This article has been accepted for publication in a future issue of this journal, but has not been
fully edited. Content may change prior to final publication. Citation information: DOI
10.1109/TNANO.2014.2310512, IEEE Transactions on Nanotechnology
TNANO-00020-2014.R1
Activated Carbon Modified by CNTs/Ni-Co Oxide as Hybrid Electrode
Materials for High Performance Supercapacitors†
Qianqian Li, Jipeng Cheng, Binbin Wang, and Li Zhang, Senior Member, IEEE
 oxides, have potentially pseudocapacitive properties,
Abstract—Hybrid materials of carbon nanotubes (CNTs)
coated with nickel-cobalt (Ni-Co) oxide nanoparticles were
synthesized using electroless plating. Transmission electron
microscopy (TEM) observations showed that Ni-Co oxide
nanoparticles were dispersively distributed on the external
surface of CNTs. The composites of Ni-Co oxides modified CNTs
were used as additives of activated carbon (AC) to improve the
electrochemical performance of the electrode materials for
supercapacitors. The electrochemical properties of the
supercapacitors were investigated by galvanostatic charge-
discharge, cyclic voltammetry (CV), and alternating current
impedance techniques. The maximum specific capacitance
reached 215 F g-1, approximately 23% higher than that without
addition of the CNT-based composite, while the resistance of the
electrode was also reduced by addition of the composite. The
results revealed that the supercapacitor had an excellent charge-
discharge cycle behavior and electrochemical stability after 1200
continuous cycles. The improved performance of the
supercapacitor can be attributed to the modified structure and
high electrical conductivity of the electrode materials due to the
addition of the hybrid nanocomposite, which is promising for
energy storage applications.
I. INTRODUCTION
S upercapacitors are one kind of electrochemical energy
storage devices with a high specific power density, which
are very promising in many energy-related applications, and
currently can fill the gap between batteries and traditional
capacitors. They are generally classified into three different
types, i.e. electrochemical double-layer capacitor (EDLC),
pseudocapacitor and hybrid supercapacitor, according to
Conway [1].
Carbon nanotubes (CNTs) have been widely studied
their discovery in 1991 [2], and in 1997, Niu et al. [3]
that CNTs could be used as an electrode material of
supercapacitors owing to their tubular structure, nanoscale
dimensions, high surface area and excellent electrical
conductivity [4-13]. Moreover, CNT-based hybrid materials,
such as the composite consisting of CNTs and transition metal
Manuscript received January 13, 2014; revised March 1, 2014
Q. Q. Li is with Institute of Applied Mechanics, Zhejiang University,
Hangzhou 310027, China
J. P. Cheng, is with Department of Materials Science and Engineering,
State Key Laboratory of Silicon Materials, Zhejiang University, Hangzhou
310027, China (e-mail: chengjp@zju.edu.cn).
B. B. Wang is with epartment of Materials Science and Engineering, State
Key Laboratory of Silicon Materials, Zhejiang University, Hangzhou 310027,
China
L. Zhang is with Department of Mechanical and Automation Engineering,
and Shun Hing Institute of Advanced Engineering, The Chinese University of
Hong Kong, Hong Kong SAR, China (e-mail: lizhang@mae.cuhk.edu.hk).
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representing an important breakthrough in developing new-
new-generation of supercapacitors [6], [14-18]. However, the
specific capacitance of CNTs as an electrode material is not as
high as that was originally expected. Among various
carbonaceous materials, activated carbon (AC) has many
advantages including a much lower cost and less complexity
fabricating supercapacitor electrodes than CNTs.
its intrinsic poor electrical conductivity and low capacitance
retention at a high charge-discharge rate still require
revolutionary strategies to overcome.
In this report, we use AC as a main building block
material and the nanocomposite consisting of nickel-cobalt
(Ni-Co) oxide nanoparticles and CNTs as an additive of the
electrode materials, in order to develop a novel high-
performance supercapacitor. The results indicate that the
electrochemical performance of the supercapacitors is
improved through the addition of the composite of Ni-Co
oxide modified CNTs, and such kind of supercapacitors is a
promising candidate for energy storage applications [19-23].
II. EXPERIMENTAL METHODS
CNTs used here were prepared by CVD method as reported
elsewhere [24], and pretreated as follows prior to the
deposition of Ni-Co oxide nanoparticles. To modify the
surface of CNTs, they were boiled in high-concentration nitric
acid for 3 hours. After this, to sensitize the surface of CNTs,
0.5 g CNTs was dispersed into 20 ml SnCl2 solution with a
centration of 0.1 M by sonication, and stirred at room
temperature for more 20 minutes, and filtrated. Subsequently,
they were added into a 0.014 M PdCl2 solution and stirred for
20 minutes for activation of the CNTs surface. The activated
CNTs were then collected after filtration for the following
electroless plating of Ni-Co. The formula and experimental
conditions of the electroless plating solution are summarized
in Table 1. The as-synthesized nanocomposites consisting of
CNTs and Ni-Co nanoparticles were obtained after 2 h
annealing in an ambient atmosphere at 400 C. In addition,
pure CNTs, used as a control sample, were also modified
through boiling in nitric acid.
Table 1. Formula and operation condition of the electroplating bath
Formula Experimental conditions
NiCl2.6H2O (CoCl2.6H2O) 22 g/L
NaH2PO2.2H2O 15 g/L
NaHC6H5O7.1.5H2O 5 g/L
NH4Cl 60 g/L
Temperature 90C
Heating type Microwave
pH value 9.0
Electrochemical plating time 20 min
This article has been accepted for publication in a future issue of this journal, but has not been fully edited. Content may change prior to final publication. Citation information: DOI
10.1109/TNANO.2014.2310512, IEEE Transactions on Nanotechnology
TNANO-00020-2014.R1 2

AC powder (from China Forest Energy Corporation) was

selected as a main building block of the electrodes. Powder
polyvinylidene fluoride (PVDF) and N-methyl-2-pyrrolidone
(NMP, PuYang MYJ Technology Co., Ltd) were used as the
binder and solvent, respectively. The mass ratio of AC, the
hybrid of Ni-Co oxides coated CNTs and the binder was 8:1:1.
The mixtures were stirred for 6 hours at room temperature and
then were painted on nickel foams as electrodes. Then two
prepared electrodes were sandwiched by a polypropylene film,
tightly fixed by double plexiglass plates as a prototype of
supercapacitor, and were fully wetted with 6 M KOH
electrolyte. AC electrodes with pure CNTs as additive and
without additive were also prepared as the control samples, as
presented in Table 3.

III. RESULTS AND DISCUSSION

A typical TEM micrograph in Fig. 1a shows the
morphology and microstructure of the as-prepared
nanocomposite of Ni-Co oxide nanoparticles coated on CNTs.
The diameter of CNTs is in the range from 20 to 40 nm which
is a proper size for EDLCs electrode as reported in the
literature [24]. These metal oxide nanoparticles are uniformly
deposited and distributed on the external surface of CNTs.
Many structural defects should exist on the surface of CNTs
after chemical treatment in nitric acid, enabling more active
sites for the nucleation of metal oxide nanoparticles. Fig. 1b
shows the diameter distribution of Ni-Co oxide particles on
the surface of CNTs in the range from 3 nm to 8 nm. A high
resolution TEM image in Fig. 1c shows the regular lattice
fringes of 0.25 nm, corresponding to the (311) interplanar
spacing of Ni-Co oxide.
The phase composition of the Ni-Co oxides coated on
CNTs with different Ni/Co molar ratios (electroplating baths
for pure Ni, Ni-Co and pure Co as listed in Table 1) were
examined by XRD, and the corresponding patterns are shown
in Fig. 2. For the electroless plating solution only containing
Ni as a metal source, the presence of Ni crystalline phase
(JCDS NO. 04-0850) was accompanied by a diffraction peak
from NiO crystalline phase (JCDS NO. 44-1159), indicating
the existence of nickel oxide. When a mixed electroplating Fig. 1. (a) TEM image of CNTs coated with nickel-cobalt oxide nanoparticles;
solution was used, the Ni-Co oxide crystalline phases (b) diameter distribution of Ni-Co oxides nanoparticles; (c) high resolution
appeared. While for the electroplating of pure Co, only cobalt TEM image of Ni-Co oxide nanoparticles from sample 4.
oxide, i.e. Co3O4 (JCDS NO. 42-1467) appeared in the XRD
pattern, which revealed that cobalt particles were completely Nyquist plots of impedance curves show the relationship
oxidized under the subsequent annealing process. between the capacitance and the frequency [1].
It is notable that SnO2 phase could be found in all Electrochemical impedance spectroscopy (EIS) is a
samples. The SnO2 phase was introduced in the first step for nondestructive technique for evaluation of the kinetic and
surface modification before the chemical plating, implying mechanistic information of electrode materials. Fig. 3 shows
that Sn2+ was not been completely substituted by Pd2+. And it the Nyquist plots of the supercapacitors prepared with
turned out that more PdCl2 solution was required in order to different additives of electrodes, in which all the spectra are
completely react with Sn2+. However, it is not necessary to do similar in shape. The EIS measurements were performed
so, not only because Pd is an expensive noble metal for between 0.1 to 105 Hz. In the high frequency region, the
processing but also the residual SnO2 phase can act as an semicircle is related to the sum of the resistance of the
electrode material for supercapacitor with a high specific electrode [27-28], while in the low frequency region a vertical
capacitance, thus no negative effects on the performance of line represents the domination of the capacitive behavior at the
electrode would be introduced. [25-26] electrolyte and electrode material interface [29]. Furthermore,
model of equivalent circuit, shown in Fig. 3 inset, is applied to
quantitatively evaluate electric

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This article has been accepted for publication in a future issue of this journal, but has not been fully edited. Content may change prior to final publication. Citation information: DOI
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TNANO-00020-2014.R1
Fig. 2. XRD patterns of the nanocomposites composed of CNTs and metal
oxide particles: (a) nickel solution, (b) mixture of Ni-Co solution, and (c)
cobalt solution.
resistance for supercapacitors [30]. The simulation work was
carried out for samples 1, 2 and 4 using the software Zview®
based on the equivalent circuit. Fig. 3 shows that the simulated
curves have a good agreement with the experimental ones in
the high frequency range, while there is a little deviation in the
low frequency region for sample 4, mainly owing to some
pseudocapacitance introduced by the electrochemical reaction
of small amount of metal oxide in the electrode. The ideally
polarizable capacitance should exhibit a straight line in the
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Fig. 3. Nyquist plots of the electrodes with different addition of conductive
agents. Sample 1 is AC, sample 2 is AC with CNTs only and sample 4 is AC
with nanocomposite of Ni-Co oxide coated CNTs as conductive agents,
respectively (also see Table 2). The frequencies were tuned from 1 mHz to
100 KHz. The inset shows the model of equivalent circuit.
Table 2. The resistance value of Samples tested in Figure 3
Sample No. Ri () Cc (mFg- Rc () W (s- Cd (Fg-1)
1 1/2
) )
1 4.4 0.44 3.4 0.92 12.5
2 1.9 2.12 1.1 1.2 60
4 1.0 5.7 0.5 1.2 186
experimental data, which is generally parallel to the Z axis,
whereas, due to ohmic resistance, this line has a slight
deviation for a real device, representing the diffusive
resistance of the electrolyte within the pores of the electrode.
The diffusive line approaches to an ideal case for sample 4,
where the nanocomposite of Ni-Co oxide coated CNTs was
used as the additive of the conductive agent. The
corresponding resistance values were also calculated by the
software, as shown in Table 2, in which the symbols of Ri, Cc,
Rc, W, and Cd, represent the parameters of internal resistance,
contact capacitance, contact resistance, Warburg diffusion
rate, and the capacitance inside the pores, respectively. And
the value of Zw can be obtained according to the equation, Zw
= W/√jω, where j = √-1, and ω is the angular frequency [31].
One can find out that the resistance of the electrodes decreases
with the addition of CNTs (sample 2) or modified CNTs
(sample 4), while the resistance of the electrode of pure AC
(sample 1) is the highest among them. The decreased
resistance of the electrode by adding CNTs can be attributed
to the formation of CNTs networks in the electrode resulting
in an improvement of electrical conductivity. Furthermore, the
impedance curves in Fig. 3 indicate that the electrical
conductivity is the highest for the sample containing the
nanocomposite of Ni-Co oxide/CNTs (also shown in Table 2
for sample 4), which can be understood that the addition of the
nanocomposite of Ni-Co oxides/CNTs into the AC electrode
will modify the interfaces between the additive and AC
material, resulting in a larger interface area. This increases the
chance for the ions of the electrolyte to penetrate into the
porous AC structure through the enlarged interfaces, resulting
in the improvement of the specific capacitance and the charge-
discharge properties of the EDLC device.
This article has been accepted for publication in a future issue of this journal, but has not been fully edited. Content may change prior to final publication. Citation information: DOI
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TNANO-00020-2014.R1
Fig. 4. CV curves of the electrodes with different conductive agents. Sample 1
is pure AC, sample 2 using CNTs and sample 4 using the nanocomposite of
Ni-Co oxides coated CNTs as conductive agents, respectively.
The cyclic voltammograms (CV) tests were conducted
for the three samples, i.e. the sample of pure AC (sample 1),
with CNTs (sample 2) and with the composite of Ni-Co
oxide/CNTs (sample 4) added as a conductive agent, at a scan
rate of 10 mV/s, as shown in Fig. 4. The profiles of the CV
curves without obvious peaks indicate that the samples exhibit
dominantly double layer capacitance behavior. Nevertheless,
by careful inspection in the region of about 0.2 V for sample
4, a weak pseudocapacitance is present during the discharging
process owing to the existence of a small amount of metal
oxide in the electrode. The integrated value of the enclosed
area of CV curves for sample 4 is much larger than those of
samples 1 and 2, because of the structural modification and a
higher interface density. In addition, the integrated area of
sample 4 is also larger than those of samples 3 and 5, where
the CNTs are coated with NiO and Co3O4 as the conductive
agents, respectively (not shown in the figure), that is because
Ni-Co mixed oxides possess a higher electrochemical activity
than those of nickel and cobalt oxides as a single metal oxide
phase alone [32].
To evaluate the potential of the synthesized
nanocomposites for supercapacitor applications, the
corresponding mass-specific capacitances were calculated
from galvanostatic charge-discharge profiles (see Fig. 5) given
in Eq. (1).
C g  2It  /Vm 
(1)
where Cg (F g-1) is the mass-specific gravimetric capacitance,
I (A) is the current loaded, ∆t (s) is the discharge duration of
the negative process in the evaluated region, ∆V (V) is the
potential change during the discharge process and m (g) is the
mass of activated materials of the electrode.
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Fig. 5. The charge-discharge curves of the electrodes with different
conductive agents, in which sample 1 is AC, sample 2 with CNTs, sample 3,
4, and 5 with different CNTs-based nanocomposites (see Table 3).
Fig. 5 show typical charge-discharge curves in the
potential range of 0.01-1.0 V at a current density of 0.5 A g-1.
The approximately symmetric triangles in Fig. 5a indicate that
the circulation of the supercapacitors is excellent, which also
reveals that all the electrodes after the addition of Ni-Co oxide
nanocomposites are electrochemically stable, and that the
charge-discharge processes are reversible. The better stability
of the samples composed of nanocomposite additives than that
of sample 1 made by pure AC material can be observed in Fig.
5, in which the voltage dropped suddenly from 1.0 V to 0.85 V
just after charge finished for the case of sample 1. The
galvanostatic charge-discharge curves of all the electrodes are
almost symmetric, therefore, the corresponding values of
capacitance can be calculated from the DC discharge process.
The insert in Fig. 5 shows the discharge curves of potential vs.
time for all the samples. Their mass-specific capacitances
were also calculated according to Eq. (1), as listed in Table 3.
Table 3. The specific capacitances of the samples with different compositions
of the addtives
Sample No. Composition Specific capacitance
1 Without CNTs 175 F/g
2 CNTs 100 F/g
3 CNTs/NiO 124 F/g
4 CNTs/Ni-Co oxide 215 F/g
5 CNTs/Co3O4 161 F/g
The specific capacitance of sample 1 is 175 F g-1, slightly
higher than those of sample 2 (100 F g-1), sample 3 (124 F g-1)
and sample 5 (161 F g-1), but a much longer discharge period
is needed due to the higher resistance of the pure AC
electrode. The specific capacitance can reach the maximum
value of 215 F g-1, when the nanocomposite is used as the
additive of the electrical conductive agent (i.e. sample 4). The
enhanced performance of the supercapacitor can be attributed
to its higher electrical conductivity and the modified
microstructure of the electrode resulting from the larger
interface between the additive and AC materials, which can
provide more
opportunities to form EDLC. The cycling performance of the
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TNANO-00020-2014.R1
Fig. 6. The long cycling curves of sample 4 used CNTs/Ni-Co oxide as
conductive agents with charging current 0.05 A g-1. After 1200 cycles a
specific capacitance of about 250 Fg-1 was maintained.
sample 4 using CNT/Ni-Co oxide nanocomposite as the
conductive agent was further tested under a [10]
charging/discharging current density of 0.05 A g-1. The
results showed that the curve maintained nearly as a horizontal
line and a specific capacitance value of about 250 F g-1 was
kept after 1200 cycles in Fig. 6, indicating that the electrode
has an excellent cycling stability.
IV. CONCLUSIONS
Nanocomposites of CNTs coated with Ni-Co oxide
nanoparticles were synthesized using electroless plating,
which were then applied as the conductive agents of AC
electrode for supercapacitors. The resistance of the electrode
after the addition of nanocomposite of Ni-Co oxide coated
CNTs was the minimum in all the samples. The maximum
mass-specific capacitance of 215 F g-1 was obtained.
Moreover, the electrode showed an excellent cycling stability
even after 1200 continuous cycles. The results showed that the
specific surface, porosity, electrical conductivity, as well as
electrochemical activity can be tuned by adjusting the molar
ratio of nickel and cobalt in the electroless plating process.
More importantly, the modification of the conductive agent for
the electrode can significantly improve the electrochemical
performance of supercapacitors and pave the way for their
future applications in energy storage.
ACKNOWLEDGMENT
The authors thank the Micro and Nano Fabrication
Laboratory of The Chinese University of Hong Kong for
technical support. This work was financially supported by
Zhejiang Provincial Natural Science Foundation of China
(LY13E020002 and LZ12E06001), “the scholarship award for
excellent doctoral student from the Ministry of Education”
(Grant No. 188310-720907/014), and by the project No. RNE-
p4-13 of the Shun Hing Institute of Advanced Engineering,
The Chinese University of Hong Kong (CUHK).
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REFERENCES
[1] B. E. Conway, Electrochemical supercapacitors: scientific fundamentals
and technological applications, Springer, 1999.
[2] S. Iijima, “Helical microtubules of graphitic carbon”, Nature, vol. 354,
pp. 56-58, 1991.
[3] C. M. Niu, E. K. Sichel, R. Hoch, D. Moy, and H. Tennent, “High power
electrochemical capacitors based on carbon nanotube electrodes”, Appl.
Phys. Lett., vol. 70, pp. 1480-1482, 1997.
[4] J. P. Issi, L. Langer, J. Heremans, and C. H. Olk, “Elecctronic-properties
of carbon nanotubes – experimental results”, Carbon, vol. 33, pp. 941-
948, 1995.
[5] A. G. Pandolfo and A. F. Hollenkamp, “Carbon properties and their role
in supercapacitors”, J. Power Sources, vol. 157, pp.11-27, 2006.
[6] E. Frackowiak and F. Beguin, “Carbon materials for the electrochemical
storage of energy in capacitors”, Carbon, vol. 39, pp. 937-950, 2001.
[7] B. Zhang, J. Liang, C. L. Xu, B. Q. Wei, D. B. Ruan and D. H. Wu,
“Electric double-layer capacitors using carbon nanotube electrodes and
organic electrolyte”, Mater. Lett. vol. 51, pp.539-542, 2001.
[8] Q. Jiang, M. Z. Qu, G. M. Zhou, B. L. Zhang and Z. L. Yu, “A study of
activated carbon nanotubes as electrochemical super capacitors electrode
materials”, Mater. Lett., vol. 57, pp. 988-991, 2002.
[9] C. S. Li, D. Z. Wang, T. X. Liang, X. F. Wang, and L. Ji, “A study of
activated carbon nanotubes as double-layer capacitors electrode
materials”, Mater. Lett. vol. 58, pp. 3774-3777, 2004.
X.Y. Tao, X.B. Zhang, L. Zhang, J. P. Cheng, F. Liu, J. H. Lou, and H.
J. Geise, “Synthesis of multi-branched porous carbon nanofibers and
their application in electrochemical double-layer capacitors”, Carbon,
vol. 44, pp.1425-1428, 2006.
[11] L. Dong, X. Tao, L. Zhang, X. Zhang, and B. J. Nelson, “Nanorobotic
spot welding: controlled metal deposition with attogram precision from
copper-filled carbon nanotubes”, Nano Lett., vol. 7, pp. 58-63, 2007.
[12] L. Dong, K. Shou, D. R. Frutiger, A. Subramanian, L. Zhang, B. J.
Nelson, X. Tao, and X. Zhang, “Engineering multiwalled carbon
nanotubes inside a transmission electron microscope using nanorobotic
manipulation”, IEEE Trans. Nanotech. vol. 7, pp. 508-517, 2008.
[13] J. Fang, M. Li, Q. Li, W. Zhang, Q. Shou, F. Liu, X. Zhang, J. Cheng,
“Microwave-assisted synthesis of CoAl-layered double
hydroxide/graphene oxide composite and its application in
supercapacitors”, Electrochim. Acta., vol. 85, pp. 248-255, 2012.
[14] M. Hughes, G. Z. Chen, M. S. P. Shaffer, D. J. Fray, and A. H. Windle,
“Electrochemical capacitance of a nanoporous composite of carbon
nanotubes and polypyrrole”, Chem. Mater. vol. 14, pp. 1610-1613, 2002.
[15] C. Y. Lee, H. M. Tsai, H. J. Chuang, S. Y. Li, P. Lin, and T. Y. Tseng,
“Characteristics and Electrochemical Performance of Supercapacitors
with Manganese Oxide-Carbon Nanotube Nanocomposite Electrodes”, J.
Electrochem. Soc. vol. 152, pp. A716-A720, 2005.
[16] L. H. Su, X. G. Zhang, C. Z. Yuan, and B. Gao, “Symmetric Self-Hybrid
Supercapacitor Consisting of Multiwall Carbon Nanotubes and Co–Al
Layered Double Hydroxides”, J. Electrochem. Soc. vol. 155, pp. A110-
A114, 2008.
[17] F. L. Gao, L. J. Zhang, and S. M. Huang, “Fabrication horizontal aligned
MoO2/single-walled carbon nanotube nanowires for electrochemical
supercapacitor”, Mater. Lett., vol. 64, pp. 537-540, 2010.
[18] Q. Li, F. Liu, L. Zhang, B. J. Nelson, S. H.Zhang, C.Ma, X. Y.Tao, J. P.
Cheng, X. B.Zhang, “In situ construction of potato starch based carbon
nanofiber/activated carbon hybrid structure for high-performance
electrical double layer capacitor”. J. Power Sources vol. 207, pp. 199-
204, 2012.
[19] Q. Shou, J. Cheng, L. Zhang, B. J. Nelson, and X. Zhang, “ Synthesis
and characterization of a nanocomposite of goethite nanorods and
reduced graphene oxide for electrochemical capacitors”, J. Solid State
Chem., vol. 185, pp. 191-197, 2012.
[20] W. F. Zhang, C. Ma, J. H. Fang, X. B.Zhang, J. P. Cheng, S. R. Dong,
and L. Zhang, “Asymmetric electrochemical capacitors with high energy
and power density based on graphene/CoAl-LDH and activated carbon
electrodes”, RSC Adv., vol. 3, pp. 2483-2490, 2013.
[21] M. Zhi, C. Xiang, J. Li, M. Li, and N. Wu, “Nanostructured carbon–
metal oxide composite electrodes for supercapacitors: a review”,
Nanoscale, vol. 5, pp. 72-88, 2013.
[22] J. Cheng, X. Chen, J. Wu, F. Liu, X. Zhang, V. P. Dravid, “Porous cobalt
oxides with tunable hierarchical morphology for supercapacitor
electrodes”, CrystEngComm, vol. 14, pp. 6702-6709, 2012.
This article has been accepted for publication in a future issue of this journal, but has not been fully edited. Content may change prior to final publication. Citation information: DOI
10.1109/TNANO.2014.2310512, IEEE Transactions on Nanotechnology
TNANO-00020-2014.R1 6

[23] X. Chen, J. Cheng, Q. Shou, F. Liu, X. Zhang, “Effect of calcination

temperature on the porous structure of cobalt oxide microflowers”,
CrystEngComm, vol. 14, pp. 1271-1276, 2012.
Jipeng Cheng received his Ph.D. degree
[24] Y. Li, X. B. Zhang, X. Y. Tao, J. M. Xu, F. Chen, L. H. Shen, X. F. in materials science and engineering at
Yang, F. Liu, G. Van Tendeloo, and H. J. Geise, “Single phase MgMoO4 Zhejiang University in 2005 and
as catalyst for the synthesis of bundled multi-wall carbon nanotubes by is an associated professor in the State
CVD”, Carbon, vol. 43, pp. 1325-1328, 2005.
[25] F. Li, J. Song, H. Yang, S. Gan, Q. Zhang, D. Han, A. Ivaska, L. Niu,
Laboratory of Silicon Materials and
“One-step synthesis of graphene/SnO2 nanocomposites and its Department of Materials Science and
application in electrochemical supercapacitors”. Nanotechnology, vol. Engineering, Zhejiang University. His
20, pp. 455602, 2009. current field of interest is functional
[26] R. Selvan, I. Perelshtein, N. Perkas, A. Gedanken, “Synthesis of
hexagonal-shaped SnO2 nanocrystals and SnO2@ C nanocomposites for
nanomaterials.
electrochemical redox supercapacitors”; J. Phys. Chem. C,vol. 112, pp.
1825-1830, 2008.
[27] C. S. Li, D. Z. Wang, T. X. Liang, G. T. Li, X. F. Wang, M. S. Cao, and
J. Liang, “Oxidation behavior of CNTs and the electric double layer
capacitor made of the CNT electrodes”, Sci. China Ser. E-Technol. Sci.,
Binbin Wang received his bachelor
vol. 46, pp. 349-354, 2003. degree from the Department of Materials
[28] B. Z. Fang and L. Binder, “A Novel Carbon Electrode Material for Science and Engineering at Jinan
Highly Improved EDLC Performance”, J. Phys. Chem. B, vol. 110, pp. University in 2011. He is pursuing his
7877-7882, 2006.
[29] Y. W. Ju, G. R. Choi, H. R. Jung, and W. J. Lee, “Electrochemical
M.S. degree in the Department of
properties of electrospun PAN/MWCNT carbon nanofibers electrodes Materials Science and Engineering at
coated with polypyrrole”, Electrochim. Acta, vol. 53, pp. 5796-5803, Zhejiang University with a research topic
2008. on synthesis of nanomaterials.
[30] C. W. Huang, C. H. Hsu, P. L. Kuo, C. T. Hsieh and H. Teng,
“Mesoporous carbon spheres grafted with carbon nanofibers for high-rate
electric double layer capacitors”, Carbon, vol. 49, pp. 895-903, 2011.
[31] C. W. Huang and H. Teng, “Influence of carbon nanotube grafting on the
impedance behavior of activated carbon capacitors”, J. Electrochem. Li Zhang (SM'12) received the B.S.
Soc., vol. 155, pp. A739-A744, 2008.
[32] Y. H. Lee, K. H. An, W. S. Kim, Y. S. Park, Y. C. Choi, S. M. Lee, D.
degree from the Department of
C. Chung, D. J. Bae, and S. C. Lim, “Supercapacitors using single- Science and Engineering, Zhejiang
walled carbon nanotube electrodes”, Adv. Mater. vol. 13, pp. 497-500, University, Hangzhou, China, in 2000,
2001. the M.S. degree from the Department of
Materials Science and Engineering,
Qianqian Li received the B.S. degree in Christian Albrechts University, Kiel,
Department of Material Science and Germany, in 2002, and the Ph.D. degree
Engineering from University of Jinan, from the University of Basel, Basel, Switzerland, in 2007.
Jinan, China, in 2009 and M.S. degree in Afterwards, he joined the Institute of Robotics and Intelligent
Department of Materials Science and Systems (IRIS), Swiss Federal Institute of Technology (ETH)
Engineering from Zhejiang University, Zurich, Switzerland, as a postdoc in 2007, and as a senior
Hangzhou, China in 2011. She is currently scientist from 2009 to 2012.
pursuing the Ph.D. degreee in Insitute of He is currently an Assistant Professor in the Department of
Applied Mechanics from Zhejiang Mechanical and Automation Engineering and an associate
University, Hangzhou, China. faculty member in the Biomedical Engineering Programme at
From 2009 to 2011, she did some research on double layer The Chinese University of Hong Kong. His main research
supercapacitor using active carbon or carbon nanotubes as interests include micro-/nanomachines for biomedical
electrode materials. From 2011-2014, her research focused on applications, and nanomaterials for energy storage and
in situ TEM study of the reaction mechanism of anode environmental applications.
materials for lithium ion battery. She was awarded Dr. Zhang is a senior member of IEEE and a member of
“Scholarship Award for Excellent Doctoral Student Granted MRS. Since 2004 he has authored and co-authored over 80
by Ministry of Education”. peer-reviewed papers.

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