Anda di halaman 1dari 6

i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 8 ( 2 0 1 3 ) 4 7 9 2 e4 7 9 7

Available online at www.sciencedirect.com

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

Electrode structure optimization combined with water feeding


modes for Bi-Functional Unitized Regenerative Fuel Cells
Xiaolong Zhuo, Sheng Sui*, Junliang Zhang
Institute of Fuel Cell, Shanghai Jiao Tong University, 800# Dongchuan Rd., Shanghai 200240, China

article info

abstract

Article history:

Bi-functional Unitized Regenerative Fuel Cells (URFCs) based on proton-exchange mem-

Received 7 October 2012

brane (PEM) electrolyte are promising in the field of energy storage. Their performance was

Received in revised form

investigated with catalyst loadings, carbon paper hydrophobicity and water feeding modes

20 December 2012

in both fuel cell (FC) and water electrolysis (WE) operations. The optimum membrane

Accepted 19 January 2013

electrode assembly (MEA) is with 0.20 mg cm2 Pt (in 50% Pt/C catalyst) for the hydrogen

Available online 21 February 2013

electrode (HE), and a total catalyst loading of 0.80 mg cm2 for the oxygen electrode (OE).
And its performance can reach 2.18 A cm2 at 1.80 V in WE test and 0.64 A cm2 at 0.60 V in

Keywords:

FC test with air oxidant. Comparison of different carbon papers reveals that suitable hy-

Electrode structure optimization

drophobicity of OE carbon papers is obtained when the PTFE content accounts for

Unitized Regenerative

26.95 wt.%. Choice of water feeding modes, which has an influence on URFC performance

Fuel Cells (URFCs)

in WE mode, is proven to have relations with current density and carbon paper hydro-

Water feeding mode

phobicity in a sophisticated way.

Catalyst loading

Copyright 2013, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights

Hydrophobicity

1.

Introduction

As one of the most promising energy generation systems, fuel


cells, especially PEMFCs (proton-exchange membrane fuel
cells) have attracted worldwide attention because of their high
efficiency and zero emission. Based on proton-exchange
membrane (PEM) electrolyte, unitized regenerative fuel cells
(URFCs) can produce H2 and O2 in water electrolysis (WE)
operation for energy storage, or generate electrical power in
H2/Air (O2) fuel cell (FC) operation [1]. It has advantages like
higher energy density and capability of long-term energy
storage without self-discharge [2,3], over secondary batteries.
Combined with solar cells or wind power systems, URFCs are
potentially interesting in the application of renewable energy.
First attempts to build URFCs using PEM technology were
made early in the 1960s [4]. At that time, systems were of low
efficiency with high metal loading. As the polarization of the

reserved.

URFCs is mainly caused by redox reaction of oxygen, the key


task for URFC researches is the fabrication of membrane
electrode assemblies (MEAs) with high efficiency in oxygen
reduction reaction (ORR) and oxygen evolution reaction (OER).
In developing novel MEAs, some researchers mainly
focused on catalyst composition [5,6]. Until now, no single
element is found to be electrochemical active for both ORR
and OER. Usually in bi-functional PtIr catalyst of OEs, Pt
mainly contributes to ORR in FC mode while Ir promotes OER
in WE mode. Yim [2,7] studied the performance and energy
conversion efficiency of different combinations of Pt, Ru and
IrOx catalysts and pointed out that PtIr catalyst exhibited high
round-trip efficiency and stability during cycling tests. In
detail, Jung [8] gave a comprehensive evaluation of the unsupported PtIr electrocatalyst and further concluded that
Pt85Ir15 catalyst showed the highest round-trip efficiency
when estimated at different current densities.

* Corresponding author. Tel./fax: 86 21 34206249.


E-mail address: ssui@sjtu.edu.cn (S. Sui).
0360-3199/$ e see front matter Copyright 2013, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.ijhydene.2013.01.137

i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 8 ( 2 0 1 3 ) 4 7 9 2 e4 7 9 7

Others focused on preparing methods of the electrocatalyst [9,10]. Zhang [11] in DICP employed chemical reduction of H2PtCl6 on the surface of IrO2 to obtain IrO2-supported
Pt catalyst, which had a better use of space occupied by IrO2
and thus a lower loading was obtained. Zhang [12] in Tsinghua
University synthesized a bifunctional RuO2eIrO2/Pt electrocatalyst through colloid deposition. The URFCs with the above
supported catalyst produced higher performance than that
with mechanically mixed Pt/IrO2 catalyst. As for catalyst layer
structure, Altmann [13] studied the bifunctional electrodes
with various multilayer arrangements and different segmented configurations with single catalyst (Pt or IrO2) areas.
And he came to the conclusion that the mixture of Pt and IrO2
performed the best on the present stage of electrode development, reaching 0.60 A cm2 at 0.60 V (FC) and 1.30 A cm2 at
1.65 V (WE). Chen [14] reported studies on eight structures of
catalyst layer with various ink deposition combinations on
membranes and GDLs. The cell potentials of the URFCs with Pt
layers sprayed directly onto GDLs are about 0.10 V higher than
those with Pt layers sprayed onto membranes at 0.80 A cm2
in FC operation. Unsupported Pt and Ir are often adopted in
URFCs as it is difficult to find a suitable carrier which is stable
in high potential in WE test. In our previous works, supported
Ir/TiC and PteIr/TiC catalysts were synthesized for URFCs
[15e17]. The effect of anode catalyst loading, Nafion content,
thickness of carbon papers on high performance PEMWEs was
also investigated [18].
Some researchers also concerned hydrophobicity and other
properties of diffusion layer materials [19]. Ioroi [20] prepared
gas diffusion backings (GDBs) with PTFE loading from 0 to
594 mg cm3 on both electrodes and examined the relation
between PTFE loading and cell performance. The results
showed that the appropriate loading on GDBs is 16 mg cm3.
Chen [21] developed a new electrode with pyrolyzed Nafion to
improve water management and minimize mass transport
limitations. By using novel MEAs, the cell performance and
round-trip efficiency at 0.70 A cm2 was enhanced 13.5% and
10.8%, respectively. Hwang [22] studied on the relation among
porosity, fiber diameter of Ti-felt GDLs and cell performance.
And he reported that cell performance was not noticeably
affected by a change in PTFE content or porosity when fiber
diameter on OE side was as small as 20 mm. Moreover, the cell
performance with diameter of 20 mm was better than those of
40e80 mm at a high current density.
The objective of this work is to study effects of MEA preparation, hydrophobicity of GDLs, and different water feeding
modes. Based on the sophisticated water transport phenomenon in FC and WE modes, the optimum strategy of preparing
and operating URFCs is suggested with considering the relation between electrode structure and manner of test
operation.

2.

Experimental

2.1.

Cell components and configurations

The mixture of nanoscale Ir black and Pt black (Johnson &


Matthey) were chosen as OE catalysts. On HEs, 60 wt.% Pt/C
(9100 HiSPEC, Johnson & Matthey) or Pt black were used.

4793

The home-made MEAs were prepared by catalyst coating


on membrane (CCM) method and then hot-pressured with
two pieces of hydrophobic carbon paper. Firstly, a mixture of
5 wt.% Nafion solution (Dupont), metallic catalyst and isopropanol (Nafion: catalyst 1:6) was dispersed to form a slurry
in ultrasound agitator for 10 min and then the slurry was
sprayed over a Nafion membrane (NR212, Dupont) in temperature range from 35  C to 40  C under infrared lamp. Secondly, two pieces of carbon paper (TGP-H-060, Toray) were
treated with 10e20% PTFE solution (TF-5203Z, 3M) and then
baked out in an oven at the temperature of 380  C for 2 h.
Thirdly, after 30 mins drying, the Nafion membrane with one
catalyst layer on each side was hot-pressed together with the
above two pieces of carbon-coated (XC-72R, Cabot) carbon
papers. About 40% of the weighted catalysts were deposited
on the membrane.
The URFC set consists of an MEA, two high density graphite
plates with serpentine flow-channels (1 mm in width and
1 mm in height), two gold-plated copper plates and two titanium end plates.

2.2.

SEM characterizations

The cross-section images of MEAs were characterized by SEM


(Sirion 200, FEI). And the elementary analysis of the two sites
on fiber surface of hydrophobic carbon papers was determined by EDX (Oxford INCA X-Act).

2.3.

Performance evaluation of FC and WE operations

Performance evaluation was carried out in a single cell with


an active area of 3.3*3.3 cm2. In FC test, the cell was operated at
65  C with H2/Air feedings at atmospheric pressure. And the
utilization ratio of H2 is 60% while that of air is 30%. The humidification temperature of H2 and air was 60  C, 5  C lower
than that of the cell. A Multi-range Fuel Cell Test System (850e,
Scribner) was used. In short-time WE test, cell temperature
was 65  C and the voltage applied by a regulated DC power
supply (PWR400L, Kikusui) ranged from 1.40 to 1.80 V. The
data used in the graph was obtained from the last second of
every different voltage. On average, every cell was tested in FC
and WE modes for about 20 h including activation process.

3.

Results and discussion

3.1.
MEA micro structures and carbon paper
hydrophobicity
Fig. 1 shows the cross-section SEM image of the MEA after
about 20 hs test in both FC and WE modes. It can be seen that
there are close contact among Nafion membrane, catalyst
layers and GDLs (carbon papers). Therefore much less resistance can be expected in proton and electron transfer. The
carbon papers used in the MEAs are 190 mm thick with the
density of 0.44 g cm3. The HE catalyst (Pt/C) layer in Fig. 2a is
about 7e8 mm thick. The OE catalyst (PtIr) layer is thinner as
about 3e4 mm thick and its denser than the HE catalyst.
Fig. 2b, which is magnified from Fig. 1, is an SEM image of HE
catalyst. It shows that catalyst particles are in a fluffy way.

4794

i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 8 ( 2 0 1 3 ) 4 7 9 2 e4 7 9 7

carbon papers are detected as shown in Fig. 3 and their element compositions are listed in Table 1. A thin film, which
may be some adhesive between fibers, coated on fiber surface
at the site of spectrum 2. After hydrophobic treatment, as
shown at the site of spectrum 1, PTFE partially coat the surface
of fibers and form a transparent film, in which fluorine content is higher than that of spectrum 2. In the treated carbon
papers, the hydrophobic part which is covered by PTFE is for
gases to go through, and the rest hydrophilic part for water
transport.

3.2.

Fig. 1 e SEM image of cross-section of MEA with HE on the


upper side.

Moreover, in the HE catalyst layer, pore size is about 0.2 mm


generally.
To describe hydrophobicity, two sites (named spectrum 1
and spectrum 2) of elementary analysis on the fiber surface of

Fig. 2 e SEM images of Pt/C catalyst on HE side.

The effect of HE catalyst loading

Generally due to fast rate of hydrogen oxidization reaction


(HOR), the catalyst loading on HEs in PEMFCs is 0.05 mg cm2
or less [23]. In URFCs, bifunctional HEs contribute to hydrogen
redox and their catalyst loading is in the range of
0.40e1.0 mg cm2 [4,12,13]. In the present work, compared
with 0.40 mg cm2 Pt black, Pt loading (in Pt/C) on HEs was
investigated from 0.08 mg cm2 to 0.20 mg cm2 while at OEs
the catalyst remained as 0.80 mg cm2 (0.60 mg cm2 Pt
black 0.20 mg cm2 Ir black).
The loading effect of Pt in FC and WE tests is shown in
Fig. 4. It can be observed that an MEA with 0.20 mg cm2 Pt
loading (in Pt/C) on HE side performs the best, reaching
2.18 A cm2 at 1.80 V (WE) and 0.90 A cm2 at 0.48 V (FC). Even
the MEA with Pt (in Pt/C) loading of 0.12 mg cm2 performs
slightly better than the one with 0.40 mg cm2 of Pt black, as
shown in the enlarged view in Fig. 4. Thus for both FC and WE
reactions, Pt loading on HE side can be reduced to 0.2 or even
0.12 mg cm2. The above work shows when supported catalyst
is used at HEs, the metal loading can be reduced by at least
50%. Compared with Pt black, carbon-based Pt has a much
higher surface area and therefore provides more active sites.
Moreover, water electrolysis and fuel cell reactions have
different polarization characteristics and reaction properties,
for example different catalysis and mass transfer mechanisms. In Fig. 4, the difference in FC test is not as big as that in
WE test. This is because anode catalyst loading is not a main
influencing factor for FC operation.

Fig. 3 e Sample sites of EDX spectrums on the fiber.

4795

i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 8 ( 2 0 1 3 ) 4 7 9 2 e4 7 9 7

Table 1 e EDX statistics of the two spectrums of Fig. 4.

Spectrum 1

Spectrum 2

Element

Weight%

Atomic%

CK
OK
FK
CK
OK
FK

91.71
1.38
6.91
95.87
1.18
2.95

94.44
1.07
4.50
97.21
0.90
1.89

Pt&Ir 0.96mg/cm2
Pt&Ir 0.8mg/cm2
Pt&Ir 0.48mg/cm2
Pt&Ir 0.32mg/cm2

1.6

Voltage (V)

Samples

1.8

1.4

0.8

Standard: C(CaCO3); O(SiO2); F(MgF2) 1-Jun-1999 12:00 AM.


0.6

3.3.

The effect of OE catalyst loading

0.4

The OE catalyst contributes the main part of over-potential in


URFCs. In this experiment, the mass ratio of Pt and Ir at OEs was
fixed at 3:1 and total metal loading was changed from 0.32 to
0.96 mg cm2, while at HEs remained 0.32 mg cm2 Pt (in Pt/C).
The effect of OE catalyst loading in FC and WE tests is
shown in Fig. 5. The MEA with metal loading of 0.96 mg cm2
performs better than that of 0.80 mg cm2 in lower current
densities under 0.50 A cm2 in FC operation. On the other
hand in WE mode, the polarization curves of MEAs with total
loading of 0.80, 0.64 and 0.48 mg cm2 partially overlap with
each other, reaching current density of 1.90 A cm2 at 1.80 V,
as shown in the enlarged view. But when total loading is
0.32 mg cm2, the current density drops 1.20 A cm2 at 1.80 V,
meaning that OER rate is hindered by insufficient catalysts.
Compared to Fig. 4 in FC mode, the difference in FC mode in
Fig. 5 is larger. This is because the reaction rate at HEs is quite
fast and ORR is the determining step in whole process, OE
catalyst has much more influences on FC performance than
HE catalyst.
Accordingly, it can be concluded that the loading of
0.20 mg cm2 Ir and 0.60 mg cm2 Pt is able to exhibit the
comparatively optimum performance in both modes. While

1.8

pure Pt 0.4mg/cm2
Pt/C 0.2mg/cm2
Pt/C 0.12mg/cm2
Pt/C 0.08mg/cm2

0.0

0.5

1.0

1.5

2.0

Current Density (A/cm2)

Fig. 5 e Polarization curves of the URFC in FC and WE


operations using different OE catalysts: a) 0.96 mg cmL2
Pt&Ir. b) 0.80 mg cmL2 Pt&Ir. c) 0.64 mg cmL2 Pt&Ir. d)
0.48 mg cmL2 Pt&Ir. e) 0.32 mg cmL2 Pt&Ir. HE catalyst:
0.32 mg cmL2 Ptin Pt/C. PTFE contents of carbon paper: 15%
(HE)/20% (OE). Cell temperature: 65  C.
other researchers usually employed higher catalyst loading as
1e4 mg cm2 [2,8,12]. This is because in manufacturing MEAs,
different researchers adopt different materials which may
have great effect on cell performance. And more importantly,
these two different modes are somehow contradictory and
they have different influencing factors. When one intends to
achieve higher performance in WE mode through adjusting
the catalyst properties or the carbon paper hydrophobicity, it
may inevitably have some influences on FC performance. J.C.
Cruz et al. [24] adopted ATO as a support for OE catalyst. In
their FC and WE tests, the performance can reach
1.118 A mg1 at 1.8 V in WE mode and 0.565 A mg1 at 0.3 V in
FC mode. Although the supported OE catalyst performed
poorer than those reported in the present paper, its noble
metal loading was reduced. Through improving the active
surface area of catalyst and electrical conductivity, better
performance can be obtained.

1.6

Voltage (V)

3.4.

The effect of hydrophobicity of OE carbon papers

1.4

0.8

0.6

0.4
0.0

0.5

1.0

1.5

2.0

2.5

Current Density (A/cm2)

Fig. 4 e Polarization curves of the URFC in FC and WE


operations using different HE catalysts: a) 0.40 mg cmL2 Pt;
b) 0.20 mg cmL2 Pt in Pt/C; c) 0.12 mg cmL2 Pt in Pt/C;
d) 0.08 mg cmL2 Pt in Pt/C. OE catalyst: 0.60 mg cmL2
Pt D 0.20 mg cmL2 Ir. PTFE contents of carbon paper: 15%
(HE)/20% (OE). Cell temperature 65  C.

Water condition is a key factor in URFC systems. Especially at


OEs, there are reverse water transport processes (draining or
water supplying), i.e. water in WE operation is consumed
while in FC operation produced. For the ORR in FC operation,
water is produced by oxygen reacting with proton coming
through the electrolyte membrane. Carbon papers as diffusion
layers are treated to form micro hydrophobic pores and
channels. Generally treated carbon papers with 10e30% content of PTFE are preferred. Otherwise, flooding phenomenon
will occur. While in WE operation, sufficient water needs to be
supplied through GDLs and reach three-phase boundaries
near catalyst particles. Excess PTFE content in carbon papers
may block water access. Therefore the balance of hydrophobicity and hydrophilicity in diffusion layer is considered.
The effects of OE carbon papers with different hydrophobicities were compared in Fig. 6. The treated carbon papers

4796

1.8

i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 8 ( 2 0 1 3 ) 4 7 9 2 e4 7 9 7

1.80

PTFE20.68%
PTFE26.95%
PTFE29.97%

1.75

1.6

Voltage (V)

Voltage (V)

1.70

1.4
0.8

1.65

1.60

0.6

1.55

0.4

1.50

0.0

0.5

1.0

1.5

20.68% (HE-feed)
26.95% (HE-feed)
29.97% (HE-feed)
20.68% (dual-feed)
26.95% (dual-feed)
29.97% (dual-feed)
20.68% (OE-feed)
26.95% (OE-feed)
29.97% (OE-feed)

0.0

2.0

0.5

1.0

1.5

2.0

Current Density (A/cm2)

Current Density (A/cm2)

Fig. 6 e Polarization curves of the URFC in FC and WE


operations using different OE carbon papers in which PTFE
contents: a) 20.68%; b) 26.95%; c) 29.97%. HE catalyst:
0.32 mg cmL2 Pt (in Pt/C). OE catalyst: 0.60 mg cmL2
Pt D 0.20 mg cmL2 Ir. 15% PTFE contents of carbon paper
(HE). Cell temperature 65  C.

Fig. 7 e Polarization curves of the URFC in WE operations


using different water-feed modes with different PTFE
contents of OE carbon paper. HE catalyst: 0.32 mg cmL2 Pt
(in Pt/C). OE catalyst: 0.60 mg cmL2 Pt D 0.20 mg cmL2 Ir.
15% PTFE contents of carbon paper (HE). Cell temperature
65  C.

contained 20.68%, 26.95% and 29.97% PTFE respectively. In WE


tests, cell performance with the former two is almost at the
same level, reaching 1.8 A cm2 at 1.80 V, better than that of
the one with 29.97% PTFE. More PTFE content in carbon papers
will block water/gas channels and therefore cause much
resistance in water transfer. It leads to dry environment
around three-phase boundaries when large amount of water
is consumed. The 26.95% PTFE sample shows the best performance in FC operation which reaches 0.8 A cm2 at 0.53 V.
It is consistent with general understanding that more PTFE
content is preferred if it doesnt affect water supply in WE
operation.

starvation may occur at the anode in WE mode. For example,


the high hydrophobicity sample like the 29.97% one, when
loading voltage is about 1.75 V, OE feeding sample is not as
good as others. On the contrary, the HE feeding and dual
feeding MEAs perform well as water is mainly consumed on
OE side. In higher current density conditions, large amounts of
water is needed at the electrode. Driven by concentration
gradient, water can go through membrane from HE to OE side
to keep MEAs functioning well as too much PTFE may hinder
water supply in OE GDLs. By adopting HE feeding in WE mode,
high hydrophobicity of OE carbon papers can be maintained
for better FC performance.
Moreover, in different feeding modes (HE feeding, OE
feeding or Dual feeding), the performance order of hydrophobicity samples is the same as 20.68% > 26.95% > 29.97%
(PTFE content).

3.5.

Water feeding modes in WE operation

Water feeding from hydrogen, oxygen and both electrodes


was investigated in WE operation. The WE performance with
different water feeding modes is shown in Fig. 7.
In comparatively low hydrophobicity level, for example the
20.68% and 26.95% PTFE samples, cells in OE and dual feeding
modes perform better than the one in HE feeding mode. Due to
water is largely needed in proton transfer from OE to HE side
and around the three-phase boundaries, itll be just proper if
water is directly fed to where it is consumed, i.e. the OE catalyst layer. While in HE feeding mode, there isnt enough
water provided to OEs. This is because water flow direction in
HE feeding mode is opposite to that of proton transfer,
resulting in insufficient water supply. For the 20.68% PTFE
sample, the performance of OE feeding mode is slightly better
than that of dual feeding mode. This may due to exceed
amounts of water in GDLs sends up gas pressure, therefore
hinders further generation of gases.
OE works in both FC and WE modes, so it is with hydrophobicity and hydrophilicity. At high current densities, water

4.

Conclusion

Optimum home-made bi-functional MEA was with Pt (in Pt/C)


loading of 0.20 mg cm2 for HEs and a mixture catalyst loading
of 0.8 mg cm2 (0.6 mg cm2 Pt black 0.20 mg cm2 Ir black)
for OEs. Its performance can reach to 2.18 A cm2 at 1.80 V
(WE) and 0.64 A cm2 at 0.60 V (FC) in short time tests. Different water feeding modes have a great effect on WE operation. And the effect changes with different PTFE content of
carbon papers: in the orders of OE feeding Dual feeding > HE
feeding with 20.68% PTFE, and Dual feeding > HE feeding > OE
feeding with 29.97% PTFE. It is also found that in different
feeding modes, PTFE content shows the same effect order (in
performance) as 20.68% > 26.95% > 29.97%. Therefore, a high
performance of bi-functional URFCs is achieved by optimized
combination of MEAs, GDLs and water feeding modes.

i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 8 ( 2 0 1 3 ) 4 7 9 2 e4 7 9 7

Acknowledgments
This work was financially supported by the National High
Technology Research and Development Program (863 Program) of China (Grant No. 2009AA05Z116) and Science and
Technology Committee of Shanghai Municipality (Grant No.
09510701400). SEM characterization was completed at the
Instrumental Analysis Center of Shanghai Jiao Tong University (IAC-SJTU).

references

[1] Dihrab Salwan S, Sopian K, Alghoul MA, Sulaiman MY.


Review of the membrane and bipolar plates materials for
conventional and unitized regenerative fuel cells. Renewable
and Sustainable Energy Reviews 2009;13(6e7):1663e8.
[2] Yim Sung-Dae, Park Gu-Gon, Sohn Young-Jun, Lee WonYong, Yoon Young-Gi, Yang Tae-Hyun, et al. Optimization of
PtIr electrocatalyst for PEM URFC. International Journal of
Hydrogen Energy 2005;30(12):1345e50.
[3] Smith W. The role of fuel cells in energy storage. Journal of
Power Sources 2000;6(1e2):74e83.
[4] Grigoriev SA, Millet P, Porembsky VI, Fateev VN.
Development and preliminary testing of a unitized
regenerative fuel cell based on PEM technology. International
Journal of Hydrogen Energy 2011;36(6):4164e8.
[5] Pettersson J, Ramsey B, Harrison D. A review of the latest
developments in electrodes for unitised regenerative
polymer electrolyte fuel cells. Journal of Power Sources 2006;
157(1):28e34.
[6] Pi Yi-Hao, Tseng Chun-Wei. Preparation and
characterization of bifunctional graphitized carbonsupported Pt composite electrode for unitized regenerative
fuel cell. Journal of Power Sources 2012;202:28e34.
[7] Yim Sung-Dae, Lee Won-Yong, Yoon Young-Gi, Sohn YoungJun, Park Gu-Gon, Yang Tae-Hyun, et al. Optimization of
bifunctional electrocatalyst for PEM unitized regenerative
fuel cell. Electrochimica Acta 2004;50(2e3):713e8.
[8] Jung Ho-Young, Park Sehkyu, Popov Branko N.
Electrochemical studies of an unsupported PtIr
electrocatalyst as a bifunctional oxygen electrode in
a unitized regenerative fuel cell. Journal of Power Sources
2009;191(2):357e61.
[9] Cruz JC, Baglio V, Siracusano S, Ornelas R, Arriaga LG,
Antonucci V, et al. Nanosized Pt/IrO2 electrocatalyst
prepared by modified polyol method for application as dual
function oxygen electrode in unitized regenerative fuel cells.
International Journal of Hydrogen Energy 2012;37(7):5508e17.
[10] Lee Hankyu, Kim Jiyun, Park Jongho, Joe Yungil, Lee Taehee.
Performance of polypyrrole-impregnated composite
electrode for unitized regenerative fuel cell. Journal of Power
Sources 2004;131(1e2):188e93.

4797

[11] Zhang Yining, Zhang Huamin, Ma Yuanweis, Cheng Jinbin,


Zhong Hexiang, Song Shidong, et al. A novel bifunctional
electrocatalyst for unitized regenerative fuel cell. Journal of
Power Sources 2010;195(1):142e5.
[12] Zhang Yangjian, Wang Cheng, Wan Nianfang,
Mao Zongqiang. Deposited RuO2eIrO2/Pt electrocatalyst for
the regenerative fuel cell. International Journal of Hydrogen
Energy 2007;32(3):400e4.
[13] Altmanna Sebastian, Kazb Till, Friedrich Kaspar Andreas.
Bifunctional electrodes for unitised regenerative fuel cells.
Electrochimica Acta 2011;56(11):4287e93.
[14] Chen Guobao, Zhang Huamin, Ma Haipeng, Zhong Hexiang.
Effect of fabrication methods of bifunctional catalyst layers
on unitized regenerative fuel cell performance.
Electrochimica Acta 2009;54(23):5454e62.
[15] Sui Sheng, Ma Lirong, Zhai Yuchun. Investigation on the
proton exchange membrane water electrolyzer using
supported anode catalyst. Asia-Pacific Journal of Chemical
Engineering 2009;4(1):8e11.
[16] Ma Lirong, Sui Sheng, Zhai Yuchun. Preparation and
characterization of Ir/TiC catalyst for oxygen evolution.
Journal of Power Sources 2008;177(2):470e7.
[17] Sui Sheng, Ma Lirong, Zhai Yuchun. TiC supported PteIr
electrocatalyst prepared by a plasma process for the oxygen
electrode in unitized regenerative fuel cells. Journal of Power
Sources 2011;196(13):5416e22.
[18] Ma Lirong, Sui Sheng, Zhai Yuchun. Investigations on high
performance proton exchange membrane water
electrolyzer. International Journal of Hydrogen Energy 2009;
34(2):678e84.
[19] Hiramitsu Yusuke, Sato Hitoshi, Hori Michio. Prevention of
the water flooding by micronizing the pore structure of gas
diffusion layer for polymer electrolyte fuel cell. Journal of
Power Sources 2010;195(17):5543e9.
[20] Ioroi Tsutomu, Okub Takanori, Yasuda Kazuaki,
Kumagai Naokazu, Miyazaki Yoshinori. Influence of PTFE
coating on gas diffusion backing for unitized regenerative
polymer electrolyte fuel cells. Journal of Power Sources 2003;
124(2):385e9.
[21] Chen Guobao, Zhang Huamin, Cheng Jinbing,
Ma Yuanwei, Zhong Hexiang. A novel membrane
electrode assembly for improving the efficiency of the
unitized regenerative fuel cell. Electrochemistry
Communications 2008;10(9):1373e6.
[22] Hwang Chul Min, Ishida Masayoshi, Ito Hiroshi,
Maeda Tetsuhiko, Nakano Akihiro, Hasegawa Yasuo, et al.
Influence of properties of gas diffusion layers on the
performance of polymer electrolyte-based unitized
reversible fuel cells. International Journal of Hydrogen
Energy 2011;36(2):1740e53.
[23] Litster S, McLean G. PEM fuel cell electrodes. Journal of Power
Sources 2004;130(1e2):61e76.
[24] Cruz JC, Rivas S, Betran D, Meas Y, Ornelas R, Osorio-Monreal G,
et al. Synthesis and evaluation of ATO as a support for PteIrO2
in a unitized regenerative fuel cell. International Journal of
Hydrogen Energy 2012;37(18):13522e8.