Electrocatalytic performance of fuel cell reactions at low catalyst loading and high mass transport

被引:166
作者
Zalitis, Christopher M. [1 ]
Kramer, Denis [1 ]
Kucernak, Anthony R. [1 ]
机构
[1] Univ London Imperial Coll Sci Technol & Med, Dept Chem, London SW7 2AZ, England
基金
英国工程与自然科学研究理事会;
关键词
OXYGEN REDUCTION REACTION; GAS-DIFFUSION ELECTRODES; HYDROGEN OXIDATION; OXIDE COVERAGE; PLATINUM; CARBON; ELECTROCHEMISTRY; TEMPERATURE; OPERATION; SURFACES;
D O I
10.1039/c3cp44431g
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
An alternative approach to the rotating disk electrode (RDE) for characterising fuel cell electrocatalysts is presented. The approach combines high mass transport with a flat, uniform, and homogeneous catalyst deposition process, well suited for studying intrinsic catalyst properties at realistic operating conditions of a polymer electrolyte fuel cell (PEFC). Uniform catalyst layers were produced with loadings as low as 0.16 mu g(Pt) cm(-2) and thicknesses as low as 200 nm. Such ultra thin catalyst layers are considered advantageous to minimize internal resistances and mass transport limitations. Geometric current densities as high as 5.7 A cm(Geo)(-2) were experimentally achieved at a loading of 10.15 mu g(Pt) cm(-2) for the hydrogen oxidation reaction (HOR) at room temperature, which is three orders of magnitude higher than current densities achievable with the RDE. Modelling of the associated diffusion field suggests that such high performance is enabled by fast lateral diffusion within the electrode. The electrodes operate over a wide potential range with insignificant mass transport losses, allowing the study of the ORR at high overpotentials. Electrodes produced a specific current density of 31 +/- 9 mA cm(Spec)(-2) at a potential of 0.65 V vs. RHE for the oxygen reduction reaction (ORR) and 600 +/- 60 mA cm(Spec)(-2) for the peak potential of the HOR. The mass activity of a commercial 60 wt% Pt/C catalyst towards the ORR was found to exceed a range of literature PEFC mass activities across the entire potential range. The HOR also revealed fine structure in the limiting current range and an asymptotic current decay for potentials above 0.36 V. These characteristics are not visible with techniques limited by mass transport in aqueous media such as the RDE.
引用
收藏
页码:4329 / 4340
页数:12
相关论文
共 57 条
[1]  
[Anonymous], 2009, COMMUNICATION
[2]   Influence of Nafion loading in the catalyst layer of gas-diffusion electrodes for PEFC [J].
Antolini, E ;
Giorgi, L ;
Pozio, A ;
Passalacqua, E .
JOURNAL OF POWER SOURCES, 1999, 77 (02) :136-142
[3]   AN EXPERIMENTAL STUDY OF MODE OF OPERATION OF POROUS GAS-DIFFUSION ELECTRODES WITH HYDROGEN FUEL [J].
AUSTIN, LG ;
ALMAULA, S .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1967, 114 (09) :927-&
[4]   Cathode development for alkaline fuel cells based on a porous silver membrane [J].
Bidault, F. ;
Kucernak, A. .
JOURNAL OF POWER SOURCES, 2011, 196 (11) :4950-4956
[5]   MODELING OF A DOUBLE-LAYERED PTFE-BONDED OXYGEN-ELECTRODE [J].
BJORNBOM, P .
ELECTROCHIMICA ACTA, 1987, 32 (01) :115-119
[6]   A survey of platinum hydrous oxide electrochemistry at elevated temperature: Evidence for a new component in the beta-deposit [J].
Burke, LD ;
Morrissey, JA .
JOURNAL OF APPLIED ELECTROCHEMISTRY, 1996, 26 (06) :593-601
[7]   Electrocatalysis under conditions of high mass transport: Investigation of hydrogen oxidation on single submicron Pt particles supported on carbon [J].
Chen, SL ;
Kucernak, A .
JOURNAL OF PHYSICAL CHEMISTRY B, 2004, 108 (37) :13984-13994
[8]   A thermostatic cell with gas diffusion electrode for oxygen reduction reaction under fuel cell relevant conditions [J].
Chen, Yan-Xia ;
Li, Ming-Fang ;
Liao, Ling-Wen ;
Xu, Jie ;
Ye, Shen .
ELECTROCHEMISTRY COMMUNICATIONS, 2009, 11 (07) :1434-1436
[9]   ULTRAPURIFICATION OF WATER FOR ELECTROCHEMICAL AND SURFACE CHEMICAL WORK BY CATALYTIC PYRODISTILLATION [J].
CONWAY, BE ;
ANGERSTE.H ;
SHARP, WBA ;
CRIDDLE, EE .
ANALYTICAL CHEMISTRY, 1973, 45 (08) :1331-1336
[10]  
Damjanovic A., 1969, MODERN ASPECTS ELECT, V5, P369