12 Synthesis of Graphene-Based Nanomaterials and Their Application in Energy-Related and Environmental-Related Areas

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Synthesis of graphene-based nanomaterials and their application in energyrelated and environmental-related areas
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Published on 26 July 2012 on http://pubs.rsc.org | doi:10.1039/C2RA20990J
Guixia Zhao, Tao Wen, Changlun Chen and Xiangke Wang*

Received 20th May 2012, Accepted 23rd July 2012
DOI: 10.1039/c2ra20990j
As a fascinating two-dimensional carbon allotrope, graphene has triggered a gold rush all over
scientific research areas especially since the Nobel Prize for Physics in 2010. To exploit the prominent
properties of graphene-based nanomaterials, two important problems are focused in this review: one
is the synthesis of these graphene-based nanomaterials with different kinds of well-defined structures,
and the other is the effective application of them as active nanomaterials in functional devices or
processes. In this critical review, from the viewpoint of chemistry and materials, we give a brief
overview of the recent significant advances in the synthesis of graphene-based nanomaterials and their
applications in energy-related areas and environmental pollution remediation areas, including
supercapacitors, lithium ion batteries, solar cells, adsorption, and degradation of organic/inorganic
pollutants from large volumes of aqueous solutions in environmental pollution cleanup. The main
challenges and perspectives of the materials for future research are also discussed.
1. Introduction
Owing to its extraordinary structure and properties, graphene, a
honeycomb network of sp2 carbon atoms, with single-atom
thickness, has attained a central position as a miraculous
material in the beginning of the 21st century. Graphene exhibits
excellent electronic, optical, mechanical and thermal properties, such as the high values of its mobility of charge carriers
(200 000 cm2 V21 s21),1 fracture strength (125 GPa),2 Youngs modulus (y1100 GPa),2 thermal conductivity (y5000 W m21 K21),3
specific surface area (theoretical value of 2630 m2 g21),4 and high
optical transmittance.4 These attractive properties have triggered
huge interest from different research fields concerned with energy
conversion/storage and environmental pollution remediation,
both of which are the most pressing and hottest issues in modern
society. However, for those practical applications in supercapacitors, lithium ion batteries, solar cells, adsorption and
degradation of different kinds of pollutants from large volumes of
aqueous solutions, graphene needs to be available and processable in large quantity and good quality. To fully utilise the
superior properties of graphene, fabrication of graphene composites with other functional materials is another important
academic and technological endeavor, for which extraordinary
performances have been witnessed in many scientific research
areas. For instance, in energy-related areas, modified graphene
materials have been used in solar cells5 while metallic/metal
oxides combined with graphene have been used in lithium ion
batteries,6 supercapacitors7 and in fuel cells as catalysts.8 In the
Key Laboratory of Novel Thin Film Solar Cells, Institute of Plasma
Physics, Chinese Academy of Sciences, Hefei, 230031, China.
E-mail: xkwang@ipp.ac.cn; Fax: +86-0551-5591310;
Tel: +86-0551-5592788
9286 | RSC Adv., 2012, 2, 92869303
environmental pollution remediation area, many graphene and

magnetic graphene nanomaterials have been used as adsorbents
for heavy metal ions and organic pollutants9 while several
transition-metal oxide graphene hybrids have been used for the
degradation of toxic organic pollutants.10 Some graphene-based
materials have been fabricated as sensor devices for pollutant
analysis.11 These treatments toward graphene not only improve its pristine properties, but also introduce some specific
functional groups or other functional nanomaterials on the
surfaces of graphene layers. Thus, these studies have extended
the research and application of graphene-based nanomaterials
in multidisciplinary areas. Although some researchers have
studied the toxicity of graphene nanosheets,12 we believe that
their intriguing properties outweigh possible biohazards and it
is hoped that any possible toxicity can be reduced or avoided in
the near future.
Herein, the recent significant advance in the synthesis of
graphene-based nanomaterials and their applications in energyrelated areas and environmental-related areas, including supercapacitors, lithium ion batteries, solar cells and organic/
inorganic pollutant management, are focused and reviewed.
We believe that this comprehensive review will provide a general
understanding to the present research about graphene-based
nanomaterials and their perspective in future nanomaterials
research, although clearly it can not include all of the published
work, due to the large activity of this field.
2. Synthesis of graphene-based nanomaterials

Since the micromechanical exfoliation of graphene in 1999, a
wide variety of studies have been focused on its fabrication. To
realize their various applications, graphene-based nanomaterials
This journal is The Royal Society of Chemistry 2012
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are firstly needed to be synthesized with controlled size, thickness

and morphology. Therefore, the development of effective
approaches for their synthesis is of crucial importance. Up to
now, there are two main strategies for the synthesis of graphene
originated from different carbon sources, the top-down and
bottom-up approaches.

2.1. The top-down approach

The graphitic materials, such as 0D fullerenes, 1D nanotubes and
3D graphite, can be chosen as carbon source for the synthesis of
graphene. The most popular top-down method is via the
oxidative exfoliation of graphite through the Staudemaier,
Brodie and Hummers methods.13 The prepared graphite oxides
are further expanded into one- or few-layered graphenes by fast
heating-treatment or exfoliated into individual graphene oxide
nanosheets by ultrasonic treatment in aqueous solution. In
Chens group, a lot of research on the controlled synthesis of
graphene oxides has been carried out.14 Fig. 1 shows the basic
process of the oxidative exfoliation. The graphene oxides are
then reduced into graphene by means of thermal annealing,15
solvothermal reduction,16 electrochemical reduction,17 hydrogen
plasma treatment,18 or radiation-induced reduction,19 etc.
Among these methods, the most frequently used method is
chemical reduction using reductants such as hydrazine, sodium
borohydride, metal Fe, Vitamin C, dimethylhydrazine, alcohols
and hydroquinone.20 By using sulfur-containing compounds
such as NaHSO3, Na2SO3, Na2S2O3, Na2S, Chen et al.21 found
that the reducing ability of NaHSO3 is comparable to that of
hydrazine, with the advantages of low toxicity and nonvolatility. However, these reductions are processed at high
reduction temperature. Recently, great efforts have been devoted
to develop mild reduction processes. For example, Kaminska
et al.22 proposed an easy and environmental friendly method for
the reduction and simultaneously noncovalent functionalization
of graphene oxide by using dopamine at room temperature.
Under a similar condition, Tung et al.23 presented a solutionbased approach to synthesize large-scale and single-layer
chemically converted graphene by directly dispersing graphene
oxide paper in pure hydrazine. At a lower temperature (i.e.,
subzero temperature), a new reducing agent system, hydriodic
acid with trifluoroacetic acid can chemically reduce graphene

oxide into graphene according to Cui et al.24 The above
mentioned methods are processed in solution, while Liang
et al.25 put forward a facile green approach for flexible graphene
film by the reduction of graphene oxide in the gas phase, in
which a solid graphene oxide film can be efficiently reduced by
hydrogen at room temperature with a small amount of Pd as
catalyst. Thermal expansion of graphite oxide is a useful method
for the synthesis of functionalized single-layered graphene.15a,26
McAllister and co-workers26 provided a detailed analysis on the
thermal expansion mechanism. It is considered that the
exfoliation takes place when the decomposition rate of the
epoxy and hydroxyl sites of graphite oxide exceeds the diffusion
rate of the evolved gases.26 Peng et al.17 introduced an
electrochemical method to reduce graphene oxide under constant
potential. By control of the electrical current, applied voltage,
reduction time and the amount of precursor (graphene oxide),
high quality electrochemically reduced graphene oxide film with
controllable size and thickness was obtained. More conveniently,
Kumar et al.19 reported the radiation-induced reduction of
graphene oxide by using sunlight, UV light and KrF excimer
laser. It has been found that after prolonged irradiation under
sunlight or ultraviolet light, graphene oxide can be well reduced.
Within a short time under laser irradiation, graphene with
negligible oxygen functionalities can be obtained.19
It is obvious that the exfoliation of the graphite oxide and the
subsequent chemical reduction are convenient for the mass
production, functionalization and solution processing of graphene. However, this method inevitably introduces large
amounts of defects into the graphene framework because of
the formation of oxygen-containing groups, the ultrasonic
treatment and the incomplete reduction. These defects lead to
deterioration of the electronic properties of the reduced graphene
oxide. Several groups reported that pristine graphite could be
exfoliated to defect-free graphene monolayers in different
solvents such as N,N-dimethylformamide (DMF), ortho-dichlorobenzene, N-methylpyrrolidone (NMP), benzylamine, ionic
liquid, or in some surfactantwater solutions. For example, as
shown in Fig. 2, Hernandez et al.27 demonstrated that through
dispersion and exfoliation of graphite in organic solvents such as
Fig. 1 (A) Outlined oxidization/intercalation process for the preparation of FGO and GO; (B) XRD patterns of FGO and GO.14b
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Fig. 2 Electron microscopy of graphite and graphene: (a) SEM image

of sieved, pristine graphite (scale bar: 500 mm). (b) SEM image of
sediment after centrifugation (scale bar: 25 mm). (ce): Bright-field TEM
images of monolayer graphene flakes deposited from c-butyrolactone
(GBL) (c), 1,3-dimethyl-2-imidazolidinone (DMEU) (d) and NMP (e),
respectively (scale bar: 500 nm). (f), (g), Bright-field TEM images of a
folded graphene sheet and multilayer graphene, both deposited from
NMP (scale bar: 500 nm). (h), Histogram of the number of visual
observations of flakes as a function of the number of monolayers per
flake for NMP dispersions.27
N-methylpyrrolidone, whose surface energy matches that of

graphene, the graphite layers can be exfoliated because the
required energy for the exfoliation is balanced by the solvent
graphene interaction. One of the problems for this method is that
the effective solvents often have high boiling points, which makes
it difficult to remove the solvents. According to ONeill et al.,28
the exfoliation of graphene at higher concentration in lowboiling point solvents such as chloroform and isopropanol can
be achieved, with a thickness of less than 10 layers. Apart from
these exfoliation methods, high-yield graphene with good quality
was also prepared via the exfoliationreinteractionexpansion of
graphite, where graphite was treated with oleum without
excessive chemical functionalization.29 Through fluorination of
graphite, thermal expansion process and the followed ultrasonic
treatment, the obtained graphene can be dispersed well in
organic solvents or in aqueous solutions containing sodium
dodecylbenzene sulfonate as surfactant according to Lee et al.30
There is also a more facile method for the exfoliation of
graphite oxide by using laser excitation other than using any
chemical reducing agent.31 Abdelsayed et al.31a reported a
solution processable synthesis of individual graphene nanosheets
in water without reductants. According to their report, the
authors confirmed the high performance of graphite oxide and
laser converted graphene in the conversion of the laser radiation
into usable heat. More specifically, Sokolov et al.31b found
that graphene features could be produced via continuous-wave
(532 nm) or pulsed (532 and 355 nm) laser excitation of graphite
oxide. According to the Sokolov et al.,31b initial excitation results
in electronhole plasmas within the material. Then the strain
associated with the oxygen-containing groups leads to the
trapping of excitons and holes. The phonon coupling results in
efficient heating and material removal, which lead to an
expanding plasma plume. Finally, the formation and growth of
graphene nanoparticles/sheets in the gas phase and on the
surface are realized.31b
Another interesting carbon source for top-down synthesis of
graphene is carbon nanotubes (CNTs), especially for the
synthesis of graphene nanoribbons (GNRs). The chemical
unzipping of CNTs resulted in elongated graphene strips by
9288 | RSC Adv., 2012, 2, 92869303
using acid reactions,32 plasma treatment,33 liquid NH3 and Li

intercalationexfoliation34 and catalytic approaches.35 According to Kosynkin and co-workers,32 a high-yielding procedure for
the fabrication of single- and few-layered GNRs through
oxidative longitudinal unzipping of multiwalled carbon nanotubes (MWCNTs) in sulfuric acid was realized. However, due to
the excessive oxidation, those narrow ribbons derived from the
inner tubes are readily destroyed while the contiguous regions of
the basal plane from the wider ribbons are often disrupted,
resulting in holes of various shapes and sizes; as a consequence
the electronic performance is detrimentally affected.32 To overcome this disadvantage an improved method was further
proposed and changes in the reaction conditions such as acid
ratio, time and temperature were investigated (see Fig. 3). It was
found that sufficiently concentrated H2SO4 (y90 vol%) and the
elevation of the reaction temperature to 60 uC were important
for the formation and exfoliation of GONRs, and the addition of
10 vol% of a second acid (H3PO4 or trifluoroacetic acid) can
greatly enhance the quality of the GONRs.36 In Dais group,37
the atomic structures, Raman spectroscopic and the electrical
transport properties of individual graphene nanoribbons
obtained by sonochemical unzipping of MWCNTs were clearly
investigated, and they found that a large fraction of GNRs were
bent with smooth edges, and most of them were two-layered.
To better control the quality of graphene layers along with the
high-field preparation, Shinde et al.38 used electrochemical
oxidation to accurately control the degree and sites of oxidation
under ambient conditions with the unique advantage of thickness
and orientation control. In their method, an interfacial electric
field is able to orient the CNTs and longitudinal unzipping is
more favorable instead of a random breakdown in chemical
methods because possible CC cleavage initiated at topological
defects has sufficient strain which makes the CC cleavage is
easy to realize.
In 2011, Perdigao and co-workers39 reported graphene
formation by the thermal induced decomposition of C60 in
combination with a Ni thin film. The formation of graphene was
verified by releasing the resulting layers by etching the metal
substrate. The main processes are illustrated in Fig. 4. They also
found that the carbon present at a buried metal/SiO2 layer can
diffuse and segregate at the surface, and graphene can grow from
the adsorbed carbon.39 However, from the high D/G intensity
ratio in the Raman spectra, it can be concluded that graphene
produced by this method appears to be highly defective.
There are some new methods for graphene synthesis.40
Theoretically, Miyamato et al.40a proposed to use ultrashort
laser pulses to detach graphene monolayers from graphite, one at
a time. After calculations by an ab initio study, the authors
inferred that photo-exfoliation should be able to produce intact
graphene monolayers free of contaminants and defects at a high
rate. Laser-induced melting of graphite under different pressure
conditions has been investigated by Garcia and Jeschke.40b Their
results showed that two steps were involved in the laser-induced
melting process: the destruction of the graphite sheets via bond
breaking and merging of the melted layers. Under the external
pressure (10 GPa), the separation of the two steps is more
evident for graphite, although it is also present in graphite films
at normal pressure. Experimentally, Carey et al.40c investigated
the interaction between the laser and graphite from various laser

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Fig. 3 a Previously published conditions and results.32 b Weight equivalents of KMnO4 relative to MWCNT weight in the starting material. c Weight
gain (%) upon isolation of the product relative to the starting weight of MWCNTs. d All scale bars are 100 nm. e Weight percent remaining at 250 uC by
TGA at 10 uC min21 under Ar. f Weight percent remaining at 950 uC. g Recorded in water. h The darker portion in the TEM micrograph is part of the
lacey carbon grid. i Preferred conditions for optimized GONRs.36
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Fig. 4 Graphene synthesized from C60 buried under a nickel film on a

SiO2 surface. (a) The preparation procedure performed in vacuum: (I)
y1.6 nm of C60 was deposited on a predegassed SiO2 surface, (II) nickel
film was grown by evaporation, and then (III) the whole assembly
was annealed at a chosen temperature for 15 min. (bd) tapping mode
2 6 2 mm AFM images of samples taken out after stages IIII,
respectively. (e) Raman spectra of transferred graphene prepared at
different annealing temperatures, with the peak assignments D, G, D9,
2D and D + G shown by dashed lines.39
and graphite parameters, which supports well the formal

theoretical researches. Recently, Zhao et al.40d attempted to
synthesize graphene by etching of graphite using a lowtemperature plasma technique. The firstly introduced H2O2
plasma technique is an easy and environmental friendly method
although the yield, as yet, is not high enough. The oxidation and
etching of reduced graphene oxide by thermal oxidation in air,
ultraviolet-generated ozone, microwave oxygen plasma and
scanning tunneling microscopy lithography have been investigated by Sols-Fernandez et al.41 It was found that reduced
graphene oxide exhibited a higher reactivity toward oxidation
than the pristine graphite. Another new wet chemical bulk
functionalization route using pristine graphite was achieved by
coupling reductive graphite activation with oxidative arylation
by organic aryldiazonium salts in a single-step procedure,
resulting in single-layered graphene without reaggregation and
substrate-induced doping.42
Graphene obtained through the top-down approach has been
used to blend with other components to synthesize functional
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composites because of the intriguing properties derived from the

synergistic effects of the components and graphene. For example,
Chidembo et al.43 employed an efficient and versatile in situ spray
pyrolysis method to synthesize globular metal oxidegraphene
composites (rGO-Co3O4 or rGO-NiO) with highly porous
morphologies. Zhao et al.44 mixed a graphene oxide solution
with a Ni(NO3)2 solution, then added NH4HCO3 to produce basic
nickel carbonate depositing on both sides of graphene layers. The
precursor was heated at 400 uC to obtain graphene/NiO
nanocomposites. Liang et al.45 reported well-distributed TiO2
nanocrystals grown on graphene as shown in Fig. 5. This synthesis
process has been applied to obtain other transition-metal oxides/
graphene composites, such as MnO2/GNS,46 Fe3O4/GNS,47 TiO2/
GNS,48 SnO2/GNS,49 Co3O4/GNS.50
Apart from complexation with inorganic compounds, graphene
also has been utilized in the synthesis of polymergraphene
composites. For instance, in situ reduction of graphite oxide in
polymer powder has been carried out using focused solar
electromagnetic radiation, where graphene oxide is completely
reduced in polyvinylidene fluoride (PVDF) through photochemical reduction, resulting in highly conducting graphene
PVDF composites.51 Tang et al.52 reported a simple casting of a
polymer solution which contains dispersed graphene oxide,
followed by thermal reduction, for producing nanocomposites
containing well-isolated monolayer reduced-graphene oxide
nanosheets. Potts et al.53 firstly reported polymer composites
using microwave-exfoliated graphite oxide (MEGO) to produce
MEGO/polycarbonate composites at various loadings, which
resulted in improvements of multifunctional properties as
compared with neat polycarbonate. In these composites, graphene
and polymer are noncovalently mixed together. By chemically
grafting an organosilane, 3-aminopropyl triethoxysilane, onto the
graphene skeleton, a covalent functionalization of graphene
nanosheets (f-GNS) was realized by Wang and co-workers.54
The top-down approach is widely used for graphene synthesis
in large quantity, and the resulting graphene nanosheets can be
Fig. 5 (a) SEM image, (b) low magnification and (c) high magnification
TEM images of TiO2 nanocrystals grown on GO sheets. The scale bar is
400 nm for the SEM image in (a) and 20 nm for the TEM image in (b).
(d) An XRD pattern of the graphene/TiO2 nanocrystals hybrid.45
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conveniently complexed with other functional components.

However, this method has several disadvantages such as: (i)
use of hazardous and toxic reagents (i.e., concentrated sulfuric
acid, organic solvents) in the synthesis processes; and (ii) the asprepared graphene frameworks contain a large amounts of
defects, which limit the application of synthesized graphene in
many research areas.

2.2. The bottom-up approach

Different from the top-down chemical approach, which starts
from graphitic materials and provides a feasible way for the mass
production of graphene, the bottom-up approach starting from
small organic molecules is another important method for precise
control over the morphology and structure of graphene. It has
been well documented that the decomposition of hydrocarbons
into graphitic materials can be catalyzed by metal surfaces
through chemical vapor deposition (CVD).55 Hydrocarbon gases
such as methane were chosen as carbon source and large
domains of single-crystalline graphene were successfully grown via
different CVD processes on various metal substrates. One of the
best templates for the deposition is the Ni(111) surface due to the
small lattice mismatch of this surface with the graphene surface.
It has been reported that graphene films with resistances of
280 V sq21 (80% transparent) and 770 V sq21 (90% transparent)
were realized through the growth of graphene on Ni film.56
Furthermore, the control in graphene scale makes CVD the most
attractive method for devices fabrication. However, precise
controlling the edge structure and topology of graphene is still a
great challenge for the CVD method. Xu et al.57 produced
extended single-layer and centimeter-scale graphene on a nickel
surface deposited on a highly oriented pyrolytic graphite substrate
by the diffusion of carbon atoms through the nickel template.
Their results demonstrate the optimization of the relevant
parameters for graphene growth (annealing time and temperature)
to yield fine control of thickness and structure of the graphene
layers. Fig. 6 shows the synthetic process for patterned graphene
film growth on the thin nickel layers.
In Ruoffs group and Kaners group, more researches were
focused on CVD growth of graphene on Cu substrates.55,58
Bhaviripudi et al.59 presented the role of kinetic factors in CVD
synthesis of uniform large area graphene using Cu catalyst. It
was found out that the growth of graphene varied from a
monolayer at low methane concentration (ppm) to multilayers at
higher methane concentration (510% by volume) under atmospheric pressure. One difficulty in the CVD synthesis on Cu
substrates is that the domain size of the resulting graphene is not
large enough.55a Li et al.55c studied the effect of growth
parameters and developed a two-step CVD process to synthesize
graphene films with an area of hundreds of square micrometers.
In Ahn and Hongs group,60 a new route to large-scale synthesis
of high-quality graphene films was demonstrated by using
centimeter-scale Cu substrates. This cost- and time-effective
roll-to-roll production method resulted in 30-inch graphene films
and simultaneously provided an efficient synthesis of graphene
with large scale and good quality for practical application.60
From the work in Kongs group61 and Ruoffs group,62 the
transfer of these deposited graphene onto arbitrary substrates
was also been launched.
Fig. 6 Novel Ni(111)/HOPG(0001) system for production of highquality single-atomic graphene layers: (a) schematic diagram of graphene
growth system and formation mechanism; (b) graphene on Ni(111)/
HOPG (0001) (size: 2 cm 6 2 cm); (c) AFM image of our graphene sheet;
(d) constant current STM image of the as-prepared graphene sheet. The
top-right and bottom-left insets show a two-dimensional fast Fourier
transform taken from the STM image and STM image superimposed by
the honeycomb lattice of graphene, respectively.57
Another common method for graphene synthesis is the

epitaxial growth of graphene on SiC wafer surfaces through
the decomposition of SiC followed by the desorption of Si from
the surface.63 By using in situ low-temperature scanning
tunneling microscopy to study the epitaxial growth, Huang
et al.63d inferred the bottom-up growth mechanism. According to
Heer et al.,63a the quantum Hall effect was suppressed due to the
absence of localized states in the bulk of the as-prepared
material. The advantages of the epitaxial growth can be
summarized by: (i) the resulting material does not need to be
transferred from the metal to another dielectric substrate; (ii)
there are no trapped impurities under the graphene; and (iii) the
growth can be directed by proper tailoring of the substrate.63c
Interestingly, an organic synthesis method for graphene has
been put forward, in which precursors are those discotic
aromatic hydrocarbons with precise chemical structures and
functional groups.64 In cyclodehydrogenation of well-defined
polyphenylene precursors, dendritic polyphenylene is easier to
process in solution due to its good solubility, which decreases p
p stacking significantly.65 By designing the structure of the
precursor monomers, a wide range of nanographenes with
various topologies and widths can be produced.65b,66 In the
organic synthesis field, there are some researches on nanographene synthesis, where the crucial problem is the practical
processability of large polycyclic aromatic hydrocarbons
(PAHs). It is found that PAHs which are larger than
hexabenzocoronene (C42H18), are not soluble in organic solvents
or not sublimable without decomposition because of strong
intramolecular pp interactions.67 One strategy to solubilize the
nanographenes is to introduce the long, flexible aliphatic chains
to the edge of the planar nanographene.68 However, with the size
of graphene increasing, such a strategy makes less difference.
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Thus, it is seriously needed to develop new methods to solve this

problem. Without using aromatic polymers, Sun et al.69 carried
out the deposition of large area and high-quality graphene with
controllable thickness using different solid carbon sources, such
as polymer film (polymethyl methacrylate) molecules, where a
metal catalyst substrate and a temperature as low as 800 uC was
used. This method stands as a complementary method to CVD
growth with the advantage of permitting growth at low
temperature and overcoming the limitation in the use of gaseous
materials in the CVD method.
Although the bottom-up approach introduces much less
defects on the graphene surfaces as compared the top-down
approach, the operation is relatively more difficult and costs
more. In summary of the two approaches, both of which have
their advantages and disadvantages, it is still needed to develop
new methods or make some improvements on these known
methods for the preparation of high-quantity and high-quality
graphene nanomaterials. To clearly understand the synthesis
methods for graphene, the mature methods mentioned above are
summarized and listed in Table 1, including the used chemicals,
and the structures and properties of the resulting graphene
nanomaterials.
3. Application of graphene-based nanomaterials in

energy-related areas
Due to the special one-atom thick layer 2D structure and its
superb characteristics of large surface area, high electrical
conductivity and chemical stability, graphene is emerging as a
particular carbon material for application in energy storage
device such as supercapacitors, solar cells and lithium ion
batteries.
3.1. Application as supercapacitor materials
Usually, supercapacitors can be divided into two types, denoted
electrochemical double-layer capacitors (EDLCs) and pseudocapacitors due to the different mechanism of charge storage.
Different from those conventional high-surface-area materials
such as activated carbons and CNTs, the available surface area
of graphene nanomaterials as capacitor electrodes is independent
of the pore distribution in the solid state.70 Vivekchand et al.71

reported graphene materials prepared from the thermal treatment of graphite oxide and used them as electrodes for EDLCs.
At a scan rate of 100 and 1000 mV s21 with H2SO4 aqueous
solution as the electrolyte, the capacitance of graphene was 117
and 100 F g21, respectively. In Chens group,72 graphene sheets
synthesized by simultaneously exfoliating and reducing graphite oxide under low-temperature plasma also showed high
specific capacitance and good electrochemical stability. It is
obvious that graphene with less agglomeration, fewer layers,
higher effective surface area should be expected to exhibit a
better supercapacitor performance.73 Therefore, the chemical
modifications of graphene are focused in many research
groups.70a,74 According to Zhang et al.,75 the performance of
supercapacitors using chemically modified graphene as electrode
depends on the flexible graphene sheets, not on the rigid, porous
structure of activated carbon to provide its large surface area.75
Du et al.76 synthesized two kinds of functionalized graphene
nanosheets through thermal exfoliation of graphite oxide at low
temperature in air and at higher temperature in N2 conditions. It
was found that the former functionalized graphene showed much
higher specific capacitance than the latter. Similar to Du et al.,
Lv et al.77 reported a high capacitance (up to 264 F g21) of a
functionalized graphene by vacuum-promoted and low-temperature exfoliation of graphite oxide. The high capacitance of this
kind of functionalized graphene is due to the oxygen-containing
groups on the surface such as hydroxyl, carboxyl and epoxy
groups, which can bring in the fast redox processes for the
pseudocapacitance. Yang et al.78 reported a multilayered
graphene film with highly open pore morphology, which allowed
the electrolyte solution to access the individual sheet surfaces
using water as an effective spacer to prevent the restacking of
graphene layers. The as-prepared film gave a specific capacitance
as high as 215 F g21 in aqueous solution. Another porous 3D
graphene network was reported by using Ni foam as a sacrificial
template in a facile CVD process with ethanol as the carbon
source (Fig. 7). The obtained NiO/graphene composites exhibited a high specific capacitance of y816 F g21 at a scan rate
of 5 mV s21, with a stable cycling performance even after
2000 cycles.79
Table 1 The approaches, methods and used chemicals for the synthesis of graphene nanomaterials, and the structures and properties of the resulting
graphene nanomaterials
Approach
Method
Chemicals used
Structure(s)
Properties or applications
Top-down
approach
Exfoliation
Graphite, concentrated
acid (H2SO4 ,HNO3, H3PO4),
KMnO4
One- or few-layered
graphene oxide nanosheets
Unzipping
Carbon nanotubes,
concentrated acid (H2SO4,
HNO3, H3PO4), KMnO4
Hydrocarbon gases,
metal substrates
SiC substrates
Narrow graphene
nanoribbons
1. to be reduced by reductants to
form reduced graphene oxide
2. to be blended with other components
to synthesize functional composites
3. to remove pollutants from aqueous solutions
1. to be blended with other components
to synthesize functional composites
2. to be applied as biosensors
1. to be used as transparent conductive films
for device fabrication
1. to be used in electronic devices such as
field effect transistors
1. to be used as transparent conductive films
for device fabrication
2. to be constructed with other components
for application in lithium ion batteries
Bottom-up
approach
Chemical vapor
deposition
Epitaxial growth
Organic synthesis
Large polycyclic
aromatic hydrocarbons
or solid polymer film and
a metal catalyst substrate
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Patterned graphene films

Graphene films
Nanographene

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Fig. 7 Photographs of (a) Ni foam before and after the growth of graphene, and (b) y0.1 g 3D graphene networks obtained in a single CVD process
after removal of the Ni foam. SEM images of (c) 3D graphene networks grown on Ni foam after CVD, and (d) 3D graphene networks after removal of
Ni foam.79
One feasible strategy to prevent the aggregation of graphene in

the solution and functionalization process is to use other
materials such as carbon black,80 CNTs,81 or metal oxide
nanoparticles 49,82 to separate 2D graphene nanosheets and
further to obtain high surface areas. For instance, Fan et al.83
constructed a novel 3D CNT/graphene sandwich (CGS) and
used it as an electrode in supercapacitors, where CNT pillars
were grown in the graphene layers. A maximum specific
capacitance of 385 F g21 was obtained with a scan rate of
10 mV s21 in 6 M KOH solution owing to the comprehensive
utilization of pseudocapacitance from a catalyst and the doublelayer capacitance from graphene, adding to the rapid transport
of the electrolyte ions or electrons throughout the sandwich
structure. Wang et al.84 did similar research by using a simple
green hydrothermal route to prevent restacking of individual
graphene sheets. Guo and Li85 reported a self-assembly
approach to synthesize a hierarchical nanostructure comprised
of carbon spheres and graphene nanosheets. The carbon spheres
act as a nanospacer to separate graphene nanosheets, resulting in
a high power density of 15.4 kW kg21 and long cycle life of the
supercapacitor.
The most popular pseudocapacitive materials are transitionmetal oxides. Recently, there have been many reports on
graphenemetal oxide/hydroxide composites, such as SnO2,49,86
Mn3O4,87 Fe3O4,88 Co3O4,89 Co(OH)2,90 and ZnO.49,82a Chen
et al.91 synthesized grapheneCo(OH)2 nanocomposites and
found that the specific capacitance of the composites reached a
high value of 972.5 F g21, with a significant improvement
relative to the individual components. A spherical a-Ni(OH)2
nanoarchitecture grown on graphene was realized and used as an
advanced electrochemical pseudocapacitor material, whose
maximum specific capacitance was found to be high up to
1760.72 F g21 at a scan rate of 5 mV s21 according to Yang

et al.92 Similarly, Zhao et al.44 applied monolayer graphene/NiO
nanosheets with two-dimensional structure for supercapacitors.
It was found that the NiO nanoparticles (57 nm) were
uniformly dispersed on the graphene surface, and the twodimensional structure enhanced the supercapacitive performance, with a high specific capacitance of 525 F g21 at a
current density of 200 mA g21 (Fig. 8). Other reduced graphene
oxidemetal oxide materials have also been applied in supercapacitors such as rGOCo3O4,93 rGOZnO,49 and rGO
SnO2.49,94 In Dais group, an advanced asymmetrical supercapacitor obtained by coupling Ni(OH)2/graphene and RuO2/
graphene hybrids were firstly fabricated, which showed high
specific capacitances and high energy and power densities.95 For
the first time, Zhao et al.96 synthesized few-layered MnO2
nanosheets using graphene oxide nanosheets as templates. The in
situ replacement of carbon atoms on graphene oxide framework
by the edge-shared [MnO6] octahedron resulted in this special
graphene-based nanomaterial, which showed a notable capacitance of y1017 F g21 at a scan rate of 3 mV s21, and y1183 F g21
at a current density of 5 A g21.
As important synthetic organic capacitor materials, polymers
are often complexed with graphene to form graphene/polymer
nanocomposites, which have turned out to show excellent
performance in supercapacitors.74,97 Graphene oxide and graphene nanosheets were often doped into a polyaniline
matrix.7,74c,98 For example, Wang et al.7 prepared a graphene/
polyaniline composite paper (GPCP) by in situ anodic electropolymerization of aniline on graphene paper, and its electrochemical capacitance was as high as 233 F g21. Mini et al.97 have
developed high performance supercapacitor electrodes based on
graphene/poly(pyrrole). The composites were synthesized by
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Fig. 8 The first three cycles of CV curves of (a) bare NiO and (b) graphene/NiO. (c) Galvanostatic charge/discharge curves of NiO and graphene/NiO
at 200 mA g21. (d) Rate capacitance of NiO and graphene/NiO with increasing current density. (e) Galvanostatic charge/discharge curves of graphene/
NiO at 0.2, 2, 4 and 6 A g21. (f) Cycle life of NiO and graphene/NiO at 200 mA g21 in 6 M KOH solution.44
using electrophoretic deposition of graphene and then the

poly(pyrrole) layer was electropolymerized upon the graphene.
The specific capacitance was found out to be 1510 F g21, with
area capacitance of 151 mF cm22 and volume capacitance
of 151 F cm23 at 10 mV s21.97 Another nanocomposite,
poly(sodium 4-styrensulfonate) (PSS)-graphene, proved to have
very high cycle stability, the specific capacitance (190 F g21)
decreasing by only by 12% after 14 860 cycles.99 It is commonly
considered that the excellent capacitive performance of these
graphenepolymer composites is due to the good EDL capacitance and pseudocapacitance, besides their good electrical conductivity. In Ruoffs group, a high-performance supercapacitor
comprising a poly(ionic liquid)-modified reduced graphene oxide
(PIL:RG-O) electrode and an ionic liquid (IL) electrolyte showed
a stable electrochemical response up to 3.5 V operating voltage, a
maximum energy density of 6.5 W h kg21 and a power density of
2.4 kW kg21.74a
In summarizing the research on transition-metal oxide/
graphene hybrids, the excellent specific capacitance and cycle
performance at high charge/discharge current can be attributed
to three factors: (i) enhanced electronic conductivity of the
composite because of graphene matrix; (ii) uniform dispersion of
the transition-metal oxide nanoparticles among the graphene
nanosheets ensure good interconnection of transition-metal
oxide nanoparticles at the surface and interior of the electrodes;
and (iii) graphene can act as a buffer for the volume change
9294 | RSC Adv., 2012, 2, 92869303
between the oxidized form and reduced form in the whole

process, which ensures a good cycling performance of the
composites. As promising electrode materials for supercapacitors
the development of graphenemetal oxide materials is still in its
early stage and requires further research.
3.2. Application in lithium ion batteries
In the modern society, rechargeable lithium ion batteries (LIBs)
are widely used in portable devices. Thus, a great effort is being
made to improve the performance of LIBs, especially their
energy density, rate capability and cycling stability, which are
largely dependent on the electrode materials since the recharge of
LIBs is completed with the lithium ion insertion/extraction
process in the electrodes. Because the commonly used graphite
has low specific capacity many workers have turned their
attention to alternative anode materials. It has been discovered
that disordered carbon shows a higher capacitance than the
ordered graphitic carbons.100 Thus it is reasonable for randomly
organized graphene nanosheets to show excellent lithium storage
capacity, due to the high specific surface areas, especially though
the facile functionalization of oxygen-containing functional
groups in the graphene oxide precursor through the chemical
route.101 In order to prevent restacking of graphene nanosheets,
CNTs or C60 molecules were introduced as spacers, which led to
an increase in capacity of LIBs from 540 mA h g21, to 730 and
784 mA h g21, respectively.102

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Metal oxide nanoparticles are attractive anode materials

owing to their high specific capacities.6,103 However, the huge
volume variation during the charge/discharge processes causes
the pulverization of the electrode, which results in poor
reversibility, although by reducing the size of these materials to
nanoscale this drawback can be partly improved. Recently, high
specific capacity and good cycling performance of graphene
metal oxide hybrids as active materials in LIBs have been
reported. The metal oxides mainly include Co3O4,104 NiO,105
Mn3O4,106 CuO,107 TiO2,108 SnO2105,109 and Co(OH)2.110 These
nanoparticles not only play an important role as spacers between
graphene layers, but also provide as active materials to interact
reversibly with lithium ions. Taking SnO2 for example, it has
high specific capacity (782 mA h g21) theoretically as an anode in
LIBs. However, its cycling performance is not satisfactory
because of pulverization. By incorporating SnO2 with graphene
to form a delaminated, 3D, flexible structure, the lithium storage
capacity and cycling performance have been improved significantly according to the work from Paek et al.111 In these hybrid
materials, graphene nanosheets act as not only lithium storage
electrodes, but also electronically conductive channels. At the
same time, the volume expansion upon lithium insertion is
limited due to the dimensional confinement of SnO2 nanoparticles by the surrounding graphene. Furthermore, the developed
pores between graphene and SnO2 act as buffer spaces during
charge/discharge processes. However, in fact, this kind of
structure is difficult to operate in a controlled fashion. Xu
et al.112 synthesized MoO2/graphene oxide composites by a
simple solvothermal method. It was found that with the addition
of graphene oxide and the increase of graphene oxide content in
the precursor solutions, MoO3 rods changed to MoO2 nanorods
and further to MoO2 nanoparticles, both of which were
uniformly distributed on the graphene surfaces. As shown in

Fig. 9, the MoO2/graphene oxide composite with 10 wt%
graphene oxide shows a reversible capacity of 720 mA h g21
with a current density of 100 mA g21 and 560 mA h g21 at a high
current density of 800 mA g21 after 30 cycles. A two-step
solution-phase reactions to fabricate Mn3O4/graphene hybrids
was reported by Dais group.113 The intimate interaction
between the Mn3O4 nanoparticles and graphene gave the hybrid
a high specific capacity (y900 mA h g21) as an anode material
for LIBs. Another kind of nitrogen-doped MnO/graphene
nanosheets (N-MnO/GNS) hybrid material was obtained
through a hydrothermal method and subsequent annealing by
ammonia. The nanostructured hybrid material exhibited a
reversible electrochemical lithium storage capacity of 772 mA h g21
at 100 mA g21 after 90 cycles and even a high capacity of
202 mA h g21 at a high current density of 5 A g21.114 In the work
of Peng et al.,115 a facile ultrasonic synthesis of CoO quantum dot/
graphene nanosheet composites at room temperature using
Co4(CO)12 as cobalt precursor was proposed. The nanosized
CoO quantum dots with high dispersity on conductive graphene
provide not only large amounts of accessible active sites for
lithium-ion insertion but also good conductivity and short
diffusion length for lithium ions, resulting in high capacity and
rate capability.
Interestingly, a hierarchically nanostructured composite of
MnO2/conjugated polymer/graphene was fabricated by selfassembly.116 The enhanced performance of the composite can
be attributed to: (i) the interlayer spacing of y0.72 nm in MnO2
promotes efficient lithium intercalation/deintercalation; (ii) the
polymer coating directs the ordered growth of MnO2 and
prevents the aggregation, thus large volume expansion can be
avoided; and (iii) the highly conductive 3-D graphene material
Fig. 9 Electrochemical performance of MoO2/GO composites and MoO2. (a) Cycling performance of MoO2/GO composites prepared by adding 3, 5
and 9 mL of GO suspension, respectively, at a current density of 800 mA g21. (b) Discharge/charge voltage profiles of MoO2/GO composite (with 5 mL
of GO suspension) at a current density of 100 mA g21. (d) Rate performance of MoO2 and MoO2/GO composite (with 5 mL of GO suspension)
between 0.005 and 3.00 V with increasing current density from 100 to 800 mA g21.112
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ensures a fast charge/discharge rate. This work provides a

universal method to fabricate hierarchically nanostructured
composites for energy conversion/storage systems.
Most of the nanomaterials mentioned above are derived from
graphene oxide obtained by the chemical top-down approach.
There are also some graphene-encapsulated metal or metal oxide
nanoparticles synthesized by the in situ, bottom-up method, in
which the particle formation and encapsulation process are
conducted simultaneously.117 For instance, the carbon/Co3O4
composites were synthesized by solid-state pyrolysis of organic
cobalt precursors.117a The resulting graphene-coated Co3O4
showed a high capacity of 940 mA h g21 even after 20 cycles.
It is noted that in these LIBs, after a loss in the initial capacity
the subsequent electrochemical lithium storage performance is
much better, which may be due to the formation of a solid
electrolyte interphase (SEI) layer.50,118 Considering the large
surface area of graphene-based materials, the effect of the SEI
layer may be larger than that of other anode materials.
In brief, graphene-based nanomaterials can largely decrease
the volume variation of the active anode materials during the
charge/discharge process, thus the high specific capacities of
metal oxide nanoparticles (or other active components) can be
maintained. As for the graphitic material itself, the high specific
surface area compared with graphite and the good electrical
conductivity ensure graphene-based materials are good alternative anode materials.
3.3. Application in solar cells
Due to the great potential for transparent and conductive
electrodes in solar cells, graphene has been widely studied as
different parts of solar cells in terms of their low cost, flexibility
and high efficiency. As an ideal 2D material that can be
assembled into film electrodes with low roughness and high
conductivity, large surface area, thin graphene films are often
used as window or/and counter electrodes, electron and hole
transport materials, and buffer layers in solar cells.119 Wang
et al.120 first reported a 10 nm-thick graphene film with a transparency of more than 70% and a conductivity of 550 S cm21 by
the thermal reduction of a graphene oxide film. This graphene
was then used as a window electrode in dye-sensitized solar cells
(DSSC), in which the currentvoltage characteristics showed a
short-circuit photocurrent density (Isc) of 1.01 mA cm21, with an
open-circuit voltage (Voc) of 0.7 V, a calculated fill factor (FF) of
0.36, and an power-conversion efficiency of 0.26%. The excellent
performance is considered due to the low transmittance of the
electrode and the series resistance of the device. Up to now,
many efforts have been made to enhance the transparency
and conductivity of such graphene thin films for application
as electrodes in solar cells.121 However, these graphene films
produced from solution often have many grain boundaries and
defects which significantly increases the resistance. One strategy to tackle this problem is to incorporate other conductive
filler materials such as silica,122 polymer123 or CNTs124 into the
graphene matrix. For example, a nanocomposite of chemical converted graphene and CNTs gave a film resistance of 240 V sq21 at
86% transmittance.124a Su et al.125 used large aromatic molecules such as pyrene-1-sulfonic acid sodium salt (PyS) and
the disodium salt of 3,4,9,10-perylene-tetracarboxylic diimide
9296 | RSC Adv., 2012, 2, 92869303
bis-benzenesulfonic acid (PDI) to functionalize graphene,

obtaining the enhancement in both the conductivity and
electronic structure of graphene. The subsequent thermal
reduction of graphene nanosheets led to a great increase of
the conductivity and the overall power efficiency of 1.12% of
the solar cells.
Besides the solution process, a more commonly used route for
high-quality graphene is CVD process, especially for their
application as transparent conductive electrodes in photovoltaic
devices.126 Yao et al.126b synthesized graphene film on Ni filmcoated SiO2/Si wafers by the CVD method, and further
transferred it to other substrates directly by dry-transfer
technology. It was found that the average resistance of the 6
30 nm-thick graphene films varied from 1350 to 210 V sq21 with
an optical transparency from 91 to 72% in the visible light
wavelength range, which was much lower than that of graphene
oxide films processed from solution oxidation. In the report of
Yan et al.,127 soluble graphene quantum dots were employed as a
sensitizer for dye-sensitized solar cells (DSSC), in which an opencircuit voltage of 0.48 V and a short-circuit current density of
200 mA cm22 were obtained, with a fill factor of 0.58.
Apart from DSSC, graphene has also been used in organic
solar cells.5b,128 Compared with indium tin oxide (ITO), which
suffers from rising cost and brittleness, graphene has many
advantages in terms of its low cost, transparency, chemical
robustness, flexibility and high electrical conductivity. Wang
et al.129 reported high-performance organic solar cells by
interface engineering of layer-by-layer stacked graphene anodes.
The key for the further improvement in PCE is to reduce the
sheet resistance of graphene, which can be achieved by increasing
the carrier mobility via interface control or by more effective
doping.
Differently, another graphene-based film from the nanographene molecules of large polycyclic aromatic hydrocarbons
(PAHs) were also employed as a window electrode in organic
solar cells.5b The 4 nm-thick films hold a transparency of 90% at
a wavelength of 500 nm. Furthermore, the highest external
quantum efficiency (EQE) of the solar cell was found to be 43%
at a monochromatic light of 520 nm, suggesting that the output
voltage of this graphene-based cell is comparable to that of ITObased solar cells.5b Many applications of graphene-based
materials as a transparent conductive electrode in solar cells
have been reported in recent years,130 which are not mentioned
specifically here. In conclusion, the present research of graphene
on solar cells is mainly focused on three aspects: (i) the
development of advanced techniques for graphene-based electrodes with high transparency and excellent conductivity; (ii) the
synthesis of graphene nanomaterials as efficient acceptors to
favor more efficient electronhole separation; and (iii) the use of
graphene-based films as an efficient hole transport layer.
Besides acting as a transparent conductive electrode, graphene
has other potential uses for photovoltaic devices. For instance,
through incorporation into conjugated polymers, graphene has
largely improved the exciton dissociation and charge-transport
properties.131 In Chens group, organic solution-processed
graphene material has been applied as an electron acceptor in
organic bulk heterojunction (BHJ) photovoltaic devices with
P3HT and P3OT as electron donor.131,132 By controlling
annealing, the device performance is improved considerably,

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and under simulated 100 mW cm22 AM 1.5 G light illumination

a best power conversion efficiency of 1.4% was obtained.
Solution-processed graphene was further used as a transparent
anode to fabricate bulk heterojunction polymer organic photovoltaic devices, which displayed a power-conversion efficiency of
0.13%.133 Wu et al.5a also demonstrated organic light-emitting
diodes with these solution-processed graphene thin films as
transparent conductive anodes. Guo et al.130c used a simple
bottom-up approach to create a novel electron transfer system
based on layered graphene/CdS quantum dots, which showed a
significantly improved photoresponse and offering a promising
path for the development of photovoltaic devices. Organic
photovoltaic devices were also fabricated by using graphenebased materials by Yin et al.,121b Park et al.134 and Zhu et al.135
In summary for the published results, graphene-based
materials are appropriate for photoconversion due to their
strong light absorption, high charge mobility, good stability and
good HOMO/LUMO matching.136
4. Application of graphene-based nanomaterials in

environmental-related areas
Environmental pollution remediation is another hot issue that
needs serious concern in scientific research. Due to the development of economies and the expansion of industrial activities,
contamination of heavy metal ions and toxic organic compounds
in water has been increased over the past decades. Considering
their high specific surface area, which would give the sufficient
contact area for pollutants, various studies have been focused on
the application of graphene-based nanomaterials for the highperformance removal of different organic and inorganic pollutants from aqueous solutions, such as through adsorption to
reduce concentration, decomposition to less toxic molecules, and
reduction to low-valent species. In other words, graphene-based
materials have been applied as adsorbents, photodegradants and
photoreductants in environmental pollution cleanup.
4.1. Application as adsorbents for pollutant removal from aqueous
solutions
Due to its large surface area, graphene is believed to be a good
adsorbent for many pollutants. For example, Li et al.137
obtained monolayer or few-layered graphene nanosheets by
ultrasonication and centrifugation of a 1-methyl-2-pyrrolidinone
(NMP) suspension, and further removed NMP for the adsorption of fluoride from aqueous solutions, resulting an adsorption
capacity of up to 35 mg g21. To improve the dispersion of
graphene in the aqueous solutions, many researches were carried
out using the modified graphene as adsorbents for pollutant
removal, among which, graphene oxide nanosheets are commonly used as adsorbents for heavy metal ions owing to the
abundant functional groups such as hydroxyl, epoxide, carboxyl
and carbonyl on the surfaces, which are expected to form strong
surface complexes with toxic metal ions. According to the
reports from Wangs group, the synthesized few-layered graphene oxide showed a high adsorption ability toward many
heavy metal ions such as Pb(II),138 Cd(II),139 Co(II)139 and
U(VI).140 In their reports, the maximum adsorption capabilities
were 842 mg g21 for Pb(II), 106.3 mg g21 for Cd(II), 68.2 mg g21
Fig. 10 Sorption isotherms of Cd(II) (A) and Co(II) (B) on graphene

oxide nanosheets (0.1 g L21) at different temperatures: pH = 6.0 0.1, I
= 0.01 M NaClO4. The solid and dashed lines correspond to Langmuir
and Freundlich model simulations.139
for Co(II) and 97.5 mg g21 for U(VI), which are all much higher
than that of other adsorbents. Fig. 10 shows the sorption
isotherms of Cd(II) and Co(II) on graphene oxide nanosheets,
and from their report, one can see that the sorption of Cd(II) and
Co(II) on graphene oxide nanosheets is far from saturation.
Deng et al.141 also reported the removal of Pb(II) and Cd(II) ions
from wastewater using one-step synthesized ionic-liquid-functionalized graphene nanosheets directly from flake graphite, with
adsorption capacities up to 406 mg g21 for Pb(II) and 73 mg g21
for Cd(II), respectively.
Besides metal ions, there are also many reports on the
adsorption of organic pollutants. Reduced graphene oxide was
used to remove anionic dyes by Ramesha et al.,142 which turned
out to be a good adsorbent because of the high surface area and
the lack of negative surface charge. Zhao et al.9 used sulfonated
graphene for the removal of naphthalene and 1-naphthol from
aqueous solutions, and obtained maximum adsorption capacities
of 2.33 mmol g21 for naphthalene and 2.41 mmol g21 for
1-naphthol (Fig. 11 and 12), which are much higher than for
other reported materials.
For the full utilization of graphene building blocks in
environment remediation, some functional nanoparticles are
combined with graphene in composites to give some additional
properties to graphene. Typically for the adsorption of
pollutants, magnetic Fe3O4 nanoparticles are incorporated to
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Fig. 11 (A) The synthesis processes of sulfonated graphene from graphite. (B) SEM image of sulfonated graphene on Si substrates. (C) AFM image of
sulfonated graphene on Si/SiO2 substrates (SiO2 ca. 300 nm). The SEM and AFM images show that few-layered sulfonated graphene sheets are
formed.9
facilitate separation in the pollutant treatment. For example,

Shen et al.143 synthesized graphene oxidemagnetic nanocomposites through a high temperature reaction of ferric triacetylacetonate with graphene oxide in 1-methyl-2-pyrrolidone. Many
similar magnetic graphene nanocomposites have been proposed
through solvothermal method or in situ chemical coprecipitation.144 Wang et al.144 applied graphene/Fe3O4 composites for
the removal of organic dyes from aqueous solutions, with the
adsorption capacity for fuchsine as high as 89 mg g21, and He
et al.145 obtained an adsorption capacity of 190 mg g21 for
methylene blue and 140 mg g21 for neutral red cationic dyes
using as-prepared magnetic graphene hybrids. Very similar to
He et al., Xie et al.146 reported the adsorption capacities
of superparamagnetic graphene oxideFe3O4 composites for
methylene blue and neutral red were 167.2 and 171.3 mg g21,
respectively. The magnetic graphene hybrids were also used to
adsorb As(III) and As(V), resulting in arsenic removal to as low
as 1 ppb in aqueous solutions.147 These hybrids also showed an
endothermic and spontaneous adsorption process toward Co(II)
from aqueous solutions, with the maximum adsorption capacity
up to 12.98 mg g21 at room temperature according Liu et al.148
The growth of noble metal nanoparticles such as Au, Pt and Pd
on graphene showed enhanced electronic properties due to the
spatial confinement and synergetic electric interactions between
the metal and graphene. These kinds of composites are mainly
applied as catalysts in organic synthesis and transformation and
less so for water purification.149 Only Sreeprasad et al.150
reported the use of graphene-Au composites supported on river
sand for the excellent uptake of Hg(II) from aqueous solutions.
More research about the application of graphenemetal compo9298 | RSC Adv., 2012, 2, 92869303
sites in pollutant removal is expected. Besides the usual

composites mentioned above, complex composite components
such as CoFe2O4 and ZnFe2O4, also play an important role in
the application of nanomaterials in environmental pollution
cleanup. For example, magnetic CoFe2O4-functionalized graphene nanosheets were used to adsorb methyl orange from
aqueous solution with an adsorption capability of 71 mg g21.79
In conclusion, the excellent adsorption capabilities of graphenebased nanomaterials toward pollutants are due to: (i) the
inherent high specific surface area of graphene; (ii) the decreased
restacking and agglomeration of graphene layers; and (iii) the
strong interaction between the adsorbates and the surface of the
modified or functionalized graphene nanosheets. It should be
noted that the interaction mechanism of organic pollutants with
graphene-based materials is different to that of inorganic
pollutants with graphene-based materials. Thereby, in the
application of graphene-based materials in the removal of
organic or inorganic pollutants from aqueous solutions, different
types of graphene-based materials should be selected, and this
will lead to much future research.
4.2. Application as degradants for pollutants in aqueous solutions
Except for the adsorption of the pollutants in water, many toxic
compounds can be eliminated by photocatalytic degradation
with the aid of photocatalysts such as ZnO, TiO2 and CdS
incorporated with graphene, which shows prominent activity in
photocatalytic application due to the novel electronic property of
graphene and its zero-band gap. Furthermore, the nanoparticles
on the graphene surface prevent the aggregation between the

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Fig. 12 (A) Effect of sulfonated graphene content on the adsorption of

naphthalene and 1-naphthol on sulfonated graphene. C(naphthalene/1naphthol)initial = 0.2 mmol L21, pH = 7.0 0.1, I = 0.01 M NaClO4, T =
293 K. (B) Adsorption isotherms of naphthalene and 1-naphthol on
sulfonated graphene (0.04 g L21 for naphthalene; 0.08 g L21 for
1-naphthol); pH = 7.0 0.1, I = 0.01 M NaClO4, T = 293 K,
C(naphthalene)initial = 0.100.39 mmol L21, C(1-naphthol)initial = 0.17
0.70 mmol L21.9
graphene layers in some extent, so that it is understandable to

expect efficient properties in the pollutant treatment. For
instance, Liang et al.45 synthesized graphene/TiO2 nanocrystal
hybrids through the growth of TiO2 on graphene oxide
nanosheets by hydrolysis and further hydrothermal treatment,
and studied their photocatalytic activity on the degradation of
rhodamine B. It is demonstrated that the as-prepared graphene/
TiO2 nanocrystal hybrids show an impressive three-fold photocatalytic enhancement relative to P25 particles (Fig. 13). TiO2
graphene nanocomposites were also used for the efficient
photocatalytic degradation of butane in the gas phase by
Stengl et al.48 Zhao et al.10 also synthesized graphene/TiO2
composites and the results of photocatalytic degradation of
methylene blue over UV and visible-light spectrum regions
indicated that the enhanced photocatalytic activity was due to e2
adsorption and transportation in the presence of graphene, as a
result of which, graphene/TiO2 was able to absorb a high amount
of photo-energy in the visible-light region and drive efficient
photochemical degradation reactions. According to Zhang
et al.,151 the enhanced degradation performance was originated
Fig. 13 (a) Schematic illustration of the photodegradation of rhodamine B molecules by graphene/TiO2 nanocrystals hybrid under irradiation by a mercury lamp. The inset shows the solution of the graphene/
TiO2 nanocrystals hybrid. (b) Photocatalytic degradation of rhodamine
B monitored as normalized concentration change vs. irradiation time in
the presence of free TiO2, P25, graphene/TiO2 nanocrystals hybrid and a
graphene/TiO2 mixture. (c) Average reaction rate constant (min21) for
the photodegradation of rhodamine B with free TiO2, P25, graphene/
TiO2 nanocrystals hybrid, and graphene/TiO2 mixture. The error bars are
based on measurements on at least four different samples.45
from three attributes: (i) the increasing adsorption of pollutants

on graphene-based nanomaterials; (ii) the extended light
absorption range; (iii) facile charge transportation and separation. Li and Cao152 synthesized ZnO/graphene composites via a
chemical deposition route and demonstrated their efficient
photosensitized electron injection, slow electron recombination
and enhanced photocatalytic activity under UV and visible light.
Similar research was reported by Xu et al.153 As a well-known
IIVI semiconductor, CdS has attracted extensive attention in
photocatalytic research because of its suitable band gap (2.4 eV),
which corresponds well with the spectrum of sunlight, and
extensive attention has been paid to CdSgraphene composites.154 Liu et al.154d utilized as-prepared CdS-reduced graphene
oxide composites for photocatalytic reduction of Cr(VI), and
they found that: (i) CdS-graphene composites exhibited a better
photocatalytic performance than CdS; (ii) the performance was
dependent on the proportion of graphene in the composites, with
the composites containing 1.5 wt% graphene achieving the
highest Cr(VI) removal rate of 92%. The more complex
composites, such as CoFe2O4 and ZnFe2O4, have also been
studied for the degradation of organic pollutants. According to
Wangs research group, the combination of CoFe2O4 or
ZnFe2O4 nanoparticles with graphene leads to high activity for
organic pollutant degradation.155 They noticed that CoFe2O4
showed an excellent degradation ability toward methylene blue,
rhodamine B, methyl orange, active black BL-G and active red
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RGB without the presence of H2O2 under visible light

irradiation.155a For the magnetic ZnFe2O4-graphene nanocomposites, the experimental results showed that these composites
can serve as both photoelectrochemical degrader for organic
molecules and the generator for hydroxyl radicals via photoelectrochemical decomposition of H2O2 under visible light
irradiation with no noticeable change in the structure and
composition.155b
The photocatalytic degradation of organic pollutants is an
environmental friendly method to eliminate organic pollutants
from aqueous solutions in environmental pollution cleanup.
First, the high surface area assures the high adsorption of
organic pollutants on the surface of graphene-based nanomaterials. Furthermore, the high dispersion of metal oxides on
graphene nanosheets and the graphene as electron transfer
channels make the degradation process occur efficiently on these
graphene-based nanomaterials. Therefore, the synthesis of
graphene-based composites with high photocatalytic capacity is
important for the degradation of organic pollutants.
5. Summary and outlook

As a unique 2D carbon material, graphene has shown a
continuously growing research upsurge since its appearance.
Very soon, more researches will be focused on the modification of
graphene and the incorporation of graphene with other functional
nanoparticles and their further applications in multidisciplinary
areas. In this critical review, we have covered recent researches on
the synthesis of graphene-based materials and their applications in
energy-related and environmental pollution remediation areas,
both of which are the issues of most concern. Specifically, the
utilization of graphene-based materials in supercapacitors, lithium
ion batteries, solar cells, adsorption and degradation for the toxic
pollutants from large volumes of aqueous solutions are covered. It
is concluded that graphene-based materials, synthesized through
top-down or bottom-up methods, show prominent properties
in the energy-related and environmental-related areas, compared
with other nanomaterials.
However, there are still many difficulties waiting for efficient
solutions. Firstly, the top-down synthesis often results in large
amounts of defects on the graphene framework, while the
bottom-up method is difficult to realize for mass production in
practical applications. New approaches for the synthesis of highquality graphene in large scale at low price are thus required.
Secondly, although graphene-based materials are used as active
materials for charge collection and transportation in electronic
devices, there are still numerous critical problems requiring
further study for the improvement in quality and function, which
include the morphology of graphene, defects, functional groups,
assembly behavior between graphene and other functional
particles. Thirdly, for the application in environmental pollutant
remediation, although the functionalized graphene-based nanomaterials show prominent ability in the removal of many
pollutants from aqueous solutions, the selective adsorption for
specific pollutants is rarely reported; and degradation reactions
mainly focus on organic dyes, and relatively less on other toxic
organic pollutants or high-valent metal ions. Furthermore, the
research for the understanding of the relationship between
graphene-based nanomaterials and improved performance is still
9300 | RSC Adv., 2012, 2, 92869303
at its early stage, which also hinders the further design for the
effective functional graphene-based materials. It is necessary to
point out that the synthesis of graphene-based materials is still
expensive and in low scale at present, which limits the
application of graphene-based nanomaterials in practical environmental pollution cleanup. With the development of technology, no doubt that these problems will be solved and more
functional graphene-based materials will find extensive use in the
near future.
Acknowledgements
Financial support from 973 projects of MOST (2011CB933700),
NSFC (20971126, 21071147, 21071107, 91126020), and open
foundation of State Key Lab of Pollution Control and Resource
Reuse are acknowledged.
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RSC Adv., 2012, 2, 92869303 | 9303

12 Synthesis of Graphene-Based Nanomaterials and Their Application in Energy-Related and Environmental-Related Areas

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12 Synthesis of Graphene-Based Nanomaterials and Their Application in Energy-Related and Environmental-Related Areas

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Guixia Zhao, Tao Wen, Changlun Chen and Xiangke Wang*

9286 | RSC Adv., 2012, 2, 92869303

environmental pollution remediation area, many graphene and

2. Synthesis of graphene-based nanomaterials

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are firstly needed to be synthesized with controlled size, thickness

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2.1. The top-down approach

acid with trifluoroacetic acid can chemically reduce graphene

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Fig. 2 Electron microscopy of graphite and graphene: (a) SEM image

N-methylpyrrolidone, whose surface energy matches that of

using acid reactions,32 plasma treatment,33 liquid NH3 and Li

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Fig. 4 Graphene synthesized from C60 buried under a nickel film on a

and graphite parameters, which supports well the formal

composites because of the intriguing properties derived from the

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conveniently complexed with other functional components.

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2.2. The bottom-up approach

Another common method for graphene synthesis is the

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Thus, it is seriously needed to develop new methods to solve this

3. Application of graphene-based nanomaterials in

of the pore distribution in the solid state.70 Vivekchand et al.71

9292 | RSC Adv., 2012, 2, 92869303

Patterned graphene films

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One feasible strategy to prevent the aggregation of graphene in

1760.72 F g21 at a scan rate of 5 mV s21 according to Yang

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using electrophoretic deposition of graphene and then the

between the oxidized form and reduced form in the whole

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Metal oxide nanoparticles are attractive anode materials

uniformly distributed on the graphene surfaces. As shown in

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ensures a fast charge/discharge rate. This work provides a

bis-benzenesulfonic acid (PDI) to functionalize graphene,

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and under simulated 100 mW cm22 AM 1.5 G light illumination