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abstract
Article history:
brane (PEM) electrolyte are promising in the field of energy storage. Their performance was
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
electrode assembly (MEA) is with 0.20 mg cm2 Pt (in 50% Pt/C catalyst) for the hydrogen
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-
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
in WE mode, is proven to have relations with current density and carbon paper hydro-
Catalyst loading
Copyright 2013, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights
Hydrophobicity
1.
Introduction
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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.
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2.2.
SEM characterizations
2.3.
3.
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.
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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.
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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
3.3.
0.4
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
1.6
Voltage (V)
3.4.
1.4
0.8
0.6
0.4
0.0
0.5
1.0
1.5
2.0
2.5
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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
3.5.
4.
Conclusion
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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
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