Energy & Environmental Science: Perspective

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PERSPECTIVE
Published on 30 September 2014. Downloaded on 28/09/2015 07:08:38.
Cite this: Energy Environ. Sci., 2015, 8,

31
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Tailored graphene systems for unconventional

applications in energy conversion and storage
devices
Chuangang Hu,a Long Song,a Zhipan Zhang,*a Nan Chen,a Zhihai Fengb
and Liangti Qu*a
Graphene-based materials have shown great potential in various elds across physics, chemistry, biology,
and electronics, due to their unique electronic properties, facile synthesis, and ease of functionalization. In
this review, we summarize the signicant advances in tailored graphene systems for the recently developed
unconventional energy conversion and storage devices reported by our group and others, namely focused
on their tunable and controllable preparation and remarkable applications in new types of supercapacitors,
lithium ion batteries, photovoltaic cells, and other emerging generators. This featured article also highlights
Received 16th August 2014

Accepted 30th September 2014
the working principles and outlines the problems hindering the practical applications of graphene-based
materials in these energy-related devices. Future research trends towards new methodologies in the
DOI: 10.1039/c4ee02594f
design and synthesis of graphene-based systems with unique properties for emerging energy storage
www.rsc.org/ees
and energy conversion devices are also proposed.
Broader context
Energy and environmental issues, including the depletion of fossil fuels, waste pollution, and global warming, pose great threats to the sustainable development
of human society. Consequently, nding reliable ways of eciently producing and conveniently storing clean energy is of paramount importance. A practical
solution to these problems lies in two aspects. First, energy should be eciently converted from inexhaustible or renewable sources, such as solar, wind, water,
and geothermal energy, into applicable forms such as electricity or fuels; and in this consideration, photovoltaic cells, photoelectrochemical cells, and fuel cells
are the prevailing devices currently under intense investigation. Second, eective, low-cost, and environmentally benign energy storage devices are needed to
complement the new power generating systems, due to the sporadic and o-grid features of most renewable energy sources, which is furthermore creating a high
demand for supercapacitors and lithium-based rechargeable batteries. Recently, due to graphene's unique properties of large surface area, high electric/thermal
conductivity, and excellent stability, there has been an ongoing trend to employ graphene materials to replace/reduce the usage of noble and rare metals in the
present energy conversion and energy storage devices with materials incurring lower costs and having a higher environmental benignity. For example, nitrogencontaining graphene sheets, instead of Pt, could be used as catalysts for the oxygen reduction reaction (ORR) in fuel cells. Moreover, specially designed graphene
structures also enable the fabrication of high-eciency miniaturized devices with high exibility and a light weight for use in wearable electronics, as shown in
several recent paradigm products. In this review, we summarize the recent progress in tailoring graphene structures for unconventional applications in energy
conversion and storage devices to meet the various requirements of modern devices and gadgets.
1. Introduction
Graphene, a two-dimensional (2D) form of carbon atoms with a
hexagonal lattice structure has attracted enormous research
interest since its rst use in 2004.1 As the rst true 2D material,
graphene has demonstrated many intriguing properties, such
as its intrinsically superior electrical conductivity, excellent
mechanical exibility, remarkable thermal conductivity, high
Key Laboratory of Cluster Science, Ministry of Education of China, Beijing Key

Laboratory of Photoelectronic/Electrophotonic Conversion Materials, School of
Chemistry, Beijing Institute of Technology, Beijing 100081, P. R. China. E-mail:
zhipan@bit.edu.cn; lqu@bit.edu.cn
State Key Laboratory of Advanced Functional Composite Materials, Aerospace

Research Institute of Materials and Processing Technology, Beijing 100076, P. R. China
surface area, etc.2,3 For instance, graphene shows an ambipolar

electric eld eect with high charge carrier mobilities of ca.
15 000 cm2 V1 s1 at room temperature,1 while suspended
graphene exhibits a strikingly high mobility approaching
200 000 cm2 V1 s1 at low temperatures.4 Optically, the light
absorption of a graphene monolayer is only 2.3% with a negligible reectance of <0.1%.5 Thermally, graphene is highly stable
and conductive (thermal conductivity of 30005000 W m1
K1).6 In addition, graphene has a large theoretical specic
surface area (ca. 2600 m2 g1)7,8 and a high chemical diusivity
of Li+ of 107 to 106 cm2 s1.9,10 Its unique structure and these
outstanding properties qualify graphene as one of the most
important materials for a wide range of applications in electronics,11,12 high-strength materials,13 chemical and biosensors,1416 catalysts,17 and various high-power-density/high-
These authors contribute equally to the work.
This journal is The Royal Society of Chemistry 2015
Energy Environ. Sci., 2015, 8, 3154 | 31
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Energy & Environmental Science
energy-density energy storage and conversion devices, such as

lithium ion batteries,1821 capacitors,2225 fuel cells,2633 and solar
cells.3437 Recently, ongoing eorts in the development of electronics has led to the emergence of various types of future
electronics in unconventional forms, including smart skins,
human friendly devices, and exible/stretchable circuitries and
energy devices.3853 These advanced devices can perform
sophisticated motions and/or deform into desirable shapes
under external stimuli of bending, stretching, compressing, and
twisting without sacricing their device performance and reliability, thus attracting broad interest in many diverse applications, ranging from robots to memory chips to integrations into
stretchable and wearable electronics.5461
In this review, we aim to summarize the very recent developments, contributed by us and other groups, of graphenebased systems in emerging and unconventional forms of energy
conversion and storage devices, mainly in supercapacitors,
lithium ion batteries, photovoltaic cells, and other power
generators. As graphene may play dierent roles in these
devices, the current work is accordingly structured to discuss its
property-motivated applications in each type of device. Finally,
future trends in designing and improving smart devices for
energy conversion and storage are also envisaged.
2. Tailored graphene systems for

energy storage
2.1
Graphene-based supercapacitors
With the recent boom in studies on powering electric vehicles

and portable electronics, electrochemical capacitors, also
known as supercapacitors, have attracted increasing attention,
due to their high power density, high rates of chargedischarge,
long cycling life, and their ability to complement secondary
batteries in reducing the cycling duty and, therefore, in
extending the battery life.6266 However, conventional supercapacitors are usually heavy and bulky, whereas there is
currently a strong demand for highly ecient, exible, miniaturized supercapacitor devices compatible with exible and
wearable electronic energy storage devices to cater for the power
requirements of modern gadgets.6771 Furthermore, the simple
and low-cost assembly of these exible and lightweight supercapacitors would enable the easy fabrication of capacitor arrays
via a convenient design and integration that is compatible with
the existing electronic industry, making them industrially viable
for powering a range of small/micro devices in dierent
scenarios.
2.1.1 Flexible and compressible graphene supercapacitors.
Graphene-assembled three-dimensional (3D) macroscopic
materials, such as foam and aerogel, have a tunable hierarchical
morphology with high surface areas and can form large-sized
monolithic materials. These properties provide a new design
platform, characterized by a light weight, high porosity, high
mechanical stability, and electrical conductivity, thus oering
great technological promise for supercapacitors.7274 Graphenebased porous bulk materials are usually fabricated by chemical
vapor deposition over a porous template,75,76 dip-coating on a
32 | Energy Environ. Sci., 2015, 8, 3154
Perspective
porous framework,77,78 or solgel reactions.7983 However, these

materials are usually brittle, and have low compression resilience ratios.75,81,84 Hence, skeletons of elastomeric polymers are
introduced to the graphene materials to enhance their exibility
and compressibility for practical applications. Choi et al.
demonstrated an all-solid-state exible supercapacitor by
assembling a lm electrode of Naon-functionalized reduced
graphene oxide (f-RGO) and solvent-cast Naon electrolyte
membranes as the electrolyte and separator (Fig. 1a).85 The
functionalized-RGO lm showed high exibility (Fig. 1b), and
the obtained supercapacitor was demonstrated to have a high
capacitance of 118.5 F g1 at 1 A g1 and a good performance
durability under 1000 cycles of bending and relaxing, owing to
the improved adhesion and the facilitated charge/ion transport
at the electrode/electrolyte interfaces (Fig. 1c and d). Alternatively, Cheng et al. developed a graphenecellulose paper (GCP)
membrane by simply ltering a suspension of graphene nanosheets (GNSs) through a slice of lter paper (Fig. 1e and f).86 Due
to the strong interactions between the abundant functional
groups on the cellulose bers (CFs) and the negatively charged
GNSs, GNSs uniformly covered the CFs to form an interconnected conductive framework (Fig. 1g), thereby combining
the porous and ductile nature of the cellulose lter paper with
the good electrical conductivity and electroactivity of GNSs. As a
result, the strain on the GCP membrane was 3% elongation,
about three times higher than that of the graphene paper
(0.76%). The excellent exibility and strength of the GCP
membrane enables the construction of more sophisticated
devices and, as shown in Fig. 1h, a exible interdigital supercapacitor was conveniently fabricated by solidifying two interdigital GCP electrodes on a polydimethylsiloxane (PDMS)
substrate with a polymer gel electrolyte. Since the interdigital
supercapacitor can be very thin, it is deemed ideal for powering
ultrathin electronic devices and micro-electromechanical
systems.
Polyaniline (PANI) and polypyrrole (PPy) are well-studied
conducting polymers that are widely used in energy conversions and storage systems, mostly because of their good
conductivity, easy-to-handle synthesis, the low cost of their
monomers, environmental stability, and the high redox pseudocapacitive charge storage associated with the multiple redox
states.73,8790 To further improve the electrochemical performance of the exible supercapacitor, PANI was included to
fully exploit the unique potential of graphene paper as a freestanding electrode by the in situ anodic electropolymerization
of aniline monomers on the graphene paper (Fig. 2ac).91 The
obtained electrode contained graphene/polyaniline composite
sheets as the building blocks, and showed a favorable tensile
strength of 12.6 MPa and a stable large electrochemical
capacitance of 233 F g1 over 1500 cycles. In another approach,
Chen et al. deployed a dipping and drying strategy to coat the
cellulose bers (CFs) of the paper with a thin and uniform
surface layer of graphene oxide (GO), and then assembled the
GO sheets into reduced graphene oxide (RGO) networks to
form a RGO/CF composite paper rich in micro-sized pores
(Fig. 2d).92 Such a composite structure could simultaneously
alleviate the agglomeration of RGO in the pores of the paper
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Fig. 1 (a) Image and schematic presentation of the all-solid-state exible supercapacitor. (b) Image of the f-RGO lms showing the exibility.
Images (c) and cyclic voltammograms (d) of the exible supercapacitor in the normal and bent states (reprinted with permission from ref. 85.
Copyright 2011 American Chemical Society). Illustrations of (e) fabrication of the GCP membrane and (f) structural evolution of GCP as the GNS
loading increases. (g) TEM image of a cellulose ber in a GCP membrane, showing GNSs anchored on the ber surface. (h) Image of a exible
interdigital GCP supercapacitor (reprinted with permission from ref. 86. Copyright 2011 Wiley-VCH).
and promote the diusion of ions in the electrolyte, fully

utilizing the interconnected CF network and the porous nature
of the paper (Fig. 2e). PANI can be further deposited onto the
RGO surface to achieve a high specic capacitance of 464 F g1.
The excellent exibility and conductivity of the PANI-RGO/CF
composite papers enable their direct application as electrodes
for exible supercapacitors with a narrow Pt wire as the current
collector, eliminating the need to resort to heavy and bulky
metallic foils or foams that are generally used as current
collectors in conventional supercapacitors (Fig. 2f). An allsolid-state supercapacitor based on the PANI-RGO/CF paper
attained 89% of the maximum capacity aer 1000 cycles and
lost only about 3.4% and 5% of its maximum capacity when
bent to 10% of its original length and folded by 180 (Fig. 2g),
respectively, proving its candidacy as a novel kind of exible
electrode for wearable and roll-up devices.
Recently, Yu and coworkers reported a convenient one-step

method to fabricate free-standing, low-density graphene paper
with good electrical conductivity, where PANI nanorod arrays
could electrochemically grow in situ to form exible graphene
PANI composite paper (Fig. 3a).93 The composite electrode was
highly exible (Fig. 3b), exhibiting an enhanced capacitive
performance of 763 F g1 at a discharge current of 1 A g1, and a
good cycling stability with 82% capacity retention aer 1000
cycles (Fig. 3c). The pronounced improvements both in the
specic capacitance and stability were ascribed to the unique
structure of the PANIgraphene composite. On the one hand,
the PANI nanorods render a high surface area, thus facilitating
ion diusion at the electrolyte/nanorod interface, and the high
conductivity of the graphene paper favors the quick transport of
electrons across the device. On the other hand, the vertically
aligned PANI nanorods make graphene paper a perfect base for
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(a) Illustration of the anodic electropolymerization of aniline on the graphene paper. Digital camera images of (b) two free-standing
graphene papers (30 mm 10 mm) and (c) a exible graphene paper (reprinted with permission from ref. 91. Copyright 2009 American Chemical
Society). (d) Schematic diagram of preparing PANI-RGO/CF composite paper. (e) Illustration of the nanostructure of the RGO/CF composite
paper. (f) Schematic diagram of a compact supercapacitor based on PANI-RGO/CF paper, where the inset is an optical image of four compact
supercapacitors lighting an LED. (g) Variation of the specic capacitance of the all-solid-state supercapacitor in dierent folding states, with the
inset showing an LED illuminated using four integrated supercapacitors in folding states (reprinted with permission from ref. 92. Copyright 2014
Wiley-VCH).
Fig. 2
relaxing the mechanical strain and deformation that occur

during the charge/discharge process, mitigating the swelling
and shrinking of the electrode materials against serious
collapses by the insertion/extraction process of the counter
ions.
Besides PANI, PPy was also introduced to enhance the
specic capacitance of the exible graphene electrodes. Lu et al.
proposed a novel exible graphene-polypyrrole/carbon nanotube (G-PPy/CNT) ternary composite lm through a owassembly method (Fig. 3d), where coaxial PPy/CNT nanocables
were uniformly sandwiched between the graphene sheets, so
that the mechanical stability of the PPy chains was signicantly
improved by the exible graphene sheets and the rigid CNT core
(Fig. 3e).94 The specic capacitance of the GN-PPy/CNT
composite reached 211 F g1 at a discharge current of 0.2 A g1,
and an excellent cycling stability of 5% capacity loss aer 5000
cycles. Additionally, He et al. reported a type of MnO2-coated
freestanding, exible, lightweight, and highly conductive threedimensional (3D) graphene network, on which a remarkably
high mass loading of 92.9% MnO2 was achieved.95 These hybrid
exible electrodes exhibit a high areal capacitance of 1.42 F
cm2 and a high specic capacitance of 130 F g1 (Fig. 3f), and
more importantly, they could be twisted or bent to a large extent

without suering any performance loss (Fig. 3g). To this extent,
we have designed a unique strategy for the in situ formation of
PPygraphene (PPyG) foam, and have demonstrated a highly
compression-tolerant graphene-based supercapacitor.29,96 The
PPyG matrix could sustain large-strain deformations (e.g., 3
50%) under manual compression and could recover most of the
material volume without structural fatigue within seconds.
Consequently, the fabricated deformation-tolerant supercapacitors showed no signicant change with a 50% applied
strain over 1000 measured cycles, highlighting the excellent
electrochemical stability of the compressible supercapacitor
based on PPygraphene foam electrodes.
Graphene nanoribbons (GNRs) elegantly combine the
structure and properties of carbon nanotubes (CNTs) and graphene sheets.9799 GNRs feature a at crystal surface that
extends into a one-dimensional structure with high length-towidth aspect ratios compared to exfoliated graphene sheets of
irregular sizes and shapes. Measurements and simulations on
individual GNRs have revealed fascinating electrical and
thermal properties.99,100 Tour et al. demonstrated the splitting of
vertically aligned CNTs with preservation of their vertical
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(a) Schematic illustrations of the formation process of graphenePANI paper. (b) Photograph of the exible graphenePANI paper (3 1.5
cm) with an electrochemical deposition time of 10 min. (c) Galvanostatic chargedischarge curves of graphene paper, PANI lm on the Pt
electrode, and graphenePANI paper at a current density of 1 A g1 (reprinted with permission from ref. 93. Copyright 2013 Royal Society of
Chemistry). (d) Schematic representation of the microstructure and energy storage characteristics of the GN-PPy/CNT lm. (e) TEM image of
GN-PPy/CNT (reprinted with permission from ref. 94. Copyright 2011 Elsevier B.V.). (f) Cyclic voltammograms of the exible supercapacitors at
scan rates of 50, 100, 200, 400, and 1000 mV s1. Inset shows the CVs of the exible supercapacitors with bending angles of 0 and 90 at a xed
scan rate of 10 mV s1. (g) Digital photographs showing the curled 3D graphene network and the exible supercapacitor in the bent state
(reprinted with permission from ref. 95. Copyright 2013 American Chemical Society).
Fig. 3
integrity to produce a mixture of split multi-walled carbon

nanotubes (MWNTs) and GNRs.101 The largely opened spaces
and the aligned vertical structure not only increased the eective surface area for the ions, but also provided facilely accessible paths for fast ion transport. The energy density and power
density are in the range of 5.29.4 W h kg1 and 1.1103 kW
kg1, respectively, superseding those of the prevailing electrochemical capacitor technology102 and some single-walled
carbon nanotube (SWNT) electrode materials.103 When a pristine vertically aligned CNT carpet was used as the active material, a maximum energy density of 3.1 W h kg1 was measured,
and the maximum power density was 35 kW kg1 at an energy
density of 0.95 W h kg1. Also, Baughman et al. fabricated long
and narrow GNRs that could be assembled and aligned into the
rst large GNR sheets, and then into macroscopic neat GNR
bers with high conductivity and good mechanical
performance.104 The gravimetric capacitance of the graphene

yarns was much higher than that of conventional twist-spun
MWNT yarns, reaching a maximum value of 99 F g1, which
compares favorably to a value of 20 F g1 obtained by the
starting MWNT yarns. This novel conversion process was scalable and could be employed for the industrial production of
GNR yarns that would be useful as woven electrodes for exible
supercapacitors.
2.1.2 Graphene micro-supercapacitors. The recent soaring
demand in portable electronics has triggered the urgent need to
miniaturize energy-storage units. In 2012, El-Kady et al.
employed a standard LightScribe DVD optical drive to perform
the direct laser reduction of graphite oxide lms to laser-scribed
graphene (LSG),105 an approach that eectively prevents the
aggregation of graphene sheets and enables the LSG to feature
an open network structure with a large specic surface area of
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Fig. 4 (a) Schematic illustration of the fabrication of laser-scribed graphene-based electrochemical capacitors (reprinted with permission from
ref. 105. Copyright 2012 the American Association for the Advancement of Science). (b) Schematic diagram showing the fabrication process for
laser-scribed graphene micro-supercapacitors. (c) Demonstration of more than 100 micro-devices produced on a single run. (d) A digital
photograph of the laser-scribed micro-devices with 4, 8, and 16 interdigitated electrodes (reprinted with permission from ref. 106. Copyright
2013 Nature Publishing Group).
1520 m2 g1 and a high electrical conductivity of 1738 S m1

(Fig. 4a). Superthin symmetrical capacitors with a total thickness of less than 100 mm could be achieved by the assembly of
two identical LSG electrodes, qualifying them as potential
power systems for micro-device applications. The same group
further reported the direct fabrication of interdigitated graphene micro-supercapacitors by etching a computer-designed
circuit onto the lm (Fig. 4b).106 In contrast to conventional
micro-fabrication methods, this mask-free method is able to
work under ambient conditions to facilely build supercapacitor
arrays with a high areal density, where 112 micro-supercapacitors can be produced on a DVD disc in a single run
(Fig. 4c). As the LightScribe has a lateral spatial resolution of
20 microns, micro-devices with dierent numbers of interdigitated electrodes could be easily fabricated, commensurate
with the working domain of the conventional micro-fabrication
techniques in the order of 100 mm. The LSG produced in this
method had an even higher conductivity of 2350 S m1, and the
micro-capacitors with 16 interdigitated microelectrodes
demonstrated a power density of 200 W cm3, representing

one of the highest values for any supercapacitor ever reported.
Again, the LSG supercapacitors were highly stable, and maintained 96% of their initial performance aer 10 000 consecutive
chargedischarge cycles.
Following a similar procedure, Ajayan and coworkers
demonstrated the application of hydrated GO as an ionic
conductor as well as an electrical insulator, making it suitable to
work simultaneously as a viable electrolyte and electrode separator in the micro-supercapacitor.107 In-plane and sandwiched
supercapacitors, with dierent geometries in the RGO-GO-RGO
conguration, were built by layer writing and patterning
without the use of any external electrolyte (Fig. 5a). The device
with the in-plane concentric circular pattern had the highest
specic capacitance of about 0.51 mF cm2 and a power density
of 1.7 W cm3 (Fig. 5b), while scanning electron microscopy
(SEM) revealed the porous nature of the laser-reduced RGO,
which was due to gases released from decomposing the functional groups and the water vapor under localized laser heating
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(a) Schematics of the laser-patterning of free-standing hydrated GO lms to fabricate RGO-GO-RGO devices with in-plane and sandwich
geometries. The bottom row shows images of the patterned lms. (b) Image of an array of concentric circular patterns fabricated on a freestanding hydrated GO lm. (c) SEM image of the interface between GO and RGO (scale bar, 100 mm), with yellow arrows indicating a long-range
pseudo-ordered structure generated by laser-beam scanning (reprinted with permission from ref. 107. Copyright 2011 Nature Publishing Group).
(d) Fabrication of RGO/PANI microelectrodes. (e) SEM image of PANI nanorods on the RGO pattern (reprinted with permission from ref. 108.
Copyright 2012 Wiley-VCH).
Fig. 5
(Fig. 5c). The performance of the micro-supercapacitor could be

signicantly improved if an external electrolyte, even a drop of
deionized water, was used to improve the ion transport.
Nevertheless, the hydrated GO lms represented a completely
dierent type of porous solid electrolyte, and capable of making
the current micro-capacitors potentially much lighter and more
compact. To further improve the capacitive performance of the
micro-supercapacitor, Xue et al. adopted a solution-based
method to electrochemically grow a uniform layer of ordered
PANI nanorod arrays vertically on patterned RGO thin lms
(Fig. 5d).108 The PANI nanorods were shown to be densely
packed on the surface of RGO, with a diameter of about 20 nm
and a height of around 100 nm to 200 nm, leading to a synergistic eect in supercapacitive storage that decreased the ionic
diusion resistance and the charge-transfer resistance. The allsolid-state RGO/PANI micro-supercapacitor exhibited a specic
capacitance as high as 970 F g1 at a discharge current density
of 2.5 A g1, with 90% performance retention aer 1700
consecutive cycles, making it ideal for powering exible miniaturized electronic devices.
2.1.3 Graphene ber supercapacitors. The recent successful demonstration of the assembly of 2D graphene sheets into
macroscopic graphene bers (GFs) has now made the
construction of GF supercapacitors possible.109111 We have thus
designed a series of unique hierarchical structures to fabricate
dierent GF supercapacitors. A sheath of a 3D porous graphene
framework was deposited onto a GF core to form an all graphene core-sheath ber supercapacitor (Fig. 6a), where the high
electronic conduction of the core graphene ber and the highly

exposed surface of the 3D graphene network were well
combined (Fig. 6b).112 The assembled ber supercapacitor was
highly exible (Fig. 6c) and could be conveniently woven into a
textile for wearable electronics (Fig. 6d). In a further eort, an
all-in-one ber graphene supercapacitor was fabricated by
rationally integrating the two electrodes and the separator on a
single GF, without involving any extra bonding agent or
assembly process (Fig. 6e).113 The controllable laser reduction of
the GO ber could facilely realize a RGO-GO-RGO conguration
(Fig. 6f), where the RGO parts had an approximate width of 1/4
diameter of the ber along the surface, acting as the active
electrode materials and current collectors, and the remaining
GO part between the RGO layers worked as the separator
(Fig. 6g). This all-in-one ber supercapacitor inherited the
mechanical exibility of GF and could be deliberately bent to
dierent radii of curvature, while maintaining its original high
capacitance (Fig. 6h).
In a recent work, Gao and coworkers presented a coaxial wetspinning assembly strategy to prepare sodium carboxymethyl
cellulose (CMC) coated graphene core-sheath bers (Fig. 7a
c).114 As CMC is an ionic conducting but electrically insulating
polyelectrolyte, two individual 40 cm long coaxial CMC-coated
graphene coresheath bers could be directly employed to
interweave a cloth supercapacitor (Fig. 7d and e). The cloth
supercapacitor demonstrated a capacitance of 28 mF at a
current of 10 mA, and the corresponding chargedischarge
curves remained undistorted under the bending angle of 180
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Fig. 6 (a) Schematic illustration of a graphene coresheath ber supercapacitor with a polyelectrolyte. The lower part shows the advantage of
the graphene coresheath ber in charge collection and ion diusion. (b) Cross-section SEM image showing the core GF surrounded by standing
graphene sheets. Images of the ber supercapacitor (c) in the bending state and (d) embedded in the textile (reprinted with permission from ref.
112. Copyright 2013 Wiley-VCH). (e) Representation of the structure of the all-in-one ber supercapacitor. (f) Schematic of the laser reduction of
GO ber for the formation of RGO-GO-RGO ber. (g) Optical image of the RGO-GO-RGO ber. (h) Scheme of the bent state of the RGO-GO-RGO
ber capacitor with a certain radius of curvature (R1 to R3), where R0 stands for the initial state (reprinted with permission from ref. 113. Copyright
2014 Royal Society of Chemistry).
along all three directions (Fig. 7f), conrming its excellent

tolerance to arbitrary bending actions. Also, by wet-spinning, Yu
et al. described the scalable synthesis of hierarchically structured carbon microbers of a single-walled carbon nanotube
(SWNT)/nitrogen-doped RGO sheet interconnected network
architecture (Fig. 7g and h).115 As the RGO renders a large
surface area for ion adsorption and the aligned SWNT network
reduces the RGO interlayer resistance, the as-prepared dry
hybrid bers showed a good tensile strength of 84 MPa to 165
MPa, excellent electrical conductivity of 20 S cm1 to 102 S
cm1, and a large specic surface area up to 396 m2 g1.
Consequently, micro-supercapacitors fabricated with these
bers featured volumetric energy densities of up to 300 F
cm3, with no loss in the cyclic stability or rate capability. The
hybrid bers were robust enough to be assembled in parallel by
incorporating up to 40 bers, and the overall capacitance of the
array followed a linear increase with the number of bers
(Fig. 7i), showing the good scalability of micro-supercapacitors
based on the hybrid ber.
We also reported a simple and facile method for continuously
producing graphene/PPy bers via a direct wet spinning
strategy.116 A roll of initially produced GO/PPy ber with a length
of 0.5 m was collected in FeCl3 solution within only 5 s and the
subsequent HI treatment yielded graphene/PPy bers, with
diameters ranging from 15 to 80 mm that could be tuned by
controlling the diameter of the needle of a single-capillary spinneret and the concentration of GO. The graphene/PPy bers had a
tensile strength of up to 80 MPa and thus led to highly exible allsolid-state ber supercapacitors with high electrochemical
capacitances of up to 100 mF cm2 under repetitive deformations.
In other attempts, we designed other interesting hybrid structures

toward exible ber capacitor applications. One-dimensional (1D)
macroscopic CNT/graphene hybrids with a large surface area and
high exibility were prepared by directly growing CNTs along
graphene bers with embedded Fe3O4 nanoparticles as catalysts
for chemical vapor deposition (CVD) of the nanotubes (Fig. 8a).117
The as-formed textile of the CNT/graphene bers was still very
exible (Fig. 8b) and the supercapacitor using the CNT/graphene
ber textiles as electrodes could light a commercial LED either in
the at or bended state, though the charge voltage was only 0.6 V
(Fig. 8ce). Meanwhile, a novel hybrid ber of MnO2-modied
graphene on GF (MnO2/graphene/GF) was developed by forming
the core-sheath graphene on GF rst and then depositing MnO2
nanostructures.118 The SEM images clearly show the morphology
change from the pristine GF (Fig. 8f) to the coating of the interpenetrating networks of graphene sheets on the GF (Fig. 8g), and
nally to the formation of a densely deposited layer of MnO2 along
the whole graphene/GF scaold (Fig. 8h). Due to the incorporation of the electrochemically active MnO2 component, the
symmetrical solid supercapacitors of two intertwined MnO2/graphene/GFs showed an area-specic capacitance of 9.1 mF cm2 to
9.6 mF cm2, far exceeding that of all graphene core-sheath ber
supercapacitors (ca. 1.2 mF cm2 to 1.7 mF cm2). Additionally,
the deposition of MnO2 did not compromise the mechanical
property of the ber supercapacitor, and the performance of the
MnO2/graphene/GF ber capacitor remained unchanged during
1000 repetitive straight-bending cycles, showing the exceptional
tolerance of the MnO2/graphene/GF supercapacitor to mechanical
deformations and its great potential to be woven into a textile for a
range of wearable electronics (Table 1).
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Fig. 7 (a) Schematic showing the coaxial spinning process. (b) A single intact wet CMC-coated graphene core-sheath ber. (c) Polarized-light
optical microscopy image of the wet ber, indicating the core-sheath structure and the well-aligned GO sheets in the core part. (d) Cloth woven
by two individual coaxial bers. (e) Supercapacitor device based on the cloth fabricated by two coaxial bers. (f) Chargedischarge curves of the
cloth supercapacitor, where 1 represents the initial cloth supercapacitor without bending, and 2, 3, and 4 show the cloth supercapacitor with
bending angles of 180 along three directions. Scale bars are 5 mm (b) and 100 mm (c) (reprinted with permission from ref. 114. Copyright 2014
Nature Publishing Group). (g) Synthesis of the carbon hybrid microbers. (h) Image of the as-prepared bers collected in water.(i) Schematic and
equivalent circuit for the scalable integration of multiple bers in micro-supercapacitors in parallel (left) and the relation between the total device
capacitance and number of bers integrated (right) (reprinted with permission from ref. 115. Copyright 2014 Nature Publishing Group).
2.2 Graphene-based exible and unconventional lithium ion

batteries
Lithium ion batteries have emerged as a main power source for
portable electronic devices, due to their high energy density,
large output voltage, appreciable life, and environmentally
benign operation.119,120 To match the rapid development of
exible electronics, the current trend in portable battery
research is focused on making lighter, thinner, and smaller
exible batteries to drive various bendable, deformable, and
wearable electronic devices. As graphene-based exible lithium
ion batteries have been well summarized lately,52,61,121 we hereby
focus on the recent progress in this eld.
As graphene paper is mechanically strong and electrically
conductive, it is deemed to be an ideal binder-free electrode
material in lithium ion batteries. Liu et al. mechanically pressed
a graphene aerogel to prepare a unique graphene paper with a
folded structure of graphene sheets (Fig. 9a and b).122 The graphene paper was free-standing and very exible (Fig. 9c), with a
high electronic conductivity of 18 S cm1. Impressively, the
folded structure of the graphene sheets with fewer layers
provided more lithium insertion active sites with an easy access
of the electrolyte, leading to improved coulombic eciencies
of up to 98% and a reversible capacity of 568 mA h g1 at
100 mA g1 aer 100 chargedischarge cycles (Fig. 9d). In

another approach, Cheng and coworkers developed a graphene
foam as a 3D conductive network for simultaneously collecting
electrons and transporting ions, and based on this platform,
they demonstrated thin, lightweight, and a exible LiFePO4/
graphene foam cathode and Li4Ti5O12/graphene foam anode
capable of charging and discharging at rates of up to 200 C
(Fig. 9e).123 The total thickness of the exible full battery was
less than 800 mm, and it was highly tolerant to the mechanical
deformations of repeatedly bending to a radius of <5 mm
(Fig. 9f). The exible battery showed an excellent stability in a
cyclic bending test, retaining 97% and 95% of its original
capacity in the rst 15 cycles under the at state and the
following 15 cycles under the bent state with a bend radius of
5 mm (Fig. 9g).
To obtain electrode materials with a high capacity, Wang
et al. designed a ternary self-assembly of metal oxides, surfactants, and graphene to synthesize ordered nanocomposites
composed of metal oxide and graphene stacks that could be
used as an additive-free and binder-free electrode in the
battery.124 Anionic surfactants were rst absorbed on the surface
of graphene stacks (Fig. 10a), and then they functioned as the
fundamental building blocks for binding to the metal cations,
thereby forming an ordered nanocomposite (Fig. 10b). Finally,
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Fig. 8 (a) Fabrication scheme of CNT/graphene bers. (b) Image of CNT/graphene ber textile, and the inset showing the bent state. (c)
Schematic illustration of a exible supercapacitor using the textile of CNT/G bers as electrodes. Images of the fabricated textile supercapacitor
in the (d) at and (e) bending state, respectively, where the insets show a light-emitting-diode (LED) lighted by the textile supercapacitor in the
corresponding state. The scale bars 0.5, 1, and 1 cm for (b), (d), and (e), respectively (reprinted with permission from ref. 117. Copyright 2014 Royal
Society of Chemistry). SEM images of (f) GF, (g) graphene/GF, and (h) MnO2/graphene/GF. (i) The stability of the MnO2/graphene/GF ber
supercapacitor undergoing 1000 repetitive straight-bending cycles (reprinted with permission from ref. 118. Copyright 2013 Elsevier B.V.).
alternating layers of graphene stacks and metal oxide nanocrystals could assemble into layered nanostructures aer crystallization and the removal of surfactant (Fig. 10c), while
hexagonal mesoporous metal oxidegraphene nanocomposites
could also be obtained by the direct assembly of metal oxides
with the surfactant into a hexagonal mesophase on the surface
of the stacked graphene (Fig. 10d). The layered metal oxide
graphene nanocomposites featured as free-standing exible
lms of 5 to 20 mm thickness (Fig. 10e). The SnO2graphene
nanocomposite electrodes showed a steady specic capacity of
625 mA h g1 aer 10 cycles at a current density of 0.01 A g1
and 760 mA h g1 at a current density of 0.008 A g1 over 100
cycles (Fig. 10f and g), conrming the good adhesion between
SnO2 and the sandwiched graphene layers resistant to the phase
transformation and volume change upon lithiation/delithiation. In another attempt to boost the capacity of the battery,
Mukherjee et al. found that defects in the graphene lattice could
work as seed points to trap lithium metal within the interior of a
thermally reduced, free-standing porous graphene network
(PGN) (Fig. 10h).125 The PGN eectively prevented dendritic
growth and exhibited exceptional specic capacities higher
than 850 mA h g1, also with an excellent reversibility and
coulombic eciencies above 99% in 1000 chargedischarge
cycles (Fig. 10i). A full-cell composed of PGN anodes and lithiated PGN cathodes could be easily fabricated from a large-scale
GO paper with an area of 30 cm2 in a similar process
compatible with the conventional Li-ion battery, demonstrating
the versatility and scalability of the PGNs in developing lowweight, all-carbon lithium batteries.
We also prepared a hierarchical graphene-on-graphene
hybrid structure as a exible, binder-free, all-graphene anode of
the lithium ion battery.126 3D graphene (3DG) interconnected
frameworks were homogenously connected with the few-layer
graphene lm, where the pore-rich 3D graphene networks
promoted the Li+ diusion and the few-layer graphene worked
as a non-metallic current collector to provide a potent scaold
to support the 3DG and extract the charge from/to the 3D graphene networks during the charge and discharge processes
(Fig. 11a and b). Compared to the metallic current collector, the
few-layer graphene possesses advantageous characteristics of
light weight, chemical stability, excellent electrical conductivity
and tolerance to corrosion and oxidation. As a result, the hybrid
structure showed an excellent specic capacity of 770 mA h
g1 with an energy density of 388 W h kg1, superseding those
of commercial graphitic anodes.
Very recently, Peng and coworkers demonstrated safe wireshaped lithium-ion batteries with low weight, high exibility,
and high energy density.127 Li4Ti5O12 (LTO) and LiMn2O4 (LMO)
nanoparticles were well-incorporated into two aligned MCNT
yarns that functioned as the anode and cathode, respectively
(Fig. 11d). A thin layer of GO coating was applied on the surface
of the anode to stabilize the structure with an improved capacity
retention. The aligned nanostructure and high electrical
conductivity of the MCNT yarns made the current collector and
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Table 1
Comparison of the materials, preparation methods, specic performance, and characteristics of the reported supercapacitors
Samples
Preparation methods
Performance
Characteristics
Ref.
Naon-functionalized RGO
lm
Graphene-cellulose paper
Filtration and hydrazine

reduction
Filtration
Capacitance: 118.5 F g1 at

1 A g1
Capacitance: 81 mF cm2
All-solid-state; exible
85
86
Graphene/polyaniline
composite sheets
Filtration and anodic

electropolymerization
PANI-RGO/cellulose bers
GraphenePANI composite
paper
G-PPy/CNT composite
Dipping and drying

HI treatment and in situ
electrochemically growth
Flow-assembly method
MnO2-coated 3D graphene
network
Electrodeposition
PPygraphene foam
Hydrothermal process and

electrodeposition
Laser-scribed graphene
Laser reduction
Interdigitated graphene
Etching circuit onto a lm
Gravimetric capacitance: 233

F g1; volumetric
capacitance: 135 F cm3
Capacitance: 464 F g1
Capacitance: 763 F g1 at a
1 A g1
Capacitance: 211 F g1 at
0.2 A g1
Gravimetric capacitance:
130 F g1; volumetric
capacitance: 1.42 F cm3
Gravimetric capacitance:
350 F g1; volumetric
capacitance: 14 F cm3
Capacitance: 3.67 mF cm2
at 1A/gLSG in 1.0 M H3PO4;
4.04 mF cm2 in 1.0 M
H2SO4
Power density: 200 W cm3
Binder-free; free-standing;
exible
Free-standing; exible
RGO-GO-RGO patterns
Layer writing and patterning
PANI nanorod arrays on

patterned RGO lms
G@3D G core-sheath ber
Electrochemically grow
RGO-GO-RGO ber
CMC coated graphene coresheath bers

SWNT/N-doped RGO sheet
network
Graphene/PPy bers
CNT/graphene hybrid
MnO2/graphene/GF

electrodeposition
Laser reduction
Wet-spinning assembly and

HI treatment
Wet-spinning and
hydrothermal treatment
Wet-spinning and HI
treatment
Hydrothermal process
chemical vapor deposition
electrodeposition
Capacitance: 0.51 mF cm2;

power density: 1.7 W cm3
Capacitance: 970 F g1 at 2.5
A g1
Capacitance: 1.21.7 mF
cm2
Capacitance: 1.2 mF cm2 at
80 mA cm2; 0.45 mF cm2
at 200 mA cm2
Capacitance: 28 mF at 10 mA
Volumetric energy densities:
300 F cm3
Capacitance: 100 mF cm2 at
0.24 mA cm2
Capacitance: 0.74 mF cm2
at 10 mA cm2
Capacitance: 9.19.6 mF
cm2
binders in conventional lithium ion batteries redundant, and

therefore, the wire-shaped battery could be conveniently woven
into various exible structures, such as electronic textiles
(Fig. 11e and f). The wire-shaped battery could be placed around
an elastic substrate into a spring structure to give a very elastic
device, where the elastic battery was able to uninterruptedly
illuminate an LED whilst it was continuously stretched by 100%
(Fig. 11g). The stretchable lithium ion battery only suered a
less-than-10% decrease in its specic capacity when its length
was doubled, and it retained over 80% of its capacity performance aer 200 cycles of stretching by 100% (Fig. 11h), due to
the unique spring-like structure and the excellent elasticity of
the substrate and gel electrolyte, thereby, qualifying these
materials as highly desirable for diverse applications in wearable and portable electronics (Table 2).
91
Flexible; wearable; rolling-up

Low-density; free-standing;
exible
Uniformly sandwiched;
exible
Freestanding; exible;
lightweight
92
93
Lightweight; compressible
96
All solid-state; exibility;

lightweight; microdevice
105
High areal density;

superthin
In-plane; sandwiched;
lightweight
All-solid-state; exible;
miniaturized
Flexible; wearable
106
109
All-in-one; exible
110
Cloth supercapacitor;
exible; wearable
Tensile; exible
111
All-solid-state; tensile;
exible
Flexible; wearable
All-solid-state; exible;
wearable
94
95
107
108
112
113
114
115
3. Tailored graphene systems for

power generation
3.1
Graphene-based photovoltaic devices
Due to the high transparency and in-plane conductivity of

single-layer graphene and the tunable catalytic activity of doped
graphene frameworks, tailored graphene structures have been
intensively studied as transparent conducting lms for charge
collection29,128,129 and as catalytic counter electrodes (CEs)130132
in a range of photovoltaic devices. Besides these applications,
Guo et al. demonstrated that graphene could eectively work as
the electron acceptor in CdS quantum dot (QD) solar cells.133
The nanoscale layer-by-layer assembly of graphene and CdS
(Fig. 12a) seemed to alleviate the inherent problems of charge
collection and transport in QD solar cells. Energy-level diagrams
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Fig. 9 (a) Illustration of the formation process of graphene paper. Digital images of (b) a graphene aerogel and (c) graphene paper. (d) Cycle
performance of the graphene paper as a lithium ion battery anode at dierent current densities (reprinted with permission from ref. 122.
Copyright 2012 Wiley-VCH). (e) Schematic of a free-standing exible battery containing a 3D interconnected graphene foam anode and cathode.
(f) Photograph of a bent battery encapsulated by PDMS, showing its good exibility. (g) Cyclic performance of the battery under at and bent
states (reprinted with permission from ref. 123. Copyright 2012 National Academy of Sciences).
indicated that, compared to that of SWNTs, the work function of

graphene is better positioned for a more balanced charge
transfer from the QDs and the following electron collection by
the collection electrode (Fig. 12b). Meanwhile, Liu et al. reported the application of solution-processable isocyanate-functionalized graphene as the electron acceptor in the bulk
heterojunction (BHJ) solar cell.134 In a dierent attempt, we
studied the viability of using electrochemically synthesized
graphene quantum dots (GQDs) as a better electron acceptor
(Fig. 12c and d).135 The large surface areas of GQDs can conveniently aord ample interfaces for exciton dissociation, while
the high electron mobility of GQDs could be expected to
increase the conductivity of the active layer and greatly facilitate
the charge transport through the active layer. Without any
device optimization in this primary study, a power conversion
eciency of 1.28% was achieved. Later, aniline-functionalized
GQDs (ANI-GQDs) were further employed as the electron
acceptor in poly(3-hexylthiophene) (P3HT) based on an optimized cell structure, where P3HT/ANI-GQD lms showed a
heterogeneous nanoscale phase separation commensurate with
the diusion length of excitons (10 nm), which leads to an
enhanced performance.136
Additionally, graphene can also function actively as the
exciton generator in sensitized solar cells. Li and coworkers
synthesized a series of well-dened GQDs with substituted
phenyl groups functionalized at the edge of the graphene
core.137 The introduction of multiple 1,3,5-trialkyl-substituted
phenyl moieties eectively shields the GQDs from one another
by wrapping them three-dimensionally, thus separating the
GQDs in all three dimensions and reducing their tendency to
form insoluble aggregates (Fig. 12eg).138 By this strategy, GQDs
with a 168-carbon core were highly soluble in various common

organic solvents, with solubilities up to 30 mg mL1 at room
temperature and an absorbance maximum at 591 nm with a
molar extinction coecient of 1.0 105 M1 cm1, about an
order of magnitude larger than those of the widely used sensitizers based on metal complexes (Fig. 12h). Unfortunately, the
lack of any anchoring group led to a low anity of the GQDs to
the TiO2 lm in a pure physical adsorption, and consequently
resulted in a slightly colored lm despite its long time sensitization and a limited photocurrent in mA cm2. Nevertheless, it
was found that these defect-free, colloidal GQDs featured an
exceptionally slow hot-carrier cooling process, where the lifetimes of the hot-carriers were about 2 orders of magnitude
longer than those in bulk graphene materials.139 As the hotcarriers survived for up to hundreds of picoseconds, intersystem crossing could eciently compete with internal
conversion, thereby, potentially increasing the access to triplet
states with notably longer lifetimes and triplet excitons with
larger diusion lengths.140 Recently, the dynamics of the hotcarrier injection and subsequent charge recombination was
studied by monitoring the photoexcitation of a similar GQD
molecule of a 132-C graphene core anchored to the TiO2 (110)
surface via a carboxylic acid anchoring group (Fig. 12i).141 The
ultrafast electron injection from GQDs to the TiO2 conduction
band took place in less than 15 fs, followed by charge recombination in a fast channel (80130 fs) associated with the
instantaneous recombination of the bound electronhole pair
right at the interface and a slow one (0.52 ps), where the hot
electrons underwent a process of injection, cooling down,
driing back to the interface, and ultimately recombining.
Besides the excitation photon energy, the slow channel was also
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Fig. 10 (ad) The ternary self-assembly approach to ordered metal oxidegraphene composites. (a) Graphene stacks with surfactant hemimicelles. (b) The transition into the lamella mesophase toward the formation of metal-oxidegraphene nanocomposites. (c) Metal oxide
graphene layered nanocomposites. (d) Self-assembled metal oxide precursor with nonionic surfactants on graphene stacks. (e) Side-view SEM
image of a self-assembled SnO2graphene nanocomposite, where the inset shows a disk-like 3 cm diameter SnO2graphene nanocomposite
electrode on the left and a folded electrode on the right. (f) A Li-ion battery conguration directly using the metal oxidegraphene nanocomposite. (g) Specic capacity of SnO2 as a function of the chargedischarge cycles in the SnO2graphene nanocomposite electrode at a
current density of 0.01 A g1 (top) and at dierent chargedischarge current densities (bottom) (reprinted with permission from ref. 124.
Copyright 2010 American Chemical Society). (h) Reduction of GO paper to produce a free-standing PGN, tested as an anode material in lithium
ion batteries. Scale bars are 2 mm (left) and 200 nm (right). (i) Capacity and coulombic eciency versus cycle index of the PGN anode. (j)
Macroscopic pouch cell powering an LED device, where the inset is an image of a large-scale GO paper (reprinted with permission from ref. 125.
Copyright 2014 Nature Publishing Group).
strongly dependent on the sample temperature, whereby it

slowed down with increasing temperatures, presumably due to
the decreased mobility of the electron polarons (Fig. 12j). Based
on these results, it was proposed that graphene absorbers are
needed to be at least hundreds of nanometers to micrometers in
size to ensure multiple excitations in each molecule under
normal solar radiation, which necessitates more eort to be
devoted to judiciously design the corresponding graphene
structure and device conguration for harvesting hot-carriers in
a real device.
For exible electronics oriented applications, Peng and
coworkers developed a range of exible graphene-based bers
as ecient CEs in wire-shaped dye-sensitized solar cells. A CNT
ber was rst treated with an oxidizing solution, and then
reduced to form a core-sheath structure with the surface
covered by graphene nanoribbons and other carbonaceous
residues (Fig. 13a).142 As shown in the SEM image in Fig. 13b,
the dense CNT core was clearly visible and the carbonaceous
sheath was postulated to be 20 nm in thickness. Such a coresheath structure integrated the high tensile strength and electrical conductivity of aligned CNTs with the high electrocatalytic
activity of the edge-rich sheath materials, and as a result, wire-
shaped dye-sensitized solar cells with energy conversion eciencies of up to 6.83% could be achieved (Fig. 13c). In another
work, they spun graphene into exible bers and electrodeposited platinum nanoparticles on to them to serve as the CE
(Fig. 13d).143 Cyclic voltammetry results showed that with
increased Pt loadings up to 7.1%, graphene/Pt composite bers
produced higher current densities and lower peak-to-peak
voltage separations (VPP), which are indicative of the improved
catalytic activities for CEs (Fig. 13e). The JV characteristics
revealed that the open-circuit voltage (Voc) remained nearly the
same at 0.73 V, while the short-circuit current density (Jsc) and
the ll factor (FF) improved from 12.67 mA cm2 to 17.11 mA
cm2 and from 0.42 to 0.67, respectively as the Pt content
increased from 0% to 7.1%, eventually reaching a maximized
photo-to-electricity conversion eciency of 8.41% at a Pt
loading of 7.1% (Fig. 13f). Recently, the same group further
synthesized a new range of graphene/CNT composite bers with
graphene sheets incorporated among neighboring CNTs to
work as eective bridges to facilitate the charge transport,
because of the strong pp interactions between CNT and graphene sheet (Fig. 13g).144 With the deposition of Pt nanoparticles, a wired dye-sensitized solar cell with the graphene/
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Fig. 11 (a) Schematic procedure and mechanism for the formation of a 3DG/few-layer graphene hybrid structure. (b) Image of the 3DG/fewlayer graphene with good exibility. Scale bar is 1 cm. (c) Cycling test of the 3DG/few-layer graphene electrode at a current density of 50 mA g1.
(d) Structure of the exible wire-shaped lithium-ion battery with the aligned MWNT/LTO anode and MWNT/LMO cathode. (e and f) Wire-shaped
batteries woven into exible textiles. (g) Images of an elastic battery used to power a light-emitting diode at increasing strains, with stretching and
releasing process illustrated. (h) Dependence of the specic capacity on the strain (reprinted with permission from ref. 127. Copyright 2014 WileyVCH).
CNT/Pt composite ber CE showed conversion eciencies of

8.36% 0.10%, which compares favorably to those of its
counterpart with a bare Pt wire (6.66% 0.15%). Furthermore,
the wire-shaped solar cells could be facilely integrated into a
photovoltaic textile, with stable and high energy conversion
eciencies under bending (Fig. 13h and i). Additionally,
symmetrical wire-shaped supercapacitors of two intertwined
graphene oxide/CNT composite bers showed specic capacitances up to ca. 31.50 F g1 (4.97 mF cm2 or 27.1 mF cm1) with
no notable decay in capacitance aer 5000 chargedischarge
cycles, validating the concept of using these miniaturized wireshaped devices in exible and portable electronic facilities
(Table 3).
3.2 Graphene-based nanogenerators harvesting mechanical
energy
When graphene is seamlessly coupled with a layer of piezoelectric material, the device is able to harvest acoustic or impact
energy through the deformation-induced piezoelectric eect.

Earlier studies on graphene-based piezoelectric nanogenerators
involved sandwiching a layer of ZnO nanostructures145,146 or
Pb(ZrxTi1x)O3 (PZT) ribbons147 between the upper and lower
graphene layers, as well summarized in a recent review,148 while
recent research has focused on developing exible, lightweight
and/or transparent nanogenerators. For this purpose, Lee et al.
developed a stretchable transparent piezoelectric nanogenerator using a polymeric piezoelectric material of poly(vinylidene uoride triuoroethylene) [P(VDF-TrFE)] sandwiched between mobility-modied graphene electrodes grown
by chemical vapor deposition (CVD) (Fig. 14a).149 With excellent
mechanical properties, the PDMS-supported, completely exible device exhibited high sensitivity to any external mechanical
energy, such as a small bending or even exposure to sound. The
measured peak to peak output voltage varied from 50 mV to
600 mV when the exposure of the device to sound changed from
82 decibels (dB) to 110 dB at 100 Hz, a response signicantly
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Table 2
Comparison of the materials, preparation methods, specic performance, and characteristics of the reported lithium ion batteries
Samples
Preparation methods
Performance
Characteristics
Ref.
Graphene paper
Pressed a graphene aerogel

Hydrothermal deposition
Binder-free free-standing;
exible
Thin; lightweight; exible
122
LiFePO4/graphene and
Li4Ti5O12/graphene
SnO2graphene
nanocomposite
Porous graphene network
Filtration and rapid heating
Graphene-on-graphene
hybrid lm
Chemical vapor deposition

and spontaneous reduction
of GO
rolled method
Capacitance: 568 mA h g1 at

100 mA g1
Capacitance: 170 mA h g1 and
164 mA h g1 at 744 mA g1
10 mA g1; 760 mA h g1 at
8 mA g1
372 mA g1; energy density:
547 W h kg1
372 mA g1; energy density:
388 W h kg1
Energy densities: 27 W h kg1;
power densities: 880 W kg1
GO-coated LTO and LMO/

MWNT yarns
Self-assembly
123
Additive-free; binder-free;
exible
124
Free-standing; binder-free
125
All-graphene; exible;
binder-free
126
Stretchable; exible;
wearable; low weight
127
Fig. 12 (a) Fabrication of the layered graphene/QDs on the indium tin oxide (ITO) glass. (b) Energy-level diagram of the bilayer system (reprinted
with permission from ref. 133. Copyright 2010 Wiley-VCH). (c) TEM image of the as-prepared GQDs. (d) Schematic (left) and energy levels (right)
of the BHJ solar cell based on GQDs (reprinted with permission from ref. 135. Copyright 2011 Wiley-VCH). (e) The shielding of graphenes (blue)
from one another in three dimensions by covalently attaching 1,3,5-trialkyl phenyl moieties. (f) Molecular structure of GQD containing the
graphene moiety with 168 conjugated carbon atoms (blue) and the three solubilizing groups (black). (g) A theoretically energy-minimized
conguration of the GQD, showing the three-dimensional enclosure of the graphene core by the alkyl chains (black). (h) Absorption spectrum of
the GQD in dichloromethane (reprinted with permission from ref. 138. Copyright 2010 American Chemical Society). (i) Structure of the GQD
molecule of a 132-C graphene core and functionalized with two 2,4,6-trialkylsubstituted phenyl groups and a carboxylic acid group. (j) Timeresolved second harmonic generation (TR-SHG) spectra (dots) of GQD/TiO2 at a pump photon energy of 2.41 eV and at dierent sample
temperatures, with biexponential ts for the solid curves (reprinted with permission from ref. 141. Copyright 2013 American Chemical Society).
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(a) Schematic illustration of the core-sheath nanostructured ber. (b) SEM image of a core-sheath ber with the sheath part peeled o to
unveil the CNTs. (c) SEM image of a wire-shaped dye-sensitized solar cell (reprinted with permission from ref. 142. Copyright 2014 Wiley-VCH).
(d) Illustration (top) and SEM image (bottom) of a wired solar cell prepared by using a graphene/Pt composite ber as the CE and a Ti wire
impregnated with TiO2 nanotubes as the working electrode. (e) Electrocatalytic characterization of graphene/Pt composite bers and (f) JV
characteristics of the wired cell with increasing Pt content. The inset of (e) shows the peak-to-peak voltage separation (VPP) as a function of Pt
content. (reprinted with permission from ref. 143. Copyright 2013 Wiley-VCH). (g) Schematic illustration of the structure of the graphene/CNT
composite ber. Photographs of the photovoltaic textile woven from six wire-shaped solar cells (h) before and (i) after bending, respectively
(reprinted with permission from ref. 144. Copyright 2014 Wiley-VCH).
Fig. 13
higher than that of a similar nanogenerator constructed on

polyethylene naphthalate (PEN) lm (10 mV to 22 mV). Alternatively, upon its exposure to an air ow, the device could
generate piezoelectric voltages of up to 3.9 V with the air ow
speed varying from 0.5 ms1 to 3 ms1, and maintained a
continuous output voltage, owing to the vibration of the PDMS,
which served as a stretchable mechanical spring. In another
work, Bae et al. demonstrated a graphene/P(VDF-TrFE)/graphene acoustic actuator and its application as a nanogenerator
during the bending/unbending process.150 When the device was
subjected to a bending test with an applied strain of 0.3% at a
rate of 60 mm s1, it showed an average output voltage of 2.5 V
(maximum value 3 V), a current density of over 0.2 mA cm2
(maximum value 0.37 mA cm2), and an energy conversion
eciency of 8%, with a reasonably stable performance for >500
cycles.
Interestingly, without the incorporation of any piezoelectric
materials, graphene-based electrostatic nanogenerators were
able to work on the asymmetrical variation in the charge
amount of the adjacent top and bottom electrodes during the
mechanical deformation if a GO layer was sandwiched in a

Al/GO/PEDOT:PSS conguration151 or embedded in the poly(methyl methacrylate) matrix.152 The Al/GO/PEDOT:PSS device
fabricated by Que et al. was highly sensitive and even responded
to a vibrating sound fork with a power output of 0.424 nW and a
conversion eciency of acoustic to electrical energy of 12.1%
(Fig. 14b). A later work by Tian et al. adopted GO lms with a
release structure, and reported a exible GO nanogenerator that
could generate an output power as high as 60 nW with a peak
voltage of 2 V upon a 15 N force applied at 1 Hz frequency
(Fig. 14ce),153 providing another viable solution to eectively
harvest repetitive acoustic and impact energy.
Very recently, and following the successful demonstration
of the exible triboelectric nanogenerator,154 stretchable and
transparent graphene nanogenerators working on triboelectricity have been realized by separating two wrinkled and
rippled graphene electrodes with a plastic spacer (Fig. 14f).155
Owing to its excellent mechanical property, graphene was
found to be compatible with an arbitrarily shaped substrate
with high exibility and stretchability (Fig. 14gi). The output
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Table 3
Comparison of the materials, preparation methods, specic performance, and characteristics of the reported photovoltaic devices
Samples
Preparation methods
Performance
Characteristics
Ref.
Graphene and CdS

composite
Layer-by-layer assembly
Graphene as electron
acceptor; balanced charge
transfer
133
Graphene and P3HT

composite
Spin-coating
Electron acceptor; balanced

charge transfer
134
Graphene quantum dots
Electrochemical corrosion
approach
Electron acceptor; high

electron mobility
135
Aniline-functionalized GQDs
and P3HT
Spin-casting
Electron acceptor;
heterogeneous nanoscale
phase
136
Phenyl-functionalized GQDs
Suzuki coupling reactions
Exciton generator; large

extinction coecients
137
1,3,5-Trialkyl-substituted
phenyl moieties
functionalized GODs
Solution synthesis method
Exciton generator; large

extinction coecients
138
Colloidal graphene quantum

dots
Exciton generator; increased

eciency of hot electron
extraction or multiexciton
generation
Exciton generator; long
lifetimes and triplet excitons
139
Monodispersed graphene
quantum dots
GQD and TiO2 composite
Chemically anchored
method
Hot carrier chromophores;

ultrafast electron injection
141
CNT@ graphene
nanoribbons
Graphene/Pt composite
bers
Oxidation-reduction method
Counter electrode; tensile;

exible
Counter electrode; exible;
wearable; lightweight
142
Graphene/CNT/Pt composite
ber
Biscrolling method and

electrodeposition
Quantum eciency at 400

nm: 16%; photoresponse:
1.08 mA cm2 under light
illumination of 100 mW cm2
Power conversion eciency:
0.88%; open-circuit voltage:
0.77 V; short-circuit current
density: 3.72 mA cm2
density: 6.33 mA cm2
density: 6.33 mA cm2; ll
factor: 0.53
As a new type of light
harvesting media for
photovoltaics
An absorbance maximum at
591 nm with a molar
extinction coecient of 1.0
105 M1 cm1
Faster component of 18 3
ps and slower one ranging
from approximately 100 ps
to nanoseconds
Relaxing into triplet states
and emitting both
phosphorescence and
uorescence
Electron injection from
GQDs to the TiO2
conduction band: less than
15 fs; charge recombination:
80130 fs; instantaneous
recombination of the bound
electronhole pair: 0.52 ps
Energy conversion
eciencies: 6.83%
Open-circuit voltage: ca. 0.73
V; short-circuit current
density: from 12.67 to 17.11
mA cm2; ll factor: from
0.42 to 0.67
Conversion eciencies:
8.36% 0.10%;
capacitances of two
intertwined bers: ca. 31.50
F g1 (4.97 mF cm2 or 27.1
mF cm1)
Spinning and
electrodeposition
performance of the device diminished with the growing

number of randomly stacked graphene layers but improved
when regularly stacked few-layer graphene was employed, an
eect mainly related to the dierence in the work function
and in the accessible amount of friction. A device
Counter electrode; exible;

wearable; miniature devices
140
143
144
constituting single-layer graphene electrodes showed an

output voltage of 5 V and a current density of 0.5 mA cm2
under a vertical compressive force of 9.88 N, qualifying it as
an attractive candidate to drive low-power portable devices
and self-powered exible electronic systems (Table 4).
View Article Online
Perspective
Fig. 14 (a) Fabrication of a graphene-based stretchable transparent piezoelectric nanogenerator, where the right panel shows the corresponding SEM or optical images at each step (reprinted with permission from ref. 149. Copyright 2013 Royal Society of Chemistry). (b) Schematic
of the fabrication of a GO-based acoustic energy harvesting device (reprinted with permission from ref. 151. Copyright 2012 Wiley-VCH). (c)
Schematic view of the exible GO-based nanogenerator. (d) Images showing the device's exibility, front side, and back side. (e) Schematic
representation of the device fabrication (reprinted with permission from ref. 153. Copyright 2013 Royal Society of Chemistry). (f) Schematic
diagrams of graphene triboelectric device fabrication. (gi) The exibility, stretchability, and adjustability of graphene with the crumpled substrate
are shown (reprinted with permission from ref. 155. Copyright 2014 Wiley-VCH).
3.3 Moisture-triggered motor, uid-induced generator, and

beyond
Apart from the above-mentioned power generators, there are
other graphene-based devices that could harvest other types of
energy and convert them to electricity. Continuing our eort in
developing unconventional applications and exploring the full
potential of GFs, we reconstructed the intrinsic conguration of
graphene within the ber body and achieved a new type of
moisture-driven rotational motor by rationally designing the
rotary processing of the freshly spun GO ber hydrogel
(Fig. 15a).156 Due to the presence of oxygen-rich functional
groups in GO, a relatively fast and reversible expansion/
contraction of GO layers took place through the adsorption/

desorption of water molecules, and accordingly, caused a large
deformation of 5% upon increasing/decreasing the relative
humidity (RH) of the environment between 20% and 85%. As a
result, the twisted GO ber (TGF) served as a superb reversible
rotary motor, with a rotary speed of up to 5190 revolutions per
minute, presenting us with a prototype of a moisture-triggered
electric generator when a magnet bar was attached to the end of
the TFG and put at the center of several copper coils (Fig. 15b).
When the whole device was exposed to an environment with
varied humidity, the TGF drove the magnet in reversible rotations, and according to Faraday's law, the periodic change of the
View Article Online
Perspective
Table 4 Comparison of the materials, preparation methods, specic performance, and characteristics of the reported nanogenerators
Samples
Preparation methods
Performance
P(VDF-TrFE) sandwiched
between mobility-modied
graphene
Graphene/P(VDF-TrFE)/
graphene
Chemical vapor
deposition
Output voltage varied from 50 mV to 600 mV when the

sound changed from 82 dB to 110 dB at 100 Hz
Sandwiched Al/GO/
PEDOT:PSS
Poly(methyl methacrylate)/
GO
GO lms
Wrinkled and rippled
graphene electrodes
Doping layer
method
Assembly
Soaking
Filtration and
assembly
Chemical vapor
deposition and
transferred method
Flexible; high
sensitivity;
stretchable
Under a bending test with an applied strain of 0.3% at a rate Acoustic
of 60 mm s1, an output voltage of 2.5 V, a current density of actuator;
0.2 mA cm2, and an energy conversion eciency of 8%
bendable;
exible
Vibrating sound fork with a power output of 0.424 nW and a
Highly sensitive;
conversion eciency of 12.1%
exible
Maximum output electrical power from the device was
Flexible
6 109 W
Output power of as high as 60 nW with a peak voltage
Flexible
of 2 V upon a 15 N force at 1 Hz frequency
Output voltage of 5 V and a current density of 0.5 mA cm2
Stretchable;
under a vertical compressive force of 9.88 N
transparent;
exible
magnetic ux in the copper coils induced an electromotive force

(EMF) of up to 1 mV, without any systematic device optimization in this preliminary study.
Alternatively, an inducted voltage could also be generated by
uid owing over the graphene sheets. Dhiman et al. observed
induced voltages for few-layer graphene of a few orders of
magnitude higher than for MWNTs with hydrochloric acid
(HCl) owing over the surface (Fig. 15c and d).157 The power
generation was believed to originate from the coupled movement of free charges in the ow direction induced by a physical
dri of the adsorbed Cl ions on the continuous graphene lm
surface, and the larger induced voltage of graphene over MWNT
could be attributed to the high electron mobility, structure
integrity, and the at nature of the graphene sheets. The power
generated was 85 nW for a 30 16 mm graphene lm with a
ow of 0.6 M HCl solution at 0.01 ms1, equivalent to a power
density of 175 W m2. Lee et al. further studied the owinduced voltage generation in graphene perpendicularly
aligned to the ow of the non-ionic liquids.158 It was found that
a notable voltage of tens of mV could still be generated when the
non-ionic liquids owed in a perpendicular direction, and also
that the polarity of the uid was inuential in determining the
magnitude of the voltage generated. Due to the absence of salt
ions, the observed voltage was understood to be associated with
instantaneous potential dierences induced in the graphene by
interacting with polar liquids, and also from the momentum
transferred from the owing media to the graphene. Similarly,
Sun and coworkers studied the ow-induced current in 3D
graphene foam, and demonstrated that the value of the induced
current was closely related to the ow velocity and the polarity of
the liquid, but was independent of the ow direction and the
external bias voltage.159,160 Lately, in contrast to the previous
reports with liquids streaming over immersed graphene
surfaces, Yin et al. found that a waving potential of up to 0.1 V
could be induced if a liquidgas boundary was moving along
apiece of monolayer graphene sheet (Fig. 15e), and, furthermore, that the phenomenon could not be understood by any
Characteristics
Ref.
149
150
151
152
153
155
mechanism used to explain ow-induced voltage.161 Theoretical

calculations showed that Na+ was more favorably adsorbed onto
graphene rather than Cl, thus forming an electric double layer
comprising the compact layer of adsorbed Na+ and the diuse
layer of attracted Cl under equilibrium, hence making the
graphene p-doped. During the insertion/extraction of the graphene electrode from the liquid, the moving boundary of the
electric double layer caused a local surplus/deciency of Na+,
driving a hole current from/to the boundary (Fig. 15f). The
induced voltage was proportional to the moving velocity and
was even capable of stimulating a sciatic nerve of a frog. Additionally, the induced voltage and current at lower velocities were
multipliable simply via series/parallel connections of multiple
graphene sheets, demonstrating the viability and scalability of
building self-powered sensors and monitors in remote areas
with sea wave energy (Table 5).
4. Summary and future outlook

Ten years has elapsed since the discovery of graphene from the
mechanical cleavage of graphite, and scientists have now
developed various methods to synthesize functionalized graphene materials of desirable dimensions to fully exploit their
outstanding electronic, optical, thermal, and mechanical
properties for application in a range of scientic elds, ranging
from material science to biology, chemistry, and physics.
Recently, with the advent of portable and wearable electronics,
the ongoing search for low-cost, lightweight, and robustly
deformable material has rmly focused on graphene as one of
the most promising candidates in device fabrication, integration, optimization, and energy provision. In this featured
article, we have discussed tailored graphene materials for
unconventional energy conversion and storage applications,
particularly in exible and miniaturized forms, while unconventional applications of graphene in other types of energy
devices, such as fuel cells are also emerging and are envisaged
to grow signicantly in the next few years.162164
View Article Online
Perspective
Fig. 15 (a) Scheme of the TGF fabrication, with the arrow indicating the direction of rotation. The right panel shows SEM images of the initial TGF
at RH 20% (1), on exposure to a high RH of 85% (2), and returning to a RH of 20% (3). The scale bars are 100 mm. (b) Schematic rotation of a TGF
with a paddle driven by the increased humidity. The paddle can be reversed to the initial state when the moisture decreases. The right panel
shows an illustration of the alternating current generator based on the humidity-responsive TGFs (reprinted with permission from ref. 156.
Copyright 2014 Wiley-VCH). (c) Scheme of the uid owing parallel to the graphene lm. (d) The induced voltage as a function of the uid ow
velocity for the graphene lm and for a MWNT lm (reprinted with permission from ref. 157. Copyright 2011 American Chemical Society). (e)
Schematic illustration of the wave generating potential in graphene moving across the surface of seawater. (f) Schematic of the electric double
layer and its boundaries by ion adsorption (left) and desorption (right) on the surface of graphene during the insertion and pulling out processes,
respectively. The induced potential dierence and hole concentration gradient in the graphene sheet are also illustrated. (g) Peak voltage as a
function of the insertion velocity of graphene into 0.6 M NaCl solution. The insets zoom in on the signals at velocities of 2.25 cm s1 and 45.1 cm
s1 (reprinted with permission from ref. 161. Copyright 2014 Nature Publishing Group).
To date, the developments of these emerging devices are still

in their infancy, with more than 80% of our references coming
from the past three years. However, the current quest for energy
devices compatible with exible and wearable electronics has
provided a golden opportunity and the much needed resources
for academia to scrutinize on what graphene could potentially
oer. Despite all the current and recent research, at least the
following challenges or issues still remain. First, unconventional devices require high-quality tailored graphene materials.
Unfortunately, there are no cost-ecient and eco-friendly
techniques for the large-scale preparation of tailored graphene
materials. Second, such a demand-driven scenario poses rigid
standards for the stability, compatibility, feasibility, and
stretchability of graphene-based devices. However, still only
limited examples can be found in the design of exible electronics and their application in recycling schemes. Third,
several important intrinsic properties of tailored graphene
materials, such as swelling, diusion of molecules and ions
within the gels, and the rheological and mechanical properties,

have only rarely been studied. An in-depth understanding of
these properties will not only facilitate the elucidation of the
intrinsic structures of tailored graphene materials, but also
provide an important clue on how to develop high-performance
unconventional devices for energy conversion and storage.
Finally, the tailored graphene materials for unconventional
energy conversion and storage that we have discussed in this
paper are mainly in the miniaturized form, but it demands
additional eort to increase the capacitance and power density
of the devices to approach practical scenarios.
To meet these requirements, we believe the following issues
deserve special attention. First, it is important to have simple and
inexpensive methods to controllably assemble the graphene
building blocks into desired structures with reasonable reproducibility, thus rendering the material as a basis for further
device evolution. Second, a continuous emphasis is needed on
increasing the device performance (energy density, power
View Article Online
Perspective
Table 5
Comparison of the materials, preparation methods, specic performance, and characteristics of the other generators
Samples
Preparation methods
Performance
Characteristics
Ref.
Spun GO ber hydrogel
Wet-spinning
Moisture-driven motor;
exible; screwable
156
Few-layer graphene sheets

and transferred method
Voltage driven from uid

ow with ionic liquids
157
Graphene
Voltage driven from uid

ow with non-ionic liquids
158
3D graphene foam
The value of induced current

is related to the ow velocity
159
3D graphene foam
Current induced when the

mixtures of ethanol and
water owed
High voltage; high sensitivity
160
Monolayer graphene sheet
GO ber served as a superb

reversible rotary motor with
a rotary speed of up to 5190
revolutions per minute; the
periodical change of
magnetic ux induced an
electromotive force (EMF) up
to 1 mV
The power generated was
85 nW for a 30 16 mm
graphene lm by the ow of
0.6 M HCl solution at 0.01
ms1, equivalent to a power
density of 175 W m2
Tens of mV could still be
generated when non-ionic
liquids owed
10 mA was induced when the
water owing velocity was 10
cm s1
20 mA was induced when the
volume mixing ratio of
ethanol : water 75 : 25
0.1 V could be induced if a
liquid-gas boundary was
moving along the piece of
monolayer graphene sheet
density, conversion eciency, etc.), and also the accessible lifetime should be highly considered, as this could make the technology a practical and viable solution to power real devices
eciently to compete with existing technologies. Third, developing multifunctional integrated devices with the ability to
harvest and store dierent types of energy would be advantageous. For instance, a supercapacitor or lithium ion battery that
could harvest thermal energy has the potential to turn the
unwanted heat produced by the working portable electronics
back into desired electricity, and thus could extend the discharge
cycle for powering. Last, the integration of appropriate smart
compositions, such as the recently developed self-healing materials, into energy conversion and storage devices could possibly
help to repair the structural micro-fractures of electrodes, retain
the electrical properties of the active components, and restore the
conguration integrity of the devices in cases of longtime,
repetitive cycling with loads or from unpredicted mechanical
damage. With the increasing amount of eort devoted to this
dynamic research eld, we believe these emerging graphenebased energy conversion and storage devices will become more
durable and more powerful and nd greater application in exible, wearable electronics and in small/micro gadgets.
Acknowledgements
We thank the nancial support from the 973 program
(2011CB013000, 2011CB605802) of China and NSFC (21325415,
21301018, 21174019 and 51161120361), Fok Ying Tong
161
Education Foundation (no. 131043), the 111 Project 807012. ZZ

thanks Excellent Young Scholars Research Fund of Beijing
Institute of Technology for the nancial support.
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Published on 30 September 2014. Downloaded on 28/09/2015 07:08:38.

Cite this: Energy Environ. Sci., 2015, 8,

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Tailored graphene systems for unconventional

Received 16th August 2014

and energy conversion devices are also proposed.

Key Laboratory of Cluster Science, Ministry of Education of China, Beijing Key

State Key Laboratory of Advanced Functional Composite Materials, Aerospace

surface area, etc.2,3 For instance, graphene shows an ambipolar

These authors contribute equally to the work.

This journal is The Royal Society of Chemistry 2015

Energy Environ. Sci., 2015, 8, 3154 | 31

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