Applied Surface Science 444 (2018) 399–406

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Applied Surface Science

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

Full Length Article

Green synthesis of amphipathic graphene aerogel constructed by using

the framework of polymer-surfactant complex for water remediation
Jingjing Cao a, Ziyuan Wang a, Xianhou Yang a, Jing Tu b, Ronglan Wu a,⇑, Wei Wang a,c,⇑
a
Key Laboratory of Oil and Gas Fine Chemicals, College of Chemistry and Chemical Engineering, Urumqi 830046, China
b
Xinjiang FLY’C Oil Co., Ltd, Urumqi 830032, China
c
Department of Chemistry and Centre for Pharmacy, University of Bergen, Bergen 5020, Norway

a r t i c l e i n f o a b s t r a c t

Article history: Graphene aerogels have been extensively studied in water treatment and oil remediation. We report a
Received 12 October 2017 mild and green method to prepare a 3D-columnar graphene aerogel. The aerogel was synthesized by
Revised 12 February 2018 using polyvinyl alcohol (PVA) and stearic acid (SA) as crosslinking agents to construct a framework of
Accepted 28 February 2018
reduced graphene oxide (RGO). The interaction between PVA, SA, and stacked RGO sheets created a
Available online 1 March 2018
mechanically very robust aerogel. The aerogel possesses ultra-light performance with the destiny ranging
from 4.9 to 10 mg cm
3. The aerogel also demonstrated ultrafast oil absorption, good fire-resistance, and
Keywords:
excellent mechanical properties. The adsorptive capacities are in the range of 105–250 times of its orig-
Ultrafast adsorption
Green synthesis
inal weight for various organic liquids after the absorption. The aerogel also exhibited a strong durability
Wastewater treatment and reusability, and after ten cycles of absorbing-squeezing, the adsorptive capacity is nearly unchanged,
Oil/water separation indicating potential application in practical oil remediation.
Oil spill Ó 2018 Elsevier B.V. All rights reserved.

1. Introduction
Water/oil separation is a regular process in chemical engineer-
ing [1,2]. In recent years, due to frequent oil leakage and accidents
in chemical industrial, special focus has been put onto the materi-
als that absorb oil and remediate water, such as cellulose [3], clay
[4–6], sponges [7,8], polymer-based composites [9,10], carbon-
based materials [11] and etc. Among the carbon-based materials,
graphene aerogels exhibit great potentials due to high absorption
capacity and excellent physicochemical properties. These physico-
chemical properties include large surface area, high porosity
(>99%), chemical stability, low bulk density (5–10 mg/cm3) and
elastically and reversibly deformable [12]. All these properties
are desired characteristics of ideal oil sorbent materials [13].
Recent studies on graphene-based aerogels focused on superhy-
drophobic sponges and sponge-like materials, such as graphene-
polymer aerogels [14], carbon-nanotube-graphene aerogels
[15,16], graphene sponges [17,18], carbonaceous-nanofiber aero-
gels [19], and etc. With regard to the synthesis of the graphene-
based aerogels, many different methods have been reported in
order to improve the synthesis procedure. Graphene sponge could
be assembled with graphene oxide sheets by hydrothermal treat-
⇑ Corresponding author at: Department of Chemistry and Centre for Pharmacy,
University of Bergen, Bergen 5020, Norway.
E-mail address: wei.wang@kj.uib.no (W. Wang).
ment with the assistance of thiourea, and the absorptive capacity
for diesel oil reached 129 g/g [17]. Qu et al. reported to use pyrrole
to synthesize N-doped graphene framework [20]. The N-doped gra-
phene framework showed excellent absorptive capacity, and the
adsorptive amount of oils was up to 200–600 times its own weight.
This absorptive capacity was much higher than other typical car-
bonaceous sorbents, such as graphene foam (10–37 times) [21],
sponge (20–86 times) [22], carbon aerogel (16–50 times) [23], car-
bon nanofiber aerogels (51–139 times) [24], and carbon-nanotube
(CNT) sponge (80–180 times) [25]. Graphene aerogel was also syn-
thesized directly by freeze-casting technique and followed by heat
treatment up to 1000 °C in an inert atmosphere [26]. The absorp-
tion capacity could improved to over 600 times of the aerogel
weight. Recently, a very simple and mild method was applied to
construct the 3D graphene oxide aerogels. Graphene oxide with
different lateral sizes was crosslinked by PVA [27]. The aerogel
showed adequate absorption capacity, and the mechanical proper-
ties were exceedingly improved. PVA was also used in the synthe-
sis of CNT aerogels [28]. In the aerogel, PVA acted as a crosslinking
agent, which also improved the mechanical properties of the aero-
gel. As to the reducing agents used in the synthesis, Zhou et al.
compared the effect of reducing agents on the absorptive capacity
of graphene aerogels [29]. Among ammonia, ethanediamine and
vitamin C (VC), the graphene aerogel reduced by ammonia pos-
sesses the lowest density and highest specific surface area. How-
ever, this sample revealed the worst mechanical strength, which

https://doi.org/10.1016/j.apsusc.2018.02.282
0169-4332/Ó 2018 Elsevier B.V. All rights reserved.
400 J. Cao et al. / Applied Surface Science 444 (2018) 399–406
led to a sharp decrease of the absorptive capacity during
adsorbing-squeezing experiments. Graphene aerogel reduced by
VC possessed the most outstanding performance for mechanical
strength and re-utilization but have poor adsorptive capacity.
Based on these studies, it is still a challenge to synthesize graphene
aerogels with good absorptive capacity and mechanical properties
by using green and non-toxic reactants.
In this study, we report a one-step synthesis of graphene aero-
gels with high mechanical properties and absorptive capacity.
Based on the previous studies, we employed PVA as a crosslinking
agent for graphene, combining with SA to improve oleophilicity,
and ethylenediamine and ammonia as reducing agents. The as-
prepared aerogel exhibits excellent adsorptive capacity and
mechanical properties. The process of absorption only takes less
than one second. Both PVA and SA are non-toxic chemical agents.
Furthermore, the hydrogen bonding between PVA and graphene
reduces the hydrophilic nature of PVA. The final aerogel is oleophi-
lic, meanwhile, slightly hydrophilic, indicating that the absorptive
capacity measured in laboratory is close to it in field.
2. Materials and methods
2.1. Materials
Graphite powders (325 mesh) and PVA were purchased from
Aladdin Corp. (Shanghai, China). The degree of polymerization for
PVA was 1800, and 88% hydrolyzed. Sulfuric acid (98%) was pur-
chased from Fengchuan Chemical Co., Ltd. (Tianjin, China).
Hydrochloric acid (37%) and potassium permanganate (99.5%)
were purchased from Tianjin Chemical Co., Ltd. (Tianjin, China).
Sodium nitrate (99.0%) was purchased from Body Chemical Co.,
Ltd. (Tianjin, China). Hydrogen peroxide (30%) was purchased from
Yongsheng Chemical Co., Ltd. (Tianjin, China). Stearic acid (99.5%)
was purchased from Shengao Chemical Co., Ltd. (Tianjin, China).
Ammonia (25%) was purchased from Zhiyuan Chemical Co., Ltd.
(Tianjin, China). All chemicals were used as received. Milli-Q water
with resistivity of 18 MX cm was used in all experiments.
2.2. Preparation of graphitic oxide (GO)
Hummer’s method was used to prepare GO [30]. Sodium nitrate
(1.5 g) was mixed with sulfuric acid (70 mL, 98%) in a ice bath. Gra-
phite powder (3.0 g) was added into the mixtures and transferred
into a 250 mL round-bottom flask. The suspension was cooled to 0
°C and potassium permanganate (9.0 g) was added. Then, the flask
was heated up to 40 °C stirred for 12 h. The suspension was mixed
with 600 mL water, and slowly 15 mL hydrogen peroxide was
added. After 10 min, the color of the suspension changed from dark
brown to yellow. Then, the suspension was centrifuged and
washed with HCl solution (1:10, HCl:H2O) to remove metal ions,
followed by washing with water to removed the residual acid.
The obtained brown suspension was centrifuged at 8000 rpm for
5 min and repeated for several times to remove the unexfoliated
particles. The supernatant was collected, and dialyzed for two
weeks. It was afterwards freeze-dried, and used freshly.
2.3. Preparation of RGO aerogel
GO solution (10 mL, 2 mg mL
1) was ultrosonicated for 1 h.
Ammonium hydroxide (100 lL) was added into the GO solution
and stirred for 30 min. The mixture was put into a autoclave, and
the reacted at 120 °C for 12 h. The formed hydrogel was dialyzed
in water for 3 days. The hydrogel was freeze-dried for 2 days to
form RGO aerogel.
2.4. Preparation of stearic acid/reduced graphene oxide aerogel (SRGO)
The synthetic route is presented in Fig. 1. We ultrasonicated GO
(5 mL, 4 g L
1) aqueous dispersion for 1 h. Stearic acid (5 mg) and
ammonium hydroxide (100 lL) was added in a beaker containing
5 mL water, and the solution was stirred for 1 h to ensure stearic
acid fully dissolved in the solution, and added 25 lL ethylenedi-
amine. Then, the GO suspension and the stearic acid solution were
mixed in a 25 mL Teflon-lined autoclave. The mixture was ultra-
sonicated again for 10 min and reacted at 120 °C for 12 h. The auto-
clave was cooled down to room temperature, and a hydrogel of
black cylinder of RGO was formed. The hydrogel was carefully
moved out and put in ethanol solution (50 wt%) for dialysis. After
throughly washed, the hydrogel was frozen at
10 °C for 12 h, then
freeze-dried for 2 days to obtain the SRGO aerogel.
2.5. Preparation of PSRGO aerogel
The same procedure was used for preparing PSRGO aerogel with
slight changes in preparing the SA solution, as shown in Fig. 2.
After the SA solution was prepared, 0.1 mL PVA solution (0.1 g
mL
1) was added into the solution. After PVA was fully dissolved
in the solution, 25 lL ethylenediamine was added. The GO suspen-
sion and the PVA/SA solution was mixed in a 25 mL Teflon-lined
autoclave. The reaction conditions and the purification were the
same as they were for SRGO aerogel.
2.6. Characterization
Powder X-ray diffraction (XRD) patterns were recorded on a D8
Bruker diffractometer (Bruker, Germany) with a Cu Ka (k = 1.5418
nm) radiation. Fourier transform infrared (FTIR) measurements
were performed with IR Prestige-21 (Shimadzu, Japan) over a
range of 400–4000 cm
1. Thermogravimetric analysis (TGA) was
carried out on STA7300 (Hitachi, Japan) in temperature of 25–
800 °C. Scanning electron microscopy (SEM) images were captured
by S-4800 (Hitachi, Japan) with an accelerating voltage of 15 kV.
Transmission electron microscopy (TEM) images were captured
by JEM-2010F (Japan) with an accelerating voltage of 100 kV. X-
ray photoelectron spectroscopy (XPS) measurements were carried
out on a ESCALab220i-XL electron spectrometer (VG Scientific)
using a 3000 W Al Ka radiation. The static mechanical properties
were measured on a benchtop tester H5KT (Tinius Olsen, Horsham,
PA, USA). This process typically involves loading a PSRGO aerogel
both a compressible head and pressure sensor, where the displace-
ment and corresponding stress values were recorded. The stress-
strain measurements for PSRGO aerogel were conducted at a com-
pression speed of 5 mm/s.
2.7. Measurements of absorptive capacity
Various organic solvents were used to investigate the absorp-
tive capacity of the aerogels. The oils were mixed with water in
volumetric ratio of 1:1. The aerogels (30 mg) was immersed in
the oil/water mixtures. The process of the absorption is fairly quick
(about 1 s). After the absorption reached equilibrium, the soaked
aerogels were taken out and weighted. The adsorptive capacity
(Q w ) was calculated as follows.
w
w0
Qw ¼ ð1Þ
w0
In the formulae, w and w0 are the weights of aerogels before and
after the absorption.
 J. Cao et al. / Applied Surface Science 444 (2018) 399–406 401

Fig. 1. The schematic route of the synthesis of SRGO aerogel and PSRGO aerogel.

Fig. 2. The procedure of synthesize the PSRGO aerogel.

3. Results and discussion decreasing with temperature. The TGA curves for the aerogels
nearly level off at 440 °C. The mass of the residual is nearly 70%,
We compare the thermogravimetric analysis (TGA) data of GO, implying that the aerogels are heat-resistant (See Video S1). Many
SRGO aerogel and PSRGO aerogel in Fig. 3. Substantial loss of water similar materials show this property, and the aerogels are even
( 100  C) only occurred in the GO sample, accounting for 17% of stable in flames [34,35,18]. The heat-resistance is not improved
the initial mass. For the aerogels, there is negligible water loss. by adding PVA in the aerogel. This conclusion is based on the over-
Another sharp mass loss in the range of 175–225 °C is observed lapping of TGA curves for the SRGO and PSRGO aerogels.
for the GO sample, most likely due to pyrolysis of oxygen-
containing functional groups from the graphene oxide surface
[31,32]. A slight difference can be recognized for the two aerogels
below 200 °C. Water loss for PSRGO aerogel is slightly higher than
water loss of SRGO aerogel, indicating the latter is less hydrophilic.
This is understood by the chemical nature of PVA, which contains
large amount of hydroxyl groups attracting water molecules. This
water loss occurred at rather low temperature (< 50  C). While,
the curves of two aerogels are identical spanning the 200–800 °C
range [33]. The mass loss near 200 °C is consistent with the afore-
mentioned OG data. Above 225 °C, a mass loss is identified, linearly

1.0

0.8
Weight loss %

0.6

0.4

GO
0.2 SA/RGO aerogel
PVA/SA/RGO aerogel

0.0
200 400 600

Video S1.
Fig. 3. TG curves of GO, SRGO aerogel, and PSRGO aerogel.
402 J. Cao et al. / Applied Surface Science 444 (2018) 399–406

Table 1
GO Assignment of FTIR bands for (a) GO, (b) SRGO aerogel, (c) PSRGO aerogel [45]. The
SA/RGO aerogel number corresponds to the assignments in Fig. 5.
SA/PVA/RGO aerogel Sample name NO. Wavenumber and assignment
GO 1 3420 (AOH, stretching)
Intensity (A.U.)

2 1737 (C@O, stretching)

3 1622 (C@C, stretching)
4 1227 (CAO, stretching)
5 1056 (CAO, stretching for epoxy group)
SRGO aerogel 1 3309 (AOH, stretching)
2 2918 (CH2, out-of-phase stretching)
2858 (CH2, in-phase stretching)
3 1573 (NAH, stretching)
1478 (NAH, stretching)
4 1320 (COAH, stretching)
5 1169 (CAOAC, Stretching)
20 40 60 80 PSRGO aerogel 1 3441 (AOH, stretching)
2 2 2925 (CH2, out-of-phase stretching)
2858 (CH2, in-phase stretching)
Fig. 4. XRD patterns of GO, SRGO aerogel and PSRGO aerogel. 3 1573 (NAH, stretching)
1478 (NAH, stretching)
4 1401 (COAH, bending)
5 1215 (CAOAC, stretching)
The XRD patterns of GO, SRGO aerogel and PSRGO aerogel is 6 1108 (CAO, stretching)
shown in Fig. 4. GO exhibits a narrow peak at 10.59° with a d-
spacing of 0.84 nm matching with the reflection of (0 0 2) plane.
This pattern is very similar to XRD patterns reported previously
for GO [36,37]. The XRD patterns of SRGO aerogel and PSRGO aero- unoxidized sp2 (1622 cm
1), and CAO vibrations (1227 cm
1)
gel are nearly overlapping, and quite different from the precursor, [38,39]. For the SRGO aerogel, the OAH stretching vibration
GO. They shows a broader peak at 25° corresponding to the reflec- reduced substantially, indicating that the composition of the aero-
tion of (0 0 2) plane with a d-spacing of 0.36 nm, and indicating the gel contained RGO instead of GO [40]. The shape of the peak also
reduction of GO [18]. suggests that hydrogen bonding between hydroxyl groups are
FTIR spectra of GO, SRGO aerogel, and PSRGO aerogel are pre- not in favor at the presence of stearic acid. We also observed two
sented in Fig. 5. The following functional groups were identified small peaks at 2918 and 2858 cm
1, corresponding to the CH2
for GO (Fig. 5a): O-H stretching vibration (3420 cm
1), C@O out-of-phase and the in-phase stretching vibration, respectively
stretching vibration (1737 cm
1), C@C stretching vibration from [41]. The characteristic peaks at 1573 and 1478 cm
1 are attribu-
ted to NAH [42]. The peaks at 1320 and 1169 cm
1 are assigned
to the bending vibration of COAH and stretching vibration of
CAOAC bond [43]. For PSRGO aerogel, we again observed the
OAH stretching vibration due to the large amount of hydroxyl
(a)
groups on PVA chain. Because of the board OAH stretching vibra-
tion, we could suspect that the OH groups formed hydrogen bonds.
The well-defined peaks at 2925 and 2858 cm
1 are attributed to
2 the CH2 out-of-phase and in-phase stretching vibration, respec-
tively. Comparing to the IR spectrum of GO, the peak at 1737
3
cm
1 disappeared for both SRGO and PSRGO aerogels due to the
1
reduction of GO in these two samples [39,44]. A detailed assign-
4
5 ment for the peaks in Fig. 5 is summarized in Table 1.
We employed XPS to further address the bonding chemistry of
(b) PSRGO aerogel. As comparison, we also synthesized a sample with-
1
2
out adding PVA and SA (Fig. 6a, RGO aerogel). Oxygen content (O1s
intensity) in the PSRGO aerogel is much higher comparing to the
O1s peak in RGO aerogel. The variances between spectra before
and after functionalization reveal significant changes in the pro-
C-H 4 portions of carbon- and oxygen-containing functional groups
(Fig. 6). The deconvoluted C1s spectra (Fig. 6b and d) for RGO
C-H 3 5 and PSRGO aerogel shows strong Cepoxide signal (286.33 eV),
2900 2800 which increased in intensity upon reaction with SA and PVA [46]
(c) Concurrently, the peak for C@O bond (532.76 eV) increased in
the O1s XPS spectrum (Fig. 6e) and the peak of C(O)AO bond
4
(529 eV) disappeared, corroborating with its C1s spectrum and
3 5 suggesting the successful synthesis of the aerogel [31,47]. With
2
GO 6 all information of the bonding chemistry, we could not identify
SA/RGO aerogel ester groups, which are expected to form due to the existence of
1 PVA/SA/RGO aerogel hydroxyl groups on PVA and carboxylic groups on stearic acid
and partially reduced graphene oxide, specially when the reaction
4000 3000 2000 1000 temperature is above 120 °C. Therefore, the interaction between
Wavenumber (cm )
-1 RGO, SA and PVA is deemed physical in nature [12].
The micro-morphology of the aerogel was investigated by TEM
Fig. 5. The FTIR spectra of (a) GO, (b) SRGO aerogel, and (c) PSRGO aerogel. and SEM, which are presented in Figs. 7 and 8, respectively. Fig. 7a
 J. Cao et al. / Applied Surface Science 444 (2018) 399–406 403

(a) (b) (c)

C1s

O1s

N1s
RGO 292 288 284 280 536 532 528
Binding Energy (ev) Binding Energy (ev)
C-C
(d) (284.79 eV) (e)
C-O
(286.33 eV) C=O
(532.76 eV)

C=O C-O
(530.91 eV)
(288.66 eV)
PVA/SA/RGO
800 600 400 200 292 288 284 280 536 532 528
Binding Energy (eV) Binding Energy (ev) Binding Energy (ev)

Fig. 6. (a) XPS spectra of RGO and PSRGO aerogel. (b) and (d) are the deconvolution of C1s spectra of RGO and PSRGO aerogel, respectively. (c) and (e) are the deconvolution of
O1s spectra of RGO and PSRGO aerogel, respectively.

Fig. 7. TEM images of (a) GO, (b) SRGO aerogel and (c) PSRGO aerogel.

Fig. 8. SEM images of (a) SRGO aerogel and (b) PSRGO aerogel.

shows the exfoliated GO sheets. Multilayered GO sheets could be
clearly observed. The color of GO solution is dark brown as shown
in the panel of Fig. 7a. Fig. 7b shows the structure of SRGO aerogel.
The multilayer structure of GO remains unchanged. The frame of
the aerogel is homogeneous, and no micro-aggregation is observed.
Fig. 7c shows the morphology of the PSRGO aerogel. In this flock
shown in Fig. 7c, GO sheets are connected with each others, while,
preserving its monolayered nature, as shown in the panel of Fig. 7c.
The interaction between PVA-SA and RGO will be beneficial to the
absorption of oil because the large surface area of RGO is perceived
404
in the aerogels. The large surface of RGO is also relatively stable in
the presence of PVA and SA, which, on one hand, protect the mono-
layer from forming aggregates; on the other hand, stabilize the 3D
structure of aerogel from collapsing [48]. It will be further proved
in the mechanical test where the aerogel showed extraordinary
property of elasticity during compression.
The SEM images in Fig. 8 show the structure of the aerogels in a
larger scale. Fig. 8a shows the morphology of the SRGO aerogel. The
morphology of the aerogel undergo a fundamental change after
adding PVA. The SRGO aerogel is constructed by stacking and inter-
connecting layers of RGO, however PSRGO aerogel shows network.
A large amount of porous structure forms after the addition of PVA
(Fig. 8b). The size of pores are from a few micrometer to tens of
micrometer [48]. The porous structure opens channels between
layers of RGO and providing a means to convey between layers,
and facilitates the diffusion of liquid and gas in the aerogel, espe-
cially viscous oils [49].
In oil absorption, durability of materials is important factor to
take into consideration. Often, there are two processes: first, mate-
rials absorb oil; second, extract the absorbed oil from the materials.
For the later step, the most simple operation would be squeeze the
oil out. These require the material to have good absorption capac-
ity and mechanical property. Here, we investigated both oil
absorption and anti-compression.
The anti-compression experiments were performed for PSRGO
aerogel, using RGO aerogel as a reference. Both RGO aerogel and
PSRGO aerogel exhibit compression elasticity, yet PSRGO aerogel
is stiffer than RGO aerogel. The compression elasticity is demon-
strated in Fig. 9a and b for RGO and PSRGO aerogels, respectively.
The PSRGO aerogel could easily bear 50 g weight (Fig. 9b), but the
RGO aerogel was squashed by the same amount of weight (Fig. 9a).
(a)
(b)
(c) 20 30
25
Stress (kPa)
20
15
Stress (kPa)
15
10
10 5 Soybean oil
0
0 100 200 500
5 Cycles
0 Chloroform
10 20 30
Strain (%)
Fig. 9. (a) The compression of RGO aerogel; (b) the compression of PSRGO aerogel;
(c) the stain-stress curve of PSRGO aerogel. The inset in (c) shows that the stress at
50% strain changes with cycles.
J. Cao et al. / Applied Surface Science 444 (2018) 399–406
When the weigh removed, the PSRGO aerogel remained
unchanged. The RGO aerogel, while elastic, could not regain the
initial length (Fig. 9a), which is consistent with the results reported
by Zhou et al. [29].
The mechanical properties of the PSRGO aerogel was further
investigated by the strain-stress curves (Fig. 9c). In total, 500 cycles
of strain-stress test were performed, and in Fig. 9c the curves of the
2nd and the 500th cycles are presented. Under compression, the
aerogels experience typical two stages of deformation within a
low strain region, namely, linear elastic deformation, and irre-
versible plastic regimes [50]. The compression curve is not overlap-
ping with the relaxing curve, indicating hysteresis which could be
due to the structure change in the compression, especially in the
densification regime [51,52]. This phenomenon is also presented
in the reduce of stress responding to strain with regard to the num-
ber of cycles. We observed that the variation between compression
curve and relaxing curve become smaller after 100 cycles. In Fig. 9,
these two curves are partially overlapped at the 500th cycle. The
stress becomes rather low at low strain, suggesting weak elasticity
during relaxation. In the insert of the figure, the decrease of stress
responding to 50% strain is presented. A nearly linear decrease of
stress was captured in respond to the number of cycles in the first
40 measurements. At later cycles, the reduce of stress is
unnoticeable.
The PSRGO aerogel shows excellent oil absorption capacity.
Fig. 10 presents the process of oil absorption and the absorptive
capacity (Q w ) of various oils. For good contrast to show the oil,
Oil Red was dissolved in toluene. The photographs of Fig. 10 shows
that the oil could be absorbed in the aerogel in a very short time
(0.8 s), and after the absorption, the oil was completely removed
from the surface of water. The aerogel exhibits good affinity to
chloroform and dichloromethane; 1 g of the aerogel can absorb
250 g of chloroform. The good absorptive capacity can be inter-
preted by the solvent-aerogel interaction since both chloroform
and dichloromethane are good solvents to SA and RGO.
The aerogel can be reused for oil absorption due to the mechan-
ical properties. Oils absorbed by the aerogel can be squeezed out,
and the aerogel still maintain intact. Fig. 11 shows change of
absorptive capacity of squeezing-reabsorbing cycles. A block of
before absorption after absorpiton
Toluene 0.8 seconds
Water
the 2nd cycle
the 500th cycle
Hexane
Anhydrous ethanol
Toluene
Dichloromethane
40 50
0 50 100 150 200 250
Qw (g/g)
Fig. 10. The photographs illustrate the process of oil absorption, which takes 0.8 s.
The chart shows the absorptive capacity (Q w ) of various oils.
 J. Cao et al. / Applied Surface Science 444 (2018) 399–406
squeeze
absorb
100
80
Qw (g/g)
60
40
20
0 after the 1st squeeze after the 10th squeeze
0 1 2 3 4 5 6 7 8 9
Cycles
Fig. 11. The reuse of the PSRGO aerogel in oil absorption. The aerogel absorbed n-
hexane to reach the maximum absorption. Then the aerogel was squeezed to half of
its initial length and reabsorbed toluene. The Q w was recorded for each cycle as
shown in the chart.
aerogel soaked in hexane and reached the maximum absorptive
capacity. Then, the block was compressed to half of its initial
length; the absorptive capacity was recorded. Such cycle was
repeated 10 times, and Q w was plotted in Fig. 11. The overall
absorbed amount in each cycle is slightly reduced (100 g/g on
the 10th cycle). The extracted oil from each squeeze increased
due to larger increase of Q w after squeezing then the slightly
reduced reabsorption. After the 10th squeezing, the shape of the
aerogel maintained undamaged due to the excellent mechanical
properties.
4. Conclusion
In summary, we successfully synthesized the PSRGO aerogel.
The interaction between the polymer and the surfactant alkylates
the stacked RGO sheets, and created a stabilized structure. This
structure can be maintained under heavy weight, and also exhibit
elastic nature where the shape remain unchanged after 500
compression-relaxation cycles. The PSRGO aerogel also exhibited
excellent capacity in oil absorption. Due to the mechanical proper-
ties and the oil-absorption capacity, the aerogel can be an attrac-
tive material for oil/water separation, water mediation, etc.
Acknowledgement
We thank for the support from the One Thousand Talents
program.
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