Energy Storage Materials 24 (2020) 22–51

Contents lists available at ScienceDirect

Energy Storage Materials

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

Graphene-based composites for electrochemical energy storage

Bo Wang a, b, *, 1, Tingting Ruan a, 1, Yong Chen a, Fan Jin a, Li Peng c, Yu Zhou b,
Dianlong Wang a, **, Shixue Dou d, ***
a
MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of
Technology, 150001, Harbin, China
b
School of Materials Science and Engineering, Harbin Institute of Technology, 150001, Harbin, China
c
Department of Polymer Science and Engineering, Zhejiang University, Polymer Building, 38 Zheda Road, Hangzhou, 310027, PR China
d
Institute for Superconducting & Electronic Materials, Australian Institute of Innovative Materials, University of Wollongong, Wollongong, NSW, 2500, Australia

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

Keywords: Since the first exfoliation in 2004, graphene has been widely researched in many fields of materials engineering
Graphene due to its highly appealing properties. Recently, graphene-based composites have attracted increasing attention
Composite for electrochemical energy storage by combining the merits of graphene and other electrochemical materials to
Electrochemical energy storage
achieve superior electrochemical performances. In this review, we start with the properties and production
Capacitor
Battery
methods for graphene, summarize the recent research progress on graphene-based composites for electrochemical
energy storage from the structural and interfacial engineering viewpoints, and underscore the significance of the
dimensionality and compound interface characteristics in the rational construction and design of these com-
posites. We also discuss recent specific applications of graphene-based composites, from electrochemical capac-
itors and lithium-ion batteries to emerging electrochemical energy storage systems, such as metal-air and metal-
sulfur batteries. The new features and challenges of graphene-based composites for electrochemical energy
storage are also summarized and discussed. This review is specifically aimed at offering new perspectives on the
combination of graphene with other electrochemical materials to optimize their performances, and will outline
ways to further improve graphene-based composites towards the next generation of electrochemical energy
storage devices.

1. Introduction
Currently, realizing a secure and sustainable energy future is one of
our foremost social and scientific challenges [1]. Electrochemical energy
storage (EES) plays a significant role in our daily life due to its wider and
wider application in numerous mobile electronic devices and electric
vehicles (EVs) as well as large scale power grids [2]. Metal-ion batteries
(MIBs) and electrochemical capacitors (ECs) represent two important
families of EES systems [3]. MIBs possess high energy density through
storing charge and metal ions (especially Liþ and Naþ) in the bulk of
electrodes via comparatively slow faradaic reactions, while ECs provide
high power density at the expense of energy density, due to their fast
surface or near-surface energy storage mechanisms [4]. To meet the
growing demands of both industry and society, advancing EES systems by
pursuing higher energy density, higher power density, and better cycling
stability, is an important and pressing mission [5]. One of the critical
factors in realizing the abovementioned target is exploring ideally
structured electrode composites with the desired synergistic effects be-
tween the different functional components [6].
Recently, graphene has been attractive for broad application in EES,
due to its unique properties from both physical and chemical aspects [7],
including its outstanding electrical conductivity and extraordinary me-
chanical properties as well as large theoretical specific surface area, and
reports from many groups have verified its potential to innovate the
current EES landscape [8–11]. In theory, graphene presents a Liþ storage
capacity of 744 mAh⋅g1 and electric double-layer (EDL) capacitance of

* Corresponding author. MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engi-
neering, Harbin Institute of Technology, 150001, Harbin, China.
** Corresponding author.
*** Corresponding author.
E-mail addresses: wangbo19880804@163.com (B. Wang), wangdianlongwbhit@163.com (D. Wang), shi_dou@uow.edu.au (S. Dou).
1
These authors contribute equally to this works.

https://doi.org/10.1016/j.ensm.2019.08.004
Received 19 June 2019; Received in revised form 30 July 2019; Accepted 2 August 2019
Available online 6 August 2019
2405-8297/© 2019 Elsevier B.V. All rights reserved.
B. Wang et al.
Fig. 1. Schematic illustration of the outline for this review. GBCs represents graphene-based composites.
550 F g1 as the active material for Li-ion battery (LIB) anode and elec-
trochemical double-layer capacitor (EDLC) electrode, respectively [12].
The current experimental results on the abovementioned applications
differ significantly, however, from these theoretical values due to the
spontaneous re-stacking of graphene layers, which occurs during both
the manufacturing and the repeated charging/discharging processes of
the electrode, leading to a significant reduction of the practical active
sites for electrochemical reactions or charge storage processes [10].
Therefore, substantial efforts have been invested in exploring
graphene-based composites to inhibit the re-stacking of graphene layers
and increase the active sites and surface area [13,14].
Graphene-based composites [15], which can combine the advantages
of the graphene component and electrochemical materials to achieve
superior electrochemical performance, have thus been proposed for
application in various kinds of EES systems. Nevertheless, due to the
complexities in the microstructures and electrode processes of different
graphene-based composites, challenges for clearly understanding their
EES mechanisms have also appeared, which require systematic electro-
chemical analysis combined with adequate theoretical calculations and
advanced operando techniques [16,17]. Moreover, the introduction of
graphene components will also introduce some new features into the
composites, such as flexibility, transparency, self-healing properties, etc.
[11] Some reviews have already been published on graphene-based
composites from viewpoints of preparation strategy or structure, or
with a focus on specific EES or environmental applications [9,12,18–29],
but a comprehensive view of the graphene-based composites, combining
preparation strategies, structural designs and specific applications, as
well as emerging features and challenges for EES, is still missing.
In this review, we start with the properties and production methods
for graphene, summarize the recent research progress on graphene-based
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Energy Storage Materials 24 (2020) 22–51
composites (GBCs) for EES from the structural and interfacial engineer-
ing viewpoints, and underscore the significance of dimensionality and
compound interface properties in the rational construction and design of
these composites. We also discuss recent specific applications of
graphene-based composites from electrochemical capacitors (ECs) and
LIBs to emerging EES systems, such as metal-air and metal-sulfur batte-
ries. The new features and challenges of graphene-based composites for
EES are also summarized and discussed. This review is specifically aimed
at offering new perspectives on the combination of graphene with other
electrochemical materials to optimize their performances, and it outlines
methods for further improvement of graphene-based composites towards
the next generation of EES devices. The outline of this review is illus-
trated in Fig. 1.
2. Properties and preparation methods of graphene
2.1. Properties of graphene
Graphene, a defect-free flat carbon monolayer with theoretical spe-
cific surface area (SSA) of 2630 m2 g1, is the basic unit of the 2-dimen-
sional (2D) carbon family, which includes family members with very
different properties based on different morphologies, defects, di-
mensions, and layers (Fig. 2) [10,30–32]. Because of the unique 2D
structure, the first Brillouin zone of monolayer layer graphene possesses
two inequivalent points (Dirac points) with a crossing band, which makes
graphene a zero-gap semiconductor with both semiconducting and
metallic properties [33–35]. However, bilayer graphene exhibits para-
bolic bands without Dirac electrons, and trilayer graphene exhibits a
combined band structure of monolayer and bilayer. Generally speaking,
odd-layer graphene with AB stacking structure possesses a linear band.
B. Wang et al. Energy Storage Materials 24 (2020) 22–51

Fig. 2. Properties, preparation methods, defects and derivatives of graphene. (a) Various characteristics in terms of electrical conductivity, thermal conductivity,
mechanical behavior, opacity, SSA, and chemical behavior. (b) The most common graphene synthetic pathways in terms of graphene quality, cost, scalability, purity,
and yield. Reproduced with permission from ref. 10, copyright 2015, Nature Publishing Group. (c) Introduction of intrinsic or extrinsic defects in graphene. (d)
Schematic illustrations of the different structures of graphene derivatives. Reproduced with permission from ref. 31, copyright 2017, American Association for the
Advancement of Science. Reproduced with permission from ref. 32, copyright 2011, American Chemical Society.

With the increase of the number of graphene layers, the band structure
becomes more complex with the overlap of the conduction and valence
bands [12].
The carrier mobility of graphene at room temperature could reach
15000 cm2 V1 s1 with the charge carriers adjustable between electrons
and holes (up to a concentration of 1013 cm2) [33,35]. Moreover, mo-
bilities over 200000 cm2 V1 s1 have been achieved in suspended gra-
phene by minimizing impurity scattering [36]. Correspondingly, the
electrical conductivity of graphene is quite high, which is beneficial for
improving the electrical conductivity of the graphene-based composites
for EES. For example, the electrical conductivity of a graphene film re-
ported by Chao Gao’s group reached ~106 S m1 [37]. Recently, Pablo
Jarillo-Herrero’s group found an interesting superconductivity
phenomenon in twisted bilayer graphene (with a small angle of ~1.1 ),
which could lead to insights into the physics of high-critical-temperature
superconductors and quantum spin liquids [38,39]. It should be
mentioned that the electrical conductivity of graphene is significantly
influenced by the number of layers and the stacking orders, as well as the
amount and type of defects with very complex influencing mechanism
[40–43]. High-temperature treatment (>2000  C) has been demon-
strated could effectively reduce the defect concentration of graphene by
healing the defect configurations to enhance its electrical conductivity
[37,44]. In addition, foreign atoms doped graphene could also improve
the electrical conductivity with appropriate doped position and quantity
[45]. Typically, Zhongshuai Wu et al. confirmed that the doped graphene
with N and/or B atoms could enhance its electrochemical reactivity and

24
B. Wang et al.
electrical conductivity with superhigh rate and large capacity for LIB
anodes [46].
The opacity of graphene is ~2.3% in a broad wavelength ranged from
ultraviolet to near infrared due to its special 2D microstructure with
single-layered atomic thickness [47,48]. An experimental transparency
value in the visible range has reached ~97% [49]. On the other hand, the
researchers also found that the transmittance of graphene decreases
linearly as the layers increase [50–52]. It is worth noting that, when the
input optical intensity is above a threshold value, the absorption becomes
saturated, resulting in a non-linear optical behavior [53]. Because of its
superior optical properties, graphene is considered as a potential material
for transparent applications in the future, not only limited to EES devices,
but also for solar cells, smart windows, and other optoelectronic devices.
The thermal conductivity of suspended graphene is very high
(4840–5300 W m1 K1), which is superior to those of other carbon
materials (e.g., carbon nanotubes and diamond) [54,55], making it a
potential substance that can be used to enhance the thermal conductivity
of electrochemical materials through different composite-forming pro-
cesses, which is beneficial for dissipating the heat generated in the case of
high current loads or abuse conditions for the final fabricated EES de-
vices. Alexander A. Balandin et al. reported that, by including 5 and
10 vol% graphene, thermal conductivities could be improved by ~500%
and ~2300% for graphene-metal and graphene-polymer composites,
respectively, which mainly resulted from the intrinsically high thermal
conductivity of the graphene component combined with its strong syn-
ergetic effects with metal and polymer components [56,57]. Similar to
the electrical conductivity, the thermal conductivity is also largely
influenced by the quality of graphene, such as the lateral size and defect
factor [42]. Recently, Li Peng et al. reported a macroscopic graphene film
composed of large-sized and defect-heald graphene sheets, which could
exhibit a high thermal conductivity of 1940 W m1 K1 after
high-temperature (3000  C) and high-pressure (300 MPa) treatment
[37].
The mechanical properties of graphene are very excellent because of
the strong σ bonds (C–C bonds), in terms of having a high Young’s
modulus and strong fracture strength [58]. James Hone et al. demon-
strated that graphene has a Young’s modulus of ~1 TPa, which seems to
depend upon the layers and defects of graphene [58]. Moreover, the
breaking strength of graphene is almost 200 times higher than that of
steel [58]. The superior mechanical properties of graphene make it a
great basic candidate for flexible and wearable EES devices. In addition,
both experimental tests and theoretical calculations have demonstrated
that uniaxial stress and anisotropic strain have different levels of influ-
ence on the electrical properties of graphene [48,59]. Keun Soo Kim et al.
studied the interplay of mechanical and electronic properties of gra-
phene. They found that the resistance in the bent direction increased
almost one order of magnitude, which was due to the difference in
stretching along the parallel and perpendicular direction [48]. In another
case, Mark A. Bissett et al. demonstrated that the mechanical strain could
change the structure of graphene, and dramatically improve the chemical
reactivity of graphene [60]. It should be mentioned that the existence of
defects in graphene may remarkably influence its mechanical properties,
which decrease as the number of defects increase. Normally, recon-
struction and healing of vacancy-type defects are the main strategies to
minimize these detrimental effects [61].
In the case of chemical properties, perfect-structured graphene is
quite inert, so that it generally interacts with other components via
physical adsorption (e.g., π-π interaction) [62]. In order to realize higher
reactivity, defects (e.g., vacancies, edges, deformations, etc.), foreign
atoms (e.g., H, F, N, B, etc.), or surface functional groups (e.g., carboxyl,
carbonyl, or amine groups, etc.) are usually introduced into graphene
[46,63]. For example, the existence of defects in graphene may result in
locally curved structures, which could give rise to the local doping sites,
and thus influence its chemical reactivity [64]. When the foreign atoms
and functional groups are grafted into graphene, the highly extended π
electron cloud would be disrupted, leading to the change of its original
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Energy Storage Materials 24 (2020) 22–51
electrical properties [53]. Moreover, It should be noted that an important
derivative of graphene – graphene oxide (GO), is hydrophilic in nature,
and thus, it has been widely used in combination with other materials in
appropriate aqueous systems for the synthesis of graphene-based com-
posites [65–67].
2.2. Preparation methods of graphene
The most common preparation strategies for graphene are shown in
Fig. 2b, and these play crucial roles in determining the qualities and
properties of the products [68]. Among these strategies, mechanical
exfoliation [69], epitaxial growth on SiC [70,71], and bottom up syn-
thesis from organic precursors [72,73] have relatively limited scalability
combined with high cost, which restrict their large-scale application in
both fundamental research and commercial applications. Although
chemical vapor deposition (CVD) of hydrocarbons (e.g., CH4, C2H2, etc.)
[74–77] is a mature technique for the preparation of graphene in in-
dustry, it is inappropriate for mass production for EES, due to its high
cost, relatively low yield, and mediocre product quality.
Apart from the above-mentioned methods, liquid-phase exfoliation
[78–80] and reduction of GO [81–83] are two general strategies for
mass-production of graphene. In the first strategy, the treated graphite
particles (e.g., expanded graphite) are firstly dispersed in a suitable sol-
vent to lower the strength of van der Waals attraction between the
adjacent layers. Then, an exterior driving force (e.g., ultrasonication
[78], electric field [79], mechanical shearing [80], etc.) is employed to
exfoliate the graphite bulk into high-quality graphene sheets. Moreover,
this strategy is suitable for preparing graphene in bulk quantities because
of its high scalability and low cost. The existence of considerable amounts
of unexfoliated or less-exfoliated graphite results in a low yield for this
technique, however.
In the second strategy, GO is first prepared by oxidizing pristine
graphite, followed by dispersing it in a liquid medium through stirring or
ultrasonication [84]. The product then needs to be reduced to recover the
π network and electrical conductivity for application in EES [85].
Correspondingly, many reduction processes (e.g., chemical [86], thermal
[87], electrochemical [88], etc.) have been adopted to obtain reduced
graphene oxide (RGO). Although the product yield of this strategy is high
and the cost can also be effectively contained, the quality of the product
mainly ranges from low to average levels owing to the inevitable residue
of both intrinsic (e.g., edges, deformations, etc.) and extrinsic defects
(e.g., O and H-containing groups), as shown in Fig. 2c. Actually, in
comparison with graphene (including RGO), GO is much easier to
disperse into numerous solvents [89]. This peculiarity enables GO to be
combined with other materials through different chemical routes to
construct GO-based composites, which could be applied directly or
alternatively (e.g., further reduction to RGO-composites) for EES
applications.
In addition, many other methods, such as carbon nanotube unzipping
[90] and direct arc-discharge [91], have also been reported for the syn-
thesis of graphene (or graphene derivatives, Fig. 2d) for laboratory
research. Because of their high costs and low yields, however, these
strategies remain marginal and unsuited to mass-production. Actually, in
order to realize the practical application of graphene in widespread
areas, exploring effective strategies to prepare high quality graphene in
large-scale quantities is still the most ambitious challenge [7]. This sit-
uation is especially prominent considering the likely application of gra-
phene in EESs for powering millions of electric vehicles (EVs) and hybrid
electric vehicles (HEVs) in the future [1,8,68]. Recently, electrochemical
exfoliation of graphite has been considered as a promising strategy to
prepare graphene materials with high-quality on large scale at an
affordable cost, which normally introduces an electrical current for
encouraging structural deformation of a graphite working electrode in a
liquid electrolyte [92–96]. Xinliang Feng and Klaus Müllen’s group re-
ported a (2,2,6,6-tetramethylpiperidin-1-yl)oxyl-assisted electro-
chemical exfoliation method to produce graphene in large quantities
B. Wang et al.
with high quality [93]. The obtained graphene sheets exhibited a large
lateral size (5–10 μm) and low Raman ID/IG ratio (<0.1). In addition,
Zhong-Shuai Wu et al. further demonstrated the electrochemical exfoli-
ation could also realize the scalable production of high-quality hetero-
atom-modified (e.g., F) graphene [96]. Although the electrochemical
exfoliation approach has attracted widely interest, it is still in infancy,
which needs further endeavour from both industrial and academic fields
to push this technology to maturity [92].
From the perspective of industrial progress to obtain graphene, CVD,
exfoliation of graphite and reduction of GO are still the main production
techniques so far by comprehensive consideration of technical maturity
and cost [53,68]. Exfoliation of graphite and reduction of GO are the
most widely used methods for the industrial production of small gra-
phene sheets, and CVD is the most used strategy for the growth of gra-
phene films [68]. With the significant progress in these approaches, the
mass production of graphene materials with yields of thousands of tons of
graphene powder (or suspensions) and hundreds of thousands of square
meters of graphene film has been realized [53]. However, producing
uniform monolayer and few-layer graphene sheets with high yield, high
efficiency and controlled cost is still the universal challenge for all these
mass production techniques. Rodney S. Ruoff’s group [53] and Huiming
Cheng’s group [68] have made some excellent reviews of this field.
3. Synthesis and structural engineering of graphene-based
composites
3.1. Synthesis strategies
Over the last few years, significant efforts have been spent on
developing synthesis methods for preparing graphene-based composites
with all kinds of morphologies, dimensions, structures, and properties.
The synthesis methods reported to date for graphene-based composites
could be divided into in-situ and ex-situ strategies, as illustrated in Fig. 3.
The term graphene in this review is not only limited to monolayer gra-
phene with perfect crystallinity, but also includes graphene derivatives
(e.g., RGO, foreign-atom-doped graphene, bilayer and multilayer gra-
phene, etc.) and graphene-based macroscopic structures (e.g., graphene
Fig. 3. Schematic illustration of typical synthetic strategies for producing graphene-based composites with different dimensions. (a) In situ strategy including one-step
in situ growth, multi-step in situ conversion, and in situ growth of graphene on other materials. (b) Ex situ strategy.
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Energy Storage Materials 24 (2020) 22–51
films, frameworks, sponges, etc.), as shown in Fig. 2d. In the following
contents, we will discuss the corresponding strategies and the prepared
composites in detail.
3.1.1. In-situ strategies for graphene-based composites
In-situ strategies for graphene-based composites have been used
extensively for EES specifically, which can be classified into three types:
(i) one-step in-situ generation of other materials on graphene, (ii) multi-
step in-situ conversion of other materials on graphene, and (iii) in situ
growth of graphene on other substances (Fig. 3a). Among them, the one-
step in-situ method primarily concerns the direct growth of crystal nuclei
on an existing graphene substrate and with subsequent development into
the desired materials with different dimensionalities, including nano-
particles [97,98], nanowires [99], nanorods [100], nanoplates [101],
nanoflowers [102], etc. The main difficulty for this approach is avoiding
the use of protective surfactants or additional linker molecules, which
normally requires a cumbersome synthesis program and influences the
performance of the final obtained composites.
Various chemical and physical synthesis technologies, such as hy-
drothermal and solvothermal processes [103–105], co-precipitation
[106,107], gas-phase deposition [108,109], sol-gel treatment [110,
111], atomic layer deposition (ALD) methods [112,113], etc. [87,114,
115], have been applied for the in-situ strategy. In the literature, hy-
drothermal and solvothermal processes are the most common reported
[116]. The one-pot method can be used to construct high crystallinity
materials without a following high temperature treatment [97,107]. For
example, Kening Sun’s group reported TiO2 quantum dots with diameters
of 4–8 nm that were in situ grown on the surfaces of graphene nanosheets
through a facile one-step hydrolysis procedure [117]. Similarly, Chenxin
Cai’s group designed a unique FePO4 hollow sphere/graphene composite
via a hydrothermal route using urea as the precipitant [118]. Moreover,
Yanwen Ma and Wei Huang’s group synthesized a graphene/polyaniline
(PANI) composite films using GO and aniline as the raw materials
through a one-step large-scale electrochemical synthesis strategy [119].
Unlike the one-step in-situ generation strategies, the multi-step in situ
conversion techniques usually include a pre-loading process for
anchoring the precursors on the surface of graphene and subsequent
B. Wang et al.
conversion procedures to construct the desired composites. A variety of
materials, e.g., Sn [120], SnS2 [121], TiO2 [122], Co3O4 [123], VN [124],
LiFePO4 [89], LiMn1-xFexPO4 [125], LiCoO2 [126], Li4Ti5O12 [127],
carbon cages [128], etc., have been manufactured on graphene following
this method. The desired composition and structure can both be simul-
taneously realized via rational design of the multi-step strategy, and thus,
could be used to fabricate complex architectures with ideal functions.
Recently, we demonstrated that pre-loaded Fe3O4 quantum dots on the
surfaces of graphene nanosheets could be transformed in-situ into
zero-dimensional (0D) amorphous carbon coated LiFePO4 (LFP) active
quantum dots [126]. Moreover, Bin Luo et al. realized the in-situ trans-
formation of the pre-loaded metal oxide nanoparticles into
one-dimensional (1D) carbon encapsulated metal nanocables or 2D
metal/metal disulfide nanosheets on the surface of graphene [120,121].
In another case, Junhong Chen’s group reported a technique that
involved the pre-loading of zeolitic imidazolate framework-8 (ZIF-8) on
the surface of graphene, before using an in-situ confinement pyrolysis
strategy for achieving ZIF-8 derived three-dimensional (3D)
nitrogen-enriched meso-microporous carbon nanocages on graphene
[128]. It is expected that, in the future, the above-mentioned in-situ
methods could be further extended to the design of various ideal
graphene-based composites with desired structures, which definitely
would encourage extensive applications in various EES areas [128].
In-situ growth of graphene on other materials is suitable in cases
where the desired materials were prepared beforehand. This is an
attractive method to encapsulate these electrochemical materials
through in-situ growth of graphene on their surfaces, which not only
offers tight mechanical support of the preformed nanostructures, but also
improves electronic conductivity throughout the whole electrode. CVD
strategies have been most frequently introduced for in-situ generation of
graphene on the surfaces of different electrochemical materials, such as
Si nanowires [108], Si nanoparticles [129], Ge quantum dots [130], etc.
In addition, the arc-discharge method [131] and the in-situ mechanical
peeling process [132] have also been employed for in-situ coating of
graphene on active materials as well.
3.1.2. Ex-situ strategies for graphene-based composites
Ex-situ strategies mainly concern the preparation of objective elec-
trochemical materials with the ideal nanostructures and morphologies in
advance, with subsequent modification and grafting to the graphene
surface via covalent or noncovalent interactions (Fig. 3b) [133]. For
these approaches, either graphene or the desired component (or both)
may need to be modified with functional groups. In contrast to the in-situ
strategies, ex-situ approaches contribute to overcoming the in-
compatibility between the processes for synthesizing precursors and
composites. Generally, GO instead of graphene is preferred for combining
with other materials because of its abundant oxygen-containing groups,
promoting connections with other functional groups through covalent
interactions [134,135]. For example, a graphene/Fe3O4 composite was
designed through self-assembly of partially reduced graphene (with an
appropriate amount of functional groups) and Fe3O4 nanoparticles in
water by forming new bonds (e.g., –COO–) between them [136]. In
addition, many polymeric chains can also be easily grafted to GO, e.g.,
poly(ethylene glycol), polylysine, polyallylamine, poly(vinyl alcohol),
etc., for preparation of graphene-polymer composites [137].
Various kinds of non-covalent interactions, such as electrostatic,
dispersive, and inductive interactions and exchange repulsion, have also
been utilized to synthesize graphene-based composites [63,67]. Among
them, electrostatic interactions have most frequently been used, because
of the general potential for attaching different functional materials to
graphene without disturbing its electrical network [63]. As is well
known, both GO and RGO are intrinsically negatively charged due to
their oxygen-containing groups, which could easily be assembled with
positively charged materials via electrostatic interactions [138]. For
example, a facile electrostatic method to construct RGO-encapsulated
composites was developed by an initial co-assembly of GO and
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Energy Storage Materials 24 (2020) 22–51
aminopropyltrimethoxysilane (APS) modified materials (e.g., SiO2
[139], Co3O4 [139], LiFePO4 (LFP) [135], etc.) and subsequently, the GO
component could be reduced to RGO through a subsequent physical or
chemical process without influencing the pre-constructed
nanostructures.
3.2. Structure and interface engineering
It is well established that the structure of the active material and its
interface exposed to electrolyte have a significant impact on the elec-
trochemical performance of the final EES system [140]. In this section,
we will summarize the research advances on graphene-based composites
for EES from the viewpoint of structure and interface engineering, in-
clusive of the structural design of electrochemical materials and the
interfacial contact of the graphene component with the electrochemical
materials, as well as the interfacial contact between the composite and
the electrolyte.
3.2.1. Structural design of electrochemical materials
Electrochemical materials with ideal structures have been demon-
strated with improved EES performance by increasing the active sites for
interfacial reactions and enhancing the flux of ions across the electrode-
electrolyte boundary [134]. Recently, the progress on graphene-based
composites by effectively combining graphene with active materials
with a variety of dimensions (e.g., 0D nanoparticles [87,126], 1D
nanorods [108,120], 2D nanoplates [121,141], and 3D nanoflowers
[128]), as illustrated in Fig. 4, has led to remarkable improvements in the
EES field.
Among them, 0D nanostructured electrochemical materials are
considered as the most likely ones for commercial EES applications
because of their great mass-production potential. Adhering 0D nano-
structured materials onto 2D graphene sheets has been demonstrated as
an effective method for improving the electronic conductivity of the 0D-
2D composites, relieving the agglomeration of electrochemical materials,
and accommodating the volume changes of the electrode during the
charge and discharge reactions. Taking SnO2 material as an example,
Liqiang Mai’s group have recently attached SnO2 nanoparticles onto
graphene sheets, which exhibited much improved EES performance as
LIB anode [142]. The introduced graphene component not only offers
abundant electron transfer channels for electrochemical reactions, but
also synergistically contributes to the total capacity. Recently, we
designed graphene modified LiFePO4 quantum dots (with diameter of
~6.5 nm) as a composite through a microreactor strategy (Fig. 4), which
exhibited an ultra-high-rate performance in LIBs [126]. Many other
active materials with this kind of 0D-2D structure have also been
designed, including metals (e.g., Sn [143], Ge [144], etc.), S [145], Si
[146], SiO [147], metal oxide (e.g., Fe3O4 [148], Co3O4 [149], Mn3O4
[150], SnO2 [151], V2O5 [152], etc.), FeS2 [153], Na2/3Fe1/2Mn1/2O2
[154], etc. In addition, graphene confined single metal atom composites
(e.g., Ni [155], Ru [156], Pt [157], Fe [158,159], etc.) have aroused
widespread attention for the electrocatalysis field due to their enhanced
electrocatalytic capability, which have also started to influence some
advanced EES systems, e.g., lithium-sulfur batteries and lithium-air
batteries.
1D nanostructured electrochemical materials are potential candidates
for EES, which could offer effective 1D electron transmission pathways
and at the same time alleviate the generated mechanical strain during
charge and discharge. As with the 0D nanostructured materials, vast
investigations have also been carried out that were focused on the
structural engineering of similar 1D-2D composites [26]. Various 1D
nanostructures, such as nanowires [160] (e.g., Si [161], MnO [162], TiO2
[163], V2O5 [164], etc.), nanorods (e.g., MnO2 [165], TiO2 [166],
LaMnO3 [167], LiMn1-xFexPO4 [125], etc.), nanotubes (e.g., carbon
nanotubes (CNTs) [168], TiO2 [169], etc.), nanofibers (e.g., Li4Ti5O12
[170], polyaniline [171], Co3O4 [172], etc.), and core-shell nanocables
or nanoscrolls (e.g., MnO2@N-doped graphene [160], Sn@C [120], Si@C
B. Wang et al.
Fig. 4. Illustrations of graphene-based composites made by effectively compounding graphene with active materials with a variety of dimensions (0D, 1D, 2D and 3D),
taking LiFePO4/graphene composites as examples, 0D: Reproduced with permission from ref. 126, copyright 2017, Elsevier. 1D: Reproduced with permission from ref.
125, copyright 2011, Wiley. 2D: Reproduced with permission from ref. 184, copyright 2015, The Royal Society of Chemistry. 3D: Reproduced with permission from
ref. 198, copyright 2016, Wiley.
[108], etc.) have been successfully incorporated in composites by
combining them with graphene components. For instance, Hongjie Dai’s
group synthesized 1D LiFexMn1-xPO4 nanorods on reduced graphene
oxide via a two-step solution-phase reaction (Fig. 4) [125]. The resulting
composite had high electrical conductivity and low ionic resistance,
leading to an excellent rate performance. We recently developed a
core-sheath MnO@N-doped graphene scroll composite, in which 1D
porous MnO nanowires were confined in tubular graphene scrolls [160].
This unique structural design not only realized enhanced electron/ion
transfer kinetics but also succeeded in addressing the structural and
interfacial stability issues facing MnO-based electrodes.
2D materials (e.g., graphene) have drawn much attention recently on
account of their unique properties arising from their ultrathin 2D char-
acteristics [173,174]. Correspondingly, a great deal of effort has been put
into exploiting their possible deployment in many fields, including
electronics, optoelectronics, and EES devices [9]. By integrating gra-
phene with 2D nanostructured electrochemical materials, a wide range of
composites in the 2D-2D mode have been constructed for EES so far,
either via in-situ growth of 2D electrochemical materials on graphene, or
via ex-situ self-assembly of 2D electrochemical materials with graphene.
Due to the diversity of electrochemical materials, the reported 2D active
components combined with graphene could be classified into MXene
[175,176], phosphorene [177,178], metal [141], metal oxide [179],
metal chalcogenide [180], layered double hydroxide [181,182],
layer-structured LiMO2 (M ¼ Co, Ni) [126], and phosphate nanosheet
[183] or nanoplate [134,184] types. Recently, we reported a facile sol-
vothermal method using ethylene glycol as the solvent to prepare a
2D-2D “plate-on-sheet” LiFePO4/graphene composite (LFP@GNs) with
(010) facet oriented LiFePO4 nanoplates in situ grown on a graphene
cross-linked network (Fig. 4) [184]. In this work, ethylene glycol not only
induced the crystal orientation of LiFePO4 due to its strong binding effect
towards the (010) facet, but also enhanced the interaction between the
LiFePO4 crystals and the graphene sheets by building up a robust
hydrogen bond network between the ethylene glycol and the GO, which
28
Energy Storage Materials 24 (2020) 22–51
effectively trapped the free ions during the crystallization of LiFePO4
[184].
Active materials with 3D hierarchical structures offer large surface
areas, well-distributed channels for electrolyte infiltration and mechan-
ical stability for electrodes [185]. Analogously, by combining graphene
and 3D hierarchical-structured active components, a variety of 3D-2D
graphene-based electrode composites have been designed for EES
through both in-situ and ex-situ strategies. Typically, hydrothermal and
solvothermal processes have been most frequently employed to realize
such a goal [186–195]. For instance, Zunli Mo’s group developed a
surfactant-assisted hydrothermal route for the synthesis of a 3D
flower-like TiO2 microsphere decorated graphene composite based on
the hydrothermal reduction of graphene oxide and the formation of TiO2
microspheres in the presence of poly(vinyl pyrrolidone) [196]. In
another work, Yu Zhu’s group designed a 3D hierarchical hollow NiO/-
Ni/graphene composite derived from Ni-based metalorganic frameworks
(Ni-MOFs), in which, hierarchical NiO/Ni nanocrystals were covered
with a graphene shell, with the hollow ball-in-ball nanostructure intact
[197]. Moreover, our group also prepared a graphene modified 3D
LiFePO4 composite with 3D hierarchical LiFePO4 nanoflowers supported
by graphene sheets (Fig. 4) [198].
3.2.2. Interface engineering of graphene-based composites
3.2.2.1. Interfacial contact of graphene component with electrochemical
materials. Obviously, the graphene inside the designed graphene-based
composites plays an important role in gathering/transmitting electrons
from/to the electrochemically active materials in the charge and
discharge processes. Thereby, obtaining an ideal interfacial contact mode
of the graphene component with the electrochemical materials is also
quite important for decreasing the interfacial contact resistance between
different components [140].
Considering the dimensions of the electrochemical materials
compared to the lateral size and flexibility of graphene, the graphene-
B. Wang et al. Energy Storage Materials 24 (2020) 22–51

based composites could be mainly divided into three types: graphene-
supported composites (which include graphene-anchored composites
[199], sandwich-like campsites [200], and layered structured composites
[171]), graphene-wrapped composites (which can be further divided into
partially wrapped composites and fully wrapped composites) [201], and
graphene-mixed composites (combining the aforementioned two modes)
[114], as illustrated in Fig. 5 [10,29]. From the theoretical perspective,
the contact area of the graphene component and the second phase elec-
trochemical materials in the graphene-wrapped composites should be
larger than for the other two kinds of composites, and thus could improve

Fig. 5. Structural models of graphene-based composites, which can be mainly divided into three types: graphene-supported, graphene-wrapped, and graphene-mixed
composites (Reproduced with permission from ref. 10, copyright 2015, Nature Publishing Group). Supported: Active material particles are supported by graphene,
which include graphene-anchored composites (reproduced with permission from ref. 199, copyright 2010, American Chemical Society), sandwich-like composites
(Reproduced with permission from ref. 200, copyright 2014, Wiley), and layered structured composites (reproduced with permission from ref. 171, copyright 2010,
American Chemical Society). Wrapped: Active material particles are wrapped by graphene sheets, which can be divided into partially wrapped and fully wrapped
composites (reproduced with permission from ref. 201, copyright 2013, Elsevier). Mixed: graphene-supported and graphene-wrapped composites are mixed together
during the electrode preparation (reproduced with permission from ref. 114, copyright 2014, The Royal Society of Chemistry).

29
B. Wang et al.
stability by avoiding peeling off of the second phase component from the
graphene component [135,201]. For this mode, graphene acts as a pro-
tective layer, preventing the aggregation of the second phase electro-
chemical materials more effectively compared with the other two modes.
Numerous graphene-wrapped composites, such as graphene wrapped
particles [87,135], hollow spheres [118], nanoplatelets [134] and
nanowires [108] have been fabricated for EES. Considering of the mass
(ion) transfer process inside these composites, however the graphene
component may have some negative influence. For instance, Young Hee
Lee’s group demonstrated that the Liþ diffusion through a defect-free
graphitic plane is limited from the theoretical calculation aspect [202].
Moreover, Quanhong Yang’s group confirmed that the partially
graphene-wrapped mode affords an optimal balance between improved
electron transport and rapid ion diffusion, while the fully
graphene-wrapped mode isolates the active materials from the electro-
lyte and blocks ion diffusion [201]. Therefore, the spatial obstruction of
the mass transfer process should also be taken into consideration along
with the electron transport kinetics in designing graphene-based com-
posites for high-performance EES systems.
From the perspective of dimensions, it should be mentioned that the
1D electrochemical materials (e.g., nanotubes, nanorods, nanowires,
etc.) and 2D electrochemical materials (e.g., nanosheets, nanoplates,
nanofilms, etc.) can be grown either vertically [203–205] on or parallel
[160,184] to the surface of the graphene component. Considering the
intrinsic 2D structure of graphene, a “face-to-face” contact mode between
the graphene sheets and the other 2D electrochemical components shows
the greatest potential among the various composite architectures, which
could fully utilize the advantages of each component. In this context,
such a sandwich-like 2D-2D structure could effectively support both fast
electron and ion transport channels, and thus be favorable for the con-
struction of advanced EES systems. Recently, we proposed a general
microreactor method for preparing graphene/2D LiCoO2 sheet compos-
ites using sandwich-like graphene/Co(OH)2 nanosheets precursor, in
which amorphous carbon coated LiCoO2 nanosheets adhered to both
sides of graphene [126]. For such a composite, the graphene substrate
not only prevented the agglomeration of the adjacent LiCoO2 nanosheets,
but also provided abundant pathways for efficient electron transmission
based on their face-to-face contact mode.
3.2.2.2. Interfacial contact between the composites and the electrolyte. It is
well known that the mass (ion) transfer process is also very important for
EES, especially in high-power applications, and thus the interfacial
contact between graphene-based composites and the electrolyte are
discussed in this section to provide more detailed information [1].
Basically, the reported strategies to improve the interfacial contact be-
tween graphene-based composites and the electrolyte could be divided
into three categories: (1) building porous structure into the
graphene-based composites; (2) improving the electrolyte wettability of
the graphene-based composites; and (3) tuning the orientation of the
graphene component in the composites, as illustrated in Fig. 6.
For building porous structure into the composites, methods such as
etching holes in graphene [206], constructing graphene aerogel (GA)
structures [135], and building pores in the second phase [114] have been
successfully developed. Among them, constructing GA structure is the
most common one [207], which possesses unique advantages for pre-
paring 3D porous electrode materials, such as high porosity, large surface
area, and good electronic conductivity [134,135]. As a result, it provides
an ideal porous network for preparing graphene-based composites with
3D ion diffusion channels and good electrical conductivity. Typically,
Klaus Müllen’s group proposed a “two step” strategy to fabricate a 3D
graphene aerogel cross-linked with graphene pre-wrapped Fe3O4 nano-
spheres for LIB anodes [135]. Such hierarchical Fe3O4/graphene com-
posites provide double protection against the volume changes of Fe3O4
nanosheets during charge and discharge processes. Moreover, in order to
further improve the infiltration of the electrolyte, Hongtao Sun and Lin
30
Energy Storage Materials 24 (2020) 22–51
Mei et al. used holey GO as one of the raw materials for designing 3D
holey GA/Nb2O5 composite and realized a high mass-loading application
as LIB anode material [208].
Improving the wettability between the graphene-based composites
and the electrolyte is another vital tool to accelerate the mass transfer
dynamic process for EES [46]. Many attempts have been made to
improve the electrolyte-wettability of the graphene framework, for
instance, modifying the surface of graphene with functional groups,
introducing the defects onto the graphene surface, and doping hetero-
atoms into the plane structure of graphene [18,209–213]. Rodney S.
Ruoff’s group reported poly(ionic liquid)-modified graphene electrodes
with much enhanced capacitive performance that used an ionic liquid
(IL) electrolyte system for improving the electrolyte wettability [213].
Later, Saikat Talapatra’s group studied the effect of 1-pyrene
carboxylic-acid (PCA) functionalization of graphene on its capacitive
energy storage and found that the electrolyte wettability of the PCA
modified graphene was much improved compared with pure graphene
using 6 M KOH aqueous solution as the electrolyte [212]. Recently,
Wencai Ren and Huiming Cheng’s group demonstrated that a heteroatom
(B and N) doping strategy could also improve the electrolyte wettability
for LIBs using organic electrolyte [46]. Following their research, many
subsequent works used the heteroatom (e.g., N, S, B, P, etc.) doped
graphene as the basic unit for fabricating high performance
graphene-based composites with improved electrolyte-wettability for
application in LIBs [134,160,209].
Another way to improve the infiltration of the electrolyte is tuning the
orientation of the graphene component in the composite. Generally
speaking, the orientation of the graphene component for graphene-based
composites can be classified into three modes, including random orien-
tation, parallel alignment, and vertical orientation. Considering the fact
that many of the active ions (e.g., Liþ, Naþ, etc.) cannot pass through the
planar structure of defect-free graphene, the vertical orientation mode of
the graphene component was considered to be the most efficient mode
for the ion diffusion dynamics. Recently, CVD has been reported as an
efficient method for producing vertically oriented graphene nanosheet
electrodes [214], although the packing density of the as-obtained gra-
phene is very low [10,215]. Soon afterwards, Chengxin Wang’ group
anchored several kinds of active nanomaterials (e.g., Sn [216,217], Si
[218], SnO2 nanoparticles [219], etc.) on both sides of the vertical
aligned graphene sheets for EES and demonstrated the improved kinetics
for both ion and electron transports.
3.2.3. Structure and dimensionality of graphene-based composites
The structures of the final designed graphene-based composites have
a significant influence on their application for various EES devices, which
cover all ‘four’ dimensions in terms of 0D particles, 1D wires, 2D films,
3D bulks, and potentially 4D self-healing or self-folding types [11], as
demonstrated in Fig. 7. In this section, we will discuss how each mode
affects the properties and applications of graphene-based composites.
0D graphene-based composites, such as irregular particles [139],
spheres [220], and flowers [44], have the most potential to be used in
EES markets for practical applications, because of their facile synthesis
process and high tap density [220]. Recently, the spray-drying technique
has been frequently used for preparing 0D graphene-based composites
[221]. Zhaoping Liu’s group reported a graphene modified LiFePO4
cathode material produced by a spray-drying technique combined with
annealing process, in which the LiFePO4 primary nanoparticles were
embedded in microsized spherical secondary particles and were wrapped
with a graphene network [220]. In another case, Chao Gao’ group
designed a graphene flower-like particle through a spray-drying process
and high-temperature treatment [44]. When utilized as carbon host for a
sulfur cathode, the graphene flower particle – sulfur composite delivered
very impressive electrochemical performance in Li–S batteries (LSBs).
1D graphene-based composites, such as wires [120], scrolls [160],
and fibers [222], are also attractive due to their ability to integrate the
particular properties of individual graphene sheets and other functional
B. Wang et al. Energy Storage Materials 24 (2020) 22–51

Fig. 6. Various strategies to improve the interfacial contact between graphene-based composites and the electrolyte, which could be divided into three categories: (1)
building porous structure in the graphene-based composites; (2) improving the electrolyte-wettability of the graphene-based composites (Reproduced with permission
from ref. 212, copyright 2011, American Chemical Society); and (3) tuning the orientation of the graphene component in the composites (reproduced with permission
from ref. 140, copyright 2015, The Royal Society of Chemistry).

materials into macroscopic assemblies with superior mechanical and
electrical performances [223]. Moreover, 1D graphene-based composites
are favorable for constructing flexible and wearable EES devices, as they
can be directly molded into fabrics and textiles [224]. Furthermore, 1D
graphene-based composites can be tailored to suit different EES devices
with unconventional architectures for special applications [21]. Typi-
cally, Liming Dai’s group designed hierarchically structured
graphene-carbon nanotube fibers and demonstrated their application for
flexible all-solid-state micro-supercapacitors [222]. In another work, Wei
Huang’s group reported a flexible wire-shaped Li–S battery based on a
graphene-sulfur composite fiber cathode [225]. Graphene-based nano-
wire composite also displays immense potential for flexible and trans-
parent electrodes with excellent optical and electrical properties as well
as high durability [226].
2D graphene-based composites, such as sheets [141], films [227], and
woven fabrics [228], represent an alternative applicable macroscopic
form on account of the high aspect ratio along its lateral direction, which
can usually be obtained by vacuum filtration, CVD, wet spinning process,
etc. [229–231] Actually, lamellar graphene components can be readily
assembled into 2D macrostructures with orderly packed sheets. Gra-
phene film composites are particularly promising in film electrodes for
EES devices. Graphene-based film batteries and supercapacitors can be
viable if they can equal or surpass current EES electrodes in regard of
cost, ease of processing, and performance. The unique characteristics of
graphene may endow the graphene film composites with excellent flex-
ibility, electrical conductivity, mechanical strength, and thermal con-
ductivity as well as optical transparency, depending on the properties of
the basic graphene-based-unit and the thickness of the as-obtained film
[171,232]. Recently, Dan Li’s group reported a flexible 2D
graphene-polyaniline film electrode fabricated by in-situ chemical
polymerization of aniline on the surfaces of chemically converted gra-
phene sheets, which could provide a combination of high capacitance,
excellent rate performance, and long cycling life [227].
In the case of 3D graphene-based composites, various structures have
been reported, such as aerogels [134], foams [233], and arrays [216].
These 3D graphene-based structure can support fast electron and mass
transfer, provide accessible surfaces for the adsorption and desorption of
ions, and offer abundant pore volume for anchoring other functional
materials, leading to EES systems with the desired performance. Apart
from application in EES, the excellent electrical conductivity and
biocompatibility of 3D graphene-based composites also enable their use
as scaffolds for tissue engineering and regeneration [234]. Substantial
research efforts are currently ongoing to control the morphologies and
the properties of 3D graphene-based composites for integration into
practical EES devices [235]. Typically, Huiming Cheng’s group designed
a 3D graphene foam-graphene/poly(dimethyl siloxane) composite with

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B. Wang et al. Energy Storage Materials 24 (2020) 22–51

Fig. 7. Configurational structures of the integral graphene-based composites in terms of 0D, 1D, 2D, 3D, and potentially 4D self-healing or self-folding types. In this
example, 0D forms include particles (reproduced with permission from ref. 139, copyright 2010, Wiley), spheres (reproduced with permission from ref. 220, copyright
2011, The Royal Society of Chemistry) and flowers (reproduced with permission from ref. 44, copyright 2017,Wiley); 1D forms include wires (reproduced with
permission from ref. 120, copyright 2012, Wiley), scrolls (reproduced with permission from ref. 160, copyright 2016, Wiley) and fibers (reproduced with permission
from ref. 222, copyright 2014, Nature Publishing Group); 2D forms include sheets (reproduced with permission from ref. 141, copyright 2012, Wiley), films
(reproduced with permission from ref. 227, copyright 2013, The Royal Society of Chemistry), and fabrics (reproduced with permission from ref. 228, copyright 2015,
The Royal Society of Chemistry); 3D forms include aerogels (reproduced with permission from ref. 134, copyright 2015, The Royal Society of Chemistry), frameworks
(reproduced with permission from ref. 233, copyright 2011, Nature Publishing Group), and arrays (reproduced with permission from ref. 216, copyright 2014,
Elsevier); 4D forms include self-healing (reproduced with permission from ref. 238, copyright 2018, Wiley) and self-folding types (reproduced with permission from
ref. 239, copyright 2015, American Association for the Advancement of Science).

high electrical conductivity through the CVD technique, which shows
great potential for flexible, foldable, and stretchable conductors [233].
Afterwards, they used such a graphene foam in combination with
LiFePO4 and Li4Ti5O12 for fabricating 3D graphene foam composite
electrodes for LIBs [236].
The future of this field lies in the progress on responsive graphene-
based structures that are adaptable to their surroundings. Generally,
real-world objects, once produced, do not change their shapes or prop-
erties; a material that can transform and vary its configuration when
subjected to an environmental change would be extremely useful, how-
ever. This may lead to EES devices that are capable of self-healing or
changing shape in case of an accident or special requirement for on-
demand shape transformations. These 3D objects that change structure
over time are termed ‘4D materials’. A recent study has suggested that 4D
printing of a ‘smart object’ may, one day, give rise to the development of
such devices [237]. Recently, Takeshi Serizawa and Hongwei Zhu’s
group designed a graphene oxide/poly(acrylic acid)/amorphous calcium
carbonate (GO-PAA-ACC) composite via a facile
biomineralization-inspired process, which showed impressive reshaping
and self-healing features and may meet some specific application re-
quirements for self-healing or shape-changing EES devices [238]. In
another case, Jiuke Mu and Chengyi Hou’s group designed a graphene
oxide-polydopamine/reduced graphene oxide (GO-PDA/RGO) compos-
ite film, which exhibited an interesting self-folding property and held

32
B. Wang et al. Energy Storage Materials 24 (2020) 22–51

potential for a wide range of applications such as sensing, robotics, and
self-folding EES devices [239].
4. Graphene-based composites for electrochemical capacitors
Electrochemical capacitors (ECs), also known as supercapacitors or
ultracapacitors, with fast charge-storage mechanisms are more suitable
for high power density applications compared with other EES devices
(e.g., LIBs). The ECs can be classified into two main groups: electro-
chemical double-layer capacitors (EDLCs) and pseudocapacitors [240].
In EDLCs, the energy is stored through a non-Faradaic process by phys-
ically adsorbing ions or charged particles on the surfaces of the elec-
trodes, as illustrated in Fig. 8a [241]. In pseudocapacitors, the
electrochemical energy storage is realized by a fast and reversible Fara-
daic process, such as a redox reaction, taking place between the interface
area of the electrochemically active species and the electrolyte (Fig. 9a)
[9].
4.1. Electrochemical double-layer capacitors
In EDLCs, the amount of charge storage of the active materials is
proportional to the double layer contact with the electrolyte (Fig. 8a),
which can be evaluated per unit mass (F g1), volume (F cm3) or area (F
cm2) [185]. In principle, graphene with a theoretical specific surface
area (SSA) of 2630 m2 g1 can reach a theoretical capacitance as high as
550 F g1, which shows a great potential for boosting the energy density
of such systems [242–245]. In practice, however, this does not seem to be
the case, as the inaccessibility of the theoretical SSA of graphene results
in a lower practical gravimetric capacitance [246]. Furthermore, spon-
taneous graphene layer re-stacking, which occurs during both electrode
fabrication and cycling, significantly reduces the practical surface
available for charge storage (Fig. 3d, e) [247]. Various approaches have
been employed to mitigate these adverse impacts, such as designing
activated graphene with extended 3D meso- and microporous structure
[242], tuning the orientation of graphene so that it is perpendicular to

Fig. 8. (a) Schematic illustration of ion adsorption at the electrode surface for EDLCs. Structures and electrochemical characterizations of (b) graphene/fullerene
composite with 0D fullerene as the spacer (reproduced with permission from ref. 248, copyright 2015, Taylor and Francis Inc), (c) graphene/CNTs composite created
by incorporating 1D CNTs with graphene (reproduced with permission from ref. 254, copyright 2012, The Royal Society of Chemistry), (d) 3D graphene/carbon
nanotube sandwich-structured composite (reproduced with permission from ref. 255, copyright 2010, Wiley), and (e) 3D commercial activated carbon bulk material
combined with graphene (reproduced with permission from ref. 253, copyright 2012, The Royal Society of Chemistry).

33
B. Wang et al. Energy Storage Materials 24 (2020) 22–51

Fig. 9. (a) Schematic illustration of charge transfer near the surface of the electrode for pseudocapacitors. In this example, RuO2/graphene composite has been chosen
as the active material. Structures and electrochemical characterizations of (b) 2,5-dimethoxy-1,4-benzoquinone/RGO composite xerogel (reproduced with permission
from ref. 288, copyright 2016, The Royal Society of Chemistry), (c) MnO2 nanoflake layer-coated vertical graphene composite (reproduced with permission from ref.
289, copyright 2016, American Chemical Society), (d) Graphene/MXene composite film (reproduced with permission from ref. 175, copyright 2017,Wiley), and (e) 3D
MnNi-LDH/graphene composite (reproduced with permission from ref. 284, copyright 2017, Elsevier).

the current collector plane [215], fabricating different types of graphe-
ne/carbon composites, etc. [222].
Graphene/carbon composites can be prepared by combining carbon
species with other structures (e.g., fullerene [248], carbon black [249],
carbon nanotubes [168,222,250], porous carbon spheres [251], hollow
carbon spheres [252], activated carbon [253], etc.) with graphene via in
situ or ex situ chemical and physical methods, gaining the advantages of
each component towards improving the infiltration of the electrolyte and
enhancing the electrical conductivity of the electrode. For instance,
Zhuangjun Fan’s group reported a graphene/carbon black composite
prepared by the in-situ reduction method, in which the 0D carbon black
acted as both the conductive agent and a spacer to increase the interlayer
spacing between 2D graphene sheets for fast electron and ion transport
[249]. Analogously, Xue Qin’s group used 0D fullerene as the spacer to
realize a graphene/fullerene composite, which could reach a capacity of
135 F g1 at the current density of 1 A g1 (Fig. 8b) [248]. 1D carbon
nanotubes (CNTs) [168,222,250], 3D carbon spheres [251,252], and
activated carbon [253] have also been introduced for incorporation with
graphene to fabricate graphene-based composites with improved EDLC
performance. Typically, Liming Dai’s group fabricated a self-assembled
graphene/CNTs composite film, in which the CNTs could insert be-
tween graphene sheets parallel to its planar structure and form
well-defined nanopores. This graphene/CNTs film electrode exhibited
great promise for EDLCs with a quasi-rectangular-shaped cyclic voltam-
mogram even at an extremely high scan rate of 1 V s1 and an average
specific capacitance of 120 F g1 [229]. Afterwards, Dengsong Zhang and
Liyi Shi’s group designed a similar graphene/CNTs composite through a
modified exfoliation approach (Fig. 8c), which exhibited a much higher
specific capacitance (230 F g1) than graphene (101 F g1) at a current
density of 0.6 A g1 [254]. In another study, 3D graphene/carbon
nanotube sandwich structures with CNT pillars grown in between the
graphene layers were been fabricated by the CVD technique (Fig. 8d).
The special structure facilitated the high-rate transportation of electro-
lyte ions and electrons throughout the electrode matrix, resulting in

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B. Wang et al.
excellent capacitive performance of this composite material [255].
Additionally, Likun Pan’s group combined 3D commercial activated
carbon bulk material with graphene through a facile chemical method,
and the resultant graphene/activated carbon composite could display a
much improved specific capacitance of 181 F g1 (Fig. 8e) [253].
Although the strategies for introducing nanostructured carbons as the
separators of graphene sheets are quite promising, further engineering of
graphene/carbon composites for EDLCs are required to reduce the pro-
duction costs for practical applications [20,256,257]. On the other hand,
most of the reported graphene/carbon composites for EDLCs possess a
large number of voids (especially macropores) leading to relatively low
density, and these pores would be filled with the electrolyte, resulting in
both high weight and volume in the final device [21,175]. Therefore,
increasing the mass density of the graphene/carbon composite to reduce
the weight and volume of the final device is also very significant for the
large-scale EDLCs required to power the next generation of electric ve-
hicles and hybrid electric vehicles [11,246].
4.2. Pseudocapacitors
In the case of pseudocapacitors, the presence of electrochemically
active species in the electrode material (Fig. 9a), for instance, oxygen-
containing functional groups [258,259], conductive polymers [171],
transition metal oxides [122] (or nitrides [260], sulfides [261–263],
hydroxides [264], etc.), and MXenes [265], enables higher energy den-
sities compared with EDLCs. Nevertheless, the electrochemical behavior
of pseudocapacitors is inferior to that of EDLCs with respect to power
density and cycle life because of the poor electric conductivity and poor
structural stability of the active materials [266]. In this regard,
graphene-based composites could be available alternatives for improving
the performance of pseudocapacitors [240,267,268].
Various graphene/conductive polymers (e.g., polyaniline [137,269],
polypyrrole [270,271], polythiophene [272], etc.), graphene/metal ox-
ides (e.g., Mn3O4 [273–275], Co3O4 [276,277], SnO2 [278,279], etc.),
graphene/metal nitrides (e.g., VN [260,280], Ni3N [281], etc.), graphe-
ne/sulfides (e.g., FeS2 [282], MoS2 [283], etc.), graphene/hydroxides
(e.g., MnNi-layered double hydroxide (MnNi-LDH) [284], NiCo-LDH
[285], etc.), graphene/MXenes [175,286,287], etc., have been exploi-
ted and researched for pseudocapacitors. In these composites, graphene
provides a conductive substrate for the support or growth of the elec-
trochemically active species at the nanoscale, which enables a large SSA
with more active sites and improved mechanical stability, thus enhancing
the electrochemical performance of the final fabricated
pseudocapacitors.
Recently, Yury Gogotsi’s group reported a 2,5-dimethoxy-1,4-benzo-
quinone (DMQ)/RGO composite xerogel (Fig. 9b), in which DMQ not
only provided stable redox-active centers but also served as a spacer to
protect the RGO sheets from aggregation and construct a three-
dimensional (3D) hierarchical electrode architecture [288]. When a
binder-free 50 mm thick rolled film was tested as a pseudocapacitive
electrode, it exhibited an excellent capacitance of 650 F g1 at 5 mV s1
(780 F cm3) in 1 M sulfuric acid and an excellent capacitance retention
of 99% after 25000 cycles at 50 mV s1 [288]. In another work, a vertical
graphene composite coated with a MnO2 nanoflake layer was designed
by Weng P. Kang and Shaozhi Deng’s group (Fig. 9c), with the vertical
structure and open architecture designed for fast ion transport pathways,
providing high pseudocapacitive performance, with the overall areal
capacitance of 500 mF cm2 at the scan rate of 5 mV s1 [289]. More-
over, Jun Yan et al. designed a graphene/MXene composite film (Fig. 9d),
which could deliver an ultrahigh volumetric capacitance (1040 F cm3)
at 2 mV s1, excellent rate capability, and long cycle life. When a sym-
metric supercapacitor was assembled from it, a high volumetric energy
density (32.6 Wh L1) could be achieved in aqueous electrolyte [175]. In
addition, Songhun Yoon’s group reported a 3D MnNi-LDH/graphene
composite with MnNi-LDH impregnated into the interlayers of gra-
phene nanosheets (Fig. 9e). It exhibited a stable performance with 90%
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Energy Storage Materials 24 (2020) 22–51
capacity retention after 1400 cycles and a high energy density of
47.29 Wh kg1 at the power density of 7473 W kg1 [284]. It seems that
the key to realizing the full potential of graphene in pseudocapacitors
depends on the development of graphene-based composites that benefit
from the synergistic effects of the graphene substrate and the electro-
chemically active component to the maximum extent, combined with an
optimized spatial orientation of the graphene sheets [21,290].
5. Graphene-based composites for Li-ion batteries
LIBs have attracted vast attention from both the scientific community
and the wider society as one of the most favored types of EES devices for
applications in different fields, owing to their high energy density
(compared with ECs), long cycling life, and low self-discharging [1,134].
In LIBs, Liþ ions constantly shuttle back and forth between a
lithium-releasing cathode (e.g., layered lithium metal oxide or lithium
iron phosphate) and a lithium-receiving anode (e.g., graphite), as illus-
trated in Fig. 10a [140]. The amount of ions carried per gram of product
determines the gravimetric capacity and energy of the battery.
5.1. Graphene-based anode composites
Similar to graphite, graphene can be applied in the anode for hosting
Liþ directly or as an active material in anode composites by combined
with other Li-hosting components. Unlike graphite, single-layered gra-
phene has been theoretically calculated to host Liþ via an adsorption
mechanism on both sides with a stoichiometry of Li2C6, which results in a
specific capacity as high as 744 mAh g1, twice that of graphite
(372 mAh g1), with an Liþ intercalation mechanism between the
stacked layers [46,291]. In addition, the inherent defects and nanopores
that are constructed by the randomly arranged graphene layers can also
store Liþ ions according to the ‘house of cards’ model [292–294]. In order
to further clarify the Liþ storage mechanism of graphene, advanced in
operando techniques (e.g., in situ low-voltage transmission electron mi-
croscopy [295]) for obtaining direct evidence are still needed.
Generally, graphene material typically exhibits a high irreversible
capacity (even higher than 2000 mAh g1) during the first Liþ insertion/
extraction process, well above the theoretical capacity of monolayer
graphene [46,294]. This phenomenon is mostly caused by the irrevers-
ible reduction of the electrolyte to form a solid electrolyte interphase
(SEI) layer on the graphene surface, which is enhanced with a higher SSA
and results in a fairly high initial irreversible capacity loss in comparison
with graphite materials [46]. In the following de-insertion process, gra-
phene displays a high reversible capacity, with potentials distributed in
the range of 1–3 V vs. Li/Liþ, much higher than the classical potentials for
graphite (0–0.4 V vs. Li/Liþ). This would cause an obvious voltage hys-
teresis between Liþ insertion and de-insertion processes (due to the
storage of Liþ on defect positions, such as vacancies, edges, and
oxygen-containing groups) and lead to a poor energy efficiency for LIBs
using such graphene anodes. Moreover, the unavoidable re-stacking of
graphene will also lower the Liþ storage capacity during the repeated
cycling processes [294]. Because of the above-mentioned factors, the
cycling performance of graphene anodes is generally very poor, and
normally, the reversible capacity of graphene is rarely comparable to that
of the commercially available graphite. In this regards, pre-lithiation
[296], surface modification with functionalized groups [297] and,
especially, designing ideal graphene-based composites [20] are consid-
ered as effective strategies for preventing initial Liþ consumption and
graphene re-stacking [10].
To date, various graphene-based anode composites with different
structures have been developed through in-situ or ex-situ methods for the
purpose of improving their cycling performance and increasing their
energy density compared with bare graphene [140]. The large capacity
contribution from other active components (e.g., metal oxides [117,138,
151,191], metals [120,141], etc.), can offer reversible insertion (e.g.,
TiO2 [117]), alloying (e.g., SnO2 [151], Sn [141], etc.) or conversion
B. Wang et al. Energy Storage Materials 24 (2020) 22–51

Fig. 10. (a) Schematic illustration of the working principle of LIBs based on the graphene-based electrodes. In this example, Fe2O3/graphene and LiFePO4/graphene
composites have been chosen as the anode and cathode materials, respectively. Structures and electrochemical characterizations of (b) 3D interconnected porous
nitrogen-doped graphene foam with encapsulated Ge quantum dots (reproduced with permission from ref. 130, copyright 2017, Nature Publishing Group), (c) 3D
holey-graphene/Nb2O5 composite (reproduced with permission from ref. 208, copyright 2017, American Association for the Advancement of Science), (d) graphene
modified LFP quantum dot composite (reproduced with permission from ref. 126, copyright 2017, Elsevier), and (e) 3D porous LiFePO4/N-doped GA composite
(reproduced with permission from ref. 134, copyright 2015, The Royal Society of Chemistry).

(e.g., Fe3O4 [191], Co3O4 [138], etc.) reactions with Liþ and thus provide
considerably higher capacities. Also, the introduced electrochemically
active nanostructures are beneficial for blocking the re-stacking of gra-
phene layers by reducing the van der Waals forces [147,260]. Therefore,
these composites are less affected by the agglomeration that takes place
both in electrode preparation and cycling tests. More importantly, the
efficient conductive carbon matrix constructed from the graphene layers
not only improves the electronic conductivity of the composite, but also
buffers the volume changes during charge and discharge [141]. Despite
these promising properties, however, the graphene-based anode com-
posites still suffer from low Coulombic efficiency, which is mainly in the
range between 50-70% for the first cycle with a large charge consump-
tion of 30–50%, similar to the Coulombic efficiency of bare graphene
[135]. The performance achieved so far with graphene-based anode
composites are quite inspiring for high-energy LIBs. Recently, Runwei Mo
et al. designed a 3D interconnected porous nitrogen-doped graphene
foam with an encapsulated Ge quantum dot/nitrogen-doped graphene
yolk-shell nano-architecture for LIB anode (Fig. 10b), which exhibited
high reversible specific capacity (1220 mAh g1), long cycling capability
(over 96% reversible capacity retention from the 2nd to the 1000th cycles)
and ultra-high rate performance (over 800 mAh g1 at 40C) [130].
Moreover, Xiangfeng Duan’s group designed a 3D hole-
y-graphene/Nb2O5 composite (Fig. 10c) by systematically tailoring the
porosity in the holey graphene backbone. The charge and mass transport
in this fabricated architecture were optimized to deliver ultrahigh-rate
energy storage performance at practical levels of mass loading
(>10 mg cm2) [208]. In addition, some promising reversible capacities
are also achieved for silicon/graphene (1400 mAh g1) [298], Fe3O4/g-
raphene (1060 mAh g1) [135], and Co3O4/graphene (1029 mAh g1)
[123] composites. Nevertheless, further optimization of the structural
configuration and mass ratio distribution between graphene and the
other active components are still critical issues that should be addressed
to achieve better electrochemical performance in term of reversible ca-
pacity, rate performance, cycling life, etc. [12,140].

36
B. Wang et al.
5.2. Graphene-based cathode composites
For LIBs cathodes, LiFePO4 [299], LiCoO2 [300], and LiMn2O4 [301]
are the most common active materials for the current commercial mar-
ket, which are mixed with low-cost carbon conductive additives, such as
carbon black, acetylene black, etc. [302] Due to their amorphous struc-
ture, however, these conductive additives usually have a relatively low
electronic conductivity and poor mechanical strength compared with
more graphitic carbon materials (e.g., CNTs and graphene) [198]. Hence,
the rate capability and cycling life of these electrodes are still limited by
the fact of slow kinetics for electron and Liþ transport as well as severe
structural degradation during repeated charge and discharge [303].
Accordingly, graphene materials as superior conductive and flexible
matrices has been the object of considerable study for constructing
cathode composites to improve the electronic and ionic conductivity (by
forming a bi-continuous conductive network) of the electrode and alle-
viate the stress/strain for preserving electrode integrity [125,134].
For synthesizing graphene-based cathode composites, in-situ methods
(e.g., the hydrothermal or solvothermal method) are normally superior to
ex-situ strategies (such as the mechanical mixing strategy), because the
former ones could effectively suppress the crystal growth (to shorten the
Liþ transport distance in the crystals of active materials) and form much
stronger chemical bonds as fast electron transport pathways (supported
by theoretical calculations in some previous reports) [184,304]. In gen-
eral, GO is most frequently employed as the raw material to construct the
porous networks (leading to improved Liþ diffusion kinetics) in the
in-situ synthesis process because of its hydrophilic property, electro-
negativity, and abundant functional groups, which is subsequently
reduced to graphene to improve the electronic conductivity, while
simultaneously, the cathode precursors would turn into active materials
with various nanostructures (e.g., nanoparticles, nanowires, nano-
ribbons, etc.) [164,220,305]. For instance, our group previously pre-
pared a graphene modified LiFePO4 quantum dot (~6.5 nm) composite
through an in-situ microreactor strategy (Fig. 10d) [126], which had a
large SSA for charge adsorption and plentiful active sites for faradaic
responses, as well as desirable kinetic features for both electron and ion
transmission. It thus exhibited extremely fast, surface-dynamics
controlled lithium storage behavior, imitating the pseudocapacitive
mechanisms in terms of outstanding rate capability (78 mAh g1 at 200C)
and remarkable cycling stability (~99% capacity retention over 1000
cycles at 20C). On the other hand, based on the density functional theory
(DFT) calculations, it was found that the heterointerfaces of graphene
and LiFePO4 had an efficient hybridized electronic structure near the
Fermi level with optimal charge distribution, which increased the active
sites in this region and further enhanced the electrochemical activity.
In addition, some previous reported works on graphene-wrapped
structured cathode composites (e.g., a 3D porous LiFePO4/N-doped GA
composite developed by our group [134], Fig. 10e) have demonstrated
that the graphene layer could protect the active materials from direct
contact with the electrolyte and thus alleviate the side reactions and
dissolution of the active materials [184,201]. Nevertheless, it also was
revealed that Liþ ions are hard to pass through the graphene layer.
Taking LiFePO4 for example, Wei Wei et al. have demonstrated that a
completely graphene-encapsulated LFP composite has almost no capacity
[201]. Regardless of the high cost of graphene materials, when the
graphene-based cathode composites are used as the electrode material,
the weight ratio of the graphene component should also be considered for
practical applications. This is because too little graphene makes it
impossible to construct an effective conductive network and too much
graphene would block the Liþ transport to some extent in the electrode.
Moreover, the graphene component is almost inactive in the potential
windows of LIBs cathodes and makes a negligible capacity contribution,
which will reduce the energy density of the final electrode [87,114,306].
The graphene weight ratios for the reported cathode composites are
mainly distributed in the range of 5 wt%-20 wt%, which are much higher
than the commercial standard for using conventional carbon additives
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Energy Storage Materials 24 (2020) 22–51
(1 wt%-3 wt.%) [302]. Therefore, further optimization of the graphene
conductive network (with more effective electron and Liþ pathways) and
a lower graphene weight ratio are still the most important challenges for
graphene-based cathode composites.
6. Graphene-based composites for electrochemical energy
storage beyond electrochemical capacitors and Li-ion batteries
6.1. Na-ion batteries
Na-ion batteries (NIBs) recently have attracted extensive attention
owing to the plentiful reserves and low cost of sodium, so that the NIBs
are considered as the potential alternatives to LIBs [307,308]. The
working principle of NIBs is similar to that of LIBs, with Naþ migrating in
the electrolyte between the electrodes (cathode and anode) while the
electrons are transmitted through the outer electric circuit, as illustrated
in Fig. 11a [309]. To date, some materials have been reported for NIB
electrodes, including hard [310] or graphitic carbons [311], NaxM alloys
(M ¼ Si, Sn, Ge, Sb, P, etc.) [312] and transition metal oxides [313] or
sulfides [314] as anode materials, and layered oxides [315], polyanionic
phosphates [316,317], or pyrophosphates [318] as cathode materials.
Compared with Liþ, however, the relatively larger ionic size of Naþ
greatly limits the available kinds of host materials for NIB electrodes, and
the search for more appropriate host materials is still ongoing [319].
Pristine graphene is rarely directly used as an anode materials for
NIBs because of its lack of defects (e.g., residual oxygen-containing
groups) and poor Naþ adsorption property, which is very modest
compared to hard carbon or other active carbonaceous materials in terms
of Naþ storage capacity [200]. Although creating defects in graphene
seems can dramatically improve the Naþ storage capacity of
graphene-based anodes, the presence of defects represents low
Coulombic efficiency for NIBs as well [320]. Similar to LIBs,
graphene-based anode composites also show great potential in NIBs,
where they enable better electrochemical performance (e.g., higher
specific capacity, better rate capability and longer cycle life) compared
with bare graphene materials. Different types of anode active materials
have been combined with graphene, including transition metal oxides
(e.g., SnO2 [321], Fe3O4 [322], MgFe2O4 [323]), transition metal sulfides
(e.g., SnS2 [324], MoS2 [314]), metals or metal alloies (e.g., Sb [325], P
[326]), phosphorene [327], and NASICON-type NaTi2(PO4)3 [328], for
fabrication as promising anode composites for NIBs. Typically, Yi Cui’s
group reported a phosphorene/graphene composite made by sandwich-
ing phosphorene layers between graphene layers (Fig. 11b), which
showed a specific capacity as high as 2440 mAh g1 (based on the weight
of phosphorene) under a current density of 0.05 A g1 and capacity
retention of 83% after 100 cycles in the voltage window of 0–1.5 V (vs.
Na/Naþ) [327]. The presence of graphene layers in the composite
ensured electrical highways for electron transport and elastic buffer
space for accommodating the volume changes of phosphorene during
cycling. In another case, Yunhui Huang’s group synthesized a 3D com-
posite of graphene decorated with NaTi2(PO4)3 microspheres through a
facile spray-drying method combined with post calcination (Fig. 11c)
[328]. By combining the advantages of nanosized particles with the 3D
graphene conductive network, the ionic, electronic and mechanical
properties of the composite were significantly improved, and it thus
possessed the high reversible capacity of 130 mAh g1 at 0.1C and
excellent rate capability (38 mAh g1 at 200C) as well as great cycling
stability (77% capacity retention over 1000 cycles at 20C.
For NIB cathodes (e.g., layered oxides [315], polyanionic phosphates
[316,317], pyrophosphates [318], etc.), similar to their LIB analogues,
their relatively poor electronic conductivity is the key factor limiting
their rate capability [319]. In this regard, although graphene components
are generally inactive for SIB cathodes, many graphene-based cathode
composites (combining graphene materials with FeF3 [329],
Na3V2(PO4)3 [330], Na2/3Fe1/2Mn1/2O2 [154], etc.) have been designed
by taking advantages of the high electronic conductivity of graphene,
B. Wang et al. Energy Storage Materials 24 (2020) 22–51

Fig. 11. (a) Schematic illustration of the working principle of NIBs based on graphene-based electrodes. In this example, NaTi2(PO4)3/graphene and Na3V2(PO4)3/
graphene composites have been chosen as the anode and cathode materials, respectively. Structures and electrochemical characterizations of (b) phosphorene/gra-
phene composite created by sandwiching phosphorene layers between graphene layers (reproduced with permission from ref. 177, copyright 2015, Nature Publishing
Group), (c) composite of 3D graphene decorated with NaTi2(PO4)3 microspheres (reproduced with permission from ref. 328, copyright 2016, Wiley), (d) FeF3–Fe-RGO
cathode composite (reproduced with permission from ref. 329, copyright 2014, Elsevier), and (e) 3D Na3V2(PO4)3@C@RGO hierarchically porous composite
(reproduced with permission from ref. 330, copyright 2015, Wiley).

which all show improved rate performance compared with the bare
cathode materials. For example, Yu Zhang’s group synthesized an
extraordinary FeF3–Fe-RGO cathode material with high discharge ca-
pacity (150 mAh g1 under a current density of 50 mA g1), good cycling
stability, and high-power performance at room temperature, which
resulted from the homogeneous conductive architecture composed of
metallic Fe and RGO (Fig. 11d) [329]. In another work reported by Yan
Yu’ group, a 3D Na3V2(PO4)3@C@RGO hierarchically porous composite
with bicontinuous ion/electron pathways could realize fast charge/di-
scharge performance (e.g., 91 mAh g1 at 80C and 86 mAh g1 at 100C,
Fig. 11e) and long cycle life (64% capacity retention after 10000 cycles at
100C) [330].
6.2. Li–S batteries
Li–S batteries (LSBs) possess remarkably high theoretical specific
energy (2600 Wh kg1 or 2800 Wh L1) via a reversible electrochemical
reaction between Li anode and S cathode, as illustrated in Fig. 12a [331].
For Li anode, despite its advantages in terms of low electrochemical
potential and high theoretical specific capacity (3860 mAh g1), its main
drawback is the easy formation of dendrites during repeated Li deposi-
tion and dissolution processes [332]. Once these Li dendrites impale the
separator, a serious safety problem will exist. Some strategies have been
proposed to resolve the Li dendrite issue through (i) liquid electrolyte
additive (e.g., LiF [333], LiPF6 [334], Csþ [335], etc.), (ii) polymer and
solid electrolyte (e.g., liquid-like solid electrolyte [336], Li7P2S8I [337],
single-ion polymer [338], etc.), (iii) artificial SEI (e.g., Cu3N nano-
particles joined together by styrene butadiene rubber [339], Li3PO4
[340], poly(vinylidene-co-hexafluoropropylene) and LiF composite film
[341], etc.), (iv) membrane modification (e.g., Li6.75La3Zr1.75Ta0.25O12
coated polypropylene separator [342], mussel-inspired poly-
dopamine-treated-polyethylene separator [343], N and S co-doped gra-
phene nanosheets on polymer separator [344], etc.), and (iv) anode
structure optimization (e.g., conductive nanostructured graphene

38
B. Wang et al. Energy Storage Materials 24 (2020) 22–51

Fig. 12. (a) Schematic illustration of the working principle of LSBs with graphene-based electrodes. In this example, lithium/graphene and sulfur/graphene com-
posites have been chosen as the anode and cathode materials, respectively. Structures and electrochemical characterizations of (b) partially reduced GO/lithium film
composite (reproduced with permission from ref. 349, copyright 2016, Nature Publishing Group), (c) freestanding lithium alloy/graphene composite (reproduced with
permission from ref. 352, copyright 2017, Nature Publishing Group), (d) S/graphene-graphitic carbon nanocage composite (reproduced with permission from ref. 145,
copyright 2016, Wiley), and (e) conductive porous vanadium nitride nanoribbon/graphene composite (reproduced with permission from ref. 124, copyright 2017,
Nature Publishing Group).

scaffold [345], patterned reduced graphene oxide anode [346], 3D cur-
rent collector with a submicron skeleton and high electroactive surface
area [347], etc.), etc. [348].
Recently, it was found that the graphene materials with appropriate
oxygen-containing groups could exhibit a good “lithiophilicity”,
providing abundant active sites for the formation of Li crystal nuclei, and
thus alleviate the dendrite phenomenon [349,350]. In this regard, gra-
phene with oxygen groups has been introduced to combine with Li for the
construction of composite anodes [351]. Typically, Yi Cui’s group
designed a partially reduced GO/Li film composite electrode (Fig. 12b),
in which Li metal is stored in the interspaces of graphene layers through
lithiophilic capillarity, and it displayed stable Li plating/stripping
behavior and high Coulombic efficiency [349]. Soon after, they reported
a free-standing lithium alloy/graphene composite foil as an alternative to
lithium metal anodes (Fig. 12c). With the protection of graphene sheets,
the foil is stable in different atmospheres and exhibit stable cyclability
(400 cycles with 98% capacity retention) [352]. Further, Jiayan Luo’s
group designed a patterned RGO/Li composite anode with electric field
detoured to the edges of the patterned anodes and Li horizontally cen-
tripetal plating in the patterned voids, which could be cycled for more
than 2000 h and maintained stable voltage profiles at a large current
density of 10 mA cm2 [346]. On the other hand, Qiang Zhang’s group
[353] and Nikhil Koratkar’s group [354] demonstrated that the N-doped
atoms and defects in graphene were also lithiophilic, which could induce
uniform Li nucleation and smooth Li plating. Moreover, the high surface
area of the conductive graphene matrix can effectively enhance the
surface area and then reduce the local current density and suppress the
growth of Li dendrite. For example, Rui Zhang et al. designed a high

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B. Wang et al.
surface-area graphene framework (1666 m2 g1) with large pore volume
(1.65 cm3 g1) and good electrical conductivity (435 S cm1), when used
in Li anode, it was beneficial to regulate the Li depositing morphology
with a high Coulombic efficiency of 93% at 0.5 mA cm2 [345]. In
another case, Shan Liu et al. reported a crumpled graphene ball matrix
with large surface area to stabilize the dendrite-free Li metal anodes
[355]. Additionally, Dong-won Kim’s group demonstrated that the N and
S codoped graphene modified membrane could maintain a uniform ionic
flux on the Li metal surface and leading to the effectively suppressing
dendrite growth and stabilized cycling performance [344].
As for S cathode, although it has many advantages including abun-
dance, low cost, environmentally benignity, and high theoretical specific
capacity (1672 mAh g1), it is affected by several drawbacks: (i) very low
electronic conductivity of the redox reaction products (e.g., S, Li2S, etc.)
leading to sluggish electrochemical kinetics; (ii) the “shuttle effect” of the
soluble intermediate reaction products (polysulfides), resulting in low
Coulombic efficiency and poor cycle life; (iii) large volume changes
during charge and discharge processes, giving rise to degeneration of the
electrode [356]. Correspondingly, in order to address these problems,
various graphene materials (e.g., GO [357], RGO [358],
heteroatom-doped graphene [359], porous graphene [360], etc.) and
graphene-based composites (e.g., graphene/transition metal oxide [361],
graphene/polymer [362], graphene/micro or mesoporous carbon [363],
etc.) with different physical and chemical properties have been proposed
as both anode candidates and separators for trapping the soluble poly-
sulfides and alleviating the “shuttle effect” [364–366]. Recently, Yuguo
Guo’s group synthesized a S/graphene-graphitic carbon nanocage
(G-GCNs) composite with S nanoparticles encapsulated within GCNs
(Fig. 12d) [145]. Due to the high conductivity and the physical constraint
effect of the G-GCNs network, the S/(G-GCNs) composite achieved
improved S utilization (with a high specific discharge capacity of
1375 mAh g1) and superb high-rate capability (765 mAh g1 at 5C) as
well as a long cycle life of 1000 cycles. In another case, Feng Li’s group
reported a conductive vanadium nitride nanoribbon/graphene compos-
ite with porous structure that could accommodate the catholyte as
cathode for LSBs (Fig. 12e), which provided strong chemical adsorption
of polysulfides and electron transport highways for fast polysulfide
conversion [124]. The obtained composite exhibited a high initial ca-
pacity (1471 mAh g1) and good cycling stability (85% capacity reten-
tion after 100 cycles at 0.2C).
Although many previous reports on graphene-based composites for
LSBs demonstrated attractive electrochemical performance in terms of
capacity and Coulombic efficiency, the achieved cycling performances
are still very modest compared with LIBs, and further research to improve
LSB techniques is required (such as further improvement of the stability
of graphene/sulfur and graphene/lithium interfaces).
6.3. Li-air batteries
To meet the growing demand for energy, it is imperative to develop
more advanced EES devices with greater energy densities than com-
mercial LIBs. In this regard, the Li-air battery (LAB) with exceedingly
high theoretical energy density of 5200 Wh kg1 is believed to be one of
the most promising candidates [332]. In general, LABs are composed of a
metallic lithium anode, an Liþ ion-conducting electrolyte, and a porous
air cathode, as illustrated in Fig. 13a. The discharge process, corre-
sponding to the reduction of oxygen (O2) at the cathode exposed to air
and the oxidation of metallic Li at the anode with the generation of LiO2
and/or Li2O2, is commonly called the “oxygen reduction reaction”
(ORR). In reverse, the charge process, i.e., electrochemically decom-
posing Li2O2 and/or Li2O into Li and O2, is called the “oxygen evolution
reaction” (OER) [332,367].
Since the pioneering studies by Bruce and colleagues in 2006 [368],
the recharging of LABs has been intensively investigated. Unfortunately,
the LABs suffer severely from short cycle lifetimes, inefficient energy
utilization, and poor rate capability, caused by their limited
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Energy Storage Materials 24 (2020) 22–51
electrocatalytic performance (for the low-cost catalysts), generation of
irreversible Li2O2 by-products, undesired side reactions (between elec-
trolyte/Li and H2O/CO2 from the atmosphere), etc. Among the many
factors influencing the performance of LABs, the properties of the air
electrode (cathode) are especially important for achieving high energy
density, which is strongly influenced by the loading mass and catalytic
activity of the catalysts as well as the morphology and amounts of the
final discharge products [332,367]. In this regard, employing
graphene-based catalyst composites with large SSAs and porous nano-
structures seems to be an ideal strategy to address these issues for LABs
[369]. So far, various nanostructured noble and transition metals (or
oxides), such as Pt (Fig. 13b) [370], Co3O4 (Fig. 13c) [172], MnCo2O4
(Fig. 13d) [371], Nd0.5Sr0.5CoO3δ (Fig. 13e) [372], etc., have been
incorporated with different graphene materials and exhibited improved
performance in LABs compared with the bare catalytic materials,
although the achieved capacities are still far below those expected from
the theoretical energy density. Furthermore, in some previously reported
work, the researchers found that the functional groups and defects of
graphene materials can also play a catalytic role in the formation of
discharge products [369,373]. In order to develop more efficient
graphene-based catalyst composites, however, major studies are still
needed to further clarify the nature of the synergistic effects between the
graphene components and other catalytic materials in the composites.
6.4. Others
The recent outbreak of graphene-based composites in the EES field
have spurred research into other novel EES systems, such as magnesium-
ion batteries (MgIBs) [374] and Al-ion batteries (AIBs) [375,376].
Compared with Li and Na, Mg and Al are low-cost, environmentally
friendly and stable in atmosphere, and more importantly, they are much
safer as metallic anodes, being without dendrite formation in the
repeated plating and stripping processes. Although MgIBs and AIBs have
been proposed as emerging EES devices with high energy density for
future EES applications, the development of these batteries has been
hindered by the limited choice of appropriate electrode materials.
Recently, a few pristine graphene and graphene composite materials
have been reported as electrode materials for both MgIBs and AIBs,
although the achieved electrochemical performances still fall far short of
practical requirements [374,375]. In fact, the research on using
graphene-based composites for the abovementioned two multivalent
metal-ion batteries is still in its early stages, and more investigation needs
to be focused on this field for achieving better electrochemical
performance.
Graphene-based composites have also been reported as air electrodes
for Na-air batteries (NABs) [377] and Zn-air batteries (ZABs) [378], and
as active materials for vanadium redox-flow batteries (VRFBs) [379],
which were introduced in order to improve their performance. Similar to
LABs, NABs and ZABs also have some technical challenges hindering
their practical application, and it appeared that graphene-based com-
posites could enhance the catalytic properties of both ORR and OER
processes for these metal-air batteries through the synergistic effects
between graphene materials and other catalytic components [18]. These
technologies for NABs and ZABs are in their very early stages and require
much deeper research. In the case of VRFBs, although this type of EES
device is quite promising for practical applications, current techniques
for synthesizing their electrodes and membranes cannot satisfy high re-
quirements. Graphene-based composites have also been employed in
VRFB electrodes to improve their electronic conductivity and reversible
kinetics [379]. Graphene materials (GO or graphene) have also been used
as additives to VRFB ion-exchange membranes to reduce the vanadium
permeation and prevent ionic cross-mixing [380]. Nevertheless, the
techniques for using graphene-based composites in VRFBs are also too
immature for commercial applications.
In addition to these aforementioned EES systems, graphene-based
composites have also exhibited great potential in numerous of other
B. Wang et al. Energy Storage Materials 24 (2020) 22–51

Fig. 13. (a) Schematic illustration of the working principle for LABs containing graphene-based electrodes. Structures and electrochemical characterizations of (b) Pt
nanoparticles/graphene composite (reproduced with permission from ref. 370, copyright 2012, Elsevier), (c) Co3O4 nanofibers/graphene composite (reproduced with
permission from ref. 172, copyright 2013, American Chemical Society), (d) MnCo2O4 nanoparticles/graphene composite (reproduced with permission from ref. 371,
copyright 2012, The Royal Society of Chemistry), and (e) Nd0.5Sr0.5CoO3-δ nanorods/graphene composite (reproduced with permission from ref. 372, copyright 2016,
The Royal Society of Chemistry).

emerging EES devices, including, but not limited to K-ion batteries (KIBs)
[381], Mg–S batteries (MSBs) [382], Mg-air batteries (MABs) [383],
Al-air batteries (AABs) [384], and hybrid systems (such as Li-ion ca-
pacitors - LICs) [385], because of their promising physical and chemical
properties with synergistic effects between different components for
efficient EES. The reports on graphene-based composites for the afore-
mentioned emerging EES systems in this section are summarized in
Table 1.
7. Emerging properties of electrochemical energy storage devices
fabricated from graphene-based composites
7.1. Flexibility
The market for flexible electronics, with products currently ranging
from flexible solar cells to flexible displays as well as wearable elec-
tronics, is rapidly expanding [413]. The rise of this market is mainly due
to the further requirements from consumers and the fast progress in
research on flexible materials [413]. In the EES field, almost all of the
commercial batteries and capacitors are inflexible and unbendable (since
bending them to any large extent may cause electrolyte leakage or even
structure damage). This is because the present EES devices are mainly
based on particulate-like active materials with very poor flexibility. With
the rise of graphene, which is considered as an ideal flexible material
(due to its intrinsic properties), and graphene-based composites could
further inherit this advantage. In this regard, numerous flexible EES
systems (e.g., rollable [414], twistable [415], stretchable [416], and
wearable [417] ECs and LIBs) with tunable shapes, dimensions, and
properties are being studied based on these materials. For example, 2D
graphene-based composite films (e.g., a graphene hydrogel/polyaniline

41
B. Wang et al. Energy Storage Materials 24 (2020) 22–51

Table 1
Summary of graphene-based composites for the emerging EES systems.
EESa) Graphene-based composites Electrochemical performance Ref.
1
Rate capability (mAh g ) Cycling stability (cycles)

MgIBs MgMn2O4/RGO 211.8 (50 mA g1)/140.1 (1 A g1) 119.5 mAh g1 at 1 A g1 (1000) [386]
Mo6S8/GO/Al Unmentioned 80 mAh g1 at 50 mA g1 (10) [387]
Mg1.1Mn6O12⋅4.5H2O/graphene 194.1 (20 mA g1)/112 (100 mA g1) 88.5 mAh g1 at 100 mA g1 (400) [388]
Mo6S8/Cu/graphene 82 (1.2 A g1) 100 mAh g1 at 120 mA g1 (30) [389]
FeVO4 0.9H2O/graphene 183.8 (50 mA g1)/86.6 (500 mA g1) 98 mAh g1 at 100 mA g1 (50) [390]

AIBs Al0.16V2O5/RGO 122 (3 A g1) 247 mAh g1 at 300 mA g1 (50) [391]
VS4/RGO 80 (100 mA g1)/60 (300 mA g1) ˃ 80 mAh g1 at 100 mA g1 (100) [392]
TiO2/graphene Unmentioned 33 mAh g1 at 6.25 A g1 (100) [393]

NABs MnCo2O4/N-doped graphene Charge-discharge voltage gap of 0.39 V at current density of 0.13 mA cm2 [394]
RuO2/B-doped RGO Charge-discharge voltage gap of <0.72 V at current density of 0.05 mA cm2 [395]
Graphene nanosheets loaded with Pt nanoparticles 7574 (0.1 mA cm2) Discharge and charge voltage plateaus at about 2.38 V and [396]
3.6 V at 0.1 mA cm2 (10)
VO2/RGO Charge-discharge voltage gap of 0.64 and 1.05 V at current density of 0.01 and 0.05 mA cm2 [397]
α-MnO2 nanowires/RGO/carbon microfibers 1200 (30 mA g1) Charge-discharge voltage gap increased from 0.7 to 0.84 V at [377]
15 mA g1 (20)

ZABs CoMn2O4 nanoparticles anchored on N-doped Unmentioned Charge-discharge voltage gap increased from 0.70 V to [398]
graphene nanosheets 0.86 V at 20 mA cm2 (100)
MnNiFe metal oxide/graphene Charge-discharge voltage gap of 1.09 V at current density of 50 mA cm2 [399]
3D Fe/N/S-doped graphene 53.9 mW cm2 (50 mA cm2) Unmentioned [400]
Ni3Fe/N,S-doped CNT/graphene 180 mW cm2 (350 mA cm2) Charge-discharge voltage gap of 0.75 V (60) [401]
RGO/carbon black/cobalt borate ~76 mW cm2 (0.3 A cm2) Unmentioned [402]
Ni3Fe/Co9S8/graphene Open circuit voltage (1.45 V), a peak power density of 125 mW cm2 [403]

VRFBs GO nanosheets/multi-walled carbon nanotubes Peak potential separation of 0.15 and 0.21 V at scan rate of 5 and 100 mV s1 [379]
RGO/graphite felt 23.9 Ah L1 (150 mA cm2) Unmentioned [404]
TiNb2O7/RGO 2400 mAh (40 mA cm2)/1700 mAh 2100 mAh at 120 mA cm2 (200) [405]
(160 mA cm2)

KIBs Mn3O4/graphene 83 (1 A g1) ~130 mAh g1 at 0.1 A g1 (100) [406]
SnS2@RGO 448 (50 mA g1)/247 (1 A g1) 205 mAh g1 at 1 A g1 (300) [407]

MSBs Graphene/sulfur nanocomposite 885 (5 mA g1)/108 (45 mA g1) 219 mAh g1 at 20 mA g1 (50) [382]

MABs Mn3O4 nanowires/3D graphene/single-walled Open circuit voltage (1.49 V), a high plateau voltage (1.34 V), and a long discharge time (4177 min) at [408]
carbon nanotube 0.2 mA cm2
α-MnO2 Nanowires/graphene 96 mW cm2 at 140 mA cm2 [409]

AABs ZnO/ZnCo2O4/C@RGO Open circuit voltage (1.53 V), a high plateau voltage (1.29 V), and a discharge capacity (42.6 mAh g1) at [410]
1 mA cm2

LICs Fe3O4/graphene//3D graphene 147 Wh kg1 (150 W kg1)/86 Wh kg1 70% retention at 2 A g1 (1000) [411]
(2587 W kg1)

NICs Polyimide-graphene//RGO 55.5 Wh kg1 (395 W kg1)/21.5 Wh kg1 ~60% retention at 100 mA g1 (1000) [412]
(3400 W kg1)
a
MgIBs, AIBs, NABs, ZABs, VRFBs, KIBs, MSBs, MABs, AABs, LICs, NICs represent Mg-ion batteries, Al-ion batteries, Na-air batteries, Zn-air batteries, vanadium redox-
flow batteries, K-ion batteries, Mg–S batteries, Mg-air batteries, Al-air batteries, Li-ion capacitors and Na-ion capacitors, respectively.

composite film developed by Dan Li et al. [227]) are very popular to
application in flexible ECs [269,418].
Among the various flexible EES systems, wearable EES devices are
quite attractive, which can be incorporated into clothing and accessories
for fabricating wearable electronics [419]. T These smart garments are
expected to collect information from the users in real time [420]. Zhenan
Bao’s group first designed textile-based ECs in 2011 through coating
graphene/MnO2 composite onto porous textile fibers [421]. Recently,
great research efforts have been devoted to the development of
core-sheath and coaxial electrodes, which combine the current collector
and active materials in a single yarn that is ready for knitting or weaving
directly into textiles [422]. For instance, Chao Gao’s group reported
polyelectrolyte-wrapped graphene/CNT core-sheath composite yarns
with good flexibility and weavability that were produced via a
wet-spinning method, which could exhibit a much improved areal
capacitance up to 269 mF cm2 (Fig. 14a) [423].
7.2. Transparency
Recently, transparent devices have attracted substantial attention.
Benefiting from the research advances on transparent materials and
techniques, various transparent devices have been demonstrated for
successful application in different fields, including touch screens, smart
windows, solar cells, etc. However, the development of transparent
power sources as a key component for fully integrated transparent de-
vices remains a challenge, mainly because of the difficulty in simulta-
neously realizing the transparency of each component [424]. Actually,
the traditional multilayer structure for power source systems (e.g., LIBs)
contains electrode (anode and cathode), electrolyte, separator, pack-
aging, etc. Among them, only the electrolyte is intrinsically transparent,
whereas the other components are opaque, and the electrode is the most
difficult component for realizing transparency [11].
To make a transparent electrode, one approach is to reduce its
thickness to the nanometer scale, although this strategy would sacrifice

42
B. Wang et al. Energy Storage Materials 24 (2020) 22–51

Fig. 14. A schematic diagram showing the emerging properties of EES devices fabricated from graphene-based composites. (a) Flexibility: Polyelectrolyte-wrapped
graphene/CNT core-sheath composite yarns (reproduced with permission from ref. 423, copyright 2014, Nature Publishing Group). (b) Transparency: Graphene/CNTs
composite film (reproduced with permission from ref. 428, copyright 2010, American Chemical Society). (c) Free-standing property: Graphene/LiFePO4 quantum dot
composite film (reproduced with permission from ref. 126, copyright 2017, Elsevier). (d) Fast-charging property for batteries. (e) High-energy density for ECs. (f)
Electrochromism: Electrochromic polyaniline/graphite oxide nanocomposite film (reproduced with permission from ref. 437, copyright 2013, Elsevier). (g) Self-
healing: GO/poly(acrylic acid) (PAA)/amorphous calcium carbonate (ACC) composite (reproduced with permission from ref. 238, copyright 2018, Wiley). (h) All
graphene-based structure: A unique sandwich structure with pure sulfur between two graphene membranes (reproduced with permission from ref. 439, copy-
right 2014,Wiley).

much of the capacity [425]. Another strategy is to design a patterned
electrode with feature dimensions below the resolution limit of the
human eye [426]. With these two methods, graphene-based composites
all have great potential for fabricating the desired transparent electrodes,
because of the inherent transparency of graphene (97.7% transmittance)
and its tunable dimensions on both the micro- and the macroscale. For
example, Aldo J.G. Zarbin’s group used an innovative, single-pot syn-
thesis to chemically produce graphene/polyaniline composite film,
which exhibited good transparency and flexibility, and could be easily
transferred to many kinds of ordinary substrates for practical applications
(Fig. 14b) [427,428]. When this composite film was employed to
construct a transparent supercapacitor device, it could display excellent
pseudocapacitive behaviors with specific capacitance of 267.2 F cm3.
Therefore, it is believed that graphene-based composites will play more
and more important roles in the field of transparent power source sys-
tems in the future.
7.3. Free-standing property
Generally speaking, the electrodes of commercial EES devices such as
capacitors and batteries are fabricated by mixing particulate-like active
materials with conductive agents (e.g., carbon black) and polymeric
binders (e.g., polytetrafluoroethylene) in suitable solvents. The obtained
slurries are coated on appropriate current collectors, normally copper foil
for the anode and aluminum foil for the cathode. After drying, the
electrodes are put through a mechanical pressing process to adjust the
pore volume and density. In the electrodes, the conductive agents are
used to improve the electronic contact between the active particles,
whereas the binders are intended to glue the active materials to the
current collectors [134]. For industrial preparation technologies, how-
ever, the mass ratio of inactive conductive agents, such as binders and
current collectors, range between 20-30 wt%, which would lower the
energy densities of the fabricated electrodes. Moreover, the inhomoge-
neous distribution of insulating polymeric binders would block the
transport pathways for both electrons and ions, and thus result in poor
rate capability and low power density [126].
Many previously reported works have demonstrated that graphene-
based composites (e.g. graphene/Si film [429], graphene/metal oxide
paper [430], graphene/LFP film [126], etc.) can be directly employed as
free-standing electrodes for various EES devices without the addition of
conductive agents and binders, because of their free-standing properties
combined with excellent conductivity, tunable porous structures, and

43
B. Wang et al.
outstanding mechanical flexibility. For example, we previously reported
a graphene/LFP quantum dot composite film with good mechanical
flexibility (Fig. 14c), which could delivered a specific capacity of
~80 mAh g1 at 100C as an LIB cathode, even at a relatively high mass
loading condition (6 mg cm2) [126]. Considering the superior proper-
ties of graphene-based composites, future free-standing EES devices
based on these materials are expected to be more integrated and effective
with higher energy and power densities.
7.4. Fast-charging property for batteries
In the case of battery systems (e.g., LIBs and LSBs), with the slow
faradaic reactions generally taking place in the bulk of electrochemically
active materials, they usually suffer from low ion transfer kinetics, thus
leading to a long charging times, typically in hours, whereas the cus-
tomers are looking forwards to a much shorter charging time, in minutes
or even seconds. Taking LIBs for example, which were first commer-
cialized in 1991 by the Sony Corporation, they always take several hours
to reach the fully charged state [431]. With the development of
graphene-based composite in this field, however, the graphene provides
fast ionic and electronic transport pathways in the electrode and thus
decreases the charging time of the LIBs (Fig. 14d). Recently, we have
demonstrated that a three-dimensional porous nitrogen-doped graphene
aerogel/LiFePO4 cathode composite could realize a charged capacity of
145 mAh g1 in 60 s with a charge efficiency of 97% [126]. In another
case, David Rooney’s group designed an anatase TiO2
quantum-dot/graphene nanosheet anode composite, which could be
successfully charged and discharged at 50C, corresponding to a fast
charge and discharge process within 72 s [117]. Moreover, Huiming
Cheng’s group reported a full LIB fabricated by using a graphene
foam/Li4Ti5O12 composite anode and a graphene foam/LiFePO4 com-
posite cathode without any further introduction of binders and conduc-
tive agents [236]. Because of the outstanding electronic conductivity and
open porous structure of the composite electrodes, the designed LIB
could be fully charged in only 18 s.
In addition, the fast-charging property has also been achieved by
other battery systems based on graphene-based composites. For instance,
Qiang Zhang’s group reported an unstacked double-layer templated
graphene/S composite as cathode material for LSBs, which achieved a
fast charge/discharge process at 10C (corresponding to 6 min) because of
its excellent electron and ion transport kinetics [432]. In another work,
Lianzhou Wang’s group designed a MoS2/graphene nanosheet composite
as anode material for NIBs using commercial MoS2 bulks and graphite as
the raw materials, which exhibited a remarkably high rate capability
with capacity of 201 mAh g1 at 75C, corresponding to a fully charged
state in 48 s [433]. Actually, the fast-charging property is not only limited
to batteries, the fast charge (and discharge) property of capacitors can
also be improved by using graphene-based composites. In 2012, Douglas
Natelson and James M. Tour’s group fabricated a microsupercapacitor
based on a 3D graphene/carbon nanotube composite carpet, which could
be charged and discharged in only 0.195 ms comparable to commercial
Al-electrolytic capacitors (AECs) for alternating current (ac) line filtering
applications [434]. This microsupercapacitor, however, could deliver a
much higher volumetric energy density of 2.42 mWh cm3 (in the ionic
liquid), more than 2 orders of magnitude higher than that of AECs, which
may make it possible to realize smaller and lighter electronic devices in
the future.
7.5. High-energy density for electrochemical capacitors
Currently commercial supercapacitors are mostly based on active
carbon electrodes and organic electrolyte with the working voltage
ranging from 2.3 V to 2.8 V, which possess excellent cycling stability and
high power density, although their energy density is quite low (5–7 Wh
kg1) compared with battery systems (one order of magnitude lower). In
recent years, graphene-based composites have been studied in great
44
Energy Storage Materials 24 (2020) 22–51
detail, with the aim of increasing the energy density of ECs to the level
achieved in batteries without sacrificing their high power capability
(Fig. 14e) [257]. For example, Guangming Wu’s group designed a 3D
hierarchical porous V2O5/graphene composite aerogel for super-
capacitors, which demonstrated a high energy density of 68 Wh kg1
(comparable to lead-acid batteries) in a symmetric two-electrode systems
using 1 M Na2SO4 aqueous solution as the electrolyte, attributed to their
high electronic conductivity and unique hierarchical porous structure
[435]. In another example, Tsung-Wu Lin’s group fabricated an asym-
metric supercapacitor based on NiOOH/Ni3S2/3D graphene and
Fe3O4/graphene composite electrodes, which could be operated revers-
ibly between 0 and 1.6 V with a maximum energy density of 82.5 Wh
kg1 at a power density of 930 W kg1 [264]. In addition, apart from the
high energy density achieved in the form of mass energy density for ECs,
many other works have also focused on improving the volumetric energy
density by tuning the porous structure of graphene-based composites.
Typically, Richard B. Kaner’s group demonstrated 3D high-performance
hybrid supercapacitors based on graphene/MnO2 composites. Volu-
metric energy densities as high as 42 Wh L1 were achieved by rationally
designing the electrode microstructure and combining the active mate-
rials with electrolytes that operate at high voltages [436].
7.6. Other properties
Apart from the properties discussed in the above sections, there are
also some other unique properties that have been emerging for EES de-
vices fabricated from graphene-based composites, such as electro-
chromism [437], self-healing [258,265], all-solid-state [438], all
graphene-based structure [236,439,440], etc. For example, Zhanhu
Guo’s group reported an electrochromic polyaniline/graphite oxide
nanocomposite film with durable EES performance (Fig. 14f) [437]. A
coloration efficiency of 59.3 cm2 C1 and an areal capacitance of
25.7 mF cm2 were obtained simultaneously. In another case, Nishuang
Liu and Yihua Gao et al. designed a highly stretchable and self-healing
supercapacitor using RGO based springs (Fig. 14g), which were
composed of polypyrrole (PPy)-decorated RGO/multiwalled carbon
nanotubes (MWCNTs) [258]. The constructed supercapacitor exhibited
82.4% capacitance retention with a large stretching capacity (100%) and
54.2% capacitance retention at the third healing. This work provides an
important method for the design and fabrication of stretchable and
self-healable supercapacitors for next-generation multifunctional elec-
tronic devices.
The multifunctionality of graphene-based composites, which can be
purposefully designed to form different kinds of components for EES
devices, such as current collectors [441] and separator [442], has
resulted in all graphene-based and all-solid-state EES devices [438–440].
For example, the existing LIB techniques generally adopt metal foil as the
current collectors (with thickness mainly ranging between 20-80 μm),
which occupies a relatively large weight ratio (~10–20 wt%) of the de-
vice and contributes no capacity, reducing the overall energy density.
Correspondingly, some strategies have been developed for fabricating
graphene-based films with light weight and high conductivity (both
electronic conductivity and thermal conductivity), which could be cho-
sen as ideal current collectors for EES devices [37,441]. For instance,
Zhong-Shuai Wu’s group reported the on-chip construction of
all-solid-state planar integrated LIBs with robust flexibility, high energy
density, and extraordinary integration, in which high-quality graphene
was employed as metal-free current collector [443]. In another case,
Wencai Ren’s group demonstrated integrated micro-supercapacitors
based on in-series screen-printed graphene on various substrates, with
metal-free current collectors, high-voltage output, exceptional electrical
double-layer capacitive behaviors and outstanding flexibility [451].
There are also some reports focused on graphene-based separators for
permselective mass transport, especially in the LSB field for reducing the
“shuttle effect” of soluble polysulfides [442]. Furthermore, Huiming
Cheng’s group constructed some sandwich-like all graphene-based
B. Wang et al. Energy Storage Materials 24 (2020) 22–51

structures for LSB cathodes, which showed great potential in term of high
energy density, long life, and ultrafast-charging performance (Fig. 14h)
[439,440]. In addition, recently, Chunsheng Wang’s group [445] and
Xinliang Feng group [446] successfully fabricated all-solid-state LSBs and
pseudocapacitors, respectively, based on graphene-based materials,
which all exhibited excellent electrochemical performance and superior
safety. More details about the emerging properties discussed in this
section are summarized in Table 2.
8. Conclusion and outlook
In this review, we have summarized the recent progress on graphene-
based composites for EES, focusing on their rational structural design,
interfacial engineering, and energy storage mechanisms for different EES
applications as well as the emerging features of EES devices fabricated
from these graphene-based composites. Although graphene-based com-
posites for EES have witnessed substantial achievements and rapid
development in the past few years, there are still many challenges that
need to be addressed before practical applications of such EES in different
fields (Fig. 15).
First, the lack of feasible techniques for the mass production of both
high-quality graphene materials and graphene-based composites limits
their potential applications in the EES field to a great extent (Fig. 15a).
For example, although the strategy involving the reduction of GO to RGO
(which is a common raw material for graphene-based composites) is
relatively cheap and promising for mass production, the inevitable
presence of both extrinsic (e.g., O, H, and other foreign atoms) and
intrinsic (e.g. vacancies and deformations) defects in RGO strongly af-
fects its physical properties (e.g. electronic conductivity) and the elec-
trochemical performance of the final obtained composites. Therefore,

Table 2
Emerging properties of graphene-based composites for EES devices reported in the literature.
Features EESa) Composites Performance Ref.

Rate capability (mAh g1) Cycling stability (cycles)

Flexibility ECs Graphene/MnO2 nano-textiles ~315 F g1 (2 mV s1) ~95% at 2.2 A g1 (5000) [421]
ECs Polyelectrolyte- graphene/CNT core- Capacitance retentions of 98 and 111% for bending 200 and 1000 times [423]
sheath fibres
ECs Cellulose/RGO/Ag 683.8 mF cm2 (5 mA cm2)/347.9 mF cm2 99.6% at 60 mA cm2 (10000) [447]
(40 mA cm2)
LIBs Si/RGO 1210 (100 mA g1)/253 (2 A g1) 1
43% at 1 A g (1000) [448]
ECs RGO/polymer dots 95.3 F g1 (0.1 A g1)/68 F g1 (10 A g1) 90.6% at 0.5 A g1 (1000) [449]
NIBs 3D carbon/Fe7S8/graphene 2.12 mAh cm2 (0.25 mA cm2)/1.12 mAh 95% at 6 mA cm2 (500) [450]
cm2 (10 mA cm2)
ECs Polyaniline/graphene 4.9 mF cm2 (2 mV s1)/3.16 mF cm2 91.1% at 0.2 mA cm2 (10000) [444]
(500 mV s1)
ECs Screen-printed graphene 1 mF cm2 (5 mV s1)/0.58 mF cm2 91.8% at 0.2 mA cm 2
(10000) [451]
(500 mV s1)

Transparency ECs Graphene/polyaniline 267.2 F cm3 (10.8 μA) 88% at 10.8 μA (400) [427]

Free-standing property LIBs Graphene/Si film Unmentioned 708 mAh g1 at 50 mA g1 (100) [429]
ECs Nb2O5/graphene papers 47 Wh kg1 (393 W kg1)/15 Wh kg1 ~93% of the initial energy at 0.25 A g1 [452]
(18 kW kg1) (2000)
LIBs LFP quantum-dots/graphene 135 (20C)/78 (200C) ~99% at 20C (1000) [126]
ECs RGO/PPy 226 mF cm2 (2 mA cm2)/116.9 mF cm2 73.2% at 3 mA cm2 (10000) [453]
(6 mA cm2)
LIBs V2O5/N-graphene 290 (100 mA g1)/162 (2 A g1) 134 mAh g1 at 1 A g1 (500) [454]
KIBs S-doped RGO sponges 435 (50 mA g1)/224 (1 A g1) 229 mAh g1 at 1 A g1 (500) [455]

Fast-charging property LIBs 3D N-doped graphene aerogel/LFP ~155 (0.2C)/78 (100C) 89% at 10C (1000) [134]
LIBs TiO2 quantum-dot/graphene 161 (5C)/101 (50C) 190 mAh g1 at 1C (100) [117]
LIBs Graphene foam/Li4Ti5O12//graphene 170 (1C)/135 (200C) ~96% at 100C (500) [456]
foam/LFP
LSB Double-layer graphene/S ~1200 (0.5C)/713 (10C) 530 mAh g1 at 5C (1000)/380 mAh g1 [432]
at 10C (1000)
1 1
NIB MoS2/graphene 284 (20 A g )/201 (50 A g ) 95% at 0.3 A g1 (250) [433]
ECs 3D graphene/CNT 115 W cm3 (400 V s1) 98.4% at 0.5 mA cm2 (8000) [434]

High-energy density ECs 3D porous V2O5/graphene aerogels 68 Wh kg1(250 W kg1) 90% at 10 A g1 (20000) [435]
ECs NiOOH/Ni3S2/3D graphene//Fe3O4/ 82.5 Wh kg1 (930 W kg1)/63.1 Wh kg1 26% at 1 A g1 (2000) [264]
graphene (6.9 kW kg1)
ECs Graphene/MnO2 22 Wh L1 (~10 kW/1) 96% at 1 V s1 (10000) [436]

Electrochromism ECs Polyaniline/GO film Coloration efficiency of 59.3 cm2 C1, 53.1% capacitance retention at 3 mA cm2 (1000) [437]

Self-heal property ECs PPy-decorated RGO/MWCNTs 82.4% capacitance retention after a large stretch of 100%, and 54.2% capacitance retention [258]
after the third healing

All graphene-based LSBs Graphene-S sandwich structure 1340 (300 mA g1) 70% at 1.5 A g1 (300) [457]
structure LSBs All-graphene/S cathode 1500 (0.34 A g1)/1039 (1.68 A g1) 841 mAh g1 at 0.34 A g1 (400) [440]

All-solid-state LSBs Amorphous S/RGO 1525.6 (0.05C)/204.7 (5C) at 60  C 830 mAh g1 at 1C (750) [445]
ECs 2D thiophene nanosheets/graphene 326 F cm3 (10 mV s1)/123 F cm3 ~86% at 100 mV s1 (10000) [446]
(100 V s1)
LIBs Li2TiO3/graphene//LFP/graphene 67.7 mAh cm3 (0.2C)/47.7 mAh cm3 (2C) no apparent degradation at 5C (3300) [443]
a
ECs, LIBs, NIBs, KIBs, LSBs represent electrochemical capacitors, Li-ion batteries, Na-ion batteries, K-ion batteries and Li–S batteries, respectively.

45
B. Wang et al.
advanced material preparation strategies for synthesizing graphene and
graphene-based composites with the desired physical and electro-
chemical properties will continue to gain substantial research interests in
the future.
Second, although there are several reported compound modes and
structures of graphene-based composites (e.g., electrochemically active
materials anchored to the surface of graphene, sandwiched between
graphene sheets, wrapped or encapsulated by graphene layers, etc.) with
improved electrochemical performance, mainly because of the proposed
“synergistic effects” between the graphene component and the other
electrochemical active materials, however, it is still not clear which of
these structures could provide the best electrochemical performance in
specific EES applications. Therefore, more effects are required to
fundamentally understand the molecular interaction between graphene
and the other components in the electrode/electrolyte interface and
inner bulk under device working conditions from both experimental and
theoretical aspects (Fig. 15b). This would permit the production of
unique graphene-based composites with customized properties for
practical applications in different EES systems.
Third, the high surface area of graphene-based composites plays a
significant role in their application for supercapacitors, both EDLCs and
pseudocapacitors. Specifically, a variety of graphene-based composites
with diverse structures and dimensionalities, for instance, graphene/
CNTs, graphene/transition metal oxides (or sulfides), and graphene/
polymer composites have achieved a degree of success. The high surface
area combined with the enhanced electronic conductivity, appropriate
porous structures, and steric hindrance effect (between two components)
endows these composites with boosted supercapacitor capabilities. The
porous structure, however, significantly degrades their volumetric en-
ergy density. In this regard, there is still room to enhance the packing
46
Energy Storage Materials 24 (2020) 22–51
Fig. 15. Challenges that need to be addressed before
practical applications of graphene-based composites
in different EES fields. (a) Mass production. Repro-
duced with permission from ref. 80, copyright 2014,
Nature Publishing Group. (b) Optimized compound
mode. Reproduced with permission from ref. 126,
copyright 2017, Elsevier. (c) Optimized porous
structure. (d) Balanced electron and ion transport. (e)
Fundamental understanding. (f) Practical applica-
tion. Reproduced with permission from ref. 5, copy-
right 2016, Nature Publishing Group.
densities of graphene-based composites by optimizing their porous
structure for further commercialization in supercapacitors (Fig. 15c).
Fourth, in fact, graphene-based composites have been substantially
studied in various metal-ion batteries (e.g., LIBs, NIBs) and metal-sulfur
batteries (e.g., LSBs, MSBs) with outstanding electrochemical perfor-
mance, which mainly benefit from their high electronic conductivity,
large surface area, unique nanoporous architecture, good stability for the
formation of SEI film, etc. In most cases, however, the mass ratio of the
graphene component is quite large in these composites, normally larger
than 10 wt%, which may lower the packing density and energy density of
the batteries. Moreover, too much graphene would more easily block the
transport of ions (e. g., Liþ, Naþ), especially in a high mass-loading
condition, due to the limited diffusion through the basal plane of per-
fect graphene. Therefore, more efforts should be focused on achieving an
optimized balance between electron transport and fast ion diffusion
(Fig. 15d). In addition, the low Coulombic efficiency for the first cycle of
graphene-based composite anodes, mainly caused by their high surface
area and the existence of defects in graphene, is another challenge that
needs to be addressed for their practical application in metal-ion batte-
ries (e.g., LIBs).
Fifth, metal-air batteries (e.g., LABs, NABs) with extremely high
theoretical energy density are considered to be likely to lead a revolution
in EES history. Although several graphene-based composites (e. g., gra-
phene/Pt and graphene/Ru) have been designed with improved perfor-
mance, the achieved capacities are still far away from the theoretical
energy density. The key fundamental chemistry problems associated with
graphene-based composite application in metal-air batteries, especially
the synergistic effects between the graphene component and the other
catalytic materials in the composites, are still not completely understood.
It is important that future work must be focused on solving and
B. Wang et al.
understanding these problems before achieving the goal for the practical
application of graphene-based composites in this area (Fig. 15e).
Sixth, although the electrochemical performances of graphene-based
composites achieved in the literature are quite impressive, successful
examples of practical applications are still quite lacking. Taking LIBs for
example, apart from the relatively high cost and complex synthesis
procedure for the graphene-based composites, the gap in test conditions
between academia and industry (e.g., mass loading, amount of used
electrolyte, electrode fabrication) is another important factor. Therefore,
in order to further promote the research achievements to industry, the
electrochemical performances obtained under industrial conditions
should be considered for the promising graphene-based composites
(Fig. 15f).
In summary, there is no doubt that graphene-based composites have
already changed the blueprint of EES field because of their excellent
electrochemical performances and unique physical properties. Innova-
tive strategies have been developed for the fabrication of EES devices
with imaging features (e.g., flexibility and transparency) by employing
appropriate graphene-based composites, although it has not been
possible to realize mass production using current state-of-the-art tech-
nologies. Nevertheless, the full potential of graphene-based composites
for EES has yet to be achieved and many challenges still remain (as
discussed in the previous content). More efforts involving both experi-
mental research and theoretical calculations should be made to solve
these existing challenges. Deeper understanding of the “synergistic ef-
fects” between graphene and other electrochemically active components
from both the structure aspect and energy storage mechanism, and
further optimizing the multifunctional morphologies and di-
mensionalities of graphene-based composites will drive more potential
applications of these materials. It is expected that the research on
graphene-based composites will continue to advance rapidly in the next
two decades and make real changes in our EES systems.
Acknowledgements
We thanks for the support and suggestions of Prof. Rodney S. Ruoff
from Center for Multidimensional Carbon Materials, Institute for Basic
Science (IBS), Ulsan 44919, Republic of Korea. The National Natural
Science Foundation of China (Nos. 51604089 and 51874110), the China
Postdoctoral Science Foundation (Nos. 2016M601431and
2018T110308), and the Heilongjiang Province Postdoctoral Science
Foundation (Nos. LBH-Z16056 and LBH-TZ1707) are gratefully
acknowledged.
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