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Fabrication of electric papers of graphene nanosheet shelled cellulose fibres by
dispersion and infiltration as flexible electrodes for energy storage†
Yan-Ru Kang, Ya-Li Li,* Feng Hou, Yang-Yang Wen and Dong Su
Published on 23 March 2012. Downloaded by Tianjin University on 21/03/2014 12:32:44.

Received 10th February 2012, Accepted 19th March 2012

DOI: 10.1039/c2nr30318c

An electrically conductive and electrochemically active composite paper of graphene nanosheet (GNS)
coated cellulose fibres was fabricated via a simple paper-making process of dispersing chemically
synthesized GNS into a cellulose pulp, followed by infiltration. The GNS nanosheet was deposited onto
the cellulose fibers, forming a coating, during infiltration. It forms a continuous network through
a bridge of interconnected cellulose fibres at small GNS loadings (3.2 wt%). The GNS/cellulose paper is
as flexible and mechanically tough as the pure cellulose paper. The electrical measurements show the
composite paper has a sheet resistance of 1063 U ,
1 and a conductivity of 11.6 S m
1. The application
of the composite paper as a flexible double layer supercapacitor in an organic electrolyte (LiPF6)
displays a high capacity of 252 F g
1 at a current density of 1 A g
1 with respect to GNS. Moreover, the
paper can be used as the anode in a lithium battery, showing distinct charge and discharge
performances. The simple process for synthesising the GNS functionalized cellulose papers is attractive
for the development of high performance papers for electrical, electrochemical and multifunctional
applications.

1. Introduction
The introduction of an electric phase into a cellulose paper can
make it electrically active for applications such as antistatic
packages,1 electromagnetic shielding,2 electrodes, sensors3 and
electric smart brands.4 High performance flexible cellulose elec-
tric papers can be used for the development of novel paper
electronics and foldable energy storage devices.4–7 Traditional
cellulose-based electric paper is made with carbon black, metal
powders or carbon fibres as the electric fillers or as the conductive
deposition layers.8–10 The papers produced from these coarse
electric phases suffer from a weak adhesion and are subject to
degradation of the electric properties upon long services or under
severe bending.8 Coating the cellulose fibres with a thin electric
phase is considered an ideal approach to form high performance
electric papers to display the functional properties of the active
phase. This approach has been actively explored in the chemical
community via the chemical functionalization of cellulose fibres
with electric polymers and polyelectrolyte depositions.11–13
However, sophisticated chemical reactions are involved in this
process in order to produce sufficiently thick polymer coatings
on the cellulose fibres through multiple deposition cycles.14 Apart
Key Laboratory of Advanced Ceramics and Machining Technology
Ministry of Education, School of Materials Science and Engineering,
Tianjin University, Weijin Road 92, Nankai District, Tianjin 300072,
P. R. China. E-mail: liyali@tju.edu.cn; Tel: +86-22-27402187
† Electronic supplementary information (ESI) available. See DOI:
10.1039/c2nr30318c
from the low efficiency of these fabrications, the electric property
of the paper is limited by the low conductivity of the polymers.14
The recent development of one- and two dimensional carbon
structures (carbon nanotubes and graphene nanosheets) with
superior mechanical, electrical and thermal properties provide
novel nanoscale phases for the fabrication of high performance
functional papers. Cellulose composite papers were fabricated by
dispersing carbon nanotubes into cellulose papers2,14,15 or
imprinting them as a conductive layer,4,6,7 for the development of
flexible paper supercapacitors with promising high perfor-
mances. However, CNTs are difficult to disperse due to Van der
Waals forces and therefore require a larger amount to make the
electric connection in the paper due to agglomeration but at the
expense of the papers mechanical strength.14
Graphene is a novel two dimensional nanomaterial consisting
of mono- or small layers of graphite sheets with high specific
areas, superior mechanical properties, are electrically conductive
and have high thermal conductivity as well as other functional
properties.16 The flexible two-dimensional nanosheet geometry
of GNS, in combination with its high mechanical and electric
properties, make it an attractive material for the development of
novel electric or multifunctional cellulose papers.17–19 In the
present work, we report the fabrication of shelled GNS and
cellulose nanocomposite paper by dispersing chemically synthe-
sized GNS in a cellulose pulp and followed by infiltration. The
flexible GNS, stabilized by a surfactant in the mixed pulp, was
deposited onto the cellulose fibres and forms a coating under
controlled infiltrations (Fig. 1). The GNS coating forms
a continuous network through a bridge of cellulose fibres,

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Fig. 1 (a) A schematic of the dispersion and infiltration process for the
fabrication of the GNS/cellulose composite paper, involving the disper-
sion of the GNS nanosheets in water (stabilized by SDS) (a) and mixing
with a cellulose pulp (b) to form a homogeneous GNS and cellulose
dispersion (c), followed by infiltration to induce the deposition of GNS
onto the cellulose fiber (d) forming the final GNS-coated interconnected
cellulose composite paper (e).
providing a high electric conductivity whilst maintaining the
flexibility and toughness of the pure cellulose paper. This GNS
functionalized cellulose paper exhibits a high electrochemical
activity as an electrode in a supercapacitor and lithium battery
with a promising electrochemical performance.
2. Experimental
2.1 Fabrication of GNS/cellulose composite paper
Graphite oxide (GO) was synthesized by chemical oxidation of
the graphite powders using a mixture of H2SO4 and KMnO4
following the Hummers process.20 The GO powder was heated
at 1000  C for 1 h under argon to reduce GO into the GNS.
The GNS appears as winkled nanosheets with a lateral
dimension of 3 mm and contains 2–4 graphite monolayers.
This was observed under transmission electronic microscopy
(TEM, Tecnai G2 F20, Philip, Netherlands) by dispersing the
GNS powder in ethanol and dipping onto a copper grid
(Fig. 2). The GNS nanosheets are highly winkled, typical for
chemically synthesized GNS, which shows that they are flexible.
Fig. 2 TEM images of the GNS nanosheets used for the fabrication of
the GNS/cellulose composite paper: (a) typical morphologies and (b) an
edge view of a GNS nanosheet.
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X-ray photoelectron spectroscopy (XPS) analysis (Fig. S1†)
indicated the existence of 8.8 at.% oxygen in the GNS nano-
sheets as C–OH (12.4%), C]O (3.3%) and O]C–OH (1.0%).
The oxygen content and the C–O bonds are typical for ther-
mally reduced chemically synthesized GNS.21
The GNS powder was dispersed in water at a concentration of
0.33 mg ml
1, with the addition of sodium dodecylsulfate SDS
(CH3(CH2)11OSO3Na) as a surfactant (5 mmol ml
1). A cellulose
pulp was prepared at a concentration of 3 mg ml
1 by immersing
a filter paper into water followed by mechanical stirring for 20 h.
The GNS dispersion (30 ml) and the cellulose pulp (100 ml)
were mixed at a volume ratio of 0.3 with mechanical stirring for
30 min to form a homogeneous black mixed pulp of GNS and
cellulose fibres. The mixed pulp was moved to a filter (with a 7 cm
diameter) and infiltrated under evacuation. A black composite
paper was obtained by peeling the paper from the filter, pressing
between two plates and drying in an oven at 40  C for 10 h. A
pure cellulose paper was prepared in parallel as a reference, using
the same batch of cellulose pulp.
2.2 Characterizations
The morphologies and microstructures of the composite paper
were observed under scanning electronic microscopy (SEM,
XL30ESEM, Phlilps, Holland) by adhering a piece of the paper
onto a copper disc with conductive paste. The chemical struc-
tures of the paper were analyzed by Fourier transform infrared
spectroscopy (FTIR, FTS 6000, Bio-Rad, US) with KBr pellets
and by Raman spectroscopy (DXR, Thermo scientific, US) with
a 532 nm incident. The sheet resistance was measured by a four-
probe method using a multi-electrical measurement system
(SDY-5, Guangzhou, China). The tensile tests were conducted
on a micro tensile tester (XQ-1, Donghua, China) with a 10 mm
gauge length at a tensile velocity of 3 mm min
1.
2.3 Electrochemical measurements
The composite paper was used as an electrode for a super-
capacitor and an anode for a lithium battery. The electrolyte was
LiPF6 (1 M, ethylene carbonate, propylene carbonate, and
dimethyl carbonate with a volume ratio of 1 : 1 : 1). The super-
capacitor was assembled with two pieces of the composite paper
as the electrode, a PP/PE/PP film as the separator and two copper
foils as the current collector. The paper electrode had a weight of
2.5 mg and thickness of 200 mm. The supercapacitive behavior
was measured by cyclic voltammetry (CV) under a 1.5–1.5 V
voltage and scanning rates of 10–200 mV s
1. A galvanostatic
method in the voltage range of 0–3 V at current densities of
1–10 A g
1 on an electrochemical working station (CHI660C,
Chenhua, Shanghai, China) was also used. The specific capaci-
tance was obtained from the galvanostatic charge and discharge
measurement. The discharge time (Dt) and voltage (DV) were
obtained from the discharge curve. The specific capacitance was
calculated from the discharge current (I), Dt, DV, and the mass
(m) of GNS in the electrode was calculated according to the
equation: C ¼ (I  Dt)/(m  DV). The lithium battery was
assembled with the paper as the anode, lithium foil as the
counter, PP/PE/PP film as the separator and copper foil as the
current collector with a standard coin cell assembling process.
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The electrochemical measurements were conducted on a battery

testing system (LAND CT2001A, Wuhan Jinnuo, Wuhan,
China) in a potential range of 0–2.5 V vs. Li+/Li at three different
current densities (100, 200, 1000 mA g
1).

3. Results and discussion

3.1 The GNS/cellulose composite paper and characterizations
A homogeneous and stable black pulp, without any observable
sedimentation upon aging over three days, was formed by
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mixing the GNS dispersion and the cellulose pulp. The infil-
tration of the mixed pulp lead to the precipitation of cellulose
fibres and the deposition of GNS. The GNS tends to deposit on
the cellulose fibres, as this is the high energy site, and coats the
fibre via a hydrogen bonding interaction. A uniform black
composite paper was obtained as a thin disc with a 7 cm
diameter and a 210 mm thickness, containing 3.2 wt% of GNS.
Fig. 3a shows a photograph of the composite paper along with
a white cellulose paper fabricated in parallel as a comparison.
The paper size and thickness depended on the size of the
infiltrator and the amount of pulp. To demonstrate this,
a larger paper with a 15 cm diameter was fabricated using
a larger infiltrator (Fig. S2†).
Scanning electron microscopy (SEM) showed randomly
oriented crossed fibres, as shown in Fig. 4a. The fibres have a tap-
like morphology, typically 5–20 mm wide and 1 mm long,
similar to the morphology in the pure cellulose paper. Enlarged
views reveal the fiber has a thin coating of GNS, shown in Fig. 4b
and c, in contrast to the monolithic smooth surface of the pure
cellulose fiber (Fig. 4d). The GNS coating on the fibres is con-
nected through a bridge of cellulose fibres. Similar GNS-coated
fibres were observed beneath the surface layer after peeling off
the paper, indicating the homogeneous nano-coated structure
(Fig. S3†). The individual GNS nanosheet can be distinguished
Fig. 4 SEM images of the GNS/cellulose composite paper viewed on the
surface at a lower magnification (a), typical morphologies of the GNS
shelled cellulose fibers (b,c) and the neat cellulose fibers (d) from a pure
cellulose paper used for making the composite paper.
from the isolated flask of GNS. The GNS phase has a 2–5 mm
dimension and a thickness below 10 nm, which is on the scale of
that observed in the raw GNS powder.
The GNS/cellulose composite paper was characterized by
spectral analyses. The FTIR spectrum of the composite paper
(Fig. S4†) shows the typical absorption bands for cellulose22 and
GNS. The Raman spectrum of the composite paper in Fig. 5b
shows the G band at 1586 cm
1, D band at 1349 cm
1 and the 2D
band at 2691 cm
1, which are due to the GNS phase and the
characteristic bands at 1097 cm
1 and 2896 cm
1, which are due
to cellulose.23 The 2D band is an overtone of the D band and the
band characteristic carries the information on the structure of the
GNS.24,25 From the Raman shift (2691 cm
1) and the full width at
half maximum (45 cm
1) of the 2D band and according to the
relationship between the band shape and the GNS structure
reported in literature,24,25 it can be deduced that the GNS has 2–4
graphite sheet layers, which is in agreement with the TEM
observations.

Fig. 3 Photographs of the GNS/cellulose composite paper (black) with

a pure cellulose paper (white) as a comparison (a), the bent composite
paper, showing the flexibility of the paper (b), and a flexible super-
capacitor made with a composite paper adhered to copper foil as the Fig. 5 Raman spectra of the GNS/cellulose composite paper with a pure
electrical conductor (c). cellulose paper and GNS for comparisons.

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3.2 Electrical and mechanical properties of the composite paper min immersing. Moreover, the composite paper resists mechan-
ical scratching without separation of the GNS from the paper,
The formation of the continuous network of the GNS sheets
unlike the reference sample which can be readily scratched off.
through the cellulose fibres provides the paper with a high electric
The excellent physical and mechanical durability of the
conductivity. A four-probe measurement of the paper gave an
composite paper is due to the firm adhesion of the GNS phase as
average sheet resistance of 1063 U ,
1. The corresponding
a coating on the cellulose fibres and is important for practical
electrical conductivity is 11.6 S m
1 was calculated from the sheet
applications.
resistance and the thickness of the paper (210 mm). In contrast,
the cellulose paper reference is beyond the limit of the sheet
resistance in the 2  104 U ,
1 measurement. The conductivity 3.3 Electrochemical properties of the composite paper as
of the composite paper is much higher than 3 S m
1 for a CNT supercapacitors and lithium batteries
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and cellulose composite paper containing as much as 35 wt% of

the single walled CNTs, fabricated with similar dispersion and
infiltration,14 but the fraction of GNS here (3.2 wt%) is only one
tenth in comparison. Moreover, the electrical conductivity is
higher than 1.1 S m
1 for a nanofibrillated cellulose and GNS
composite paper with a similar GNS loading, prepared by
chemical functionalization and reduction of GO.18 The high
conductivity of the composite paper is related to the high
conductivity of the GNS, obtained by the thermal reduction and
homogeneous dispersion of GNS as a thin coating on the cellu-
lose fibres.
The GNS/cellulose paper is flexible and tough and can be
bent and fully restored freely (Fig. 3b). The tensile tests of the
GNS/cellulose paper gave a stress–strain curve which displays
a higher slope in comparison with the pure cellulose paper
(Fig. 6). The elastic modulus of the paper calculated from the
slope of the curve is 0.19 GPa, which is 58% higher than 0.12
GPa for the pure cellulose paper. The increased modulus could
be due to the mechanical locking of the cellulose fibres by the
GNS coating making it resistant to the inter-fibre sliding. The
elastic modulus increases but not at the expense of the strength
of the paper, which is 2.3 MPa and close to that of the pure
cellulose paper (2.8 MPa). The slight decrease in the strength
is associated with the reduced elongation of the composite
paper (2.8%) as compared with 4.0% for the pure cellulose
paper.
The GNS/cellulose composite paper has good stability against
liquid attack. This was tested by immersing the paper in water
and comparing with the paper containing the GNS coating by
direct infiltration (Fig. S5†). The shelled GNS cellulose paper did
not show any change after being immersed in water for over four
weeks, whereas the GNS coated papers became swollen in the
GNS coat and dropped from the paper into the water after 10
Fig. 6 Stress–strain curves of the GNS/cellulose composite paper and
a pure cellulose paper.
The electrochemical properties of the composite paper were
measured by using it as an electrode in a supercapacitor and an
anode in a lithium battery. The supercapacitor was made with
two pieces of the composite paper sandwiched with a piece of
PP/PE/PP as a separator, with the total thickness being 450 mm.
Cyclic voltammetry measurements of the double supercapacitor
in an organic electrolyte of LiPF6 shows a typical double
supercapacitive behavior (Fig. 7a). The galvanostatic
measurements were conducted at different current densities, as
shown in Fig. 7b. The capacitance is 8.5 F g
1 for the
composite paper obtained from the galvanostatic curve. The
capacitance with respect to the amount of GNS in the paper
(3.2 wt%) is 252 F g
1. The value is higher than that of 22 F g
1
for CNTs dispersed4 or imprinted on cellulose papers.6 It is also
higher than that of 120 F g
1 for GNS coated onto cellulose
paper, at a lower scanning rate of 1 mV S
1 in an aqueous
electrolyte of H2SO4.17 Moreover, the GNS/cellulose paper
exhibits a high energy density potential for high energy density
storage. The energy density attains 237 Wh kg
1 at 1 A g
1,
which is much higher than that of CNTs imprinted on CNT/
cellulose paper.4,6 The high electrochemical performance bene-
fits from the coated phase of the GNS and the good electrical
connection in the composite paper.
The capacitance decreases with the current density from 252 F
g
1 to 191 F g
1 at 2 A g
1 and to 150 F g
1 at 3.3 A g
1. Despite
the decrease, the energy density is still maintained at 153 Wh kg
1
and a powder density of 2.4 kW kg
1 at a current density of 2 A
g
1. The reduced capacitance at high current densities could be
due to the limited ion diffusion rate or the increased internal
resistance with the increasing charging rate.5,7
Moreover, a paper supercapacitor was made with the
composite paper adhered to copper foil as the current collector.
The composite paper can form a good contact with the copper
foil while remaining flexible and can be bent without separation
(Fig. 3c). The electrochemical measurement gave a CV profile
which shows typical double layer supercapacitive behavior
(Fig. 7d). Therefore, the composite paper can be coupled with
metal foils for the development of flexible paper-metal
electrodes.
Finally, the composite paper was used as an additive-free paper
anode for a lithium battery with a promisingly high charge and
discharge performance. The GNS anode shows a high initial
discharge capacity of 670–1970 mA h g
1 at the first cycle (Fig. 7e).
The initial discharge capacity is in the range of 540–2040 mA h g
1
for the GNS anode in the lithium battery.26–28 The charge and
discharge profiles, given in Fig. 7f, show the major lithium inter-
calation and deintercalation occurs in the potential range below
0.5 V (vs. Li/Li+). The inter/deintercalations in this potential range

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Fig. 7 Electrochemical properties of the GNS/cellulose composite paper supercapacitor (a–d) and lithium battery (e and f): (a) cyclic voltammograms
(CV) measured at 10 mV S
1. (b) Charge and discharge curve measured at 1 A g
1 and 2 A g
1 in 0–3 V. (c) Specific capacitance of GNS at 1, 2, 3.3, 5, 10 A
g
1. (d) A CV profile of a paper supercapacitor measured at 100 mV s
1 in
0.1 to 0.5 V. (e) Discharge capacitance of the lithium battery after different cycles
at the three different current densities. (f) Charge and discharge profiles for the 1, 2, 10, 20 and 45 cycles measured at a current density of 100 mA g
1.

is associated with the insertion of lithium ions into the graphene
planes.26 The first cycle discharge (lithium insertion) shows a step
at around 1.45 V which is due to the formation of a solid elec-
trolyte interface (SEI) layer on the electrode.29 The discharge
capacity becomes stable after 10 cycles with a reversible capacity
of 257 mA h g
1. The reversible capacity (257 mA h g
1) is higher
than that of a CNT/cellulose cathode (140 mA h g
1)5 and GNS
papers (80 mA h g
1).28,29 Higher charge and discharge capac-
ities of 290–460 mA h g
1 are reported for GNS powders mixed
with conductive agents as the anode in a lithium battery.26,27
However, the capacities decrease continuously with the cycle
number over 20 cycles. In comparison, our composite paper
anode shows a greater stability is reached after a few cycles of
charging and discharging performance. The Columbia efficiency
of the composite anode is high than 95% over the 45 cycles
measured. At higher current densities, the composite paper anode
still displays the similar stable charging and discharging behavior,
showing the potential of the composite paper as a lithium anode
for high energy density storage.
4. Conclusions
A GNS/cellulose composite paper was fabricated via a simple
paper making process by dispersion of GNS into a cellulose pulp
followed by infiltration. The GNS was able to deposit onto the
cellulose fiber and form a coating via infiltration- induced
deposition. The GNS coating on the cellulose fibres forms
a continuous phase through a bridge of the cellulose fibres,
providing the paper with a high electrical conductivity and
electrochemical activity. The GNS/cellulose is flexible and
mechanically tough and has good durability against liquid attack
and mechanical scratching. It can be used as flexible electrodes
for supercapacitors and lithium batteries with promising high
electrochemical performances.

3252 | Nanoscale, 2012, 4, 3248–3253 This journal is ª The Royal Society of Chemistry 2012

Acknowledgements
This work is supported by the National Basic Research Program
of China (Grant. No. 2010CB934700), and Key Grant Project of
Chinese Ministry of Education (309010), Fund of Key Labora-
tory of Advanced Ceramics and Machining Technology (Tianjin
University) Ministry of Education (ACMT-2008-03).
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