170 (2020) 302e326

Fig. 4. Schematic of preparation of GNPs/Cu composites, with permission from Ref. [72]. Copyright © 2018 Elsevier Ltd. (A colour version of this figure can be viewed online.)

Fig. 5. Schematic diagram of the PVD, (a) sputtering and (b) evaporation coating methods, with permission from Ref. [75]. Copyright © 2018 Elsevier Ltd. (A colour version of this
figure can be viewed online.)

such as nanowire, nanorod, nanofilm, and nanotube. For example, effective ways to improve interfacial bond strength is micro-
Cong et al. incorporated a-FeOOH nanorods and magnetic Fe3O4 alloying, which promotes the phase formation between Gr and
nanoparticles with Gr sheets to assemble Gr-based multifunctional metal matrix, and improves the mechanical properties. Some
nanocomposites [78]. Bagheri et al. self-assembled gold nanorods alloying elements such as Ti, Cr, B or Zr were added into the Gr or
onto Gr templates into long fibers [79]. Hong et al. self-assembled carbon nanotube Cu matrix composites, which promoted the car-
2e6 nm gold nanoparticles on Gr [80]. Huang et al. modified RGO bide layer at the interface (Fig. 9), and improved the interface
sheets with fluorescent Au nanodots by the synthesis and in situ bonding performance [56,84,85]. The carbide layer at the interface
assembly of metal nanostructures [81]. The advantage of the self- affected the composites susceptibility to crack initiation, and
assembly method is the strong controllability, and the assembly reduced the composite toughness [56,84,85].
is periodically ordered. The main disadvantages are the insufficient
stability, weak interaction force between molecules, and long as-
3.3. Graphene defect engineering
sembly operation.
Al was coated on Gr by chemical reduction of organic Al. The
The defects of Gr play an important role in the in-situ interface
basic principle is that Al powder (Al) reacts with the (C2H5)2Br to
modification strategy. The surface defects of Gr are usually created
prepare (C2H5)3Al. The (C2H5)3Al solution is decomposed, and the
by plasma treatment. The Gr defect region is active and favors the
formed Al atoms are deposited on the Gr to form coating, as shown
formation of interfacial oxides/carbides. The interfacial reaction
in Fig. 6 [82,83]. The grains grow through two dimensional and
between Gr and metal occurs at the defects. For example, Chu et al.
three dimensional layer, as shown in Fig. 7 [82,83]. The effects of
used plasma treatment to create graphene defects, and prepared
process parameters and reducing agent on the Al coating were also
Gr/Cu MMC by spark plasma sintering (SPS), as shown in Fig. 10
investigated. The process parameters were optimized to prepare
[86]. In the prepared Gr/Cu composites, the CuxOy oxides were
high quality Al-coated Gr, and the Al-coating coverage reached 84%
formed mainly at the defect sites (Fig. 11), and the generated CuxOy
(Fig. 8) [82,83]. This method improved the wettability between Gr
oxides coordinated at the interface, and improved the interface
and metal, and the performance of the Gr MMC. This method could
bond strength. The MMC with plasma-treated Gr exhibited excel-
be extended to other metal coatings, such as coating Mg on Gr by
lent mechanical properties [86].
chemical reduction of organic Mg.

4. Fabrication of graphene reinforced metal matrix

3.2. Micro-alloying composites (MMC)

The strong interface between Gr and metal matrix plays an The fabrication methods of Gr reinforced MMC can be divided
important role in improving the performance of Gr MMC. One of into three main categories, i.e., liquid-state method, solid-state
 Z. Zhao et al. / Carbon 170 (2020) 302e326
Fig. 6. High-resolution TEM images of the Al-coated Gr with a reaction time of (a, c) 0.5, and (b, d) 1 h, with permission from Ref. [82]. Copyright © 2019 Elsevier Ltd. (A colour
version of this figure can be viewed online.)
method and deposition processing. The liquid-state fabrication
methods mainly include stirring casting, selective laser melting and
pressure infiltration. The solid-state fabrication methods mainly
include powder metallurgy, friction stir welding, severe plastic
deformation, layer-by-layer assembly, template method and mo-
lecular level mixing. The deposition processing methods mainly
include electrochemical deposition method, cold spray forming and
in-situ synthesis. Some representative fabrication methods of Gr
reinforced MMC are shown in Fig. 12.
4.1. Liquid-state fabrication methods
4.1.1. Stirring casting
Stirring casting is a method of preparing composites in liquid
states. During the process, the metal is melted, the dispersed phase
(such as ceramic particles, Gr) is added into the melt by stirring
(Fig. 13). Among the liquid state fabrication methods, stirring
casting is the most cost effective and the simplest. For example,
Rashad et al. fabricated GNPs/AZ31 composites by the stir-casting
method, the GNPs improved the micro-hardness, tensile fracture
strain and compression yield strength [87]. Stirring casting has the
following features: the loading of the strengthening particles is less
than 30 vol%, the strengthening particles easily aggregate, and the
pores are easily formed in the melt. In order to improve the
wettability between the melt metal and strengthening particles,
the strengthening particles are often coated with metal.
4.1.2. Selective laser melting
Selective laser melting (SLM), as an advanced forming
307
technology, has been widely used in aviation, automobile and other
industries. The product is formed by selectively melting successive
layers of powders by the interaction of a high-energy laser beam
during the SLM process, as shown in Fig. 14. SLM technology can
prepare metal parts with complex shapes. Varieties of Gr MMC
have been prepared by SLM, such as TiAl/RGO MMC [88], Gr/Al
nanocomposites [89], Gr/Inconel 718 composites [90] and so on,
these composites exhibit perfect mechanical properties. For
example, the compressive strength and strain of the TiAl/RGO MMC
reached 1546.88 MPa and 5.34% [88]. The Al4C3 was formed be-
tween the Gr and Al matrix (Fig. 15) in Gr/Al nanocomposites,
which improved the wettability, the Vickers hardness of Gr-Al
composites was 75.3% higher than that of pure Al [89]. The ulti-
mate tensile strength of 1 wt% Gr/Inconel 718 composites was 53%
higher than those of pure material [90]. Though the SLM can pre-
pare high performance Gr MMC, the SLM process and the proper-
ties of parts were affected by the properties of the SLM powders,
such as high purity, high sphericity, flowability and narrow size
distribution. It was thus very strict for preparing Gr MMC SLM
powders. At the same time, the Gr can affect the laser absorptivity
of metal powders, and the defects can be easily formed in the parts,
such as pores, inclusion and deformation. The process parameters,
such as laser power, exposure time, scanning speed, scanning path
and so on, must be strictly tailored.
4.1.3. Pressure infiltration
Pressure infiltration casting is one of advanced processes for
producing MMC, the liquid metal is flown into a preform of rein-
forcement material through pressurized inert gas, as shown in
308 Z. Zhao et al. / Carbon 170 (2020) 302e326

Fig. 7. The Al coating surface (a, b), the schematic illustration indicates the Al particles with a 2D layered growth (c) and 3D island growth (d), with permission from Ref. [82].
Copyright © 2019 Elsevier Ltd. (A colour version of this figure can be viewed online.)

Fig. 8. The SEM images (a) and the EDS analysis (b) of Al-coated Gr (Blue Al element, Yellow C element), with permission from Ref. [83]. Copyright © 2018 Elsevier Ltd. (A colour
version of this figure can be viewed online.)
 Z. Zhao et al. / Carbon 170 (2020) 302e326 309

Fig. 9. Interface design of graphene/Cu composites, with permission from Ref. [84]. Copyright © 2018 Elsevier Ltd. (A colour version of this figure can be viewed online.)

Fig. 10. Schematic of graphene defect engineering and preparation of P-RGO/Cu composites, with permission from Ref. [86]. Copyright © 2018 Elsevier Ltd. (A colour version of this
figure can be viewed online.)
310 Z. Zhao et al. / Carbon 170 (2020) 302e326
Fig. 11. Interface of 1 vol% plasma treatment-RGO/Cu composites. (a, b) TEM images; (c, d) HRTEM image of selected region in (a, b); (e) HRTEM image of plasma treatment-RGO/Cu
interface region and corresponding FFT patterns recorded in e1, e2, e3 and IFFT image recorded in e4 [86]. Copyright © 2018 Elsevier Ltd. (A colour version of this figure can be
viewed online.)
Fig. 16. Pressure infiltration can overcome the shortcomings of poor
wettability between reinforcement phase and matrix. The pressure
infiltration speed is fast, which can avoid adverse reactions be-
tween matrix and reinforcement phase. During the pressure infil-
tration process, the preheating temperature, infiltration pressure,
pressing speed and pressing time affect the properties of the MMC.
At present, the preparation of Gr MMC by pressure infiltration is
mainly focused on Gr/Al matrix composites, which exhibit perfect
mechanical properties and electrical conductivity. For example,
Shao et al. prepared GNPs reinforced 5083 Al matrix composites by
pressure infiltration method, the tensile strength of MMC was
increased by 14% [91]. Yu et al. prepared GNPs/6063 alloy com-
posites by pressure infiltration and hot extrusion. The tensile
strength of the composites (276 MPa) was about 22.5% higher than
that of the alloy, the electrical conductivity of the MMC was greatly
improved [92]. Yang et al. prepared GNPs/pure Al composites by
pressure infiltration, the distribution of GNPs was uniform (Fig. 17),
the GNPs were well bonded with Al matrix [93].
However, in the pressure infiltration, the pressure is high, the
parts are easily deformed, especially the parts are composed of
short fibers or whiskers, which touch only a few points and can be
bended or broken between these points. The large and complex
parts have high requirements for manufacturing equipment, and
they are difficult to be formed. It is thus extremely important to
control the forming process, such as the preheating temperature,
infiltration pressure, pressing speed and pressing time.
4.2. Solid-state fabrication methods
4.2.1. Powder metallurgy
Powder metallurgy is one of the easiest methods to prepare Gr
MMC. The metal powders and Gr are mixed in the mixing device,
pressed into the die to form the desired shape, and then sintered, as
shown in Fig. 18. In order to improve the performance of compos-
ites, the composites are further hot extruded, hot forged or hot
rolled, as shown in Fig. 19. For example, Li et al. prepared the 0.4 wt
% GNPs/Al MMC by the powder metallurgy followed by a multi-pass
cold drawing at ambient temperature, the distribution of GNPs was
homogeneous, and the interfacial bonding was strong, as shown in
Fig. 20 [94]. The powder metallurgy can be used to prepare complex
parts at a low cost. The powder metallurgy is applied in the area of
industry extensively. Several kinds of Gr MMC have been prepared
such as Gr/Al, Gr/Gu, Gr/sliver or Gr/Ti and so on [95e101]. How-
ever, there are still some challenges to be solved, such as Gr is easily
agglomerated in the metal matrix, the interfacial reactions occur
between Gr and matrix at high temperatures, the interface bonding
strength needs be further improved.
4.2.2. Friction stir welding
Friction stir welding is a solid-state welding method for welding
the metals with low melting points. It heats the metals using the
heat produced by friction between the stir head and the base metal,
as shown in Fig. 21. Friction stir welding was invented by the British
 Z. Zhao et al. / Carbon 170 (2020) 302e326 311

Fig. 12. Some representative fabrication methods of Gr reinforced MMC. (A colour version of this figure can be viewed online.)

Welding Research Institute in 1991. After years of development, the

friction stir welding technology has been widely used in preparing
structures of light metal (such as Al, Mg alloys) and for preparing
composite materials with fewer impurities. However, it is difficult
to prepare complex parts. Many researchers have prepared Gr Al or
Mg matrix composites by friction stir welding. For example, Jeon
et al. fabricated Gr/Al MMC by the friction stir welding. The thermal
conductivity of the Gr/Al composites was increased by more than
15% in comparison with that of the Al matrix [102]. Chen et al.
prepared GNPs/Mg-based metal matrix nanocomposites by solid
state stirring, the GNPs were uniformly embedded inside the Mg
grain, and the interfacial bonding was very good, as shown in
Fig. 22 [103]. Khodabakhshia et al. fabricated GNPs/AleMg com-
posites through the friction stir processing [104].
The friction stir welding has the main advantages: without the
heat-affected zone typical for the fusion welding, low residual
stress, convenient operation process, suitable for welding different
materials, no need to add welding wire, and low cost. However,
there are still some problems restricting its development, such as
the wear of mixing head is too fast, welding speed is low, the hole
formed in the weld end is difficult to be repaired, welding work-
piece must be rigidly fixed.

4.2.3. Severe plastic deformation

Severe plastic deformation has been considered as an effective
Fig. 13. Schematic diagram of stir casting technique. (A colour version of this figure can way to refine the grains. During the process, large plastic defor-
be viewed online.) mation occurs in the alloy. The severe plastic deformation can
312 Z. Zhao et al. / Carbon 170 (2020) 302e326

Fig. 14. Schematic diagram of SLM process, with permission from Ref. [89]. Copyright © 2018 Elsevier Ltd. (A colour version of this figure can be viewed online.)

Fig. 15. TEM and HRTEM of Gr-Al composites: (a) Al4C3 with corresponding SAED patterns, and (b) Gr, Al, Al4C3 and interface, with permission from Ref. [89]. Copyright © 2018
Elsevier Ltd.

Fig. 16. The schematic preparation process of the GNPs/Al composites, with permission from Ref. [93]. Copyright © 2018 Elsevier Ltd. (A colour version of this figure can be viewed
online.)

improve the mechanical properties of metal through refining the angular pressing, torsion extrusion and so on [105e117]. Several
grains. The severe plastic deformation methods mainly include kinds of Gr MMC have been prepared by different plastic defor-
accumulative roll bonding, high pressure torsion, equal channel mation way. For example, Ferreira et al. fabricated GO reinforced Al
 Z. Zhao et al. / Carbon 170 (2020) 302e326
Fig. 17. 0.54 wt% GNPs/Al composites before the extrusion treatment. (a) Morphology and corresponding distribution of (b) Al and (c) C elements, with permission from Ref. [93].
Copyright © 2018 Elsevier Ltd.
Fig. 18. Schematic of powder metallurgy route. (A colour version of this figure can be
viewed online.)
MMC by the accumulative roll bonding, as shown in Fig. 23
[118,119]. Ultrafine structured GO/Al was obtained by rolling to 5
cycles, however, the distribution of the GO was non-homogeneous,
as shown in Fig. 24 [118]. Liu et al. also prepared GNPs reinforced Cu
MMC by accumulative roll bonding. After 6 rolling cycles, the ten-
sile strength of GNPs/Cu composites reached 496 MPa [120]. Kho-
bragade et al. prepared Gr reinforced Cu MMC by the high-pressure
torsion method. The Cu powders and Gr powders were mixed and
compressed, as shown in Fig. 25, The Gr/Cu composites prepared by
high pressure torsion exhibited excellent electrical conductivity
and mechanical property [121]. Huang et al. also prepared GNPs-
reinforced Al-based nanocomposites by the high pressure torsion,
the GNPs were dispersed and embedded within the grains, along
the grain boundaries and in relatively large agglomerates, as shown
in Fig. 26 [122]. Severe plastic deformation can be used to prepare
ultrafine structured, high performance Gr MMC, however, it is
313
difficult to prepare large and complex parts.
4.2.4. Layer-by-layer assembly
Layer-by-layer is a simple versatile method for preparing lami-
nated composites. During this process, different nanomaterials are
layer by layer combined on the substrates, as shown in Fig. 27. The
metaleGr nanolayered composites prepared by layer-by-layer as-
sembly exhibited excellent mechanical properties, ultra-high
strengths of coppereGr with 70-nm repeating layer spacing and
nickeleGr with 100-nm repeating layer spacing reached 1.5 and
4.0 GPa, respectively [6]. The basic principle of layer-by-layer as-
sembly is that the Gr is prepared by chemical vapor deposition, and
transferred onto the evaporated metal thin film on an oxidized Si
substrate, and the next metal thin film layer is evaporated [6]. By
repeating the metal deposition and Gr transfer processes, the
metaleGr nanolayered composite was prepared. The Gr can pin the
dislocation at the metaleGr interface and improve the mechanical
properties [6]. Layer-by-layer assembly can prepare ultra-high
strength Gr MMC, however, it is now limited to nanomaterials.
4.2.5. Molecular level mixing
Molecular level mixing can prevent the agglomeration of the
RGO and enhance the adhesion between RGO and Cu. During the
molecular level mixing, GO and Cu salts were mixed, and the Cu2þ
and GO were adsorbed. The Cu2þ was oxidized into CuO by NaOH
solution and decorated on GO surface, the CuO/GO composite
powders were obtained. The CuO/GO composite powders were put
into the furnace tube containing H2, the CuO was converted to Cu
after in-situ reaction with H2 and deposited on RGO surface. The
RGO/Cu composite powders were consolidated by SPS, the yield
strength of the 2.5 vol% RGO/Cu nanocomposite was 284 MPa,
which was 1.8 times higher than that of pure Cu [123].
314 Z. Zhao et al. / Carbon 170 (2020) 302e326

Fig. 19. The composites prepared by powder metallurgy and further hot extruded, with permission from Ref. [94]. Copyright © 2018 Elsevier Ltd. (A colour version of this figure can
be viewed online.)

Fig. 20. TEM and HRTEM of GNPs/Al composites. (aec) as-extruded composite rod, (def) as-drawn microwire at an equivalent strain of 6.00. (c) and (f) are magnified micrographs
of the boxes in (b) and (e), with permission from Ref. [94]. Copyright © 2018 Elsevier Ltd. (A colour version of this figure can be viewed online.)

4.2.6. Template method ~1.5 mm, the RGO is put into porous Cu preform, and the porous
The template method consists of three steps, the porous struc- structure of Cu containing RGO is hot pressed. After hot-pressing,
ture of Cu like fir wood is prepared, the pores are in rectangular the holes are eliminated, and the RGO is uniformly distributed in
shape with an average size of ~20
30 mm and a wall thickness of the cellular structure. The 1.2 vol % RGO-and-Cu nacre exhibited
 Z. Zhao et al. / Carbon 170 (2020) 302e326
Fig. 21. Schematic diagram of friction stir welding. (A colour version of this figure can
be viewed online.)
Fig. 22. HRTEM of the GNPs embedded in the Mg matrix, with permission from
Ref. [103]. Copyright © 2012 Elsevier Ltd.
Fig. 23. Accumulative roll bonding process with GO, with permission from Ref. [118]. Copyright © 2019 Elsevier Ltd. (A colour version of this figure can be viewed online.)
315
good comprehensive mechanical properties, the yield strength was
233 ± 15 MPa, the tensile strength and Young modulus were
308 ± 10 MPa and 109 ± 4 GPa, respectively [124].
4.3. Deposition processing
4.3.1. Electrochemical deposition method
Electrochemical deposition method not only modifies the sur-
face of Gr, but also can prepare the Gr MMC. For example, Zhao et al.
prepared GNPs reinforced Cu matrix composites by electrochemical
deposition, and found that the electrodeposition promoted the
formation of Ni-modified GNPs and oxygen-mediated CueOeC
bonds [72].
4.3.2. Cold spray forming
Cold spraying technology is an emerging material surface
modification technology, in order to enhance the interaction be-
tween the coating materials and the substrate, the powder particles
are accelerated to supersonic velocities using a high-pressure air,
which is forced through a nozzle and deposited on the substrate.
Upon impact, solid particles deform plastically and bond mechan-
ically to the substrate to form a coating. This method can not only
prepare the coating, but also prepare MMC as an additive
manufacturing method. The homogenous distribution of the rein-
forcing materials depends on the premixing. The properties of the
coatings or the MMC depend on the materials in terms of density,
strength and activity. Bakshi et al. prepared the multiwalled carbon
nanotube (CNT) reinforced aluminum nanocomposite coatings by
cold spraying, the nanotubes were uniformly distributed in the
matrix and improved the properties [125]. Yin et al. prepared ho-
mogeneously distributed GNP/copper powders by ball milling, and
GNPs-reinforced copper MMCs coating with lower friction co-
efficients by cold spray [126]. During the cold spraying process, the
easy deformation of solid particles caused the agglomerates of
reinforcing materials and damaged the material structures. In order
to solve this problem, Cho et al. developed a cold spraying process
at a low pressure, and prepared multi-walled carbon nanotube-
reinforced copper nanocomposite coating, the CNTs could
contribute more to improving the strength and the thermal con-
ductivity in metal matrix composites [127].
316 Z. Zhao et al. / Carbon 170 (2020) 302e326

Fig. 24. The microstructures from a 4-cycles sample periphery layer (a), one middle layer (b) and from a 5-cycle sample a periphery layer (c) and middle layers (d), with permission
from Ref. [118]. Copyright © 2019 Elsevier Ltd. (A colour version of this figure can be viewed online.)

Fig. 25. Schematic of the high pressure torsion process, with permission from Ref. [121]. Copyright © 2019 Elsevier Ltd. (A colour version of this figure can be viewed online.)

4.3.3. In-situ synthesis
In order to avoid the damage of Gr, the Gr and its derivatives
were directly in-situ synthesized on the metal surface. Chemical
vapor deposition (CVD) is a widely used technique to prepare GNPs
with high quality and good interfacial bonding between graphene
and metal. During the CVD process, the precursors, gas or vapor,
can react or be decomposed on the preselected substrate at high
temperature and vacuum in a chamber, 2D nanosheets such as Gr
or its derivatives grow on the substrate. The in-situ synthesis solves
the problem of poor dispersion and easy aggregation of Gr, and can
prepare the high performance Gr MMC, such as comprehensive
properties and corrosion resistance. Parasai et al. coated Gr as a
protective coating on the Cu or Ni alloy by CVD, the Gr coated Cu
films were corroded 7 times slower in the Na2SO4 solution than
that of bare Cu, the nickel coated with multilayer Gr was corroded
20 times slower than that of bare nickel [128]. Pu et al. coated Gr on
 Z. Zhao et al. / Carbon 170 (2020) 302e326 317

Fig. 26. HRTEM of 5 turns sample processed by high-pressure torsion at 473 K, (a) the existence of GNPs not only in the grain boundary area but also within the Al matrix, (b) part of
the curved graphene nanoplates having the same orientation with Al matrix, with permission from Refs. [122]. Copyright © 2019 Elsevier Ltd.

Fig. 27. Schematic of metalegraphene multilayer system. (A colour version of this figure can be viewed online.)

stainless steel, the Gr-covered stainless steel exhibited a low
interfacial contact resistance and excellent anti-corrosion property
[129,130].
In conclusion, more and more fabrication methods of Gr MMC
have been reported. The distribution of Gr is homogeneous, and the
interfacial bonding is strong. However, the low cost and fast
preparation methods of Gr MMC, especially for complex and larger
parts, still need be developed further.
(Fig. 28). They could pin the dislocations and grain boundaries
during the deformation process (Fig. 29), which improved the
mechanical performance of the alloy [82,133].
In summary, Gr can effectively improve the mechanical prop-
erties of the alloy, but the elongation at break of the Gr MMC is
usually reduced. How to increase the elongation while maintain an
improved tensile strength is the main research development di-
rection for future.

5. Properties of graphene reinforced metal matrix 5.2. Thermal conductivity

composites
5.1. Mechanical properties
Gr has excellent mechanical properties, for example, the
breaking strength can reach 42 N m1, which is 200 times higher
than that of steel. Its hardness can reach 400 N m1, which makes it
a promising reinforcement material in the metal composites. The
performance of Gr MMC is affected by the volume fraction of Gr,
dispersion of Gr, interfacial bonding, the type of alloy, and the
forming method. Gr has been added to Al alloy, Mg alloy, Ni alloy, Ti
alloy or Cu alloy through different fabrication methods, to improve
the mechanical properties, as shown in Table 1. Gr MMC with high
rigidity and strength can be applied in aerospace fields [131,132].
The strengthening mechanisms of Gr mainly include: grain
refinement, dislocation strengthening and load transfer. The Al-
coated Gr was reported to refine the grains of AlSi10Mg alloy
The thermal conductivity of metal ranges from 230 to
430 W$m1$K1, while the thermal conductivity of Gr is
4000 W$m1$K1. The volume fraction, distribution and
morphology affect the thermal conductivity of the Gr MMC. The
addition of Gr to the metal matrix could significantly improve the
thermal conductivity, as shown in Table 2. However, the existing
defects in the Gr MMC could reduce the thermal conductivity. For
example, Wejrzanowski et al. found that the addition of single-
layer Gr to the Cu metrics did not enhance the macroscopic ther-
mal conductivity. That was because of small pores in the MMC and
very low volume fraction of Gr. However, adding multi-layer Gr
improved the thermal conductivity [181].
Negative effects of Gr on thermal conductivity of MMC were
reported as well. For example, Yang et al. found that the addition
of a small amount of Gr would reduce the thermal conductivity of
titanium. That was because there were some pores in the
318 Z. Zhao et al. / Carbon 170 (2020) 302e326

Table 1
Mechanical properties of Gr MMC.

Matrix Materials Preparation method Ultimate tensile Yield Hardness Elongation/% Reference
strength/MPa strength/MPa

Al alloy 0.1 wt% Gr/Al Ball milling, hot isostatic pressing, 270 198 84 ± 5 HV e [134]
extrusion
0.3 wt% GNPs/Al Flake powder metallurgy 249 e e 13 [135]
0.3 wt% RGO/Al Hot pressing e e 1.59 ± 0.07 GPa e [136]
1 wt% Gr nanoflakes/Al Cryomilling and hot extrusion 248 194 e 8.3 [137]
0.3 wt% GNPs/Al Semi-powder, hot extrusion 280 ± 5 195 ± 3 85 ± 5 HV 9.53 ± 1.5 [138]
0.5 wt% Gr nanoflakes/Al Powder metallurgy, hot extruded 467 319 e 11.7 [139]
0.7 vol% Few-layer Gr/Al Hot-rolling 440 e e e [140]
GNPs/AA5052 Friction-stir processing 244.3 148.7 84 HV 20.1 [141]
0.42 wt% few-layer Gr/Al Spark plasma sintering, hot extrusion 177.5 ± 3.9 148.6 ± 2.6 18.8 ± 2.4 [142]
GO/Al Friction stir welding 191.99 28 [102]
GNPs/Al6061 Friction stir welding 141.53 ± 2.05 86.935 ± 0.685 e 14.88 ± 0.62 [143]
5 wt% GNPs/Al High-pressure torsion 350 e e 1.8 [122]
1.8 wt% GNPs/5083 Al Pressure infiltration 331.0 186.9 e 6.3 [144]
0.3 wt% GNPs/Al6063 Pressure infiltration and hot extrusion 276.7 e e 14.7 [145]
1 wt% GNPs/2009Al Powder metallurgy and multi-pass 514 398 e 10 [146]
friction stir processing
GO/Al Accumulative roll bonding e e 84.6 HV e [118]
2 wt% Gr/AleSn Mechanical alloying and vacuum hot e e 91 HV e [147]
pressing
0.7 wt% Gr/Ale10Zn-3.5Mg- Hot extrusion 610 e e e [148]
2.5Cu
0.4 wt% GNPs/Al Extrusion, cold drawing 219 ± 10.4 208 ± 8.2 e 0.84 ± 0.16 [149]
0.54 wt% Gr/Al Pressure infiltration and extrusion 275 215 e 11.7 [93]
0.3 wt% GO/Al Powder metallurgy 167 e e 11.5 [150]
40 At % Gr/Al Friction stir alloying 147 ± 5 94 ± 5 48.7 ± 0.6 HV 26 ± 1 [151]
2.5 wt% Gr/Al 3D printing 66.6 HV [89]
Mg alloy 0.18 wt% GNPs/Mge1%Ale1%Sn Semi powder metallurgy, hot extrusion. 269 ± 3 208 ± 5.3 e 10.9 ± 3.4 [152]
0.18 wt%GNPs/Mge10Ti Semi powder metallurgy, hot extrusion 230 ± 3 160 ± 5.3 e 14 ± 3.4 [153]
0.6 wt% GNPs/Mge1Al Semi-powder metallurgy, hot 265 ± 8 204 ± 9 63 ± 2 HV 4.0 ± 0.6 [154]
extrusion.
3.0 wt% GNPs/AZ31 alloy Stirring casting, hot extruded 299 ± 6.2 195 ± 4.5 68.9 HV 12.56 ± 4.3 [87]
0.6 wt% GNPs/AZ91D Thixomolding 245 e 92.1 HV 3.9 [155]
0.1 wt% GNPs/ZK60 Melt stirring, hot extrusion processes 343 ± 3.8 283 ± 3.5 75 ± 2.5 HV 17 ± 2.0 [156]
1.6 vol% GNPs/Mge6Zn semi-solid stirring, high energy 352 ± 2 271 ± 4 6.3 ± 1.0 [157]
ultrasonic processing, hot extrusion
0.3 wt% GNPs/Mge1Al Powder metallurgy and hot extrusion 246 ± 3.5 178 ± 2.9 55 ± 4 HV 16.9 ± 3 [158]
0.3 wt% GNPs/AZ31 Powder metallurgy and extrusion 275 ± 5.7 173 ± 6.2 71 ± 2.1 HV 21.7 ± 2.8 [159]
0.5 wt% GNPs/AZ91 Sintering and hot extrusion 335 ± 4.8 296 ± 3.7 88.5 ± 1 HV 8.7 ± 0.1 [160]
0.5 wt% GO/AZ91 Sintering and hot extrusion 355 ± 4.5 312 ± 4.5 96.1 ± 2 HV 11.3 ± 0.2 [161]
0.6 wt% GNPs/AZ80 Rheo-casting and by hot extrusion 325 ± 32 160 88.9 ± 5 HV 9.3% [162]
0.18 wt% GNPs/Mge1.5Al Semi powder metallurgy, hot extrusion 268 ± 4.5 209 ± 3.9 60 ± 3 12.7 ± 2 [163]
1.5 wt% GNPs/Mge6Zn Casting and hot extruded 313 ± 5.2 214 ± 2 e 21 ± 1.1 [164]
Ni alloy 0.12 wt% GO/Ni Electrodeposition e e 6.85 GPa e [165]
GNPs/Ni Electrochemical deposition e e 4.6 GPa e [166]
1 wt% Gr/Inconel 718 Selective laser melting 1417 1175 508 HV 4.3% [167]
0.25 wt% RGO/Inconel 718 Spark plasma sintering e 375 HV e [168]
Ti alloy 3.5 wt% multilayer Gr/TiAl Spark plasma sintering e e 700.3 HV e [169]
Cu alloy 2.5 vol% RGO/Cu Compacting and spark plasma sintering 335 284 e 15 [170]
1 vol % Multi-layer Gr/Cu Ball milling, high-ratio speed rolling 425.5 ± 3.3 360.5 ± 2.1 e 16.4 ± 3.6 [171]
Gr/Cu foil Electrochemical approach e e 2.5 GPa e [172]
0.8 vol% Ni-GNPs/Cu Spark plasma sintering 245 e e 9 [173]
1.0 vol% Ni-GNPs/Cu Spark plasma sintering 320 268 e e [174]
1 vol% Pore RGO/Cu Spark plasma sintering 251 ± 7.6 209 ± 9.5 e 18 ± 0.8 [175]
10 vol% GNPs/Cu Spark plasma sintering 265 e e 7 [176]
0.1 wt% Multiscale Gr/0.5 wt% Hot-pressed sintering 184.2 60.1 60.3 HV 22.8 [177]
carbon fiber/Cu
11.8 wt% GNPs/Cu Electrochemical deposition and 111.2 HV [178]
atmosphere sintering
0.3 wt% Gr/Cu Powder metallurgy 210 e 51 17.5% [179]
GNPs/Cu Accumulative roll bonding 496 e e 5% [120]
10 wt% Gr/Cu High pressure torsion e e 2.67 ± 0.08 GPa e [121]
1 wt% GNPs/Cu Mechanical milling, the hot pressing e e 62.9 HV e [180]
1.5 vol% RGO/CueTi Powder metallurgy, spark plasma 290 e 15% [84]
sintering

composites, as well as the Gr aggregates in the matrix [182]. In
summary, in order to obtain high thermal conductivity of Gr
MMC, the Gr should be distributed homogeneously, and few
defects should exist in the composites. With good thermal con-
ductivity, Gr MMC have been used in aerospace and military
fields [183].
5.3. Electrical performance
For more than 100 years, metals with intrinsically high electrical
conductivity are responsible for the power transmission. Both
electrical conductivity and mechanical properties need satisfy
higher requirements of modern devices. Unfortunately,
 Z. Zhao et al. / Carbon 170 (2020) 302e326 319

Fig. 28. The microstructure of Al-coated Gr/AlSi10Mg composites (cross section) prepared by SLM (a), the microstructure of AlSi10Mg alloy (cross section) prepared by SLM (b), with
permission from Ref. [82]. Copyright © 2019 Elsevier Ltd. (A colour version of this figure can be viewed online.)

Fig. 29. TEM of Gr/AlSi10Mg composites prepared by SLM: (a) before deformation, (b) after deformation, with permission from Refs. [82]. Copyright © 2019 Elsevier Ltd. (A colour
version of this figure can be viewed online.)

Table 2
The thermal conductivity of several common metal materials.

Matrix Composites Preparation method Coefficient of thermal conductivity (W$m1$K1) Reference

Al alloy Gr/5052-H32 Friction stir processing 171.7 at 250  C [102]

Ni alloy 0.12 wt% GO/Ni Electrodeposition 79.4 [184]
Ti alloy 10 vol% GNPs/Ti Hot press sintering 115 [98]
Cu alloy Gr/Cu Plasma-enhanced chemical vapor deposition 135e160 [185]
30 vol% GNPs/Cu Spark plasma sintering 458 [186]

conventional forming methods used to strengthen metals also
generally cause a pronounced decrease in the electrical conduc-
tivity. The Gr has a lower resistivity (106 ῼ$cm) than other ma-
terials because of its special structure [187e190]. Each carbon atom
in Gr is bonded to the adjacent three carbon atoms through a s
bond and forms sp2 hybridization. At the Gr layer, there are only
three s-bonds. The fourth bond projects upward and downward
from the plane of the layer, the electron cloud is formed and creates
a continuous p orbital across the whole Gr layer. The free move-
ment of electrons crosses the whole Gr layer (Fig. 30), which makes
Gr highly conductive. When the Gr is added into the metal, the
electrical performance is improved, as shown in Table 3. The added
Gr in the metal compromises the conflicts between the mechanical
properties and the electrical performance, and improves both
mechanical properties and electrical performance.
5.4. Anticorrosion properties
Corrosion can deteriorate the metals, and is caused by chemical
reaction between surrounding environment and metal. The metal
types and environmental conditions affect the form and rate of
deterioration. When metal corrosion occurs, it will have a negative
impact on the structure and shorten its service life. The common
method to inhibit the metal corrosion is to coat a protective coating
on the metal surface. However, the protective conductive polymers,
conductive polymer nanocomposites or thiol-based monolayers
can’t withstand high temperatures [195,196]. With inactive chem-
ical properties, stable thermodynamic properties and strong
oxidation resistance, the Gr coating can protect the metal from O2,
and inhibit the metal from corrosion (Fig. 31) [197]. For example,
Laleh et al. prepared GO coated 7049 alloy by lift up method, and
320 Z. Zhao et al. / Carbon 170 (2020) 302e326
found that a greatly enhanced corrosion resistance of GO/Al sample
(a factor of 1237 times) relative to that of untreated Al [198].
Fernandez et al. coated RGO onto Mg through electrochemical and
chemical methods, a reduced corrosion rate of 85% was obtained in
the physiological saline 0.9 wt % NaCl electrolyte [199]. Zhao et al.
coated Gr on Ag thin films, and the corrosion rate was reduced by
about 66 times [200]. The performances of Gr anticorrosion coat-
ings are summarized in Table 4. However, the existing defects in the
CVD grown Gr have limited corrosion inhibition, and even enhance
the corrosion. That is because oxide would preferentially occur at
the defects in the Gr lattice [201,202].
The Gr coating on Cu indeed offered an effective short-term
oxidation protection. However, over long time scales, this Gr
coating induced more extensive wet corrosion than that was seen
for the initial bare Cu [203]. Graphite is cathodic to Cu and pro-
motes the corrosion of Cu. However, due to the impermeability of
Gr to gases and the closer Gr metal bonding, the O2 and H2O are
separated, and a slow corrosion will occur in a short term. When
the time is long, the defects occur in the Gr, and accelerate the
corrosion [203e205].
Gr MMC preparation methods can affect the corrosion rate of
the composites. For example, Rashad et al. prepared the 0.5 and
1.0 wt% GNPs by hot extrusion, the GNPs reduced the corrosion
resistance of Al [206]. That was because the Gr particles were
cathodic relative to the matrix, and thus a galvanic corrosion was
caused in the presence of an electrolyte [206]. In summary, coating
Gr with good compactness on metal could inhibit the metal
corrosion.
6. Applications
With the aforementioned unique properties, the applications of
Gr MMC in aerospace, automotive, electronics, medical in-
struments, and so on are illustrated briefly in the following.
6.1. Aerospace industry
The development of aerospace materials towards high precision,
lightweight and high-performance applications promotes the
research of metal matrix composites. The Gr MMC can provide low
coefficient of thermal expansion and desired stiffness during the
space maneuvers. In addition, Gr MMC with excellent electrical
conductivity can improve the electrical-signal transmission
Fig. 30. The schematic of free movement of electrons across the whole Gr layer. (A
colour version of this figure can be viewed online.)
between the antenna dish and the spacecraft.
6.2. Electronics
The Gr MMC with high conductivity, tailorable coefficient of
thermal expansion and low density have broad applications in the
electronic industry, such as electronic packaging, electromagnetic
interference (EMI) shielding, and so on [213e216]. Gr/Al electronic
packages have been space-qualified and applied in communication
satellite and global positioning system satellite [64]. The metal
oxide/carbon and carbon/metal chalcogenide composites exhibit
high EMI shielding effectiveness, which could be expected to be
applied in the field of EMI shielding [217]. The Gr/Cu composites
with a high electrical conductivity can be used to fabricate indus-
trial brushes, which exhibit excellent wear resistance and con-
ductivity. The Gr/Al MMC are processed into long span overhead
wires, the transmission capacity of overhead wires is improved
effectively.
6.3. Automotive industry
With the development of automobile industry, about 50% of
global production of metal composites has been applied in the field
of automotive industry [218]. Most parts of cars are made of metal
composites. The Gr-reinforced MMCs exhibit a better wear resis-
tance, which can be used for manufacturing bearing surfaces, cyl-
inder liners, pistons, cam shafts, tappets, lifters, rockers and brake
components [218,219].
7. Conclusion and perspective
The preparation methods and properties of the Gr MMC with
good structural integrity and functional properties have been crit-
ically reviewed together wither their applications in aerospace,
automotive, electronics and military fields. Many methods to pre-
pare Gr MMC with their inheriting advantages and disadvantages
have been summarized such as powder metallurgy, stirring casting,
friction stir welding, severe plastic deformation, selective laser
melting, pressure infiltration and so on. These methods can prepare
high performance Gr MMC, i.e., homogeneous distribution of Gr,
and strong interfacial bonding. However, there are some defects in
these methods, for example, it is difficult to eliminate pores and
other defects in the products prepared by powder metallurgy. The
adding amount of Gr is limited during stirring casting, and the Gr
can be easily agglomerated. It is difficult to prepare large or com-
plex shape parts through friction stir welding, severe plastic
deformation, and pressure infiltration methods. Selective laser
melting can prepare complex shape parts, but Gr affects the laser
absorption rate of metal powders, the pores can be easily formed.
Two challenges, i.e., agglomeration of Gr and poor interfacial
bonding, need be further exploited to prepare high-performance Gr
MMC especially at a large scale. Most liquid metals are difficult to
wet the Gr and the contact angle is usually larger than 90 .
Meanwhile, both poor wettability and big density difference be-
tween Gr and metal matrix cause agglomeration of Gr in the metal
matrix. Surface engineering strategies have been disclosed to be an
effective approach to solve these two challenges. Physical (me-
chanical) and chemical bonding are two main interface modes
between Gr and metal matrix. Both bonding modes mainly involve
tailoring the alloy composition, modifying the Gr surface, engi-
neering the defects of Gr, and the method of forming the Gr MMC.
Advanced methods to design and adjust the interface between Gr
and metal are the main development direction.
Via coating metallic element on Gr, the wettability between
metal element and Gr can be improved. Meanwhile, these coating
 Z. Zhao et al. / Carbon 170 (2020) 302e326 321

Table 3
Electrical conductivity of the Gr/metal composites.

Matrix Composites Preparation method Electrical conductivity (% IACS) Reference

Cu alloy 1.6 vol% Gr/Cu Hot pressing 97.1 [191]

2.5 vol% Gr/Cu Hot pressing 93.8 [191]
0.008 vol % Gr/Cu Chemical vapor deposition 117 [192]
1 wt % Gr/Cu Ball milling and hot-pressing 94 at 600  C [180]
10 wt % Gr/Cu High pressure torsion 87 [121]
0.5 wt % RGO/Cu Powder metallurgy 96.47 [99]
Gr/carbon fiber/Cu Hot-pressed sintering More than 80 [177]
11.8 wt % GNPs/Cu Electrochemical deposition and atmosphere sintering 89.2 [178]
Gr/Cu Rolling and sintering processes 98 [193]
0.4 wt% Gr/Cu Mechanical alloying and spark plasma sintering 79 [194]
0.4 wt% Gr-3 wt% Co/Cu Mechanical alloying and spark plasma sintering 65 [194]
Sliver alloy 0.5 wt % Gr/sliver Powder metallurgy 98.62 [66]
Al alloy 0.42 wt % GO/Al Spark plasma sintering and hot extrusion 60 [142]
5 wt % Gr/Al High pressure torsion 69.5 ± 2.3% [122]

Fig. 31. Barrier effect on corrosive media of Gr film, with permission from Ref. [197]. Copyright © 2018 Elsevier Ltd. (A colour version of this figure can be viewed online.)

Table 4
Performance of Gr anticorrosion coatings [207].

Substrates Preparation method The performance of Gr film Reference

Cu Chemical vapor deposition The Cu films coated with Gr were corroded 7 times slower in Na2SO4 solution than that of bare Cu. [128]
Cu Electrochemical approach The inhibition efficiency of GNPs coated Cu was calculated to be 94.3% in 3.5% NaCl solution. [208]
Cu Acetone-derived Gr Gr-coated Cu surface exhibits 37.5 times higher corrosion resistance as compared to that of [209]
mechanically polished Cu in 3.5% NaCl solution.
Cu Chemical vapor deposition Gr films on the Cu substrate improved the corrosion performance of the material for a short period of [210]
time.
Cu Chemical vapor deposition Gr greatly eliminates the toxicity of Cu by inhibiting corrosion and reducing the concentration of Cu. [211]
Cu In-situ catalytic growth and The corrosion rate of the as-fabricated bulk Gr/Cu composites is reduced by 50% in NaCl solution. [212]
assembling
Ni/SUS304 Chemical vapor deposition The Gr coating on stainless steel can enhance its anti-corrosion property. [129]
stainless steel
Steel Electrophoretic deposition Providing good corrosion protection against hydrochloric acid aqueous [130]
Ag Chemical vapor deposition The Gr-coated Ag thin film was reduced by about 66 times and maintained the high stability and unique [200]
optical properties of Ag thin films in 0.1 M NaCl solution.
Al Lift up method A great enhancement in the corrosion resistance of GO/Al sample relative to that of untreated Al (a factor [198]
of 1237 times)
Mg Chemical and electrochemical A reduction corrosion rate of 85% was obtained in physiological saline 0.9 wt % NaCl. [199]
methods
Ni Chemical vapor deposition Direct coated nickel substrates were corroded 20 times slower than bare nickel. [128]

metal elements increase the density of Gr, which can facilitate the
dispersion of Gr in the metal matrix. Some alloy elements such as
chromium or boron can improve the interfacial bonding between
Cu and carbon fiber [64]. Some rare earth elements such as Y can
also improve the interfacial bonding between carbon fiber and Mg
[220]. Some elements can even react with Gr to form compounds,
the compound as an intermediate bridge can connect Gr with the
metal matrix, thus the interfacial bonding strength of the com-
pound between Gr and metal matrix will become strong. As a
result, it is an important direction to find alloy elements that can
322 Z. Zhao et al. / Carbon 170 (2020) 302e326
improve the wettability between Gr and metals, or the element that
can become a bridge between Gr and metal matrix. Both will be the
focus of future research studies.
Surface modification of Gr is another approach for enhancing
the interfacial bonding. The reported surface modification methods
include chemical reduction, hydrothermal, electrochemical depo-
sition, physical vapor deposition, self-assembly, coating Al on Gr by
chemical reduction of organic Al, and so on. Introducing surface
defects in Gr by advanced treatment methods, such as plasma
treatment, is another approach to enhance the interfacial bonding.
The Gr defect region is active and favors interfacial oxides/carbides
formation. The composites exhibited excellent mechanical prop-
erties. However, Gr surface modification methods with low cost
and short process time need be developed further. Meanwhile, the
Gr without any modification with a capability to improve the per-
formance of composites may be a potential area.
Gr MMC have good thermal conductivity, electrical perfor-
mance, mechanical properties, corrosion properties and so on. With
the development of forming technology and reduced cost, Gr
reinforced MMC will be widely used in rail transit, machinery,
electric wire and civil fields, and the engineering application field of
Gr MMC needs to be further expanded. However, parts with com-
plex shapes are difficult to be prepared from MMC with these
traditional methods. Proper processing methods are needed to be
developed for preparing complex final products with complex
shapes from these versatile MMC.
Although Gr MMC have excellent properties, most still remain at
experimental stage, and have not been industrialized in a large-
scale. Large scale preparation and manufacturing of MMC will be
another future direction for this area.
Declaration of competing interest
The authors declare that they have no known competing
financial interests or personal relationships that could have
appeared to influence the work reported in this paper.
Acknowledgments
The authors would like to thank the National Natural Science
Foundation of China (Grant No. 51775521), the China Postdoctoral
Science Foundation (2019M661068), the Key Research and Devel-
opment Project of Shanxi Province (201903D121009), the Natural
Science Foundation of Shanxi Province: 201801D221154, the Major
Science and Technology Projects of Shanxi Province, China
(No.20181101009, 20181102012), Science and Technology on Power
Beam processes Laboratory Foundation (JZX7Y201901SY008501),
National Key Laboratory for Remanufacturing Foundation
(JZX7Y201901SY00501).
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