Journal of Power Sources 325 (2016) 329e336

Contents lists available at ScienceDirect

Journal of Power Sources

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

A high-performance dual-scale porous electrode for vanadium redox

flow batteries
X.L. Zhou, Y.K. Zeng, X.B. Zhu, L. Wei, T.S. Zhao*
Department of Mechanical and Aerospace Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong, China

h i g h l i g h t s

A dual-scale porous electrode is developed for flow batteries.

The developed electrode offers high specific surface area.

The battery with the dual-scale electrode offers high performance.

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

Article history: In this work, we present a simple and cost-effective method to form a dual-scale porous electrode by
Received 20 April 2016 KOH activation of the fibers of carbon papers. The large pores (~10 mm), formed between carbon fibers,
Received in revised form serve as the macroscopic pathways for high electrolyte flow rates, while the small pores (~5 nm), formed
5 June 2016
on carbon fiber surfaces, act as active sites for rapid electrochemical reactions. It is shown that the
Accepted 9 June 2016
Brunauer-Emmett-Teller specific surface area of the carbon paper is increased by a factor of 16 while
maintaining the same hydraulic permeability as that of the original carbon paper electrode. We then
apply the dual-scale electrode to a vanadium redox flow battery (VRFB) and demonstrate an energy
Keywords:
Dual-scale
efficiency ranging from 82% to 88% at current densities of 200e400 mA cm2, which is record breaking as
Flow battery the highest performance of VRFB in the open literature.
Electrode © 2016 Elsevier B.V. All rights reserved.

1. Introduction made significant progress in market penetration, owing to its high

Electricity generated from intermittent renewable energy
sourcesdsuch as solar and wind need to be harnessed in order to
supplant the grid for cheap, efficient and reliable energy deploy-
ment. To do this, large-scale energy storage technologies are
indispensable for tackling the issues of intermittent supply and
variable demand [1e3]. Among the selection of energy storage
technologies, redox flow batteries (RFBs) offer unique characteris-
tics, including excellent scalability, high efficiency, long cycle life
and are generally safe [4e6]. In particular, the vanadium redox flow
battery (VRFB) has been recognized as one of the most promising
technologies, primarily because it uses the same element in both
half-cells, which avoids the issue associated with cross-
contamination between the two half-cell electrolytes [7e10].
Despite its attractive merits, however, VRFB technology has not
* Corresponding author.
E-mail address: metzhao@ust.hk (T.S. Zhao).
cost [11e14]. The capital cost, expressed in terms of the unit cost of
power (US$/kW) or the unit cost of energy capacity (US$/kWh), is
inarguably the largest contributor of high expenditure by sector.
The total capital cost of a VRFB system consists primarily of the
electrolyte cost and stack cost, which can be expressed as [12]:
.  . 
Ctot zCs þ Ce zUs t$I$Veff þ Ue Veff $UE (1)
where Ctot, Cs and Ce are the total cost, stack cost and electrolyte cost
($ per kWh), respectively; Us is the unit cost of the stack including
electrodes, membranes and bipolar plates ($ per m2); Ue is the unit
cost of the electrolyte including redox elements and supporting
salts/acids ($ per Ah); UE is the electrolyte utilization; I is the cur-
rent density (A m2); t is the designed discharge duration (h); and
Veff is the effective discharge cell voltage (V). The effective discharge
cell voltage can be estimated by Ref. [12]:

http://dx.doi.org/10.1016/j.jpowsour.2016.06.048
0378-7753/© 2016 Elsevier B.V. All rights reserved.
330 X.L. Zhou et al. / Journal of Power Sources 325 (2016) 329e336
Veff ¼ Vrev  hact  hohm  hcon (2)
where Vrev is the reversible voltage; hact, hohm, and hcon are the
activation, ohmic and concentration losses, respectively. According
to eqns. (1) and (2), a reduction in the capital cost for RFBs with
given redox couples like VRFBs can only be accomplished by
simultaneously maximizing the operating current density and
minimizing the voltage losses. Namely, improving the rate capa-
bility and efficiency of the VRFB through cost-effective approaches
is critical for commercialization.
Electrode design is essential to achieving a high performance
and efficient VRFB primarily because it contributes to the system
polarization through not only the ohmic polarization, but also
through activation polarization and concentration polarization.
Therefore, ideal porous electrodes for high-power VRFBs should
possess the following properties: i) high surface activity and spe-
cific surface area for electrochemical reactions to minimize the
activation loss; ii) large hydraulic permeability for efficient elec-
trolyte transportation to minimize the concentration loss and
pumping work; and iii) excellent electronic conductivity to mini-
mize the ohmic loss. The most commonly used materials for VRFB
electrodes are carbon fiber-based materials (graphite felts, carbon
felts, and carbon papers) for their high electronic conductivity, high
hydraulic permeability, chemical and electrochemical inertness for
a wide variety of chemicals and a wide range of potentials [15e20].
However, issues associated with the use of these materials
including low specific surface area and poor electrochemical ac-
tivity limit the VRFB to be operated at a low current density
(~50 mA cm2) [21e23]. Extensive efforts have been devoted to
improving the surface catalytic activities towards the redox re-
actions. One strategy is to introduce functional groups onto the
carbon fiber surfaces to create abundant active sites and increasing
hydrophilicity. It was found that the oxygen functional groups
introduced by simple acid or thermal treatment can effectively
catalyze the vanadium redox reactions [24e27]. Additionally, metal
and metal oxide materials have been investigated as efficient cat-
alysts for VRFBs. However, many of them are sensitive to parasitic
reactions (hydrogen evolution) or are rare metals [10]. Recently,
researchers from Pacific Northwest National Laboratory (PNNL)
reported several types of catalysts of low cost and high catalytic
activity [21,22], including Bi metal, Nb2O5. VRFBs with these cata-
lysts deliver significantly improved rate capability and cyclability.
By incorporating Bi nanoparticles onto the solid surfaces of a
negative porous electrode, the VRFB can be operated at
160 mA cm2 with an energy efficiency of 79%.
Although some progress has been made in improving the sur-
face catalytic activity of carbon-fiber based electrodes, low specific
surface area is still a central issue for developing high-power VRFBs
and has yet to be fully-resolved due to its conflict with the transport
properties of the electrode [2]. In the conventional carbon fiber-
based electrodes, the pores are several tens of micrometers in
diameter and are typically formed by the voids between the fibers.
These micron-scale pores can construct efficient electrolyte trans-
port pathways, offering high hydraulic permeability and thus low
concentration loss and pump work. However, the specific surface
area is extremely low (0.1e3 m2 g1) due to the large pore sizes
[28]. The most straightforward strategy to increase the surface area
would be to use carbon fibers with smaller dimeters to form the
electrode for a reduction of pore sizes. Unfortunately, this method
will also induce a significant reduction in hydraulic permeability,
leading to increased pump work and concentration polarization [1].
Hence, to increase the specific surface area without sacrificing too
much permeability, the common strategy is to coat high surface
area materials (such as carbon blacks, carbon nanotubes and
graphenes) onto the carbon fiber surfaces [29e34]. Although this
approach increases the surface area of the electrode, it still suffers
from several issues. For instance, dip-coating is typically adopted to
coat carbon surfaces; the major disadvantage associated with this
method is the fact that attachment between the high-surface-area
materials and the carbon fiber surfaces relies on weak Van der
Waals forces. Flowing electrolyte can easily destroy or disrupt the
attachment, causing a severe problem in durability [35]. Several
groups have reported to synthesize carbon nanotubes (CNTs), car-
bon nanofibers (CNFs) or graphene directly on the carbon fiber
surfaces via chemical vapor deposition (CVD) processes, aiming to
connect the high surface area material with carbon fiber surfaces
via covalent bonds [35e38]. However, issues associated with the
CVD process including the high price of metal precursors, and
complex and tedious preparation hinder its mass production
significantly. Furthermore, the issue of hydraulic permeability
reduction and therefore large concentration loss still stands during
battery operation, as previously reported [30]. The ideal solution
would be to compose a low-cost porous electrode structure with
high surface area that does not sacrifice permeability.
The bi-dispersed porous structure is one of the common struc-
tures in porous media and is issued in the evaporators of heat pipes.
It is composed of clusters (at macro-level), which are agglomerated
by small particles (at micro-level) [39,40]. This unique structure
features higher permeability than the mono-dispersed porous
structure that is composed of macro-level clusters as well as higher
surface area due to the micro-level particles [40]. Inspired from the
concept of a bi-dispersed porous structure, we form a dual-scale
porous electrode (DPCE) that has a bimodal distribution of pore
sizes by selecting carbon papers (CPs) that have large primary pores
(~10 mm) as starting materials and employing KOH activation
method to etch the carbon fiber surfaces to form the desired small
secondary pores (~5 nm), as shown in Fig. 1. With this unique
porous structure, large primary pores serve as the macroscopic
pathways for electrolyte flow; small secondary pores that are well-
connected to primary pores provide ample active sites for elec-
trochemical reactions. The expectation is that the surface area is
dramatically increased without compromising on the permeability
because of presence of the secondary pores. Our results match this
expectation and we show that the specific surface area of the novel
electrode structure can reach as high as 42.7 m2 g1, which is one
order of magnitude higher than conventional carbon electrodes
(2.6 m2 g1). It is demonstrated that the VRFB with the present
electrodes can stably operate at 400 mA cm2 with an energy ef-
ficiency over 80%. To the best of our knowledge, it represents one of
the highest VRFB performances in the open literature. In addition,
the preparation method is both straightforward and cost-effective
making it particularly appropriate for mass production. This dual-
scale porous electrode represents a significant step toward the
advancement of VRFBs, and in principle, other RFBs as well.
2. Experimental
2.1. Electrode fabrication
Pristine CP (SGL 10 AA), provided by Union Chemical Industrial
Co., Ltd., was selected as the starting material. The pristine carbon
paper (CP-p) was first heat treated in a tube furnace at 500  C in air
for 5 h [15]. In order to create nanopores on the carbon fiber sur-
faces, the oxidized CP was thoroughly mixed with KOH slurries at
different carbon paper/KOH weight ratios of 1:0.5, 1:1 and 1:2. The
obtained mixture was then heat treated (heating ramp rate of
3  C min1) in a horizontal furnace under a nitrogen flow at 800  C
for 1.5 h to form the DPCE. The resulting DPCE was rinsed several
times with 6 M HCl to remove inorganic salts, and subsequently
 X.L. Zhou et al. / Journal of Power Sources 325 (2016) 329e336
Fig. 1. The schematic of the conventional carbon-fiber based electrode and the proposed dual-scale porous carbon electrode.
rinsed with distilled water until the establishment of a neutral pH.
Finally, the DPCE was dried in an oven at 90  C for 3 h.
2.2. Characterization
The material morphology was acquired by scanning electron
microscope (SEM, JEOL-6700F and JSM-6300) under an accelera-
tion voltage of 20 kV. Transmission electron microscopy (TEM)
images were obtained by operating a high-resolution JEOL 2010F
TEM system with a LaB6 lament at 200 kV. The samples were
dispersed in ethanol, sonicated and dripped onto the carbon-
coated Cu grids. Surface elemental composition was characterized
with X-ray photoelectron spectroscopy (XPS, Axis Ultra DLD, UK).
N2 adsorption/desorption measurement was conducted with a gas
analyzer (ASAP2420, Micromeritics) after degassing at 120  C for
3 h to investigate the pore structure of the materials. The Brunauer-
Emmett-Teller (BET) and Barrerr-Joyner-Halenda (BJH) method
were adopted to calculate the specific surface areas and aperture
distribution of electrodes.
2.3. Electrochemical measurements
Cyclic voltammetry tests were conducted using a typical three-
electrode cell. Carbon paper was used as the working electrode
with a geometric size of 0.1 cm2, and was connected to a platinum
wire with a reference electrode (Saturated calomel electrode), and
counter electrode (Pt mesh) in 0.2 M VOSO4 in 3 M H2SO4 solution
(Sigma-Aldrich, 98%) [15]. A single flow cell with an active electrode
area of 4 cm2 was assembled for charge/discharge tests. The in-
house designed zero-gap flow battery with a serpentine flow
field was used in this study. Two layers of carbon paper were used
with the compression ratio of 60% and Nafion 212 was adopted as
the membrane material. Electrolytes of 50 ml were fed into the
compartments using the acrylic flow channels and were circulated
to and from the reservoirs at 15 ml s1 using a 2-channel peristaltic
pump (WT-600-2J, Longerpump, China). Measurements were
conducted with 50 ml 1 M V (IV) þ 3 M H2SO4 solution as the
positive electrolyte and 50 ml 1 M V (III) þ 3 M H2SO4 solution as
the negative electrolyte. Charge-discharge and cycling tests were
331
conducted using an ArbinBT 2000 at a constant current density
ranging from 200 to 500 mA cm2.
3. Results and discussion
3.1. Electrode design, fabrication and characterization
As shown in Fig. 1, the basic idea is to form the DPCE which has
pores in two different scalesdmicron-scale primary pores and
nanometer-scale secondary pores. To compose the proposed
structure, we adopted the carbon paper as starting materials which
have primary pores (~10 mm) and use KOH to etch carbon fiber
surfaces to form the secondary pores (~5 nm). It should be
mentioned that the pristine carbon papers were thermally treated
in air before etching to introduce the oxygen functional groups to
increase the surface activity and hydrophilicity [26]. The mecha-
nism of the etching process, known as KOH activation, has been
documented previously [41]. It is suggested that the activation of
carbon with KOH proceeds as 6KOH þ C / 2K þ 3H2 þ 2K2CO3,
followed by the decomposition of K2CO3 and the reaction of CO2
with C. The surface morphology of CP-air and prepared DPCEs with
KOH/CP weight ratio of 1:0.5 (DPCE-0.5), 1:1 (DPCE-1) and 1:2
(DPCE-2) are depicted in Fig. 2. Fig. 2a showed that the carbon fiber
surfaces of CP-air have nearly no pores, which is consistent with the
results reported [18]. In contrast, all of the DPCE samples have
rough surfaces with uniform nano-scale pores generated by the
well-dispersed KOH activation agent (Fig. S1). In addition, with the
increase in the KOH/CP weight ratio, the nano-scale pores will be
enlarged due to the further reaction between KOH and C.
To investigate the surface structure of the carbon fibers, TEM
images were taken. Fig. 3 revealed a relatively sharp contrast at the
edge of each carbon fiber and the depths of the created nano-scale
pores are around 20 nm, indicating that the carbon fiber surface
was successfully etched during activation and did not significantly
change the carbon fiber structure. Since the depth of the nano-scale
pores is only 20 nm, the reactant ions can easily diffuse from the
bulk electrolytes into the pores for the electrochemical reactions
and the product ions can diffuse back to the bulk electrolytes after
the reactions, as shown in Fig. 1.
332 X.L. Zhou et al. / Journal of Power Sources 325 (2016) 329e336
Fig. 2. The scanning electron microscopy images of carbon fiber surfaces of CP-air (a), DPCE-0.5 (b), DPCE-1 (c) and DPCE-2 (d).
Fig. 3. The transmission electron microscopy image of carbon fiber of DPCE-1.
To test and verify our assumption that the specific surface area
can be increased by this dual-scale porous structure, the N2
adsorption/desorption measurements were conducted. Fig. 4
showed the N2-absorption and pore-width distribution of pristine
CP, air-treated CP and DPCEs. Significantly, the DPCEs have one
order of magnitude higher specific surface area than the CP-p
(2.6 m2 g1). The specific surface area of DPCE-0.5, DPCE-1 and
DPCE-2 is 62.3 m2 g1, 42.7 m2 g1 and 26.9 m2 g1. The specific
surface area decrease with the KOH/CP weight ratio due to the
nano-scale pores were enlarged by the further reaction between
KOH and C, which is consistent with the SEM images. More
importantly, as shown in Fig. 4b, pore sizes of the created pores in
DPCEs usually range from 5 to 12 nm, which are beneficial for the
electrochemical reactions due to the reason that pores with pore
size of around 5 nm can enable fast diffusion of active species [42].
As previously reported in Ref. [42], the diffusivity of redox
species in pores with diameter of 5 nm is 100 times higher than that
in pores with diameter of 2 nm. If we assume that pores that have
diameters larger than 5 nm can provide the effective surface area
for the redox reactions, the effective surface areas of DPCE-0.5,
DPCE-1, DPCE-2, CP-a, CP-p should be 12.80 m2 g1, 14.52 m2 g1,
15.32 m2 g1, 6.21 m2 g1 and 1.04 m2 g1, respectively.
We further used XPS to characterize the surface properties of
the CP-air and DPCEs, as shown in Fig. 5. The XPS results showed
that the O/C ratio of CP decreased after the KOH activation, due to
the fact that KOH can remove oxygen functional groups at high
temperatures, as expected. In addition, the percentage of different
oxygen containing functional groups is also altered. It is apparent
that the air treated CP has a much higher number of CeOH groups
while post KOH treatment increased C]O group content, since
CeOH groups can be partially converted to C]O groups during the
activation process, as summarized in Table 1.
3.2. Electrochemical performance
The electrochemical activities of CP-air and DPCEs were inves-
tigated in a typical three-electrode system. As depicted in Fig. 6, the
peak currents of each redox reaction are mainly governed by the
diffusion of the vanadium ions to the electrode surface [43] and
thus no obvious difference was found between the different elec-
trodes, indicating that the effect of surface area on the electro-
chemical behavior cannot be well-reflected by the peak currents.
Hence, we use the potential separation for the reduction and
oxidation peaks to characterize the surface activity here. The CV
curve of the CP-air in V(IV) electrolyte showed relatively large
separation for the reduction and oxidation peaks for the V(II)/V(III)
and V(IV)/V(V) redox reactions, as shown in Fig. 6a. In contrast, the
 X.L. Zhou et al. / Journal of Power Sources 325 (2016) 329e336 333

Fig. 4. The nitrogen sorption isotherm plot (a) and the corresponding pore size distribution plot (b) of the CP-p, CP-air and DPCEs.

Fig. 5. O1s XPS spectra of CP-air (a), DPCE-0.5 (b), DPCE-1 (c) and DPCE-2 (d). The dark cyan line, blue line and orange line represent the fitted peaks of HeOeH, CeO and C]O. (For
interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.)

Table 1 To further investigate the electrochemical performance of the

Atomic fractions of C, O of CP-air, DPCE-0.5, DPCE-1 and DPCE-2. prepared electrodes, we conducted a symmetrical half-cell flow
Components CP-air DPCE-0.5 DPCE-1 DPCE-2 battery test to test the positive and negative sides of a VRFB sepa-
rately [43]. Fig. 6b and c compare the polarization curves of CP-air
O 1s (%) 6.54 4.18 3.06 2.15
C¼O (%) 1.21 1.78 1.27 0.96 and DPCEs in the negative symmetric cell (0.5 M V(II)/0.5 M V(III))
CeOH (%) 3.94 1.29 1.13 0.61 and positive symmetric cell (0.5 M V(IV)/0.5 M V(V)). It is shown
C 1s (%) 93.46 94.79 95.82 96.88 that all the DPCE samples exhibit lower overpotential than the air-
treated CP. With an increase in the KOH/C weight ratio, the per-
formance of DPCEs in the negative symmetric cell increases initially
DPCE-0.5 had much faster kinetics than the CP-air, as evidenced by and then decreases. It can be explained that the effective surface
a smaller voltage separation, which can be explained by the cata- area increases with the weight ratio but the number of functional
lytic effect of C]O functional groups, which is consistent with [33]. groups decrease and thus the surface electrochemical activity de-
The C]O functional groups may increase the density of states and creases. DPCE-1 and DPCE-2 have much larger effective surface
cause the carbon to behave more like a metal, facilitating the areas than that of DPCE-0.5. For the performance of DPCEs in the
adsorption of the positive charged ions [33,44]. In addition, the positive symmetric cell, the performance of DPCEs increases with
electrochemical activity of DPCE decreased with the increase in the increased amount of KOH loadings, which is a different trend
KOH/CP weight ratio due to fewer C]O functional groups, as with the situation in the negative symmetric cell. While the func-
expected. tional groups have a large influence on the electrochemical activity
334 X.L. Zhou et al. / Journal of Power Sources 325 (2016) 329e336

Fig. 6. a) CV in a scan rate of 10 mV s1 for CP-air, DPCE-0.5, DPCE-1 and DPCE-2 in 0.2 M V(V) þ 3 M H2SO4 solution; potentiostatic measurements of air-treated CP DPCE-0.5, DPCE-
1 and DPCE-2 with the cell active area of 4 cm2 in the negative (b) and positive symmetrical cells (c).

toward the V(IV)/V(V) reactions under the low vanadium concen-
tration, as shown in Fig. 6, it has been shown that the kinetics of
V(IV)/V(V) reaction has relatively low dependence on carbon sur-
face for high vanadium concentration solutions [43]. Hence, in the
practical case with high vanadium concentration, the influence of
carbon surface on the kinetics of V(IV)/V(V) reaction is quite limited
and the effective surface area becomes the dominant factor. Hence,
with the KOH/C ratio increase, the effective surface area increases
and thus the kinetics of V(IV)/V(V) reaction increases.
3.3. VRFB charge-discharge and cycling performance
Fig. 7a shows the charge-discharge curves of the CP-air and
DPCE samples between 0.8 and 1.65 V at a current rate of

Fig. 7. (a) Charge-discharge curves of VRFBs with CP-air, DPCE-0.5, DPCE-1 and DPCE-2 at the current density of 200 mA cm2; (b) charge-discharge curves of VRFBs with DPCE-1 at
the current densities of 200e500 mA cm2; (c) the energy efficiency and columbic efficiency of VRFBs with different electrodes at the current densities of 200e500 mA cm2; (d)
the discharge capacity of VRFBs with different electrodes at the current densities of 200e500 mA cm2; (e) the energy efficiency and columbic efficiency of VRFBs with DPCE-1
during 120 cycles; (f) the discharge capacity of VRFBs with DPCE-1 during 120 cycles.
 X.L. Zhou et al. / Journal of Power Sources 325 (2016) 329e336
200 mA cm2. The CP-air in this work can deliver an energy effi-
ciency of 73% at the current density of 200 mA cm2, which is
consistent with the value reported by other groups [27]. As
compared to the CP-air, all the DPCE samples showed remarkably
decreased overpotential in both charge and discharge processes.
The DPCE-1 exhibited the best performance among the sample
prepared, primary because of the trade-off between the effective
surface area and the surface properties, which is consistent with
the symmetrical battery test. It should be mentioned that the
pristine CP shows even poorer performance than that of the CP-air,
as shown in Fig. S2. Fig. 7b shows the rate capability of the VRFBs
with DPCE-1, showing that the battery can operate at ultra-high
current densities (400 mA cm2 or 500 mA cm2) with relative
low overpotential. Fig. 7c and d summarize the coulombic effi-
ciency, voltage efficiency, energy efficiency and discharge capacity
of VRFBs with different electrodes at current densities ranging from
200 mA cm2 to 500 mA cm2. It can be clearly seen that VRFBs
with DPCE-1 can deliver an energy efficiency ranging from 82% to
88% at current densities of 200e400 mA cm2, which is by far the
highest efficiency ever reported in the open literature [45e47],
confirming the efficiency of the porous structure of the designed
DPCEs, as shown in Fig. 8. Even at the current density of
500 mA cm2, the battery’s efficiency reaches a relatively high
energy efficiency of 76%. In addition, Fig. 7e and f demonstrate the
performance of VRFBs with DOCE-1 at the current density of
400 mA cm2, showing no obvious degradation during the 120
cycles.
4. Conclusion
In summary, we present a simple and cost-effective method to
form a dual-scale porous electrode by KOH activation of the fibers
of carbon papers. The large pores (~10 mm) formed between carbon
fibers serve as the macroscopic pathways for high electrolyte flow
rates while the small pores (~5 nm) formed in carbon fibers provide
active sites for fast electrochemical reactions. It is shown that the
Brunauer- Emmett-Teller specific surface area of the carbon paper
is increased by a factor of 16 while maintaining the same hydraulic
permeability as that of the original carbon paper electrode. We then
apply the dual-scale electrode to a vanadium redox flow battery
(VRFB) and demonstrate an energy efficiency ranging from 82% to
88% at current densities of 200e400 mA cm2. To the best of our
Fig. 8. The comparison of the performance of VRFBs with DPCE-0.5/1/2 and the VRFB
performance in the open literature.
335
knowledge, it represents one of the highest VRFB performances in
the open literature. This dual-scale porous electrode represents a
significant step toward the advancement of VRFBs, and in principle
other flow batteries as well. Further optimization of pore size and
pore shape of the dual scale porous electrode will help to further
improve the battery performance in the future.
Acknowledgements
The work described in this paper was fully supported by a grant
from the Research Grants Council of the Hong Kong Special
Administrative Region, China (Project No. 623313).
Appendix A. Supplementary data
Supplementary data related to this article can be found at http://
dx.doi.org/10.1016/j.jpowsour.2016.06.048.
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