CARBON 9 2 ( 2 0 1 5 ) 3 1 8 –3 2 6

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Enhancing electrochemical properties of graphite

anode by using poly(methylmethacrylate)–
poly(vinylidene fluoride) composite binder

Yan Wang a, Huiyuan Zheng a, Qunting Qu a,*

, Li Zhang a, Vincent S. Battaglia b,
Honghe Zheng a,*
a
College of Physics, Optoelectronics and Energy & Collaborative Innovation Center of Suzhou Nano Science and Technology,
Soochow University, Suzhou, Jiangsu 215006, PR China
b
Lawrence Berkeley National Laboratory, 1 Cyclotron Rd, Berkeley, CA 94720, USA

A R T I C L E I N F O A B S T R A C T

Article history: Poly(methylmethacrylate)–poly(vinylidene fluoride) (PVDF–PMMA) composite binder is

Received 9 February 2015
Accepted 27 April 2015
Available online 2 May 2015
adopted for preparation of graphite electrode laminate in lithium-ion batteries. Compared
to that using the traditional PVDF binder, the electrode with composite binder exhibits
significantly enhanced electrochemical performance in terms of rate capability, specific
capacity and cycling behavior. At a very high discharge rate of 50 C, the electrode with
PVDF–PMMA binder still retains more than 80% of its capacity while the electrode based on
PVDF binder only delivers 16.2% of its capacity. The significant improvement of the rate capa-
bility is due to the improvement of Li ion diffusion within the graphite anode. Electrochemical
impedance spectroscopy study shows that Li ion diffusion coefficient in the graphite anode is
increased by an order of magnitude. After 200 charge–discharge cycles, capacity retention of
the electrode is also considerably higher than with single PVDF binder. This is due to the good
stability of the solid electrolyte interphase formed on the graphite electrode.
 2015 Elsevier Ltd. All rights reserved.

1. Introduction respect, improvement of the electrochemical behavior of gra-

Graphitic carbon materials are widely adopted as lithium ion
battery (LIB) anodes in industry because they can deliver more
than 350 mAh g1 of reversible capacity (theoretically
372 mAh g1) with low working potential close to that of
lithium metal, excellent electrical conductivity, environmental
friendliness and low cost. With the increasing demand for elec-
tric vehicle (EV) and energy-storage system (ESS) applications,
large-scale LIB emerged as the most promising power source.
Electrochemical behavior of graphite anode, to a great extent,
determines the overall performance of the battery. In this
phite anode is of great significance for the fabrication of high
performance LIBs. To attain this goal, much more effort has
been made in optimizing the graphite particle structure, tex-
ture, grain size and surface conditions. However, it is still not
enough. Because the graphite electrode laminate is a compos-
ite consisting of graphitic carbon particles, polymeric binder,
and conductive carbon additive, to improve the overall electro-
chemical properties of the graphite laminate, it is clearly not
enough to consider only active material modifications.
Electrode binder joins active materials and conductive addi-
tives into a cohesive laminate and provides the adhesion

* Corresponding authors.
E-mail addresses: qtqu@suda.edu.cn (Q. Qu), hhzheng@suda.edu.cn (H. Zheng).
http://dx.doi.org/10.1016/j.carbon.2015.04.084
0008-6223/ 2015 Elsevier Ltd. All rights reserved.
 CARBON 9 2 (2 0 1 5) 3 1 8–32 6
between the laminate and the current collector. Therefore, it
plays a very important role affecting the overall electrochemi-
cal behavior of the electrode. In the past two decades,
poly(vinylidene fluoride) (PVDF) was the most widely used bin-
der material for LIB electrodes. This is attributed to its good
electrochemical stability, binding capability and ability to
absorb electrolyte [1–5]. However, PVDF is readily swollen,
gelled, or dissolved by nonaqueous liquid electrolytes to form
a viscous fluid or gel polymer electrolyte, which results in
desquamation of electrode particles and hence capacity fading
and cycle life shortening [6–8]. Besides, this binder strongly
blocks Li migration and the rate performance of the electrode
is thus significantly affected [9,10]. Many studies of binders
have mainly focused on the adoption of new binder com-
pounds to enhance the binding affinity between active mate-
rial, carbon additive and current collector. This helps to
maintain a complete electronic network with a certain level
of electrode uniformity and thus contributes to an electro-
chemical improvement of the electrode. Gelatin [11–14],
sodium carboxy-methyl cellulose (CMC-Na) and styrene-
butadienerubber (SBR) [15–20], poly(acrylic acid) (PAA) [5,21–
23], poly(methacrylic acid) (PMA) [1], poly(vinylalcohol) (PVA)
[24], alginate [25], poly(acrylamide-co-diallyldime-thylammo
nium-chloride) (AMAC) [26], poly(acrylonitrile-methyl
methacrylate) (AMMA) [6], and polyimide (PI) [27], all have been
reported as promising new binder systems replacing PVDF and
some of them have been successfully used in commercial
lithium ion batteries. However, none of the reports has
attempted to facilitate Li ion migration and improve the rate per-
formance of graphite electrode through binder optimization.
In this paper, PMMA and PVDF composite binder was
adopted for fabrication of graphite anode laminate with high
electrochemical performance. The molecular structure of
PMMA and PVDF is provided in Fig. 1. PMMA has been adopted
as polymer electrolyte in LIBs due to its high thermal stability
(decomposition temperature >330 C), and good ionic conduc-
tivity because of the excellent polymeric segmental motion
and affinity between the ester group of PMMA and the car-
bonate ester group of EC and DMC [28,29]. However, it has
rarely been adopted as electrode binder because of its poor
adhesion. Hu et al. [30] have shown that PMMA binder has
very poor adhesion with obvious debonding of active materi-
als during electrochemical cycling. To incorporate the advan-
tage of good ionic conductivity of PMMA and good binding
capability of PVDF, we prepared graphite laminates using
PVDF–PMMA composite binder. Electrochemical tests show
Fig. 1 – The molecular structures of PVDF and PMMA.
319
that the rate performance and cycling stability of the graphite
electrode is significantly enhanced. The new approach of
using composite binder to substantially improve the electro-
chemical performance of carbon anode is very promising for
preparation of high quality graphite anode to meet the high
demands of EVs and ESSs.
2. Experimental
2.1. Preparation of electrodes
Spherical graphite powders (Shenzhen Beterui new energy
Materials Group Co., Ltd. Code No AGP-8, China) were applied
as the electrode active material. Battery-grade acetylene black
(AB) with an average particle size of 40 nm was acquired from
Denka Singapore Private Co., Ltd. Poly(vinylidene fluoride)
(KF1100) binder was supplied by Kureha, Japan. PMMA binder
and N-methylpyrrolidone (NMP) solvent was purchased from
Aldrich chemical company.
Graphite anodes were prepared by casting slurries con-
taining 83% graphite, 12% PVDF, and 5% acetylene black in
NMP solvent onto copper foil by doctor blade method. The
slurry with PVDF–PMMA composite binder was prepared by
thoroughly mixing the graphite material and acetylene black
together in NMP solvent. 12% of PVDF and PMMA with a
weight ratio of 1:1 was then added into the premixed
graphite/AB/NMP mixture. The obtained slurry was further
homogenized using a FA25 superfine homogenizer at a rate
of 4000 rpm for 15 min. As a reference, electrodes using a sin-
gle PVDF and PMMA binder of 12% weight ratio were prepared
according to the same procedure.
Through varying the height of the blade, all the electrode
films were cast to have approximately the same loading of
active material (around 3.0 mg cm2). The obtained electrodes
were dried at 120 C in vacuum for 12 h to completely remove
the NMP solvent. In order to determine the electronic conduc-
tivity of the laminate, the electrode film was peeled off from
the Cu substrate. The dc conductivity measurement was per-
formed using a Double testing digital four-probe tester
(ST2263, Suzhou Jingge Electronic Co., Ltd.). To enhance the
adhesion between the active material and current collector,
the electrode laminates were pressed with a calendering
machine before use. At last, the electrodes were punched into
small disks with area of 1.33 cm2 to assemble coin cells for
electrochemical testing.
2.2. Electrochemical tests
Li//graphite cells were assembled in an Ar-filled glove box
(<0.5 ppm of oxygen and water, OMNI-LAB, VAC) using a com-
mercial electrolyte consisting of 1 M LiPF6 in ethylene carbon-
ate/diethylene carbonate/dimethyl carbonate (EC/DEC/DMC,
v/v/v = 1:1:1) (Novolyte Technologies). Celgard 2400 was
adopted as the separator.
Galvanostatic charge–discharge cycling of Li//graphite
cells were conducted at 30 C using Maccor S4000 (Maccor
Instruments, USA). Three formation cycles at C/20 charge
and discharge were applied between 0.01 and 2 V vs. Li/Li+.
Rate test of the graphite electrodes consisted of full dis-
charges at rates of C/10, C/5, C/2, 1, 2, 5, 10, 20, 30 and 50 C
320 CARBON 9 2 ( 2 0 1 5 ) 3 1 8 –3 2 6
respectively. Long-term cycling of the cells was carried out
with 0.2 C charge and 0.5 C discharge for 200 cycles. Cyclic
voltammetry (CV) was performed on an Autolab potentiostat
(PGSTAT302N, Autolab Instruments, Switzerland) in the
voltage range of 0.01–2 V at a rate of 0.05 mV s1.
Electrochemical impedance spectroscopy (EIS) was performed
on a Zahner Elektrik IM6 electrochemical work station over
the frequency range of 102–105 Hz with an alternating volt-
age of 5 mV. All impedance measurements were carried out
at the discharge state of 60% DOD (depth of discharge) after
rate tests. Before test, the cell was rested for at least 5 h at
30 C. The impedance spectra (100 kHz to 10 MHz, 5 mV per-
turbation) of the cells were then recorded.
2.3. Materials characterization
Morphologies of the graphite electrodes with different bin-
ders before and after electrochemical tests were observed by
scanning electron microscopy (SEM) using a Hitachi S-4700
operated at 15 kV accelerating voltage and energy dispersive
X-ray spectroscopy (EDX). The crystallinity of PVDF, PMMA
and PVDF–PMMA composite was characterized with an
automated X-ray diffractometer (PANalytical X’Pert PRO,
Netherlands) using Cu Ka radiation (k = 1.5406 Å). The diffrac-
tion angle (2h) was stepped between 10 and 60 with an
increment of 1 min1.
3. Results and discussion
Fig. 2 compares the electronic conductivity of the graphite
laminates with different binders measured with a four probe
technique. For the graphite laminate using PVDF binder, the
electronic conductivity is obtained to be around 4.66 S cm1.
The high electronic conductivity is due to the good binding
capability of the binder between graphite particles. When
PVDF–PMMA composite binder was used, electronic conduc-
tivity of the graphite laminate is about 4.49 S cm1. A slight
decrease of the electronic conductivity should be associated
Fig. 2 – The electronic conductivity of the graphite laminates
based on different binders.
with the decrease of adhesion between graphite particles
due to the adoption of PMMA binder. For the graphite lami-
nate with pure PMMA binder, the electronic conductivity is
only about 0.65 S cm1. The very low electronic conductivity
may result from the worse binding ability of the single
PMMA binder. Poor connectivity makes the electronic path
between graphite particles less effective in the graphite
laminate.
Fig. 3 displays the CVs of the graphite electrodes with dif-
ferent binders. For the graphite electrode with pure PVDF bin-
der, the small cathodic peak at 0.75 V vs. Li/Li+ is due to the
well known reduction of electrolyte components at the elec-
trode/electrolyte interface, leading to the formation of SEI
film. Toward negative potential, three typical cathodic peaks
are attributed to the formation of stage-4, stage-2 and stage-
1 graphite intercalation compound (GIC), respectively. By con-
trast, the electrode using PMMA binder shows strong irre-
versible reaction peak at 0.8 V vs. Li/Li+. Meanwhile,
reversible lithium intercalation and deintercalation reactions
are significantly reduced. No unexpected peak is observed in
the potential range, suggesting that the PMMA is electro-
chemically stable in the working window. It is interesting to
see, that with PVDF–PMMA composite binder, the irreversible
reduction currents arising from electrolyte reduction is very
low, while the cathodic peaks characteristic of reversible
lithium intercalation into graphite interlayer and the anodic
peaks characteristic of lithium de-intercalation from graphite
interlayer are significantly enlarged. Besides, the three catho-
dic peaks are well separated compared to that with single
PVDF binder, implying the addition of PMMA into the elec-
trode matrix facilitates the electrochemical kinetics.
The first discharge–charge curves of the graphite anode
using different binders are shown in Fig. 4. For the graphite
electrode using traditional PVDF binder, the reversible capac-
ity is obtained to be 349.3 mAh g1 and the first coulombic
efficiency is 87.4%. Meanwhile, a reversible capacity of
162.1 mAh g1 is obtained for the electrode with single
PMMA binder and the first coulombic efficiency is only
62.2%. As the electrochemical property of the electrode with
a single PMMA binder is very poor, it is not subjected to fur-
ther investigation in this work. By contrast, the electrode with
PVDF–PMMA composite binder showed a much enhanced
reversible capacity of 397.6 mAh g1 and the first coulombic
efficiency is 88.1%. This reversible capacity value exceeded
the theoretical capacity of 372 mAh g1 for graphite material.
The high reversible capacity should be attributed to two rea-
sons. One is the high utilization of the active material due
to an improved polymeric network by the addition of PMMA
binder. The other reason may be associated with the electro-
chemical lithiation of the acrylic ester polymers. Ohta et al.
[27] have reported that the carbonyl oxygen atoms in the dii-
mide ring are active sites. Carbonyl oxygen atoms of PMMA
can be the active sites which may contribute an extra capacity
to the electrode. Of course, this needs further confirmation.
Fig. 5 shows the rate capability of the graphite anode with
different binders. As shown in this figure, the graphite elec-
trode with PVDF–PMMA composite binder shows a much
improved rate performance compared to that using PVDF bin-
der. At 1 C rate of discharge, both the electrodes with PVDF–
PMMA composite binder and pure PVDF binder were able to
 CARBON 9 2 (2 0 1 5) 3 1 8–32 6
Fig. 3 – Cyclic voltammograms of the graphite electrodes
with different binders: (a) PVDF, (b) PMMA (c) PVDF–PMMA.
(A color version of this figure can be viewed online.)
deliver almost 100% of their reversible capacity. At 30 C rate,
the electrodes with PVDF–PMMA composite binder retained
more than 92% of its reversible capacity while the electrode
with PVDF binder only delivered less than 50% of its capacity.
At a very high discharge rate of 50 C, the electrode based on
PVDF–PMMA binder still retained more than 80% of its capac-
ity while the electrode with PVDF binder exhibited only 16.2%
of its reversible capacity. When the discharge rate was
321
Fig. 4 – The first charge–discharge profiles of the graphite
anode using (a) PVDF, (b) PMMA and (c) PVDF–PMMA binder.
(A color version of this figure can be viewed online.)
returned to C/20, both electrodes showed a total recovery of
their initial capacity, indicating a good cycling stability of
the graphite anode.
Fig. 5b and c shows discharge profiles of the graphite elec-
trodes based on PVDF–PMMA and PVDF binder. It can be seen,
that at low discharge currents (from C/20 to 2 C), both elec-
trodes display the typical plateaus of graphite anodes except
a slight elevation of the discharge plateau due to the polariza-
tion of the cell resulting mainly from the internal resistance
of the cell. When the discharge rate exceeds a certain value,
a sudden capacity loss of the electrode is observed, which is
mainly due to Li ion diffusion limitation in the electrode. If
there is a large gradient of the Li+ ion concentration within
the electrode, the potential will rise quickly to the cut-off
potential. It can be seen that 5–10 C is the maximum working
rate for the electrode based on PVDF binder. Further increase
of C rate leads to a dramatic drop of the available capacity.
This is because the diffusion of Li ion in the electrode
becomes the determining factor controlling the reaction rate.
As for the graphite electrode based on PVDF–PMMA binder, Li
ion diffusion controls the electrochemical reaction at around
50 C current. The result reveals that the adoption of PMMA
binder facilitates Li ion diffusion and contributes to a signifi-
cant improvement of rate performance of the electrode.
The poor rate capability of the graphite anode with PVDF
binder is associated with the strong Li blocking effects of
PVDF binder. In a previous study, we have shown the ion-
blocking property of the ionic insulating PVDF binder in
LiNi0.8Co0.15Al0.05O2 cathode [9]. Addition of PMMA may con-
tribute to a decrease of the crystallinity. This helps to reduce
Li blocking effects of PVDF binder. XRD patterns of PVDF,
PMMA and PVDF–PMMA at different states were compared.
Fig. 6a shows the XRD patterns of polymer powders. For the
PVDF polymer, X-ray diffraction data clearly shows that this
polymer consists of crystalline regions, and four diffraction
peaks can be clearly seen at 2h = 18.46, 20.08, 26.77, and
38.68. For the PMMA polymer, the typical broad peak around
2h = 13 suggests the amorphous nature of this binder. The
322 CARBON 9 2 ( 2 0 1 5 ) 3 1 8 –3 2 6
Fig. 5 – (a) Rate capability of the graphite electrodes using
PVDF–PMMA and PVDF binder. Discharge (delithiation)
profiles of graphite electrode with (b) PVDF and (c) PVDF–
PMMA at different C rates. (A color version of this figure can
be viewed online.)
significantly decreased intensity of the diffraction peaks for
PVDF–PMMA composite suggests the reduced crystallinity of
Fig. 6 – XRD pattern of the (a) polymer powders and (b)
polymer films formed by casting the polymer solutions onto
a zero background sample holder. (A color version of this
figure can be viewed online.)
PVDF by blending it with amorphous PMMA. Fig. 6b shows
XRD patterns of the dry polymer films prepared by casting
the polymer solutions onto a zero background sample holder
followed by evaporation of solvent. For the PVDF film, two
characteristic peaks are clearly observed at 2h = 20.08 and
38.68, indicating the high crystallinity of PVDF. For the
PVDF–PMMA composite, compared with pure PVDF, the disap-
pearance of the peak at 38.68 and the slight decrease of the
intensity of the diffraction peak at 20.08 confirm that the
crystallinity of PVDF was greatly reduced. The reduction of
the crystallinity should be due to the addition of amorphous
PMMA, which interrupts the ordered arrangement of PVDF
chains. The reduced crystallinity is expected to increase the
mobility of Li+ by modifying the segmental motion of polymer
chains. In this aspect, the Li+ blocking effect of the binder
resulting from the stiffness of the polymer chain is mitigated
[31–35].
In order to further confirm our conclusion that PMMA
binder facilitates Li ion diffusion in the graphite electrode,
electrochemical impedance spectroscopy measurements of
Li//graphite cells based on different binders were conducted.
 CARBON 9 2 (2 0 1 5) 3 1 8–32 6
In the Li//graphite half cells, Li foil is used as both the counter
and reference electrodes. So any changes in the impedance of
the cells through use of different binders can directly reflect
the impedance changes of the graphite electrodes. As shown
in Fig. 7, the Nyquist plot consists of two depressed semicir-
cles in high and intermediate frequency region and a straight
line in low frequency region. The first semicircle in the high
frequency region reflects the impedance of SEI film (RSEI).
The second semicircle in the intermediate frequency region
is related to the charge transfer process occurring at the elec-
trode surface (Rct). The linear parts appearing at the low-
frequency region is due to the Warburg diffusion associated
with the finite Li ion diffusion in the graphite anode [36]. By
comparison, the overall impedance of the electrode based
on PVDF–PMMA composite binder is significantly lower than
that based on PVDF binder. The significantly decreased RSEI
and Rct of PVDF–PMMA binder should be associated with the
improved properties of the electrode/electrolyte interface as
discussed below.
The Li+ diffusion coefficient (DLi) in graphite anode can be
calculated using the following equation [37]:
R2 T2
DLi ¼
2A2 n4 F4 C2 r2w
where n is electron number for each molecule during Li ion
insertion, A is the surface area of the cathode, F is the
Faraday constant, C is Li ion concentration, and r is the
Warburg factor. The lithium diffusion coefficient in the gra-
phite anode based on PVDF binder calculated from above
equation is obtained to be about 1.24 · 1015 cm2 s1. By con-
trast, DLi of the electrode based on PVDF–PMMA composite
binder is as high as 1.64 · 1014 cm2 s1, more than an order
of magnitude larger than that of PVDF based electrode.
Fig. 8 displays the long-term cycling performance of the
graphite anodes with different binders. As shown in this fig-
ure, PVDF–PMMA-based graphite anode shows a significantly
enhanced cycling performance during 200 electrochemical
cycles. It is seen that the capacity retention of the PVDF-
Fig. 7 – Nyquist plots of graphite electrodes using PVDF and
PVDF–PMMA binder after rate tests at 60% DOD. (A color
version of this figure can be viewed online.)
323
based electrode is no more than 66% while the capacity reten-
tion of the PVDF–PMMA based electrode is not less than 92%.
This result clearly reveals that binder modification also influ-
ences the long–term cycling performance of graphite anode.
Coulombic efficiency is an important factor reflecting the sta-
bility of the electrode and the electrode/electrolyte interface
during the long-term electrochemical cycles. It is noticed that
the coulombic efficiency of the graphite anode based on
PVDF–PMMA composite binder attains 99.9% after initial elec-
trochemical cycles, significantly higher than 96.9% for the
PVDF-based electrode during the long-term cycling. As
coulombic efficiency reflects the side reactions at the elec-
trode/electrolyte interface, high coulombic efficiency of the
electrode with PVDF–PMMA composite binder indicates a
stable electrode/electrolyte interface in the electrolyte.
Fig. 9 shows the SEM images of pristine graphite electrodes
based on different binders and the electrode after the long-
term cycling test. For the pristine electrode morphologies of
the PVDF based and PVDF–PMMA based graphite electrodes
seem quite similar. The spherical graphite of 10–20 l in diam-
eter can be clearly observed and the conductive carbon addi-
tive is homogenously distributed in the electrode laminate.
After long-term cycling, cracks as marked out in the oval
areas are clearly seen on electrode based on PVDF binder,
indicating the relatively high brittleness of the electrode.
The appearance of a thick film on the surface of graphite elec-
trode as compared with the fresh electrode is associated with
the growth of the solid electrolyte interphase (SEI) resulting
from side reactions at the electrode/electrolyte interface. By
comparison, for the electrode with PVDF–PMMA composite
binder, no crack or fracture is observed on the electrode sur-
face. This can be explained with the good elasticity of the
electrode due to the presence of PMMA binder. The electrode
surface also seems quite smooth and uniform, showing a
stable SEI film formed on the graphite electrode. This implies
that electrode binder greatly influences the formation of SEI
film on the electrode surface. This is consistent with the
result reported by Li et al. [25,38]. They showed that the
Fig. 8 – Cycling performance of the graphite electrodes with
different binders (solid and open symbols indicate capacity
retention and Coulombic efficiency, respectively). (A color
version of this figure can be viewed online.)
324 CARBON 9 2 ( 2 0 1 5 ) 3 1 8 –3 2 6

(a) (b)

(c) (d)

Fig. 9 – SEM images and EDX analyses of graphite electrodes with (a and c) PVDF and (b and d) PVDF–PMMA binders: (a and b)
pristine electrode, (c and d) after 200 charge/discharge cycles. (A color version of this figure can be viewed online.)

property and physical distribution of binder play an impor-
tant role in the properties of SEI layer. In this respect, the
low impedance of the graphite electrode based on PVDF–
PMMA composite binder as shown in Fig. 7 could be attributed
to the improved properties of SEI.
According to the EDX results of the graphite anode sur-
faces with different binders after 200 cycles, oxygen content
of electrode based on PVDF–PMMA composite binder is con-
siderably higher than that of the PVDF-based electrode. This
is believed to be attributed to the PMMA binder in which the
O atoms are involved in the SEI formation reaction. Komaba
et al. [1–3,5] reported that the electrostatic interaction
between the positively charged lithium ions and negatively
charged oxygen atom in the polymer should modulate the
SEI properties at the electrode/electrolyte interface. In this
sense, PMMA plays a role in the build-up of a stable SEI film
at the electrode/electrolyte interface and this explains the
good cycling performance of the electrode based on PVDF–
PMMA composite binder.
4. Conclusion
PVDF–PMMA composite binder was utilized for preparation
of graphite anode in Li-ion batteries. Compared to the
electrode using conventional PVDF binder, rate capability and
cycling behavior are considerably improved. The significant
 CARBON 9 2 (2 0 1 5) 3 1 8–32 6
improvement of the rate capability is believed to be due to the
improvement of Li ion migration within the electrode. The
adoption of PMMA binder facilitates Li ions diffusion and Li
ion diffusion coefficient within the graphite anode is
increased by an order of magnitude. The decreased crys-
tallinity of PVDF by the addition of PMMA explains superior
Li ion migration properties in the electrode. The excellent
cycling performance of the electrode based on PVDF–PMMA
binder is associated with the stable SEI formed on the gra-
phite electrode. PMMA plays a role in the build-up of the SEI
film at the electrode/electrolyte interface, which is beneficial
for the electrochemical properties of graphite anode.
Acknowledgment
This work was financially supported by the National Natural
Science Foundation of China (NSFC Nos. 51272168 and
21473120).
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