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A Large-Area, Flexible, and Flame-Retardant
Graphene Paper
Liye Dong, Chuangang Hu, Long Song, Xianke Huang, Nan Chen,* and Liangti Qu*
Similar to the paper-making process, the efficient flame retardant graphene
paper is conveniently obtained by using graphene oxide (GO) and
hexachlorocyclotriphosphazene (HCCP) aqueous pulp. The “paper pulp”
can also conceivably be used as ink to make other hydrophilic films become
flame retardant paper. Further, the as-prepared reduced GO-HCCP paper
(RGO-HCCP paper), compared with GO-HCCP paper, can maintain its intact
structure for a longer time in an ethanol flame. As a consequence of these
preparation methods, the bearing temperature of the as-prepared graphene
papers shows a significant increase.
1. Introduction
A wide range of potential applications for graphene have been
proposed based on the unique structures and multitude of
outstanding properties.[1] Graphene extends to various fields
including catalysts,[2] conductive substrates,[3] water treat-
ment,[4] and electrode materials for energy storage devices.[5]
Nevertheless, having been shown that graphene has a profound
impact in many areas, it should be noted that improving the
thermal stability of graphene still represents a challenge which
will greatly restrict the field of application in various aspects
due to its low decomposition temperature (below 600 °C in
air).[6] Actually, graphene’s unique 2D layered structure makes
it seem to be having a retardant effect, for it can act as a
carbon donor to allow an insulating cellular carbonaceous layer
(char).[7] The 2D sheet structure, with lamellae blocking effect,
can delay the heat transfer, pyrolysis products of diffusion and
escape, and oxygen diffusion and mixing.[8] But these proper-
ties of graphene will hardly suffice. Scientific research about
flame retardant graphene so far is scant.[9] In general, fire-
retardant materials generally contain elements such as nitrogen
and phosphorus.[9a] The two elements may be added in the
form of an additive to the substrate or incorporated into the
L. Dong, Dr. C. Hu, L. Song, X. Huang,
Dr. N. Chen, Prof. L. Qu
Key Laboratory of Cluster Science
Ministry of Education of China
Key Laboratory of Photoelectric/Electrophotonic
Conversion Materials
School of Chemistry
Beijing Institute of Technology
Beijing 100081, China
E-mail: gabechain@bit.edu.cn; lqu@bit.edu.cn
DOI: 10.1002/adfm.201504470
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structure of the materials. Nitrogen can
serve as foaming agent and produce large
volumes of noncombustible gases such
as N2, NH3, and NxOy when burning.[10]
On the other hand, the addition of phos-
phorus is to form, during the combustion,
an impermeable, semisolid, and vitreous
layer essentially composed of polyphos-
phoric acid and to activate the process of
formation of intumescence.[11] The flame
retardants, including nitrogen and phos-
phorus atoms, are used to improve the fire
resistance owing to the synergistic flame
retardant effect.[12]
Hexachlorocyclotriphosphazene (HCCP), with the formula
(N3P3Cl6), is constructed with alternating nitrogen and phos-
phorus atoms in a hexatomic ring structure.[13] The six P−Cl
bonds every HCCP molecule possesses are capable of reacting
with a variety of nucleophiles. The product after substitution
has a P=N inorganic backbone. Graphene oxide (GO) sheets
decorated by oxygen-containing groups can form a piece of
self-assembled paper through π−π stacking-induced crosslink
effect.[14] Therefore, the use of HCCP-modified graphene oxide
paper and reduced graphene oxide (RGO) paper will be condu-
cive to the thermal stability by introducing nitrogen and phos-
phorus atoms.
2. Results and Discussions
We employed the evaporation-induced self-assembly (EISA)
method to prepare the GO-HCCP paper, which was a facile
and time-saving method.[15] Figure 1a shows the preparation
process of GO-HCCP paper clearly. The large-area GO-HCCP
paper with high quality is displayed in Figure 1b. Addition-
ally, the paper can be adjusted to a bigger degree by using a
container with a larger bottom surface and cut into different
pieces. The GO-HCCP papers can also be folded into a variety
of shapes like paper as shown in Figure 1c (a paper airplane).
We chose scanning electron microscope (SEM) to observe the
micromorphology of the as-synthesized GO-HCCP paper. The
fracture morphology of the GO-HCCP paper was shown in
Figure 1d. Graphene oxide layers stack together to form layered
structure with a thickness of about 15 µm due to van der Waals
forces between graphene layers and HCCP with hexatomic
rings. Furthermore, EISA method was able to generate ripples
on the surface of GO-HCCP paper as shown in Figure 1e. The
self-assembled ripples in the GO-HCCP surface could be real-
ized by utilizing the stress relief process in buckling which usu-
ally leads to the formation of random twists and wrinkles.[16]
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Figure 1. a) Preparation process of the GO-HCCP paper. b) The photo of the large-area GO-HCCP paper (200 mm × 300 mm). c) Photograph of
GO-HCCP paper, it is soft and flexible enough to make a paper airplane. The SEM image of the d) fractured cross sections and e) surface of the GO-
HCCP paper.

The energy dispersive of X-ray analysis (EDS) elemental map-
ping is shown in Figure 2a, in conjunction with EDX element
content (Table S1, see the Supporting Information), revealing
that the GO-HCCP paper is mainly composed of C, N, O, P,
and Cl elements, confirming the existence of HCCP molecules
in the GO-HCCP paper. Raman spectra were conducted at
room temperature, as shown in the Figure 2b. The spectra con-
sist of two well-known and characteristic GO bands at 1348 and
1594 cm−1, respectively. The ratio between the D and G bands
(ID/IG) can be used to estimate the degree of structural disorder
and/or amorphous compounds in sp2-based carbons. The ID/IG
value of GO was calculated to be 0.98, while that of GO-HCCP
was higher (ID/IG = 1.13). This result indicates that the increase
in the ID/IG values can be attributed to the increased disorder
due to the insert of HCCP molecules between the graphene
sheets. This was also confirmed by the following structural
characterization.
In the pristine GO, the interlayer distance (d-spacing) is just
7.49 Å (2θ = 11.8°), which is well consistent with the previous
report.[17] However, in GO-HCCP paper, in which the distance
between graphene layers is about 9.81 Å (2θ = 9.0°), as shown
in Figure 2c. The extended interlayer distance of graphene
stacks can be attributed to the insertion of HCCP molecules
into GO flakes. Moreover, we found that the interlayer distance
of graphene stacks could further increase with the increasing
of mass loading of HCCP molecules (Figure S1, Supporting
Information). It means more HCCP molecules and function-
alities can readily intercalate between the graphene stacks. This
result suggested an increasing of the interlayer distance in
GO-HCCP paper.

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Figure 2. a) The EDS of GO-HCCP paper. b) The Raman, c) XRD, and d) FTIR spectra of GO and GO-HCCP paper, respectively. e) High-resolution XPS
spectra of the C 1s of GO-HCCP paper. f) The typical stress–strain curves of the GO and GO-HCCP paper.
Fourier transform infrared spectroscopy (FTIR) spectra of GO
and GO-HCCP illustrated in Figure 2d also confirm the suc-
cessful synthesis of GO-HCCP paper. The broad and intense
peak of O−H groups centered at 3431 cm−1 and the C−O
stretching peak centered at 1086 cm−1. The peak at 1734 cm−1
was the characteristic of C=O stretch of carboxyl groups situated
at the edges of the GO sheets. In the spectrum of the as-prepared
GO-HCCP, two peaks at 873 and 1214 cm−1 were assigned to the
vibration of N−P and N=P bonds, respectively, which could also
be observed in the spectrum of HCCP molecules (Figure S2,
Supporting Information).[18] The appearance of a new peak at
988 cm−1 was clearly observed, which was attributed to C−O−P
vibration,[19] indicating that a new chemical bond is formed by
the reaction of GO nanosheets and HCCP molecules.
The X-ray photoelectron spectroscopy (XPS) is also a useful
analysis technique that can provide information on the type of
functional groups and is conducted to further verify the reac-
tion between GO and HCCP. Figure 2e presents the high-res-
olution XPS C 1s spectra of GO-HCCP, we could observe the
appearance of the C−O−P to further verify the strong covalent
cross-linking between GO and HCCP molecules, which was
consistent with the IR spectra.[20]
The typical strain–stress curves of GO-HCCP paper are
shown in Figure 2f. Adding appropriate amount of HCCP mole-
cules to GO flakes to increase the tensile strength of GO-HCCP
(the mass ration ratio of GO: HCCP is 1: 0.5) paper can greatly
improve the mechanical properties. Furthermore, a wrinkled
surface texture, as shown in Figure 1e, could create mechanical
interlocking and load transfer between GO flakes and HCCP
molecules, leading to an improved mechanical strength.[21]
However, along with the increasing of HCCP molecules in
GO-HCCP paper (the mass ration ratio of GO: HCCP is 1: 1),
bonding between the GO flakes becomes weak, which causes
them to slide out of the initial position under a load much
lower than the strength of the GO-HCCP paper with the mass
ration ratio of 1: 0.5 (GO: HCCP) in Figure S3 (Supporting
Information). Moreover, such small HCCP molecules cause
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functional groups to attach to the surface of GO (increased
functionalization), which reduces van der Waals and covalent
cross-linking forces between the GO flakes and decreases the
energy required to pull them from the initial position. As a
result, the tensile strength of GO-HCCP paper could reach up
to 240 MPa, which was about 4.5 times higher than that of the
individual GO paper with 53 MPa.
Thermogravimetric analysis (TGA) was employed to evaluate
the thermal stability. The first stage of main mass loss in GO
occurred at about 190–220 °C, due to the decomposition of
oxygen-containing groups, which is the same as the GO-HCCP
paper. GO-HCCP paper exhibits higher stability in comparison
to GO paper in the second stage of TGA with a heating rate
of 10 °C min−1 as shown in Figure S4a,b (Supporting Informa-
tion), largely resulted from the loading HCCP molecules as the
good physical barrier effect between the GO layers. Meanwhile,
HCCP mainly reacts with the functional groups on graphene
to generate the esterifiable and cross-linking char layer during
combustion, which is consistent with the FTIR results. GO
paper and GO-HCCP paper were thermally unstable and started
to lose mass upon heating even below 100 °C, which was attrib-
uted to the volatilization of stored water in its π-stacked struc-
ture. The main loss of GO-HCCP paper began from about
750 to 900 °C, which was attributable to the decomposition of
the graphitic framework in air. Both the residual during thermal
degradation and combustion are important for fire-safety appli-
cations. There was almost no residual at 600 °C for pure GO
paper, while the residue yield of the RGO-HCCP paper is
54%, so it was actually entirely from the graphene oxide. From
these comparisons, it is clear that the added HCCP molecules
contribute to the fire resistance.
In order to check the real performance of GO-HCCP paper
in a combustion environment, we chose the ethanol flame
with a temperature of about 600–800 °C, which is close to the
bearing temperature of GO-HCCP paper in air. Subsequently,
the GO and GO-HCCP paper were placed synchronously in the
ethanol flame (Figure S4c,d and Movies S1 and S2, Supporting
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Figure 3. SEM observation of the a) filter paper, b) GO@filter paper, and c) the GO-HCCP@filter paper. d) Combustion process of the filter paper,
e) GO-HCCP@filter paper. f) Photos of the samples mentioned above before and after burning.
Information). The pristine GO paper completely burned off in
50 s. On the other hand, the GO-HCCP paper maintained the
initial shape with little shrinkage and without catching fire in
50 s. Even after 90 s, there was no further change in the shape
of GO-HCCP paper.
Having confirmed the structure of GO-HCCP and its dis-
persibility in water, we prepared a concentrated GO-HCCP
ink (5 mg mL−1) for further investigation of flame retardant
applications. The easily ignited filter paper was chosen as the
basement to measure the fire resistance. For the preparation of
flame retardation samples, we dipped the filter papers (10 mm ×
15 mm) into the GO-HCCP ink and confirmed that the ink
had soaked through the thin filter papers before drying. Finally,
we obtained two kinds of infiltrated filter papers with a small
load of 1 mg GO and GO-HCCP. As shown in Figure 3a, filter
papers are made of cotton fibers which are highly combustible.
Both in the Figure 3b,c, the filter papers have been coated with
GO or GO-HCCP ink. Naturally, we call them GO@filter paper
and GO-HCCP@filter paper here, respectively. The combus-
tions of the filter paper, GO@filter paper, and GO-HCCP@
filter paper in the ethanol flame are shown in Figure 3d–f. As
Figure 3f shows the GO-HCCP@filter paper can hold its shape
with some crimp under combustion for 90 s. For the compar-
ison, the filter paper completely burned off only in 5 s. Mean-
while, the GO@filter paper also could not maintain its initial
shape and burned in seconds.
The flame retardant coating GO-HCCP ink can also be coated
onto some other flammable films such as nonwoven fabrics. It
also performed excellent fire resistance (Figure S5, Supporting
Information). The GO-HCCP ink can be regarded as intumes-
cent coating containing a carbon source, an acid source, and a
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blowing agent.[22] GO could be considered as the carbon source,
while both the acid source and the blowing agent derived from
the HCCP.
In other words, GO is a material that has a large number of
functional groups (oxygen-containing groups), having a high
reactivity at high temperature. In order to obtain anoxic GO,
it is necessary to remove the oxygen-containing groups, that
is, reduce GO to better fire resistance RGO. We fabricated
the RGO-HCCP paper, as shown in Figure 4a, by thermal
reduction with thermocompressor to 300 °C. In this way, it
has been developed to RGO, while maintaining its high-flex-
ibility (Figure 4a, inset) as well as giving it a much higher
flame retardant property than its original form. The obtained
RGO-HCCP paper is composed of aligned RGO sheets with
numerous twists and wrinkles than the GO-HCCP paper
due to the decrease of oxygen functional groups, as shown
in Figure 4b. The more twists and wrinkles existed on RGO-
HCCP paper are believed to be more difficult for the non-
combustible gas produced by the N and P containing func-
tional groups to escape from the intervals. Figure 4c shows
transmission electron microscope (TEM) images of RGO-
HCCP paper. There are many dots derived from HCCP mol-
ecules on the graphene sheets. The distance between gra-
phene layers of RGO-HCCP paper is smaller at about 3.6 Å
(2θ = 24.7°, as shown in Figure 4d) than that of GO-HCCP
paper. We can infer that the distance of the layer is decreased
resulting from the remove of the oxygen-containing groups.
Furthermore, note that the ID/IG ratio of RGO-HCCP paper
increased from 0.98 to 1.04 compared with GO-HCCP paper,
as shown in the Raman spectra (Figure 4e). The ID/IG ratio
was increased when the GO reduced as the graphene because
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Figure 4. a) The photo of the large-area RGO-HCCP paper, the inset shows that RGO-HCCP
paper is flexible. b) The SEM and c) TEM images of the RGO-HCCP paper. d) The XRD, e) Raman
spectra, f) high-resolution N1s peaks, and g) high-resolution P2p peaks of RGO-HCCP paper.
of the induced defect sites and destruction in the carbon lat-
tice. The EDS and XPS further verify the presence of N and
P in RGO-HCCP paper and N, P bonding modes. The high-
resolution N1s XPS spectra (Figure 4f) can be fitted with
three different peaks which can be assigned to the nitrogen
in aromatic pyrrole-containing (400.2 eV) or pyridine-con-
taining compounds (399.1 eV) and the quaternary nitrogen
(401.8 eV), respectively.[5a,23] The High-resolution XPS spectra
with curve fittings for p2p spectra of RGO-HCCP could be
deconvoluted into two peaks (Figure 4g). The peaks at 134.3
and 133.6 eV were P−O and C−PO3,[24] which played impor-
tant roles in the fire resistance.
The impact of fire in GO-HCCP paper was limited due
to the presence of an abundant number of hydroxyl groups
on the basal plane of GO layers. Consequently, the hydroxyl
functional groups in the GO-HCCP paper can be effectively
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removed and subsequently turned into
RGO-HCCP paper by thermal reduction, so
as to improve the fire resistance. The flame
retardancy of RGO and RGO-HCCP papers
is shown in Figure 5a,b (see Movies S3 and
S4 for details in the Supporting Informa-
tion). By contrast, the pristine GO paper
has been severely deformed in 90 s. How-
ever, RGO-HCCP paper maintained its ini-
tial shape with little shrinkage and without
catching fire in 90 s. The flame retardancy
of RGO-HCCP paper is more superior to
that of RGO paper. The mass-loss rate can
be used to characterize the flame retardant
properties of these materials correctly. The
TGA curves of RGO and RGO-HCCP paper
are presented in Figure 5c. The main mass-
loss stage occurred between about 500 and
600 °C for the RGO paper. RGO paper was
burned out when the temperature reached
600 °C, while the residue yield of the RGO-
HCCP paper was more than 80%. The tem-
perature range of RGO-HCCP paper main
mass-loss was from 650 to 850 °C, which
was significantly higher than the RGO
paper.
It comes down to the following aspects:
the thermal condensation of phosphoric acid
into pyrophosphonic acid and metaphos-
phonic acid, the generation of nitrogen con-
taining noncombustible gas,[25] heat being
taken away by gas, releasing water as a
byproduct,[9a,26] and the subsequent decom-
position of the graphitic framework in air.
When the temperature is as high as 900 °C,
the remaining quality is still in excess by
10%. The results show that the RGO-HCCP
paper has much higher flame retardation
effect than the RGO paper. The research of
combustion products is also helpful to ana-
lyze the mechanism of flame retardant prop-
erties. The as-obtained combustion products
are also fully characterized by XRD, Raman,
and EDS component analysis. Results from XRD show that
the interlayer distance of the burned RGO-HCCP paper is
about 3.4 Å in Figure 5d (2θ is close to 26.5°, the [002] peak
of graphite).[27] We can infer that the distance of the layer was
decreased resulting from the remove of the grafted functional
groups. In Figure 5e, we see that the intensity ratio of the ID/IG
of the RGO-HCCP increased (ID/IG = 1.04) as it is converted
into graphene flakes with more defects in burned RGO-HCCP
(ID/IG = 1.23). The elemental mappings revealed the distribu-
tion of nitrogen and phosphorus dots onto the graphene flakes
in Figure 5g, which was also confirmed by the corresponding
EDS (Table S1, Supporting Information). The dots containing
nitrogen and phosphorus atoms were of great importance for
the fire resistance.
The GO-HCCP paper and RGO-HCCP paper were attached
to two separate circuits containing a mini LED, as shown in
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Figure 5. a) Snapshots of flame treatments of RGO (upside) and b) RGO-HCCP (below) with respect to time in 90 s. The images were captured from
the video in Movies S3 and S4 (see the Supporting Information). c) TGA of the RGO and RGO-HCCP paper. d) The XRD of the burned RGO-HCCP.
e) The Raman spectra of the burned RGO-HCCP. f) The STEM image of the sheet of the burned RGO-HCCP and elemental mappings of C, N, O, and
P, respectively.

Figure 6. Interestingly, due to extremely poor electrical con-

ductivity, the mini LED in the GO-HCCP paper circuit could
not be lit (Figure 6a). When GO-HCCP paper was placed in the
ethanol flame, graphitization occurred and caused the increase
of the electric conductivity, then the mini LED was lit (Figure 6b
and Movie S5, Supporting Information). In practice, it can be
used as a warning device for flame. Separately, the RGO-HCCP
paper can be used as a wire in the circuit both at room tem-
perature environment and in ethanol flame (Figure 6c,d and
Movie S6, Supporting Information). This is due to its effective
flame retardant and excellent conductive properties (the con-
ductivity of RGO-HCCP paper before and after burning was
shown in Table S2, Supporting Information).

Figure 6. a) Circuit constructed by an LED and GO-HCCP paper. b) The
LED can be lighted when the GO-HCCP paper is heated to glowing red.
c) Circuit constructed by an LED and RGO-HCCP paper. d) Circuit in the
flame can still work normally, LED is bright. The images were captured
from the video in movies S5 and S6 (Supporting Information).
3. Conclusion
In summary, we have developed a piece of free-standing gra-
phene paper which can be used as an efficient flame retardant.
The compound containing nitrogen and phosphorus atoms
produced by HCCP molecules has made a big contribution to
the fire resistance. The as-prepared GO-HCCP paper shows a
good flame retardant property in combustion. The GO-HCCP
ink can be coated onto any basement to obtain the fire resist-
ance as the flame retardant protective clothing. Furthermore,
the synthesized RGO-HCCP flame retardant paper has a signif-
icant promotion on the flame-retardant behavior after thermal

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reduction than the GO-HCCP flame retardant paper. All the
results indicate that these flame retardant graphene papers
can be good candidates for flame retardancy and have potential
applications in some areas such as civil, military, and aerospace
flame retardant fields.
4. Experimental Section
Materials and Sample Fabrication: The detailed fabrication procedure
of the RGO-HCCP paper is as follows. The GO solution was first
diluted with deionized water to 5 mg mL–1. At the same time, the
HCCP molecules were dissolved in N,N-dimethylformamide solution
(25 mg mL–1). Then, the two aforementioned solutions were mixed with
continuous stirring. The mixed solution was transferred into an oven at
45 °C for about 2 d, then the GO sheets and the HCCP molecules would
be assembled into GO-HCCP with layer-by-layer structure at a liquid–
air interface via slow evaporation. The thicknesses and sizes of the
GO-HCCP paper can be controlled by the added amounts of GO-HCCP
solution and the sizes of mold containers.
Characterizations: The morphology of the as-prepared samples was
investigated by scanning (SEM, JSM-7500F) and transmission (TEM,
7650B, Hitachi) electron microscopy. The XRD analysis was carried out
on D8 advanced X-ray diffractometer with Cu Kα radiation (λ = 1.5418 Å).
Raman spectra were recorded using a RM 2000 Microscopic Confocal
Raman Spectrometer (Renishaw PLC, England) with a 514.5 nm laser. XPS
data were obtained with an ESCALab220i-XL electron spectrometer from
VG Scientific using 300W Al Kα radiation. The elemental mappings were
performed on a scanning transmission electron microscope unit with high-
angle annular dark-field detector (HITACHI S-5500) operating at 30 kV.
Electrical conductivity was measured by a four-point probe technique.
Supporting Information
Supporting Information is available from the Wiley Online Library or
from the author.
Acknowledgements
This work was sponsored by NSFC (Grant Nos. 21325415, 21174019,
21301018), National Basic Research Program of China (2011CB013000),
and Beijing Natural Science Foundation (2152028).
Received: October 19, 2015
Revised: November 20, 2015
Published online: January 27, 2016
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