nano battery

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3D Ordered Macroporous MoS2@C Nanostructure for
Flexible Li-Ion Batteries
Zongnan Deng, Hao Jiang,* Yanjie Hu, Yu Liu,* Ling Zhang, Honglai Liu,
and Chunzhong Li*
Z. Deng, Prof. H. Jiang, Dr. Y. Hu, Dr. L. Zhang,
Prof. C. Li
Key Laboratory for Ultrafine Materials of
Ministry of Education
School of Materials Science and Engineering
East China University of Science & Technology
Shanghai 200237, China
E-mail: jianghao@ecust.edu.cn; czli@ecust.edu.cn
Dr. Y. Liu, Prof. H. Liu
State Key Laboratory of Chemical Engineering
School of Chemical Engineering
East China University of Science & Technology
Shanghai 200237, China
E-mail: liuyu@ecust.edu.cn
DOI: 10.1002/adma.201603020
The key feature of the 3DOM MoS2@C for boosting LIB
performance is that ultrasmall few-layered MoS2 nanosheets/
carbon hybrids form 3D macroporous structure, which avoids
the stacking/restacking of MoS2 and leaves enough space for
solving the problems related to the volume expansion during
the charge and discharge process. Consequently, the 3DOM
MoS2@C/CC anode delivers a high discharge capacity of
3.428 mAh cm−2
at 0.1 mA cm−2
with rapid charge/discharge
capability (1.361 mAh cm−2
at 5 mA cm−2
) and excellent cycling
stability (93% capacity retention after 100 cycles). Quantum
Density Functional theory (QDFT) calculations reveal that the
edge-enriched ultrasmall and few-layered MoS2 nanosheets
is favorable for enhancing lithium storage capacity. A highly
flexible full cell using as-synthesized MoS2@C/CC and com-
mercial LiCoO2/Al as anode and cathode is also assembled,
demonstrating superior mechanical strength and outstanding
electrochemical performances.
Scheme 1 illustrates the typical preparation process of the
3DOM MoS2@C incorporation structure on carbon cloth. In
the first step, a piece of positively charged carbon cloth was
obtained by the modification of polyaniline in N-methyl-2-pyr-
rolidone solvent. Then, the negatively charged polystyrene (PS)
nanospheres were homogenously dispersed into ammonium
thiomolybdate (ATM) and glucose aqueous solution, followed
by the self-assembly of PS nanospheres on the surface of
carbon cloth based on electrostatic attraction (Figure S1, Sup-
porting Information). After that, the MoS2@C/CC flexible elec-
trode was obtained by matching the ATM decomposition rate
and glucose carbonization rate during carbonization, which
will make a detailed discussion later. Importantly, the polysac-
charide compounds, i.e., glucose have dual functions: carbon
source and linker, which therefore enhance the combination
force of 3DOM hybrids and carbon cloth. Such a fascinating
flexible electrode can be directly applied as LIBs anode without
the addition of inactive binders and carbon black.
Figure 1a shows the typical 3D network morphology of the
MoS2@C/CC electrode. After magnification, it can be observed
that the surface of each carbon fiber is composed of the 3D
interconnected ordered macroporous nanostructure, as shown
in Figure 1b,c while the pristine carbon cloth shows a clean
and smooth surface (Figure S2, Supporting Information). The
average pore size is about 200 nm and the wall thickness is thin
of about 20 nm. It is noted that no obvious MoS2 nanosheets
can be found in the surface, implying the perfect embedding of
MoS2 into carbon framework. The microstructure of the 3DOM
MoS2@C has been further examined by transmission electron
microscopy (TEM) technique. The low magnification TEM
image (Figure 1d) also shows 3DOM nanostructure, which
is in accord with the SEM observations. Impressively, we can
The future trend in electronic devices is flexibility, miniaturiza-
tion, and increased portability,[1,2]
but the flexible lithium ion
batteries (LIBs) devices are still in their infancy.[3]
Searching
for the foldable and flexible electrode will greatly promote
flexible LIBs devices.[4,5]
The well-known strategy to prepare
flexible electrode is directly coating active materials on flex-
ible current collectors (e.g., carbon cloth, graphite paper)
instead of the traditional copper/aluminum foils.[6,7]
How-
ever, the weak binding force will inevitably cause the detach-
ment of active materials from current collector, resulting in
the serious capacity fading.[8]
To strengthen their interaction,
directly growing active materials on flexible substrate is one of
the interesting ways for fabricating highly integrated flexible
electrode.[9,10]
Nevertheless, their biggest challenging issue for
flexible LIBs is that during the charge/discharge process, the
remarkable volume change and partial dissolution of active
materials happen.[11]
The key to make efficient flexible elec-
trode lies in the construction of high-performance and stable
materials as well as their robust adhesion with the flexible cur-
rent collector.
Molybdenum disulfide (MoS2) nanosheets are of great
interest in lithium ion storage because of their good van der
Waals interaction between sheets.[12–14]
But practically, they
are very easy to stack/restack into the bulk material, leading to
the limited space for lithium ion storage at high rates particu-
larly.[15–17]
The biggest problem of MoS2 nanosheets for flexible
LIBs is that its implementation is greatly impeded by its poor
rate performance mainly due to the sluggish Li ion diffusion,
low conductivity, and the unsatisfactory cycling stability caused
by the huge volume variation and polysulfide dissolution during
the cycling.[18–20] To address these issues, herein, we report a
novel flexible and foldable high-performance lithium ion bat-
tery by designing 3DOM MoS2@C nanostructures and in situ
assembling them on carbon cloth (labeled as MoS2@C/CC).
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find that substantial ultrasmall few-layered MoS2 nanosheets
with lateral dimension of 5–10 nm are homogenously incor-
porated into the 3DOM carbon wall, offering rich edges which
are beneficial for enhancing LIBs, as shown in Figure 1e. The
corresponding SAED pattern (the inset of Figure 1e) proves
the hexagonal MoS2 crystalline structure (JCPDS: 37-1492)
without the existence of other crystals.[21]
The interlayer spacing
of the MoS2 nanosheets is measured to be about 0.704 nm in
Figure 1f, which is much larger than the standard MoS2 crystal
of 0.612 nm.[22]
The expansion of interlayer distance can be
mainly attributed to the involvement of glucose molecules into
the MoS2 interlamination, which will accelerate the kinetic of
Li ions transportation. We further detect the elemental distri-
bution of the as-obtained 3DOM MoS2@C hybrids, as shown
in Figure 1g–j. All of Mo, S, C elements are nearly overlapped
along with the 3DOM nanostructure, which also suggests the
successful preparation of MoS2@C incorporation nanostruc-
ture. Interestingly, such nanostructure can further realize
the strong interaction with other current collectors, such as
titanium foil (Figure S3, Supporting Information).
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Scheme 1. Schematic illustration of the preparation process of MoS2@C/CC flexible electrode.
Figure 1. a–c) SEM images and d–f) TEM images at different magnification, g–j) TEM-EDS mapping of Mo, S, C elements.

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To realize the well-embedding of few-layer MoS2 nanosheets
into 3DOM carbon wall, it is very crucial to control the matching
relationship of the generation rate of MoS2 and the carboniza-
tion rate of glucose during annealing in inert atmosphere.[23]
In order to clarify it, we constructed a thermodynamic/kinetic
model by applying the first-order reaction dynamics and transi-
tion state theory to estimate the inhomogeneity of the MoS2/C
composite (see details in Supporting Information). The relative
MoS2/C ratio
r /
(r)/
MoS /C
MoS
L
MoS
(0)
C
L
C
(0)2
2 2
R
c c
c c
)(
=
)
)
(
(
(1)
is employed to represent the inhomogeneity of the MoS2/C
composite, where c(L)
i(r) is the local concentration of compo-
nent i, c(0)
i is the total concentration of component i. According
to Equation (1), the deviation of RMoS2/C from 1 denotes the
inhomogeneity of the system. Figure 2a clearly shows the fluc-
tuation of RMoS2/C is small (10%), which means MoS2 and C
will homogeneously distribute in the composite. Notably, the
homogeneity can still be well-maintained with the increasing
of temperature (Figure S4, Supporting Information). Therefore,
T = 873 K seems to be a reasonable choice to realize the well-
incorporation of MoS2 into carbon framework.
The crystallographic structure of the as-obtained flexible
electrode is further characterized by X-ray diffraction (XRD), as
shown in Figure 2b. As a comparison, we also synthesized the
pure 3DOM MoS2/CC electrode using the same strategy only
without the addition of glucose, as shown in Figure S5 in the
Supporting Information. All the diffraction peaks can be easily
indexed to the hexagonal MoS2 phase (JCPDS: 37-1492) except
the two peaks located at 25.4° and 43.4°, which are ascribed to
the carbon cloth substrate. Notably, our MoS2@C/CC flexible
electrode exhibits a weak and broad (002) diffraction with a
d-spacing of 0.704 nm, which is in good agreement with the
TEM observation, while the MoS2/CC electrode shows a strong
and sharp (002) diffraction with a d-spacing of 0.620 nm. The
results suggest that few-layer MoS2 nanosheets exist in the
MoS2@C/CC flexible electrode with an expanded interlayer
spacing. Raman Spectroscopy further verifies the few-layer
MoS2 nanosheets (Figure 2c). The E1
2g and A1
g peaks of
MoS2@C/CC appear at 383.0 cm−1
and 406.9 cm−1
with a peak
separation (Δk) of 23.9 cm−1
(smaller than 24.2 cm−1
of four-
layers MoS2 nanosheets).[24]
The MoS2/CC electrode shows a Δk
value of 25.7 cm−1
, an indicator of multilayer MoS2 nanosheets.
The content of MoS2 nanosheets in the optimized 3DOM
MoS2@C hybrids is measured to ≈55% by weight according to
the thermogravimetric analysis result (Figure S6, Supporting
Information). In addition, we further measure the electrical
conductivity by four-point probe technology. As shown in
Figure 2d, the pure carbon cloth conductivity is ≈37.2 S cm−1
.
It is noted that the MoS2@C/CC flexible electrode possesses a
high conductivity of 15.7 S cm−1
, which is significantly higher
than the corresponding MoS2/CC electrode (only 0.5 S cm−1
).
More impressively, the microstructure and the conductivity
of our flexible electrode can be well-maintained even during
300 times bending test (Figure S7, Supporting Information).
The unique 3DOM structure with high conductivity and sta-
bility is reckoned to deliver high energy/power densities and
outstanding cycling performance.
The electrochemical performance of the MoS2@C/CC and
MoS2/CC was evaluated by directly using them as anodes to
assemble the 2016-type half cells, respectively. Figure S8a in the
Supporting Information shows the first three cyclic voltammo-
grams (CV) curves of the MoS2@C/CC within a voltage window
of 0.01–3 V at 0.2 mV s−1
. There are two peaks at 1.0 and 0.45 V
in the first discharge can be attributed to the
formation of LixMoS2 caused by insertion
of Li+
into MoS2 interlayer and the further
generation of Mo and Li2S by conversion
reaction of LixMoS2 and Li+
, respectively.
The oxidation peak at 2.25 V in the first
charge process belongs to the delithiation
of Li2S. In the subsequent two discharge
processes, a new peak is observed at 1.9 V
instead of the previous reduction peaks,
which is due to the formation of Li2S.[25]
The other peaks are from the carbon cloth
substrate (Figure S8b, Supporting Infor-
mation). To highlight the structure advan-
tage, we also investigate their Li+ diffusion
kinetics according to the CV curves of the
MoS2@C/CC and the MoS2/CC at various
scan rates (Figure S8c,d, Supporting Infor-
mation). We find that the intensity of current
peaks gradually increase with the increasing
of sweep rate. The relationship between peak
current (ip) and the square root of the scan
rate (v1/2) for MoS2@C/CC, MoS2/CC are
also respectively provided in Figure 3a,b. The
linear relationship of ip and v1/2 indicates
the reaction of Li+ insertion/extrusion is
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Figure 2. a) Thermodynamic/kinetic estimation of the relative MoS2/C ratio as a function of
reaction degree, b) XRD patterns and c) Raman spectra of the MoS2@C/CC and the MoS2/CC,
d) the electronic conductivity of the MoS2@C/CC, the MoS2/CC, and the CC.

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diffusion-controlled. Furthermore, the diffusion of Li+
kinetics
can be interpreted according to the Randles–Sevcik equation
(Equation (2))[26,27]
(2.69 10 )p
5 3/2 1/2 1/2
i n S D C v= × × × × ×
(2)
where ip is peak current, n is the charge-transfer number,
S is the electrode area, D is the diffusion coefficient of Li+,
C is the concentration of Li+, and v is the sweep rate. It can
be seen that the diffusion coefficient D is determined by the
slope in Figure 3a,b because the n, S, and C value is constant.
As expected, the MoS2@C/CC exhibits a larger slope in both
cathodic and anodic scan than the corresponding MoS2/CC,
indicating a rapid ion diffusion coefficient, which will lead to a
higher rate performance.
The initial three discharge–charge curves are also provided
in Figure S9 in the Supporting Information at 0.1 mA cm−2.
We find that the MoS2@C/CC delivers a high discharge areal
capacity of 3.802 mAh cm−2 with a Coulombic efficiency
(CE) of 88%. The CE quickly goes up to 97% and 99% in the
following second and third cycles almost without the capacity
loss, indicating the as-synthesized MoS2@C/CC electrode
possesses a high structural integrity. We
then further measure the rate capability of
the MoS2@C/CC electrode at various current
densities ranging from 0.1 to 5 mA cm−2
,
as shown in Figure 3c. It can be observed
that the MoS2@C/CC electrode delivers the
average areal capacity of 3.428, 3.105, 2.776,
2.475, 2.038, and 1.361 mAh cm−2
at 0.1, 0.2,
0.5, 1, 2, and 5 mA cm−2
, respectively. More
importantly, after deeply cycling at 5 mA cm−2
for 5 cycles, an average discharge capacity of
3.271 mAh cm−2
can be immediately recov-
ered, implying the high reversibility. For
comparison, the MoS2/CC electrode is also
evaluated, which obviously shows a much low
areal capacity of 3.106 mAh cm−2
with poor
rate capability (0.938 mAh cm−2
) because
of its limited electrons/ions transportation
caused by the stacking and restacking of
MoS2 nanosheets in MoS2/CC electrode.
We then further calculate the gravimetric
capacity of the 3DOM MoS2@C nanohy-
brids after deducting the capacity contribu-
tion from carbon cloth substrate (Figure S10,
Supporting Information), which shows a
very high specific capacity of 1130 mAh g−1
at 0.1 mA cm−2
although relatively low MoS2
content. Even at 5 mA cm−2
, 546 mAh g−1
still can be maintained (Figure S11, Sup-
porting Information). Furthermore, the
MoS2@C/CC electrode also possesses a
stable cycle life. As shown in Figure 3d, as
high as 2.471 mAh cm−2
(93% capacity reten-
tion of the second cycle) is achieved after
cycling for 100 cycles at 0.5 mA cm−2
while
only 1.701 mAh cm−2
(64% capacity reten-
tion) is obtained for the MoS2/CC electrode.
The macroporous construction of MoS2@C/CC after cycled
over 100 cycles (inset of Figure 3d) can still be preserved which
further prove the good structural stability. It is noted that the
loading mass of 3DOM MoS2@C nanohybrids on carbon
cloth is very easy to control just by tuning the dipping times
of the precursor ink. As shown in Figure 3e, when the loading
mass increases from 1.02 to 2.66 mg cm−2, all the as-formed
MoS2@C/CC electrodes exhibit high areal capacity and excel-
lent cycling stability. More interestingly, the reversible capacity
of the 3DOM MoS2@C/CC electrodes exhibits positive linear
relationship with mass loading, indicating their rapid ions/elec-
trons transportation ability (Figure 3f).
To better understand its enhancing Li+ storage mechanism,
the QDFT calculation was implemented to simulate the Li+
adsorption behavior on the exposed surface of MoS2 with dif-
ferent interlayer space. Three typical surfaces of MoS2 (named
as X, Y, and Z) are defined in Figure 4a,b. We have applied
QDFT to calculate the binding energy of Li-MoS2 under four
kinds of conditions, respectively, i.e., on the three surfaces
and inside of the nanosheet, where the calculation details are
introduced in the Supporting Information. Figure 4c com-
pares the binding energy of the three surfaces with interlayer
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Figure 3. a,b) Linear relationship of the anode/cathode peak current (ip) and the square root
of the scan rate (v1/2), c) rate capability and d) cycling performances for MoS2@C/CC and
MoS2/CC, respectively (the inset of Figure 4d showing the morphology of MoS2@C/CC after
100 cycles), e) the capacity of MoS2@C/CC with different mass loading, f) linear relationship
of the capacity of MoS2@C and different mass loading.

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spacing (H) of 0.612 and 0.704 nm,[28]
respectively, while the
corresponding structures are shown in Figure S12 in the Sup-
porting Information. For layering space H = 0.704 nm, the
binding energy on the three surfaces range from –101.8 to
–109.6 kcal mol−1
, which is stronger than the inside binding
energy of –89.5 kcal mol−1
. As the binding energy is usually
taken into account by its exponential form, exp[-Eb/(kBT)], the
absolute increment 10–20 kcal mol−1
may lead to an obvious
improvement of the adsorption amount. It is well-accepted that
ultrasmall few-layered MoS2 nanosheets possess much more
surface, leading to a stronger binding interaction. A higher
lithium storage capacity will be achieved. Comparing the
binding energies on the three surfaces, it seems the binding
energy on the X surface is stronger than others, which suggests
that exposing more X surface is more beneficial for enhancing
the specific capacity. For conventional MoS2 material where
H = 0.612 nm, however, the surface behavior is not as good as
H = 0.704 nm. It seems the binding energy on the X surface is
more sensitive to the layering space, a 0.092 nm increment of
H leads to a 19.7 kcal mol−1
increment of –Eb. This reveals the
X surface is the most important factor in surface adsorption.
To give a more detailed understanding of the charge/discharge
process, we examined the structures of MoS2 and LiMoS2
in the adsorption/desorption cycles, as shown in Figure 4d. A
lithium-induced structural transformation of MoS2 has been
found: when lithium is adsorbed first, the MoS2 plane inclined
by 37.5° comparing to its original structure, denoting a slippage
between two layers, which seems irreversible in the following
adsorption/desorption cycles. The slipped structure resulted
in a weaker binding energy, which explains the performance
degradation of electrode material in the initial several charge/
discharge cycles.
The 3DOM MoS2@C/CC electrode has several distinct advan-
tages that can endow it with superior lithium storage capability.
(a) The open and interconnected 3DOM nanostructure has
a high BET specific surface area of 145.1 m2 g−1 (Figure S13,
Supporting Information), which is helpful for accelerating Li+
diffusion and meanwhile relaxing the volumetric expansion
during Li+ insertion process. (b) The 3DOM MoS2@C/CC elec-
trode shows a much higher conductivity (15.7 S cm−1) than the
corresponding MoS2/CC electrode (0.5 S cm−1
), suggesting
the rapid electrons transfer rate (Figure 3d). Furthermore, the
ultrasmall few-layered MoS2 nanosheets (1–3 layers, 5–10 nm)
have been well-incorporated into carbon walls, which creates
the rich Li+
insertion active sites and effectively avoids the
stacking/restacking of MoS2 during charge/discharge process.
(c) Considering that the conversion mechanism of MoS2 (4Li+
+
MoS2 + 4e−
↔ Mo + 2Li2S) and the generation of interme-
diate polysulfides as lithium sulfur batteries,[29]
the MoS2@C
incorporated structure is favorable to adsorb and anchor the
lithiation products of Li2S and Mo as well as polysulfides, and
restraining the reaction of Li2S with electrolyte and the poly-
sulfide shuttle effects. (d) The polysaccharides glucose can not
only decompose into high-quality carbon, but also play the
adhesive role which further strengthens the close integration of
the 3DOM MoS2@C hybrids and carbon cloth,[30]
and therefore
achieving a stable and high-performance flexible electrode.
The performances of 3DOM MoS2@C/CC anode were fur-
ther evaluated by assembling a MoS2@C/CC//LiCoO2/Al coin-
type full cell. The full cell was galvanostatically cycled between
1.0 and 4.2 V at various current densities ranging from
0.2 to 5 mA cm−2 (Figure 5a). It can be observed that a high
initial discharge area capacity of 2.661 mAh cm−2 with CE of
79.3% is achieved at 0.2 mA cm−2. Even at 5 mA cm−2, this
device still can deliver an average reversible area capacity as
high as 1.681 mAh cm−2 with no capacity decay after another
100 cycles, demonstrating excellent rate performance and
superior capacity retention. Based on the above results, we also
demonstrate the fabrication of a flexible LIB full cell, as shown
in Figure 5b, which can be charged to ≈3.54 V (Figure S14,
Supporting Information). For comparison, the corresponding
MoS2@C powder was coated on the Cu foil by traditional tech-
nique, which then also assembled into a flexible electrode.
Obviously, our flexible electrode exhibits a more stable capacity
output during hundreds of times bending test (Figure S15,
Supporting Information). To further highlight the flexibility of
the device, we test the brightness change of a white LED (3 V,
0.2 W) under different states. As shown in Figure 5c,d, it can
be observed that the LED can easily lightened and keep the
brightness even when the cell was bended. More importantly,
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Figure 4. a,b) Structure of MoS2 crystal and the definition of X, Y, and Z directions, c) the binding energy of Li adsorbed in MoS2 on the three surfaces
and inside of the MoS2 particle, where X, Y, and Z denote the surfaces which are perpendicular to the X, Y, and Z directions, respectively, d) lithium
adsorption/desorption on the X surface of MoS2 particle. Color code: purple, Li; cyan, Mo; yellow, S.

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the device can still sustain and keep the LED brightness
after repeating the bending tests for 300 cycles (Figure 5e;
Video S1, Supporting Information), further revealing the excel-
lent flexibility.
To summarize, we demonstrate a new 3D ordered macropo-
rous MoS2/carbon nanostructure with large surface area and
ample space for constructing high-performance flexible and
foldable LIBs using PS nanospheres as the macropore template.
Different from the established MoS2/carbon hybrid nanomate-
rials, the present incorporated building shows the integrated
features of flexible substrate, ordered macroporous, and ultras-
mall few-layered MoS2 nanosheets embedded into the inter-
connected carbon wall. The resultant flexible electrode delivers
a high discharge capacity of 3.428 mAh cm−2 at 0.1 mA cm−2
with faster charge/discharge capability (1.361 mAh cm−2 at
5 mA cm−2) than that of 3DOM MoS2/CC electrode (0.938 mAh
cm−2 at 5 mA cm−2). They also have a stable capacity of
2.471 mAh cm−2 at 0.5 mA cm−2 for LIBs without morphology
change even after 100 cycles. The QDFT calculations reveal that
the edge-enriched few-layered MoS2 nanosheets is favorable
for enhancing lithium storage capacity. Furthermore, a flexible
full cell is also assembled, demonstrating superior mechanical
strength and outstanding electrochemical performances. The
excellent flexibility and impressive Li+ storage capacity make
it appropriate for flexible wearable electronics applications in
future.
Experimental Section
The Preparation of 3DOM MoS2@C/CC Flexible Electrode: Negative
PSCOOH sphere is beforehand papered by acrylic acid modification.
Typically, 5 mL styrene, 0.5 mL acrylic acid, 0.12 g Na2CO3, and
0.1 g ammonium persulfate were dissolved in
100 mL deionized (DI) water with stirring at 70 °C
for 7 h under the inert gas protection. The white
suspension is purified by dialysis for 3 d and finally
dried in the oven at 50 °C. Subsequently, a piece of
the carbon cloth (CC, WOS1002) was successively
treated by acetone and DI water to remove the
impurities, followed by vacuum drying at 60 °C.
The pretreated carbon cloth was then immersed
into polyaniline/n-methyl-2-pyrrolidone solution
(0.025 wt%) for 1 h to make it exhibit positive
charge and then dipped into the precursor ink which
is papered by adding 20 mg glucose, 40 mg ATM,
and 1 g PSCOOH sphere in 5 mL DI water with
string for 2 h. The mass loading of MoS2@C can
be easy adjusted by controlling the impregnating
time and times. Finally, the MoS2@C/CC flexible
electrode was obtained by calcination at 600 °C for
2 h in Ar steam. The MoS2/CC electrode was also
obtained by the same procedure only without the
addition of glucose.
Supporting Information
Supporting Information is available from the Wiley
Online Library or from the author.
Acknowledgements
This work was supported by the National Natural Science Foundation
of China (21522602, 91534202 and 51672082), the Shanghai Rising-Star
Program (15QA1401200), the Program for New Century Excellent Talents
in University (NCET-13-0796), the International Science and Technology
Cooperation Program of China (2015DFA51220), the Program for
Shanghai Youth Top-notch Talent, and the Fundamental Research Funds
for the Central Universities.
Received: June 8, 2016
Revised: September 29, 2016
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