Identification of Catalyst Structure during the Hydrogen Oxidation Reaction in an Operating PEM Fuel Cell

被引:31
|
作者
Siebel, Armin [1 ,2 ]
Gorlin, Yelena [1 ,2 ]
Durst, Julien [3 ]
Proux, Olivier [4 ,5 ]
Hasche, Frederic [1 ,2 ]
Tromp, Moniek [6 ]
Gasteiger, Hubert A. [1 ,2 ]
机构
[1] Tech Univ Munich, Dept Chem, Chair Tech Electrochem, Lichtenbergstr 4, D-85748 Garching, Germany
[2] Tech Univ Munich, Catalysis Res Ctr, Lichtenbergstr 4, D-85748 Garching, Germany
[3] Paul Scherrer Inst, Energy & Environm Div, CH-5232 Villigen, Switzerland
[4] ESRF, FAME Beamline BM30B, F-38000 Grenoble, France
[5] Univ Joseph Fourier, CNRS, UMS 832, Observ Sci,Univers Grenoble, F-38000 Grenoble, France
[6] Univ Amsterdam, Vant Hoff Inst Mol Sci, Sci Pk 904, NL-1098 XH Amsterdam, Netherlands
来源
ACS CATALYSIS | 2016年 / 6卷 / 11期
关键词
HOR; operando EXAFS; palladium hydride; PEMFC; RDE; X-RAY-ABSORPTION; LIMITED-VOLUME ELECTRODES; RU ANODE ELECTROCATALYST; SUPPORTED PALLADIUM; OXYGEN REDUCTION; PD; SPECTROSCOPY; HYDRIDE; EXAFS; SIZE;
D O I
10.1021/acscatal.6b02157
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
Palladium is among the most active catalysts for the hydrogen oxidation reaction (HOR) and is thus a potential candidate for replacing platinum in fuel cell catalysis. At the same time, it is well-known to absorb large amounts of hydrogen, forming a bulk hydride phase. In several electrochemical studies conducted in liquid electrolytes and temperatures between 60 and 20 degrees C, the hydrogen from the hydride phase was observed to desorb at potentials positive of similar to 32 to SO mV vs the reversible hydrogen electrode (RHE). Here, we present operando spectroscopic studies in a fuel cell configuration. We first validate our experimental setup by comparing the potential dependence of hydrogen absorption into a Pd/C catalyst under nitrogen determined both by electrochemical means and by operando X-ray absorption spectroscopy (XAS) at various temperatures between 20 and 100 degrees C. Subsequently, we investigate the structure of the Pd/C catalyst during the HOR in a fuel cell operating at 80 degrees C in a H-2-pump configuration. Our results unequivocally show that, in contrast to rotating-disk-electrode (RDE) data reported in the literature, the hydride phase is maintained during the HOR in a fuel cell anode environment. The discrepancy between our results and previously published data is explained in terms of the vastly different mass-transport limitations in a fuel cell and in a conventional liquid electrolyte based electrochemical cell and highlights the importance of investigating catalyst structure in a representative reaction environment.
引用
收藏
页码:7326 / 7334
页数:9
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