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FEATURE ARTICLE
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Recent developments in superhydrophobic graphene

Cite this: DOI: 10.1039/x0xx00000x
and graphene-related materials: from preparation to
potential applications
Jian-Nan Wang,a Yong-Lai Zhang,a,* Yan Liu,c Wanhua Zheng, d Luke P. Lee b and

Nanoscale Accepted Manuscript

Received 00th January 2012, Hong-Bo Suna,*
Accepted 00th January 2012

DOI: 10.1039/x0xx00000x In the past decade, graphene has revealed a cornucopia of both fundamental science and
potential applications due to its exceptional electrical, mechanical, thermal, and optical
www.rsc.org/
properties. Recently, increasing efforts have been devoted to exploit its new features, for
example, wetting properties. Benefit from its inherent material character, graphene shows great
potential for the fabrication of superhydrophobic surfaces that could be potentially used for
various anti-water applications. In this review, we summarize the recent developments in
superhydrophobic graphene and graphene-related materials. Preparation strategies using pure
graphene, graphene oxide, and graphene/polymer hybrids are presented; their potential
applications are discussed. Finally, the perspective of this dynamic field including both current
challenges and future demands has been discussed based on our own opinion. It is anticipated
that the cooperation of the numerous merits of graphene and superhydrophobicity will bring
new opportunities for high-performance multifunctional devices.

Introduction years. To construct binary micro/nanostructures from planar

Recent years have witnessed the increasing research interests in
graphene and the graphene-related materials, since they have
exhibited many fantabulous properties in a mere decade,
including ultra-high carrier mobility, 1-3 optical transmittance,4,5
high mechanical strength,6,7 high thermal conductivity,8
flexibility,9 chemical stability10 and biocompatibiliy.11,12 Thus
exceptional characters have made them superb choices in a
variety of applications, for example, transistors,13-16
electrodes,9,17,18 microsensors,19-21 supercapacitors,22-26 and
optoelectronic devices. 27-31 Beyond the studies that mainly
focus on their electronic properties, great efforts have also been
devoted to the surface wettability control of graphene and its
related materials, as a comprehensive understanding of the
surface property of graphene is highly desired in both
fundamental science and practical applications, especially for
exploiting new functionalities and utilizations.
Wetting behaviors of solid substrates have long been
investigated under the continued stimulation of the broad
applications both in daily life and commercial production.32,33
Generally, the surface wettability is mainly governed by the
physical architecture and the chemical composition, so solid
surfaces with extreme hydrophobicity can be rationally created
by combining hierarchical roughness and low-surface-energy
materials.34-36 According to this line, superhydrophobic
graphene surfaces have been successfully obtained in recent
graphene, a series of technologies have been employed, such as
self-assembly, electrospinning, freeze-dry; and structured
graphene surfaces with various two-dimensional or stereo
configurations have been realized, remarkably increasing the
surface roughness. Additionally, graphene and its related
materials can work as nice building blocks to construct
complicated layered assemblies, for instance through layer-by-
layer assembly;37 and the organized structures may contribute
to their surface topology control.38 On the other hand, to
generate low-surface-energy coatings, several kinds of
strategies have been generally used, for example, direct
utilization of low-surface-energy materials, modification of
low-surface-energy layers on the prepared rough surface using
molecular grafting, and post removal of surface hydrophilic
functional groups. In view of the processing capability and the
modification flexibility both brought by the abundant oxygen-
containing groups (OCGs), chemically exfoliated graphene
oxide (GO) has been firstly chosen as a preferred starting
material to achieve superhydrophobic graphene surfaces. With
the rapid progress of graphene science, high quality graphene
could be acquired by multiple means, such as chemical vapor
deposition (CVD), laser treatment, or even commercially
available in different sizes and states, which enriches the
approaches to the super-nonwetting graphene surfaces.
Gradually, investigations on the dewetting properties of

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graphene and graphene-related materials have emerged as an
active research field, which is evidenced by the evergrowing
published literatures. In the process of summarizing the
pertinent researches, we found that superhydrophobic graphene
surfaces inspired from nature creatures have attracted numerous
curious eyes of scientists from different realms including
chemistry, physics, biology, electronics, and tissue engineering.
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It has been revealed that the cooperation of graphene and
superhydrophobicity will promote the development of non-
wetting researches and provide opportunities to develop novel
graphene-based devices.
In this review, we focus on the recent developments in the
superhydrophobic graphene and graphene-related materials.
The article starts with a brief presentation of the wettability of
graphene and graphene oxide. Then, a comprehensive review of
the preparation methods is summarized in the second section,
grouped by the material categories. In the following part,
potential applications of these functional surfaces are presented
one by one. Finally, a brief discussion of the current state and
the future challenges in this area is provided in our own
perspective.
Fundamentals of superhydrophobic materials
Basic principle for the construction of superhydrophobic
surfaces
Superhydrophopbic surfaces are solid surfaces that are
extremely difficult to wet; the contact angle (CA) of a water
droplet on such a surface is larger than 150°, and roll-off
angle/contact angle hysteresis is less than 10°. For an absolutely
flat surface, wettability is determined by the surface free energy
of the solid, which can be described by the Young’s equation
(Fig. 1a).39
 sv   sl
cos Y  (1)
 lv
where γsv, γsl, γlv are the surface free energy of solid-gas, solid-
liquid, liquid-gas interfaces involved in the system, respectively.
According to this equation, a solid material with low-surface-
energy is necessary to achieve high CA. But it is not the only
factor. For a real surface that is usually rough, topological
roughness plays a crucial role in the wetting behavior of solid
surfaces. To explain the relationship between surface roughness
and wettability, two classical empirical models, Wenzel regime
and Cassie-baxter regime, have been extracted from various
experimental data. In Wenzel’s model,40 it is assumed that
liquid completely fills the grooves of the rough surface (Figure
1b), so the relationship can be explained by the following
equation.
cos W  r cos 0 (2)
where r is the surface roughness factor defined as the ratio of
the true surface contact area to the projection area, θW is the
apparent contact angle in the Wenzel model, and θ0 is the
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contact angle for liquid droplet on an ideal flat surface. The
surface roughness could amplify the original wetting nature of
the surface, either hydrophobic or hydrophilic.
In contrast, for Cassie’s case, liquid is assumed to sit on
the top of surface protrusions with air pockets strapped below
(Figure 1c). The effect of the solid/air composite interface on
the CA of surface can be derived by the following equation: 41
cos CB  f1 cos 1  f 2 cos 2 (3)
where θCB is the apparent contact angle in the Cassie-Baxter
model, f1 and f2 are the fractional areas of the solid and air of
the surface, respectively, θ1 and θ2 are the CAs for flat solid
surface and air, respectively. And we have f1+f2=1, θ2=180°as
Nanoscale Accepted Manuscript
air is considered as a completely non-wetting material. Then
equation 3 can be derived as:
cosCB  f1 cos1  1  1
(4)
Therefore, a high CA may be achieved by increasing the
surface roughness or introducing more buried air bubbles.
The above theories have been successfully adopted to
explain the underlying mechanism of the famous “lotus effect”.
It has been found that both the hierarchical micro-
nanostructures (randomly distributed micropapillaes and fine
branch-like nanostructures) and the epicuticular wax materials
(low surface energy coating) are responsible for the self-
cleaning property, in agreement with above theories.
Fig. 1 Schematic illustration of the wetting behavior of a water droplet on
different solid substrates. (a) Young’s model. (b) Wenzel’s model. (c) Cassie’s
model.
Surface wettability of graphene and graphene oxides
Surface wettability of graphene sheets plays a vital role in
determining the compatibility with the desired environment. So
a deep-understanding the wettability of graphene and its related
materials is fundamentally important for the development of
graphene-based devices. Recently, several experimental and
simulation studies have been focused on the surface property
and wettability of graphene films. Based on density functional
theory, Leenaerts et al.42 indicated that graphene is strongly
hydrophobic. They concluded that the binding energies between
water molecules are larger than the associated adsorption
energies on the graphene surface, such that water molecules
form clusters on the graphene sheet. Quantum molecular
dynamic simulations afford fundamental insight into the
wetting behavior of water nanodroplet on a free-standing
single-layer graphene sheet, and also allow incorporation of the
polarization interaction, main-body effect and hydrogen-bond
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interactions into the prediction of wettability. The simulation
results show that the graphene sheet yields a CA of 87°.43
Compared with the theoretical results, graphene grown by CVD
gives a CA of 89.4°.44 Besides, Shin et al.45 reported that
epitaxial graphene has a static contact angle (CA) of 92°and is
slightly hydrophobic regardless of its thickness, close to that of
highly ordered pyrolytic graphite (91°), while graphene reduced
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by hydrazine has a CA of 127°and a small interfacial energy
with water. Proved both theoretically and experimentally,
graphene has a natural hydrophobicity, which is essential to
understand the wetting behavior of water on the surface of such
material.
In addition to pristine graphene, another important
graphene-related material that has been widely used for the
fabrication of graphene-based devices is GO. GO is prepared by
chemical exfoliation of natural graphite, and could be
considered as a derivative of graphene with oxygen functional
groups on their basal planes and edges. Due to the presence of
OCGs, GO could be well dispersed in polar solvents such as
water. The ease of synthesis and the solution processing
capability make GO a promising precursor for the preparation
of superhydrophobic graphene surfaces. The wettability of GO
film is influenced by the contents of OCGs on the surface. With
various levels of oxidization, GO films exhibit different wetting
properties. For instance, GO film has a CA 67.4°46 compared to
that of 30.7°.47 Invariably, GO shows hydrophilicity owing to
the chemical nature of the groups, such as carboxyl, hydroxyl
and epoxy. To further increase its hydrophobicity, proper
reduction treatments (e.g., hydrazine reduction; thermal
annealing; photoreduction) would be implemented, drastically
or partially removal of the hydrophilic OCGs would lower its
surface energy, giving rise to much higher water CAs of the
reduced GO (rGO).
Preparation methods
Superhydrophobic surfaces prepared from GO
The presence of abundant OCGs endows the GO sheets with
tractable solution-processing capability and possibility for
further functionalization, therefore, many graphene-based
superhydrophobic materials have been fabricated using GO as
starting materials. Following the basic principle, artificial
superhydrophobic surfaces have been successfully prepared by
combining rough surface structures and low-surface-energy
material functionalization. In the following section, some
typical approaches to superhydrophobic GO have been
summarized.
Surface functionalization. Surface functionalization, which
can alter the surface characteristics, is an effective way to
obtain water-repellent surface; and the brought ease of
imparting superhydrophobicity to various surfaces greatly
extends the utilization of such functional surfaces. As a starting
material, GO is naturally hydrophilic, since most of the
functionalized OCGs are hydrophilic. So in order to drastically
change its surface wettability, post-functionalization of GO
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sheets with hydrophobic groups seems a simple but effective
method. As a typical example, Xue et al, obtained
superhydrophobic GO surface by functionalization GO with
polyhedral oligomeric silsesquioxane (POSS), a unique cage-
like molecular structure with eight isobutyl groups surrounding
the cubic core. 47 The amine-POSS can be covalently grafted
onto GO sheets via amide formation, and chemical
functionalization could be simply proved by the phenomenon
that POSS-modified GO moved from water phase into CHCl3
phase, as shown in Fig. 2a. The grafting leads to the
introduction of hydrophobic moities of isobutyl groups, and the
grafted graphene (POSS-graphene) becomes hydrophobic with
a water CA of 111.2° (Fig. 2b). To further increase the
hydrophobicity, the POSS-graphene was grounded into
Nanoscale Accepted Manuscript
particles and redispersed in ethanol, the regenerated film
exhibited hierarchical asperity and an enhanced CA of 157°
(Fig. 2c).
Generally, functionalization of GO sheets with large
groups would physically separate the graphene layers from each
other. As a result, the obtained GO hybrid becomes soluble in
various solvents. Such solution-processing capability will
facilitate the structuring process, making it possible to prepare
surperhydrophobic graphene through various routes.
The variety of OCGs on the GO sheets makes the molecular
functionalization flexible. Initiated from the neucleophilic
substitution between epoxy groups on GO sheets and amine of
ODA, Lin et al, also prepared superhydrophobic GO films by
octadylamine (ODA) bonding.46 The hydrophobic nature of
ODA significantly lowers the surface energy of grafted GO. A
rough ODA-grafted GO film could be easily prepared by a
simple filtration process. The obtained surface exhibited a high
CA of 163.2° and a low hysteresis of 3.1°. Through
functionalizing GO with phenylisocynate (C6H5NCO), Wang et
al changed hydrophilic GO into hydrophobic nanosheets via
solvothermal synthesis.48 Besides, (Heptadecafluoro-1, 1, 2, 2 -
tetradecyl) trimethoxysilane (HFTMS) was also employed as a
surface reactive molecule to create superhydrophobic GO
surface.49
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Fig. 2 (a) Surface modification of GO with POSS, and photographs of original GO
in water and the synthesized POSS-graphene in CHCl3. (b) SEM image of the
POSS-grafted GO film, the inset is the image of water droplet CA, ~111.2°. (c)
SEM image of a rough POSS-graphene film prepared from POSS-graphene
particles, the corresponding water CA is 157°. Reproduced with permission. 47
Copyright 2012, American Chemical Society.
Solvent modification. Owning to the large specific surface area
and the presence of OCGs, GO can adsorb large amounts of
solvent molecules when dispersed in solvents. Even after the
formation of graphene films, the adsorbed molecules may also
affect its surface energy, and change its wettability significantly.
Recently, thermally rGO with tunable wettability has been
obtained by solvent adjustment. 50 SEM images of graphene
films deposited on an aluminum substrate using pure water as
the solvent (graphene-W film) and using pure acetone as the
solvent (graphene-A film) were shown in Fig. 3a and b,
respectively. As compared to the naked substrate, the graphene-
coated samples show one to two orders of magnitude in the
average surface roughness due to the irregular stacking of
graphene sheets. Interestingly, totally different wetting
performances were observed for the graphene-W film which
was complete wetting and graphene-A film which showed a
water CA of ~160°. The opposite effect was ascribed to the fact
that the chemisorption of acetone on the defective graphene
introduces hydrophobic carbon-hydrogen bond, while
immersion in water leads to the formation of hydrophilic
carbon-oxygen bond. Additionally, the surface roughness
amplified the wettability according to Wenzel’s theory. Based
on these results, the graphene films can be tailored from
superhydrophilic to superhydrophobic with a water CA
changing from 0° to 160° by using acetone/water mixed
solvents with different proportions (Fig. 3c). Zhang et al, also
observed solvent-dependent hydrophobic phenomenon in
diverse pure organic reagents, as they prepared highly
hydrophobic films from chemically rGO via suction filtration.51
In their work, graphene were dispersed in different pure organic
solvents (methanol, ethanol, dimethylformamide, toluene,
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decanol, and so on) at the same centrifugal speeds, though there
is no clear difference observed among the surface morphologies
of the graphene films, they showed different water CAs.
Among them, films treated with ethanol and isopropanol
exhibit static CAs got close to or exceed 140°, and all films
showed CAs above 90°. Interestingly, the film showed
reversible transition from hydrophobicity to hydrophilicity
under the alternation of ultraviolet irradiation and air storage,
deriving from the adsorption and desorption of oxygen
molecules on the nanosheets surface. The solvent modification
is a simple, low-cost and flexible method for controllable
modulation of the surface chemical compositions of graphene,
providing an effective approach to tune the wettability of
graphene in a large range, from superhydrophobicity to
Nanoscale Accepted Manuscript
superhydrophilicity.
Fig. 3 SEM images of a graphene film deposited on an Al substrate: (a) with pure
acetone as the solvent (Graphene-A film), (b) with pure water as the solvent
(Graphene-W film). (c) Tunable control of the CA of a graphene film on an Al
substrate by using a water-acetone mixture as the solvent. Increasing the water
proportion in the mixture results in more hydrophilic behavior, whereas higher
acetone content yields a more hydrophobic response. (d) Contact angles of the
chemically treated and untreated graphene aerogel surface vary with
concentration. (e) SEM image of the FDTS modified graphene aerogel.
Reproduced with permission. 50,52 Copyright 2010, Wiley-VCH and 2011, American
Chemical Society, respectively.
Freeze-dry. Freeze-dry technique has been widely used to
generate porous structures. Recently, in the preparation of
superhydrophobic graphene, freeze-dry technique has been
successfully adopted as a simple and inexpensive method for
building rough graphene surfaces. For instance, Lin et al,
fabricated a serial of graphene aerogels using freeze-dry
technique, and all of them exhibited a water CA larger than
150°, even reaching 160° (Figure 3d). 52 By freeze-drying the
GO aqueous dispersion, a GO aerogels have been successfully
prepared. The surface roughness could be varied using GO
solution with concentrations increasing from 3 to 15 mg/ml,
which directly leads to the variation of water CA (Fig. 3d). In
this case, the tradeoff between aerogel density and structural
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porosity could be taken into account. The graphene aerogels
become superhydrophobic when the OCGs were thermally
removed at high temperature. In this work, both the formation
of porous structure and the removal of OCGs contribute to the
hydrophobic natural of the resultant graphene aerogel. (Fig. 3e)
To further strengthen the hydrophobicity of the samples, 1H,
1H-2H, 2H perfluorodecyl-trichlorosilane (FDTS) was applied
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to the surface, which further decrease their surface energy.
Template method. In addition to the above-mentioned
methods that construct rough graphene surface by irregular
stacking, hierarchical graphene structures could also be made in
a controlled manner. Lee et al reported the preparation of
superhydrophobic and transparent graphene films that consist
hollow graphene spheres using amine-functionalized silica
particles (NH2-SiO2) as a template. 53 The electrostatic
interactions between the negatively charged groups (-COOH, -
O-, -OH) of GO and positively charged groups (-NH2) of NH2-
SiO2 have been adopted as driving force to induced such
assembly. The GO layer coated on the surface of the SiO 2
particles was thermally reduced and the silica cores were etched
away in a HF solution, in this way, a structured graphene film
was successfully prepared. To further lower the surface energy,
the structure was treated with silane surface, and the CA of the
surface increased to 157°, reaching superhydrophobic range.
Moreover, the transmittance spectrum showed that the hollow
graphene structured surface show possibilities of transparent
device for flexible electronics, since the transmittance of
modified graphene spheres on the PET film is around
72.7±1.19% at 550 nm.
Biomimetic laser processing. Recently, photo-induced
deoxygenization of GO have become an appealing GO
reduction strategy, considering the controllable reduction
degree and flexible patterning. 54-56 Inspired from natural
butterfly wings that exhibit both superhyophobicity and
beautiful structural color due to the presence of ordered
photonic crystal structure, graphene surfaces with
superhydrophobicity and iridescence have been demonstrated
by photo-reduction.57,58 Two beam laser interference was used
for synchronous construction of periodic structure and
modulation of surface chemistry (Fig. 4a). Typically, periodic
distribution of laser intensity would lead to the formation of
grating structures, while the strong laser-matter interaction
would result in partial ablation of GO film and the drastically
removal the OCGs on the surface. The one-step procedure
endowed the graphene surface with both hierarchical roughness
and decreased surface energy, both of the two effects contribute
to the formation of a superhydrophobic surface. As shown in
the Fig. 4b, the tested water CA could reach 153° for the
graphene film with a period of 2 μm. Considering the fact that
the residual oxygen content was subject to the laser intensity,
the surface wettability would be further tuned by the laser
power.57 Moreover, the surface topology can be adjusted by the
grating period, and thus incident angle of the two laser beams
provided another way to tune the wettability. 58 What’s more,
the laser intensity distribution could also be tuned by multi-
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exposure of two beam laser interference. 2D micro-pillar arrays
were fabricated by dual laser interference with 90°rotation (Fig.
4c), and the CA of the prepared film is 155°; this would
effectively avoid the anisotropic superhydrophobicity.
Interestingly, the prepared graphene films with periodic
structures took on a wonderful iridescence, as observed by the
naked eyes.
Nanoscale Accepted Manuscript
Fig. 4 (a) Fabrication scheme of superhydrophobic graphene surfaces by TBLI and
dual TBLI with 90° rotation. (b) SEM image of the grating structure of the
graphene surface with a period of 2 μm. The layered nanostructure can be
clearly seen. The water CA is 153° vertical to the grating. (c) SEM image of the
graphene film with 2D grating-like structures. The period is 2μm and the
measured water CA is 155°. Reproduced with permission. 58 Copyright 2014,
Wiley-VCH
Superhydrophobic surfaces prepared from graphene
Generally, GO featured tractable water processing capability
and the flexibility for functionalization, so various
superhydrophobic graphene have been successfully developed
using GO as starting material. However, despite various
reduction protocols have been employed to restore the sp2
region of GO, the residual OCGs and the generated defects
dramatically alter the structure of the carbon plane, making the
rGO a substantially different material. Nowadays, with the
rapid progress of graphene preparation strategies, graphene can
be produced by micro-mechanical exfoliation of highly ordered
pyrolytic graphite (HOPG),59,60 chemical vapor deposition
(CVD)61-65, epitaxial growth66,67 and solvents exfoliation.68-70
As a result, superhydrophobic graphene have been successfully
developed based on real graphene.
CVD growth on structured templates. CVD method becomes
a promising strategy to produce graphene, since it enables the
preparation of single layer or few layer graphene with high-
quality (e.g., large area, low defects, and high carrier mobility).
However, the CVD graphene films were usually flat. Despite it
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is compatible with device fabrication, for instance, with the
help of substrates transferring technique, the flat surface set
obstacles to control its wettability. To introduce structure into
the prepared samples, template assisted CVD growth method
have been inventively proposed. 44,71-73 Dong et al, demonstrated
superhydrophobic graphene films by microwave plasma CVD
(MPCVD) using a patterned Si substrate. 71 In their research,
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vertically aligned few-layer graphene nanosheets were first
prepared on usual planar Si substrate. Though rough surface
with sharp edges were obtained, the water CA was 132.9°, even
when the surface was modified with ODA, the CA slightly
increased to 133.7°. To achieve highly nonwetting performance,
graphene sheets were grown on Si substrate with micropillar
arrays. SEM images in Fig. 5a and b show that graphene sheets
were evenly distributed on the substrate including the sides and
bottom of the pillars. With a composite structure consisted of
the microtexture inherited from the substrate and a
nanostructure originated from the sharp edges, the graphene
surface got a CA of 149.8°. After ODA treatment, water droplet
on the graphene surface presented a quasi-spherical shape (Fig.
5c) and the measured CA increased to 152.0°. As shown in the
optical microscope image (Fig. 5d), there is air trapped between
the droplet and the silicon pillars, and therefore an ideal
Cassie’s mode was used to earn the theoretical CA in this case.
Later, similar strategy was employed to create
superhydrophobic flower-like graphene surface grown on Si
nanocone arrays by hot filament CVD (HFCVD).72
Additionally, 3D hollow molds, such as foamed nickel
could also be used to prepare structured graphene.44,73
Graphene could directly grow on Ni templates by CVD
technique.73 After chemical etching of the metal sacrificial
scaffold, free-standing graphene foam was produced. The
imparted porous network and subsequent Teflon coating leaded
to the unique superhydrophobicity. Moreover, the graphene
foam exhibited superior elasticity and mechanically robustness,
as confirmed by the completely rebounding of the impacting
droplet. Conveniently, the structure of the graphene foam could
be flexibly tuned by selecting appropriate templates. To further
increase the surface roughness, carbon nanotubes can then be
grown onto the graphene/Ni scaffold by a two-step CVD.44
After the removal of nickel template, an superhydrophobic
carbon foam was prepared free of surface modification. The
superhydrophobic graphene foam holds great promise for
various functional applications such as non-wetting electrodes
and oil/water separation.
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Fig. 5 (a) SEM image of graphene grown on silicon microstructures, the
micropillars were 15 μm × 15 μm with a special interval of 35 μm. (b) Magnified
SEM image of the graphene uniformly distributed even on the sides and bottom
of the silicon structure. (c) Photo of water droplet on the ODA modified
graphene surface on microstructure. (d) Optical image of the contact line on the
water/solid interface where gas gap can be apparently seen. Reproduced with
permission. 71 Copyright 2013, Nature Publishing Group.
Dip coating. Using a structured carrier, dip coating is a rapid
and active alternative to establish superhydrophobic graphene,
as reported by Nguyen et al. 74 A common sponge was
employed as a frame for graphene coating. Benefited from the
mechanical flexibility of graphene and strong Van der Waals
forces between the nanosheets and sponge, graphene was
physically adhered to the sponge surface. Through repeated
dipping-drying process, controllable amounts of graphene could
be loaded onto the porous skeleton. The hydrophobic coating
made the powerful water-absorbing media water-proof. As the
graphene loading increased to 7.3% (defined as the weight ratio
of anchored graphene to the sponge), the graphene sponge
obtained a saturated water CA of about 162°. When it was
forced to immerse in the water, the graphene sponge was
wrapped by an air layer and exhibited a mirror-like look; while
released, it was floated on the water surface and kept dry due to
the dewetting-induced buoyancy and its low density. To avoid
the detachment of graphene and ensure the superhydrophobicity
stability, a dimethylsiloxane (PDMS) protective layer was made
in surface which is thin enough not to erase the rough feature
formed by the protrusions of the nanosheets. The as-treated
sponge can go through the squeezing test, indicating the
mechanical stiffness and the possibility for recycling use. It was
observed that the CAs of the graphene spongs were still larger
than 150° after having floated on aqueous solutions with
different pH values (2-14) for days, and thus the as-prepared
superhydrophobic foam can be applied in corrosive
environments with a long working period.
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Fig. 6 (a) Schematic illustration of the strategy for the crumpled graphene
induced from the pre-stretched substrate. SEM images of patterns developed on
the graphene sheet: (b) wrinkles form and (c) delaminated buckles as the
substrate is uniaxially relaxed, (d) crumples as the substrate is biaxially relaxed,
(e) unfolded pattern as the substrate is biaxially stretched back. (f) Atomistic
modeling results of (from left to right) crumpling of a single-layer graphene
under uniaxial compression, biaxial compression, and the Mises stress
distribution. Reproduced with permission. 75 Copyright 2013, Nature Publishing
Group.
Crumpling and unfolding. Crumpling-unfolding process
offers another simple and effective route towards the formation
of surface roughness. Zang et al developed a large-area
functional graphene with wrinkle structures by harnessing the
elongation of the supporting substrate. 75 The fabricating scheme
was schematically illustrated in Fig. 6a. With the help of a
PDMS stamp, CVD grown few-layer graphene was transferred
to a pre-stretched elastomer whose length is three times to its
original size (pre-strained by 200%). Then the substrate was
relaxed along two directions and reset to its initial size. In this
way, the adhered graphene contracted to the same degree, and
hierarchical roughness formed. As shown in Fig. 6b and c, the
graphene film developed wrinkles and delaminated buckles
when the substrate was relaxed in one direction, and then grew
crumples (Fig. 6d) as the substrate is relaxed biaxially. These
self-organized structures can also spread out and become
relatively flat (Fig. 6e), once the relaxed substrate was stretched
back. In this way, the crumpling and unfolding of the graphene
film can be irreversibly tuned. The microscopic procedure
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triggered by the stress can be reproduced by the atomistic
simulation (Fig. 6f), from which a single crumple with ridges
and vertices, as well as the corresponding stress distribution can
be clearly observed. If the substrate simultaneously relaxed in
the two directions, a different irregular pattern would appear on
the graphene surface. As the rough structure of the wrinkled
graphene is crucial for water-repellency, the wettability of the
surface can be tailored by tuning the relaxing manner (e.g.,
uniaxially or biaxially) and pre-strain level (e.g., 100% or
250%). It is worth mentioning that the graphene film can
maintain its integrity over multiple crumpling-unfolding cycles
(>50) with only a few unconnected cracks.
Doping. Arc discharge technique has been used for the
preparation of graphene ever since 2009,76-79 it is a simple and
Nanoscale Accepted Manuscript
efficient approach to prepare few layer graphene nanosheets.
Besides, this technique is very suitable for graphene doping and
modification.76,79 As mentioned previously, both the surface
roughness and the chemical composition influent the surface
wettability. Recently, in addition to the creation of rough
graphene structure, as discussed in previous sections, efforts
have been devoted to tailoring the surface chemistry of
graphene for the purpose of tuning its wetting behavior. As a
typical example, Shen et al, prepared superhydrophobic
fluorine-doped graphene using direct current arc discharge
method.80 In their synthesis, a hollow graphite rod filled with
graphite fluoride was used as the anode instead of a
conventional pure graphite rod. During the discharge process,
the graphite fluoride evaporated and the dissociative F atoms
and/or ions would react with carbon, so that F-doped graphene
was grown gradually. Morphology observation showed that the
F-doped graphene are multi-layers and there are wrinkles or
ripples on the edges of the nanosheets. According to the XPS
spectra, the content of the fluorine in the prepared graphene
was 10 wt% and doped F atoms had an ionic character. With
the difference in surface chemical composition, F-doped
graphene showed a CA of 158°.
Superhydrophobic surfaces prepared from graphene-based
hybrids
The hybridization of graphene has received significant attention
in the sense that the synergistic effect of components leads to
the improvement of performance in multiple facets and the
creation of new functionalities. In addition to the fabrication of
superhydrophobic surfaces using solo graphene and its related
materials, guest materials, for instance, polymers, have been
mixed with graphene, forming various hybrids for the
development of superhydrophobic coatings. The introduction of
other materials may provide feasibilities of controlling both the
surface morphology and the surface free energy, which
facilitates the fabrication of superhydrophobic surfaces.
Solubility modulation. Solubility modulation, which can
induce precipitation and crystallization, is a simple method to
control the morphology of various materials. By solvent
replacement, Zhang et al, established a polymer/graphene
hybrid surface composed of uniformly packed microspheres
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structure, which exhibited an average water CA of 151.6±1.4°
(Fig. 7a).81 In their work, N, N-dimethylformamide (DMF) has
been selected as a solvent to dissolve poly (vinylidene fluoride-
hexafluoropropylene) (PVDF-HFP), and graphene sheets could
suspended stably in the solution by ultrasonication. Then water
used as a non-solvent was adsorbed by the suspension. After
solvent leaching in water and freeze-drying, DMF was removed
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and a porous materials was obtained. Fig. 7b showed the
formation mechanism of PVDF-HFP/graphene microsphere.
Upon contact with the poor solvent, polymer tended to separate
from the liquid and immobilize on the graphene nanosheets.
The entanglements of the graphene sheets intercalated with the
crystallized PVDF-HFP chains finally induced the formation of
microparticle, and the surface of these particles were covered
with irregular spikes and nets in nanometer (Fig. 7c and 7d).
Thus multi-level surface structure was regarded as a critical
feature of superhydrophobic surfaces. Besides, several other
superhydrophobic polymer/graphene surfaces were constructed
through solvent replacement, 82-85 demonstrating the versatility
of this approach. Generally, in these studies, graphene
nanosheets having a large surface area provided abundant
immobilization sites for the precipitated polymer and facilitated
their crystallization. The polymer-graphene attachment can be
further strengthened by multiple forces between carbon surface
and polymer chains such as hydrophobic affinity, 81,82 π-π
interaction,83,84 dispersive, polar and hydrogen-bond
interactions.85 In addition to the change of surface morphology
and wettability of graphene, polymer may bring other
developments. For example, the deposited polymer on the
carbon surfaces may work as a spacer, preventing graphene
nanosheets from re-aggregation and improving their dispersion
stability.84 In return, Graphene may enhance the thermal
stability of the polymer as the release of volatile components
was limited by the nanosheets.83,84
Fig. 7 (a) SEM image of PVDF-HFP/Graphene microspheres. The CA of water on
the rough surface is 151.6±1.4°. (b) The formation of the graphene based hybrid
microsphere based on the entanglement and crystallization process. (c)
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Magnified SEM image of a single rough microsphere. (d) Further magnified SEM
81
image of the nanostructures on the microsphere. Reproduced with permission.
Copyright 2011, American Chemical Society.
Self-assembly. As a potent nanofabrication method, self-
assembly enable flexible construction of stereoscopic topology
from nanoscale structure units. 37 Recently, it has been
demonstrated that soft 2D graphene materials can be assembled
into robust 3D interconnected networks with the aid of
nanoparticles, building a novel superhydrophobic graphene
based materials.86 Typically, GO was mixed with FeSO 4 and
kept at 90 °C for 6 hours, then a black hydrogel containing
about 95.8 wt% water was naturally formed. The formation
mechanism can be explained as the fact that Fe2+ ions tended to
Nanoscale Accepted Manuscript
move towards GO sheets due to electrostatic attraction and then
oxidized into Fe3+, while GO sheets were in situ reduced and
assembled into 3D networks driven by π-π stacking interaction
between graphene sheets using the anchored iron oxide
nanoparticles as powerful support. Additionally, the as-formed
hydrogel exhibited a strong adsorption of heavy ions such as Cr
(VI) and Pb (II), which may be arisen from the synergistic
effects of the electrostatic interaction, ion exchange, and
surface complexation. After freeze-dry, the hybrid hydrogel
becomes to superhydrophobic graphene aerogel. Interestingly,
the ion oxide component of the graphene hybrid hydrogel can
be controlled by the pH values from α-FeOOH to Fe3O4.
Magnetic investigations revealed that the graphene/Fe 3O4
aerogel showed ferromagnetic property which can produce
strong magnetic signals at a small magnetic field. Moreover,
this method was workable to induce the self-assembly of
reduced graphene sheets with other metal oxides such as Mn 2O3
and CeO2, assisted with Mn2+ and Ce3+, respectively. This
method provides a facile way for building multifunctional and
manifold graphene derivatives.
Structural reconformation. Due to the presence of OCGs and
the water-processing capability, GO could be mixed with
various functional polymers, providing the feasibility of
fabricating diverse hybrid structures. Recently, Choi et al
demonstrated the fabrication of superhydrophobic
graphene/Nafion hybrid films through conformational
rearrangement.87 As shown in Fig. 8 (top panel), Nafion, a
fluorated polymer, was blended with GO, then chemical
reduction in hydrazine solution was implemented. The rGO can
be uniformly coated with Nafion driven by the hydrophobic
interaction between the conjugated graphene sheets and
polymer backbone. What’s more, the hydrophilic sulfonic
groups of Nafion imparted high dispersion and long-term
stability over 2 months to the rGO/Nafion (denoted as CMGN)
hybrid. To obtain thin films, the hybrid solution was then
vacuum filtrated. SEM images (Fig. 8, bottom panel) showed
that a rough surface with petal-like microstructure gradually
emerged as the ratio of Nafion component increased. The
roughness was contributed to the structural reorientation of the
hybrid sheets, that is, the favorable interactions between
graphene and Nafion cause the conformational rearrangement
of the Nafion and the wrinkle and protrusion of sheet edges.
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With the change of surface morphology, the CAs of the films
increased from ~97°to ~161°, indicating a tunable wettability
with respect to the hybrid composition. It is worth mentioning
that the electronic properties of graphene were carefully
retained in the hybrid, as the coating of individual graphene
sheet by Nafion was at molecular level, and the supramolecular
interactions made graphene sheets closely packed. 88,89
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Fig. 8 Illustration of the formation of Nafion/Graphene hybrid through
intermolecular hydrophobic interaction (top panel) and the conformational
rearrangement-induced morphological evolution of the films as the
concentration of Nafion increased from 2 wt % to 30 wt % (bottom panel). Scale
bars are 1 μm. The inset of the bottom panel is the CA photographs of the hybrid
films. Reproduced with permission.87 Copyright 2012, American Chemical Society.
Electrospinning. Electrospinning is a straightforward and cost-
effective method to provide surface roughness, it has been
widely adopted for the fabrication of superhydrophobic
surfaces. Recently, superhydrophobic graphene nanocomposite
fibers were one-step fabricated by electrospinning.90 In this
work, graphene nanoparticles worked as an additive to enhance
the surface roughness was added to the polymeric solution.
Without the particles, pure electrospun poly (vinyl chloride)
(PVC) fibers showed a water CA below 140°. In comparison,
the PVC hybrid polymer electrospun in the presence of
graphene nanoflakes achieved a high CA of 151.5°even 166.3°,
presenting a realization of superhydrophobicity. Considering
the small amount (1wt%) needed to introduce sufficient
hydrophobic character, graphene can be utilized as an effective
superhydrophobic media.
Potential applications
The combination of superhydrophobicity with graphene has
triggered a number of new functionalities and utilizations. From
the material point of view, graphene features high carrier
mobility, good conductivity, transparency, excellent mechanical
strength, and biocompatibility; while in the view point of
unique dewetting property, additional functionalities such as
self-cleaning, anti-fogging, oil/water separation could be well
imparted to graphene and graphene-based devices. Currently,
despite the fact that the fabricative strategies for
superhydrophobic graphene surfaces have been well developed,
functional applications is still limited to laboratory tests. In this
regard, we briefly summarized a series of typical applications in
this section.
Water treatment
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As a remediation of accidents, the cleanup of leaked chemicals
or oil is a global environment issue. Generally, porous materials
that have high porosity and high surface areas show great
potential in oil/chemicals pickup, however, these materials
usually shows poor selectivity towards target oil, thus easily
saturated with water. To address this issue, nanoporous
polydivinylbenzene (PDVB) with superhydrophobicity has
been successfully developed for the high-capacity and high
selectivity adsorption of organic compounds. Recently,
graphene based materials with both superhydrophobic and
superoleophilic properties44,74,91 emerge as a promising
candidate for selective absorption of oil and organic solvents
without water pickup. Fig. 9a showed the complete removal of
gasoline labeled with Sudan III from the water using a graphene
Nanoscale Accepted Manuscript
aerogel.86 The oil-saturated samples can be easily regenerated
after dried in an oven at 100 °C for 30 minutes. Notably, the
graphene hybrid aerogel kept a high adsorption capacity after
eight absorbing-drying periods for gasoline (Fig. 9b), the
excellent recyclability was a promising feature for adsorbent. In
addition to gasoline, a variety of oil and solvents such as
cyclohexane, toluene, paraffin oil, vegetable oil, phenoxin can
be sucked up (Fig. 9c). For another example, a
superhydrophobic graphene sponge also show eminent
absorption capacities ranging from 54 to 165 times their weight
for a wide range of solvents.74 The sponges could also be
renewed by a simple distillation or squeezing process, showing
a superior mechanical strength. In addition, the light weight,
chemical inertness, low cost and environmental friendliness
make the graphene sponge a powerful candidate for practical
application.
Moreover, graphene-based hydrogel was reported to show high
adsorption rates of heavy ions which are extremely toxic in
water resources of heavy ions.86 The calculated maximum
adsorption capacities for Cr (VI) and Pb (II) were 139.2 and
373.8 mg/g, respectively, which are much higher than active
carbon for Cr (VI) (69 mg/g). Therefore, functional graphene
based materials are regarded as ideal choices for water
purification.
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Fig. 9 (a) Photographs of the removal process of gasoline (dyed with Sudan III for superhydrophobic graphene have exhibited attractive potential
clear observation) from water using the graphene/iron oxide aerogel. (b)
Regeneration capacity of the hybrid for adsorbing gasoline. The graphene
in artificial muscles.75 When a voltage of 3000V was applied
aerogel can be reused after heated in the oven at 100 °C. (c) Adsorption between the graphene films, the elastomer among them
capacities of the aerogel for a range of organic solvents and oils in terms of its developed an electric field and deformed under the induced
86
weigh gain. Reproduced with permission. Copyright 2012, American Chemical
Society.
Maxwell stress. The pre-crumpled graphene films were
unfolded as the elastomer stretched over 100%, and the
transmission changed between 40-60%. The acting was fast
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Wettability switching
The manipulation of surface wettability is of great importance
in many research areas such as cell culture, microfluidics, and
water transportation. To this end, graphene surfaces with
tunable wettability may exactly meet the needs of various
applications requiring functional coatings. Several strategies
have been proposed to investigate the wettability control of
responsive and the laminate would return to the unfolded state
upon withdrawing the voltage (Fig. 10a). The procedure
mimicked the behavior of an artificial actuator with tunable
transparency. The stretchable graphene ensured the multiple
manipulation of the actuator without fracture. This work
presents a smart graphene device with dedicate design and
brings light into the possible uses of graphene-based systems.

Nanoscale Accepted Manuscript

graphene.50,51,57,58 Typically, Rafiee et al, reported a simple
route which can dramatically alter graphene surface from
superhydrophilic to superhydrophobic using solvent
modification method, as introduced in previous section. 50 In
their work, by combining water and acetone in a suitable
proportion as the solvent, graphene film with desired wetting
behavior would be achieved.
Besides, reversible wettability control of hydrophobic
graphene surface has also been realized through ultraviolet light
irradiation, as reported by Zhang et al. 51 When the graphene
film was exposed to ultraviolet light for 12h, the film show
presented a water CA of 40°; while kept in air storage for 12h,
the film displayed a high water CA of 140°. The interesting
phenomenon was bound up with the adsorption of oxygen
molecules which may result in the production of hydrophilic
groups on the graphene surface. The observed tunable
wettability could be reproduced for more than five cycles.

Transparent coatings and electrodes

Transparency is an essential requirement for many optical
devices, such as windshields, OLEDs, photovoltaic cells. To
enhance light transmission and prevent moisture permeation,
contaminant-proof or self-cleaning property is also useful or
even necessary for them. In this regard, graphene film with
transparency and superhydrophobicity seems an ideal candidate
for optical and optoelectronic materials. 53,75,87,90 Lee et al
demonstrated a simple route towards superhydrophobic
graphene film with transparency and flexibility, which exhibits
a water CA of 157° and an optical transmittance of 72.7%. 53
Cooperated with high conductivity, functional graphene film
shows great potential for transparent electrodes. 71,80 By
tailoring the surface roughness, graphene surfaces with variable
transmittance, resistance and wettability were obtained. 71 The
prepared graphene film manifested high toughness and
deformability compared with usual electrode material of gold.
The combination of stretchability, tunability and transparency
will endow graphene electrodes with sorts of potential
utilizations.
Smart actuator
Man-made actuators are helpful in many applications such as
energy harvesters and artificial intelligence. Crumpled
Fig. 10 (a) Schematic illustration (upper images) and photographs (bottom
images) of the voltage-induced working process of the graphene-elastomer
actuator. As a voltage is applied, the actuator reduces its thickness and expands
its area; and the transmittance increases. (b) Structural color of the graphene
film with 2D grating-like structures. The rose patterns are derived from pristine
photographs of the graphene film viewed from different angles by computer
design. Reproduced with permission. 58,75 Copyright 2013, Nature Publishing
Group and 2014, Wiley-VCH, respectively.
Other applications
Due to the ability to transfer charge and resist water, conductive
superhydrophobic graphene surface may also find broad
applications in electronics. For instance, it could serve as a
functional protective layer for electrostatic discharge and EMI
shielding83,84,92 to improve the operating safety and signal
stability of electronic devices; it may also prevent electronic
failures caused by water contact. In the light of these
capabilities, graphene based materials with unique
superhydrophobicity would hold great promise for practical
uses. Recently, Fang et al, reported a graphene/polymer hybrid
film holding a high conductivity of 6560 S/m and a total EMI
shielding effectiveness value of 43.7 dBcm 3/g, which is 4 times

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greater than that of traditional metal shielding materials. 84
Besides, superhydrophobic graphene could be employed as
functional papers93 and advanced textile94, which may be
promised for wearable electronics.
In addition to the potential applications in electronic, many
superhydrophobic graphene surfaces show high adhesive,
which is responsible for water transportation and cell culture,
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revealing great potential in tissue engineering. 72,49,57 Moreover,
due to the water repellency and good dispersion in polymer
solutions, polymer/graphene hybrids are considered as good
candidates for catalyst supporter. 81 Instead of black looking
appearance, superhydrophobic surface with periodic
microstructures exhibit brilliant iridescence (Fig. 10b),58 in this
regard, the colorful superhydrophobic graphene show potential
for embellishment coatings. Additionally, hydrophobic
graphene could also be used as a functional coating towards
depth filter.95 Droplet coated with superhydrophobic graphene
particles may serve as a miniaturized reactor standing on either
hydrophobic or hydrophilic surfaces.47 Currently, the research
topic “superhydrophobic graphene” is still in their infancy.
Nevertheless, we still deem that, with the progress of
superhydrophobic graphene and its related materials, it may
find more and more promising applications, both for
fundamental research and for practical usage.
Conclusions and outlook
Due to the outstanding physical/chemical properties, graphene
has been intensively investigated by diverse disciplines; in the
past decade, it has been considered as a rising star over the
horizon of material science. 95 Moreover, as numerous well-
controlled structures have been triumphantly constructed from
graphene-related materials, the development of this family has
been vigorously propelled.38 In recent years, to investigate and
utilize the surface property of graphene, different routes have
been proposed to fabricate superhydrophobic graphene surfaces
by controlling surface roughness and chemical composition of
graphene. In this review, we discussed the fabrication methods
and potential applications of superhydrophobic graphene and
related materials. In the beginning, owing to the ease of
functionalization and the tractable water-processing capability,
GO solution is regarded as a reservoir for the fabrication of
various graphene-based non-wetting surfaces. Later, with the
rapid progress of graphene production methods,
superhydrophobic graphene has been successfully prepared
based on pristine graphene. For instance, CVD method provides
an effective way for the fabrication of functional graphene
surfaces. In addition to the superhydrophobic surfaces
fabricated by solo graphene or graphene-related materials, with
the aid of polymer and inorganic nanoparticles, manifest
graphene derivatives can be also developed by hybridization.
All of these graphene-based superhydrophobic materials exhibit
great potential in a wide range of applications, such as water
treatment, wettability switching, transparent electrodes and
smart actuators. To make an overview of the state-of-the-art of
this dynamic field, we summarized the recent developments of
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superhydrophobic graphene and its related materials in Table 1.
Despite a short history, graphene has become a promising
newcomer in superhydrophobicity research. As compared with
conventional materials such as metals (including semimetals
and metal alloys), oxides, and polymers, graphene and its
related materials exhibit many superior features. To make a full
comparison, some representative properties of these
superhydrophobic materials have been briefly summarized in
Table S1 (see supporting information).
Currently, as the research of superhydrophobic graphene is
still at an early state, there are still lots of challenges that need
to be addressed. For example, a majority of the fabrication
methods are limited to laboratory research and not suitable for
large scale production. Besides, most of the superhydrophobic
Nanoscale Accepted Manuscript
graphene films generally face the problem of poor mechanical
stability. Mechanical durability is crucial to fulfill the need of
real-world applications. The third challenge is how to make full
use of the superhydrophobic graphene and its related materials.
Besides the hydrophobic nature, graphene embraces kinds of
merits, including mechanical strength, optical transparency,
high conductivity, large specific surface area, flexibility, and so
on. It could be expected that the combination of these superior
properties of graphene and superhydrophobicity would lead to
novel functions in the field of electronic devices,
optoelectronics, microfluidics and tissue engineering. Overall,
we believe that an exciting future for superhydrophobic
graphene surfaces will be witnessed since multidisciplinary
scientists and engineers have been contributing to the
understanding and the design of such surfaces.
Acknowledgements
The authors would like to acknowledge the National Basic
Research Program of China under grants No. 2011CB013000
and 2014CB921302, and the NSFC under grant No. 61376123,
51335008 and 61435005) for support.
Notes and references
a
State Key Laboratory on Integrated Optoelectronics, College of
Electronic Science and Engineering, Jilin University, 2699 Qianjin Street,
Changchun 130012, China. Fax: XX XXXX XXXX; Tel: XX XXXX
XXXX; E-mail: yonglaizhang@jlu.edu.cn; hbsun@jlu.edu.cn
b
Institute of Quantitative Biosciences & Biophysics, Departments of
Bioengineering, Electrical Engineering & Computer Science, UC
Berkeley.
c
Key Laboratory of Bionic Engineering (Ministry of Education), Jilin
University, Changchun 130022, China.
d
Nano-Optoelectronic Lab, Institute of Semiconductors, Chinese
Academy of Sciences, P. O. Box 912, Beijing, China.
† Footnotes should appear here. These might include comments
relevant to but not central to the matter under discussion, limited
experimental and spectral data, and crystallographic data.
Electronic Supplementary Information (ESI) available: Supporting Table
S1. See DOI: 10.1039/b000000x/
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Nanoscale Accepted Manuscript

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DOI: 10.1039/C5NR00719D
ARTICLE Journal Name

Table 1. Summary of the methods of fabricating superhydrophobic graphene and their potential applications

Category Method Material Potential application Ref.

Surface Covalent bond GO with ODA ODA-GO a Superhydrophobic coating 46
functionalization Covalent bond GO with POSS POSS-GO c Miniaturized reactor 47
Interfacial reinforcement
Covalent bond GO with phenyl isocynate Phenyl isocynate-GO Superhydrophobic coating 48
Covalent bond GO with HFTMS HFTMS-GO b Oil/water separation, Adhesive 49
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Solvent Solvent adjustment rGO Wettability switching 50

modulation Suction filtration rGO Adhesive, Photoresponsive, 51
Reversible wettability
Freeze-dry FDTS-rGOd 52
Template method Silane-treated rGO Transparent flexible electrode 53
Biomimetic laser processing rGO Structural color, Tunable wettability 57,58
CVD growth Two-step CVD on Ni foam Graphene/CNT Oil/water separation 44
using structured MPCVD on patterned Si ODA-Graphene 71

Nanoscale Accepted Manuscript

templates HFCVD on Si nanocone Graphene Adhesive 72
CVD on Ni foam Teflon-Graphene Flexible, Mechanical strong 73
Dip coating Graphene Oil/water separation 74
Crumpling and unfolding Graphene Transparent electrode 75
Artificial-muscle actuator
Arc discharge Fluorine-doped graphene Batteries, Wide-band gap secmiconductor 80
Nonsolvent Solvent replacement Graphene/PVDF-HFP f Catalyst supporter 81
induced Solvent replacement Graphene/PVDF e Oil/water separation 82
precipitation and Solvent leaching Graphene/MEH-PPV h EMI shielding 83
crystallization Luminescence, Thermal stability
Solvent replacement Graphene/P3HTg EMI shielding 84
Solubility modulation Graphene/PC i 85
Self-assembly Graphene/iron oxide Removal of heavy metal 86
Structural reconformation Graphene/Nafion Transparent conductive flexible 87
Electrospinning Graphene/PVC j Photovoltaic cells 90
Others Covalent graft Graphene/PVDF Oil/water separation 91
Solvothermal reduction rGO/CNTs k EMI shielding 92
Stable hydrophobicity
Microwave reduction Fluro-rGO Paper 93
Ascorbic acid reduction Silane-rGO Textile 94
Spray Phenyl isocynate-GO Depth filter media 95
a
, ODA, octadecylamine; b, HFTMS, (heptadecafluoro-1,1,2,2-tetradecyl) trimethoxysilane; c, POSS, polyhedral oligomeric silsesquioxane; d, FDTS,
1H,1H-2H,2H perfluorodecyl-trichlorosilane; e, PVDF, polyvinylidene fluoride; f, PVDF-HFP, poly(vinylidene fluoride-hexafluoropropylene); g, P3HT,
poly(3-hexyl thiophene); h, MEH-PPV, poly[2-methoxy-5-(2'-ethyl-hexyloxy)-1,4-phenylene vinylene]; i, PC, polycarbonate; j, PVC, polyvinyl
chloride; k, CNTs, carbon nanotubes

14 | J. Name., 2012, 00, 1-3 This journal is © The Royal Society of Chemistry 2012
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Journal Name ARTICLE

Yong-Lai Zhang received his BS (2004) and PhD (2009) from Jilin University, China. In 2008, he had worked in
Fritz-Haber-Institut of the Max-Planck-Gesellschaft as an exchanged PhD student. After received his Ph.D, he
joined the faculty in the State Key Laboratory on Integrated Optoelectronics, College of Electronic Science and
Engineering, Jilin University. In 2011, he worked as a research professor in Yonsei University, Korea. After that,
he was awarded a “Hong Kong Scholar” postdoctoral fellow and worked at Center of Super Diamond and
Advanced Films (COSDAF), City University of Hong Kong. His research interests include laser
micronanofabrication of biomimetic surfaces, graphene-based microdevices and Lab-on-a-Chip system.
Published on 12 March 2015. Downloaded by University of California - San Diego on 12/03/2015 15:04:37.

Nanoscale Accepted Manuscript

Hong-Bo Sun received his B.S. and Ph.D. degrees from Jilin University, China, in 1992 and 1996, respectively. He
worked as a postdoctoral researcher in the University of Tokushima, Japan, from 1996 to 2000, and then as an
assistant professor in Department of Applied Physics, Osaka University, Japan. In 2005, he was promoted as a full
professor (Changjiang Scholar) in Jilin University, China. His research interests have been focused on ultrafast
optoelectronics, particularly on laser nanofabrication and ultrafast spectroscopy. So far, he has published over
200 scientific papers, which have been cited by SCI journals more than 7000 times.

This journal is © The Royal Society of Chemistry 2012 J. Name., 2012, 00, 1-3 | 15