Journal of Physics and Chemistry of Solids 74 (2013) 635–640

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Journal of Physics and Chemistry of Solids

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

A facile one-pot synthesis of Cu2O/RGO nanocomposite for removal

of organic pollutant
Benxia Li n, Tongxuan Liu, Luyang Hu, Yanfen Wang
School of Materials Science and Engineering, Anhui University of Science and Technology, Huainan, Anhui 232001, China

a r t i c l e i n f o abstract

Article history: Gathering the photocatalysis of semiconductors and the superduper electron transmittability of
Received 9 July 2012 graphene, graphene-based semiconductor photocatalytic composites are attracting increasing interest
Received in revised form of researchers. In this paper, a Cu2O/reduced-graphene-oxide (Cu2O/RGO) nanocomposite was prepared
28 August 2012
via a facile wet-reduction process, for removal of organic pollutants. The samples were characterized by
Accepted 27 December 2012
Available online 4 January 2013
X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscopy, transmission
electron microscopy, and UV–vis spectrophotometry. The nanocomposite is composed of Cu2O
Keywords: nanoparticles with sizes of 100–500 nm attached to the RGO sheets. For photodegradation of
A. Nanostructures methylene blue (MB) under visible light, the Cu2O/RGO nanocomposites exhibited greatly enhanced
A. Semiconductors
photocatalytic efficiency compared to the pure Cu2O nanoparticles. The enhanced photocatalytic
B. Chemical synthesis
performance was mainly ascribed to the increased adsorptivity to organic dye as well as the efficient
D. Microstructures
charge transportation and separation from Cu2O to RGO.
& 2013 Elsevier Ltd. All rights reserved.

1. Introduction especially in narrow bandgap semiconductors. Therefore, it is

In the past decade, it has become increasingly prevalent to use
semiconductor materials as photocatalysts for eliminating
organic pollutants in water [1–4]. Semiconductor photocatalysis
as an advanced oxidation technology with the advantages of easy
operation, mild reaction conditions, simple equipment, and small
secondary pollution, is expected to show broad prospects in the
use of water splitting and environmental management under
sunlight irradiation [5–7]. Up to now, TiO2 and ZnO photocata-
lysts have been widely used because of their strong oxidizing
power, non-toxic nature, and low cost [8,9]. But, as we know,
these photocatalysts are wide band-gap semiconductors
( 43.2 eV), and the photocatalytic efficiency remains very low
because of the ultraviolet response. Cu2O, a well-known p-type
semiconductor, is a simple metal oxide with small bandgap
energy of 2.0–2.2 eV [10,11], which is a great advantage in
making full use of sunlight, compared to the wide bandgap
semiconductors. Therefore, the preparation Cu2O nanocrystals
for water splitting and degradation of organic pollutants under
visible light irradiation [12–14] have been widely studied. How-
ever, despite its great potential, the photocatalytic efficiency
remains very low because of the fast recombination of the photo-
generated electron–hole pairs in the single phase semiconductor,
n
Corresponding author. Tel.: þ86 554 6668649; fax: þ 86 554 6668643.
E-mail address: libx@mail.ustc.edu.cn (B. Li).
necessary to suppress the electron–hole recombination in the
semiconductor photocatalyst by incorporation of electron-
accepting materials.
As a rapidly rising star in materials science and condensed
matter physics, graphene, a single 2D sheet of sp2 hybridized
carbon atoms with the same structure as the individual layer in
graphite, has initiated an enormous number of scientific activities
due to its extraordinary properties such as high electronic con-
ductivity, large theoretical specific surface area and excellent
mechanical strength [15,16]. Other forms of graphene-related
materials, including graphene oxide, reduced graphene oxide,
and exfoliated graphite have been explored in a wide range of
applications, such as electronic and photonic devices, clean
energy, and sensors [17,18]. Particularly, the fabrication of semi-
conductor/graphene-related composites has attracted substantial
research efforts motivated by the desire to improve the photo-
catalytic efficiency [19–22]. Recent studies have revealed that
that the graphene-involved photocatalysts simultaneously cover
several excellent attributes: the increasing adsorptivity with
respect to pollutants, extended light absorption range, and effi-
cient charge transportation and separation [23,24], which are the
ideal traits of a photocatalyst we have been pursuing for. There-
fore, it is believed that loading Cu2O nanoparticles on RGO sheets
can efficiently utilize the combinative merits of Cu2O and RGO to
obtain a photocatalyst with superior performance.
In this paper, a nanocomposite photocatalyst composed of
Cu2O nanoparticles attached on RGO sheets was prepared via a

0022-3697/$ - see front matter & 2013 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.jpcs.2012.12.020
636 B. Li et al. / Journal of Physics and Chemistry of Solids 74 (2013) 635–640
mild one-pot wet-reduced process, for use in photodegradation of
organic pollutants. The morphology and microstructure of the as-
prepared Cu2O/RGO nanocomposite were characterized. The
photocatalytic performance of the Cu2O/RGO nanocomposite
was evaluated by the photodegradation of methylene blue in
water, and compared with that of pure Cu2O nanoparticles, to
highlight the enhanced photocatalytic performance of Cu2O/RGO
for maximum utilization of Cu2O photocatalyst and RGO as
electron collector and transporter in the photocatalytic degrada-
tion of organic pollutants.
2. Experimental
2.1. Materials
All chemicals were analytical grade and used as received
without further purification. Graphite powder, 37% hydrochloric
acid (HCl), 98% sulfuric acid (H2SO4), 85% phosphoric acid
(H3PO4), 30% hydrogen peroxide (H2O2), potassium permanganate
(KMnO4), copper acetate monohydrate (Cu(Ac)2  H2O), sodium
hydroxide (NaOH), ascorbic acid and absolute ethanol were
purchased from Shanghai Sinopharm Chemical Reagent Co., Ltd.
2.2. Preparation of Cu2O/RGO nanocomposite
Graphene oxide (GO) was first prepared from graphite powder
according to an improved Hummers’ method [25]. Then, the
Cu2O/RGO nanocomposite was synthesized via the following
procedure: 0.3991 g Cu(Ac)2  H2O was dissolved in distilled water
(30 mL) under constant stirring at room temperature, and 30 mL
of GO aqueous dispersion (containing 0.05 g GO) was added into
the above solution and stirred for 30 min. Then, 40 mL of NaOH
aqueous solution (0.2 mol/L) and 20 mL of ascorbic acid aqueous
solution (0.1 mol/L) were successively added into the solution.
After stirring for another 30 min at 50 1C, a claybank precipitation
was gradually formed. Finally, the precipitate of Cu2O/RGO was
filtered, and washed several times with distilled water and
ethanol, and dried at 60 1C in a vacuum oven.
For comparison, the pure Cu2O nanoparticles were prepared by
a similar method, without adding GO aqueous dispersion.
Fig. 1. Illustration of the formation process of Cu2O/RGO nanocomposite.
2.3. Characterizations of the samples
Powder X-ray diffraction (XRD) patterns were recorded on an
XRD diffractometer (Shimadzu XRD-6000) operated at 40 kV
voltage and 30 mA current using Cu-Ka radiation. The morphol-
ogies of the samples were observed by field-emission scanning
electron microscopy (FE-SEM, Sirion200) and transmission elec-
tron microscopy (TEM, H-7650). X-ray photoelectron spectro-
scopy (XPS) measurements were performed on a VGESCALAB
MKII X-ray photoelectron spectrometer with an exciting source
of Mg-Ka. UV–vis absorption spectra of the samples were
recorded on a UV–vis spectrophotometer (Perkin Elmer Lambda
950) by dispersing 1.8 mg of the sample in 5 mL ethanol.
2.4. Photocatalytic property test
The photocatalytic properties of the samples were evaluated
by the photodegradation of methylene blue (MB) in water under
visible light irradiation from a 300 W Xe lamp equipped with a
420 nm cutoff filter (CEL-HXF300/CEL-HXUV300, China). A spe-
cific experimental process is as follows: 80 mg of photocatalyst
was suspended in 100 mL of 5.0  10  5 M MB aqueous solution
under continuous stirring. Before irradiation, the dispersion was
stirred in the dark for 2 h to achieve an adsorption–desorption
equilibrium between the photocatalyst and MB molecules. After-
wards, the solution was exposed to visible-light irradiation under
magnetic stirring at room temperature. At a given illumination
time interval, about 3 mL of MB solution was sampled for
analyzing the MB concentration, and the absorption spectra of
the MB solution was recorded by a UV–vis spectrophotometer
(Shimadzu UV2550, distilled water as reference).
3. Results and discussion
3.1. The formation mechanism of Cu2O/RGO nanocomposite
In this work, Cu2O/RGO nanocomposite was fabricated by a
facile wet-reduced process, in which both the formation of Cu2O
nanoparticles and the reduction of GO were achieved in a one-pot
reaction. Fig. 1 illustrates the fabrication process and formation
mechanism of the Cu2O/RGO nanocomposite. It has been proved
that the surfaces of the chemically exfoliated GO sheets are
 B. Li et al. / Journal of Physics and Chemistry of Solids 74 (2013) 635–640
covered by a large number of hydroxyl, carboxyl and epoxy
groups which are introduced on GO sheets due to oxidation
procedures [26]. These functional groups can act as anchor sites
to enable the subsequent in situ formation of Cu2O nanoparticles
on GO sheets, which are simultaneously reduced to RGO sheets by
ascorbic acid in the reaction system. The formation of Cu2O/RGO
nanocomposite undergoes the following three distinctive stages:
(i) when the GO suspension is added to the Cu(Ac)2  H2O solution,
Cu2 þ ions will be adsorbed onto the surfaces of GO sheets due to
their bonding with the O atoms of the negatively charged oxygen-
containing functional groups via electrostatic force [27]. (ii) After
the addition of NaOH aqueous solution, the crystal nuclei of
Cu(OH)2 formed and combined with the functional groups of GO
sheets via intermolecular hydrogen bonds or coordination bonds,
acting as precursors for Cu2O nanoparticles. (iii) Adding ascorbic
acid as a reducer, Cu2O nanoparticles were formed from the
reduction of Cu(OH)2; meanwhile, RGO sheets were formed from
the reduction of GO as in Eq. (1). Thus, the Cu2O/RGO nanocom-
posite was obtained from both of the reduction reactions carried
out in one step under heating at 50 1C.
Cu(OH)2 þGOþascorbic acid-Cu2O/RGO
3.2. XRD and XPS characterizations
Fig. 2(a) shows the XRD patterns of GO sheets, Cu2O nanopar-
ticles and the Cu2O/RGO nanocomposite, respectively. All the
diffraction peaks in the XRD pattern of Cu2O nanoparticles match
Fig. 2. (a) X-ray diffraction patterns of GO, Cu2O nanoparticles and Cu2O/RGO nanocomposite, and (b–d) XPS spectra of Cu2O/RGO nanocomposite.
637
well with those of the cubic phase Cu2O (JPPDS no. 78-2076). In
the XRD pattern of GO, the characteristic (002) reflection of
graphite located at 2y ¼26.21 (JPPDS no. 75-1621) disappears,
and a diffraction peak belonging to the (001) reflection of GO
emerges at 2y ¼71. Compared with the graphite’s interlayer
spacing of 0.34 nm, the interlayer spacing of GO was enlarged
to 1.65 nm because a large amount of oxygen-containing func-
tional groups formed on carbon basal planes. The diffraction
peaks of Cu2O/RGO nanocomposite are similar to those of Cu2O
nanoparticles, and no peaks belonging to Cu or Cu(OH)2 were
detected. Nevertheless, the (001) diffraction peak at 71 of GO
disappeared in the XRD pattern of the Cu2O/RGO nanocomposite,
revealing that GO was reduced by ascorbic acid [28]. Besides, the
diffraction peaks of graphite were also absent in the composites,
indicating that the decoration of Cu2O onto RGO sheets caused the
enlargement and disorder in the layer spacing of RGO [12,22].
Further evidence for the chemical composition of the Cu2O/RGO
nanocomposite was obtained by X-ray photoelectron spectra
(XPS, as shown in Fig. 2b–d). The survey spectrum (Fig. 2b) shows
the presence of Cu and O as well as C [29]. The Cu 2p XPS
spectrum (Fig. 2c) of the nanocomposite exhibits two main peaks
(1)
at 931.93 eV and 951.78 eV, corresponding to the Cu2p3/2 and
Cu2p1/2 peaks of Cu þ , respectively [30]. Therefore, it can be
concluded from XRD patterns and XPS spectrum that Cu2O is
the only reduced product from Cu(II), and there is no CuO or Cu.
The C1s spectrum (Fig. 2d) indicates that RGO contains three
components: 50.57% non-oxygenated C (284.75 eV), 26.80% car-
bon in C–O (286.15 eV), and 22.53% carbonyl carbon (CQO)
(288.31 eV) [31]. Compared with those of GO reported previously
638 B. Li et al. / Journal of Physics and Chemistry of Solids 74 (2013) 635–640
[32,33], the relative contribution of the components associated
with oxygenated functional groups in the present RGO decreased
considerably, indicating that GO could be reduced by ascorbic
acid in the present reaction system.
3.3. Morphologies and structures of GO and Cu2O/RGO
The SEM and TEM images shown in Fig. 3 reveal the morphol-
ogies and microstructures of GO sheets, pure Cu2O nanoparticles
and Cu2O/RGO nanocomposites, respectively. As observed in
Fig. 3(a), GO sheets present crumpled surface textures with
curling edges, and the solid GO sample is severely agglomerated
because of its high specific surface area and the strong interlock-
ing of the flakes. The TEM image in Fig. 3(b) reveals the layered
structure of the GO sheets with many wrinkles through all the
surfaces of GO sheets, and the details indicate that the interlayer
bonding becomes loose and the interlayer distances are widened,
which is consistent with the result from XRD pattern of GO.
Fig. 3(c and d) shows the FE-SEM images with different magni-
fications of pure Cu2O nanoparticles obtained in the absence of
GO sheets, revealing that the Cu2O nanoparticles have ball-like
morphology with diameters around 100 nm, and some of them
Fig. 3. (a) SEM and (b) TEM images of GO sheets, (c–d) SEM images of pure Cu2O nanoparticles, (e) SEM and (f) TEM images of Cu2O/RGO nanocomposite.
tend to aggregates into larger particles (  500 nm) to reduce
their surface energies. In the presence of GO, the Cu2O/RGO
nanocomposite with particle-on-sheet morphology (Fig. 3e–f)
was obtained. The SEM image of the Cu2O/RGO nanocomposite
(Fig. 3e) indicates that the reduced GO sheets are decorated with
Cu2O nanoparticles with sizes of 100–500 nm, whereas the Cu2O
nanoparticles on RGO sheets aggregate more seriously than the
pure Cu2O nanoparticles, maybe because the presence of GO
sheets prevents the homogeneous nucleation of Cu2O. From the
TEM image of the Cu2O/RGO nanocomposite (Fig. 3f), the light-
gray thin films are the RGO sheets, and the dark regions on the GO
background are Cu2O particles, which can prevent the RGO layers
reunion in the reaction process, and maintain the large specific
surface area features of RGO. Therefore, SEM and TEM observa-
tions confirm that the Cu2O/RGO nanocomposite was obtained by
the present synthesis.
3.4. UV–vis absorption spectra and photocatalytic performance
Cu2O is a well-known p-type semiconductor possessing a
direct band gap at about 2.2 eV. In order to demonstrate the
effect of the presence of RGO on the photo-response of the
 B. Li et al. / Journal of Physics and Chemistry of Solids 74 (2013) 635–640
as-prepared Cu2O/RGO nanocomposite, UV–vis absorption spec-
troscopy was performed on the samples. Fig. 4 shows UV–vis
absorption spectra of GO, pure Cu2O nanoparticles and Cu2O/RGO
nanocomposites, respectively. The UV–vis spectrum of GO exhi-
bits a maximum absorption peak at about 237 nm, corresponding
to the p–p* transition of aromatic CQC bonds [34]. The UV–vis
spectrum of pure Cu2O nanoparticles presents a broad absorbing
band peaked at around 545 nm, similar to previously reported
Cu2O nanoparticles [13]. The Cu2O/RGO nanocomposite has
absorption in the whole UV–visible region ranging from 200 nm
to 800 nm, and the absorption increases in the visible region,
which is beneficial to making full use of sunlight for
photocatalysis.
The photocatalytic performance of the Cu2O/RGO nanocompo-
site was examined by the photodegradation of methylene blue
(MB) as a representative pollutant under visible-light irradiation
from a 300 W Xe lamp. Prior to irradiation, the photocatalytic
reaction system was magnetically stirred in the dark for 2 h
to reach the adsorption/desorption equilibrium of MB on the
surface of the photocatalyst. Fig. 5 shows the UV–vis absorption
spectra of the aqueous solution of MB (initial concentration of
5.0  10  5 mol/L, 100 mL) with 80 mg of the Cu2O/RGO nano-
composite and pure Cu2O nanoparticles as photocatalyst, respec-
tively, and exposure to visible light for various durations. When
the Cu2O/RGO nanocomposite was used as photocatalyst, as
shown in Fig. 5(a), the characteristic absorption of MB at
665 nm decreased rapidly with extension of the exposure time,
Absorbance (a.u.)
GO
Cu 2 O/RGO
Cu 2 O
200 300 400 500 600 700
Wavelength (nm)
Fig. 4. UV–vis spectra of GO, Cu2O and Cu2O/RGO nanocomposites.
Fig. 5. Evolution of the absorption spectrum of MB solution (5.0  10  5 mol/L, 100 mL) in the presence of (a) Cu2O/RGO nanocomposite and (b) Cu2O nanoparticles.
639
and almost disappeared after about 120 min. The color change
sequence (inset of Fig. 5a) in the MB solution during this process
displays that the intense blue color of the initial solution gradu-
ally disappears with increasingly longer exposure times. In the
presence of pure Cu2O nanoparticles, as shown in Fig. 5(b), MB
solution was just partly degraded after 180 min, and no signifi-
cant change emerged in the color of the MB solution during the
irradiation. The concentration of MB in the presence of the Cu2O/
RGO nanocomposite is decreased to 10% after irradiation of
120 min, whereas the concentration of MB on Cu2O nanoparticles
is lowered to 64% after 180 min. The results from photocatalytic
tests have demonstrated that the Cu2O/RGO nanocomposite
possesses an obviously enhanced photocatalytic performance
than pure Cu2O nanoparticles, highlighting the importance of
anchoring Cu2O nanoparticles on RGO sheets for maximum
utilization of the Cu2O photocatalyst and RGO as electron collec-
tor and transporter in photocatalytic degradation of organic
pollutants.
Considering the narrow band-gap (about 2.2 eV) of Cu2O and
the super electron transmittability of graphene due to its two-
dimensional p-conjugation structure [17], the degradation of MB
under visible light in the present case should be conducted
following the semiconductor-excitated mechanism, and RGO
sheets act as electron collectors and transporters, as illustrated
in Fig. 6. The primary step in the process is the photoexcited
charge separation within Cu2O nanoparticles, followed by the
transfer of electrons to RGO sheets and then to the surface-
adsorbed O2 to generate reactive oxidation species such as  OH
and O2 . Such a process effectively suppresses the recombination
of photo-generated charge carriers, leaving more charge carriers
to form highly reactive species (  OH and O2 ) and promote the
degradation of dye. Besides, some reports [23,35,36] have
800
Fig. 6. Electron transport in the photocatalytic degradation of MB, using Cu2O/
RGO nanocomposite as a photocatalyst.
640 B. Li et al. / Journal of Physics and Chemistry of Solids 74 (2013) 635–640
demonstrated that graphene-related materials can effectively
adsorb MB from aqueous solutions due to their huge specific
surface areas as well as the p–p stacking between MB and
aromatic regions of graphene, which allow good access of dye
molecules to the surface of photocatalyst in the photocatalytic
system. Therefore, the excellent photocatalytic performance of
the Cu2O/RGO photocatalyst is mainly attributed to the good
adsorptivity and the efficient charge transportation and
separation.
4. Conclusion
The Cu2O/RGO nanocomposite was prepared by a green and
facile one-pot wet-reduction process without using any hazar-
dous chemicals. The nanocomposite is composed of Cu2O nano-
particles with sizes of 100–500 nm attached to the RGO sheets.
When used for photodegradation of the organic dye MB, the
Cu2O/RGO nanocomposite displayed a greatly enhanced photo-
catalytic efficiency than pure Cu2O nanoparticles, which is mainly
attributed to the thin two-dimensional sheet support that
increases remarkably the adsorbability of photocatalysts as well
as provides a good electron acceptor favoring the transfer of
photo-generated electrons from Cu2O to RGO sheets.
Acknowledgments
Financial supports from the National Natural Science Founda-
tion of China (No. 21001003), Natural Science Foundation of
Anhui Province of China (No. 10040606Q15), and Young and
Middle-Aged Academic Backbone Training Project of Anhui Uni-
versity of Science and Technology are acknowledged.
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