Bimetallic PtSn catalyst for selective CO oxidation in H2-rich gases at low temperatures

被引:165
作者
Schubert, MM [1 ]
Kahlich, MJ [1 ]
Feldmeyer, G [1 ]
Hüttner, M [1 ]
Hackenberg, S [1 ]
Gasteiger, HA [1 ]
Behm, RJ [1 ]
机构
[1] Univ Ulm, Abt Oberflachenchem & Katalyse, D-89069 Ulm, Germany
关键词
D O I
10.1039/b008062o
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
Kinetic measurements on preferential CO oxidation in a H-2-rich atmosphere (PROX) over a bimetallic, carbon supported PtSn catalyst reveal a high activity and selectivity already at low temperatures (0-80 degreesC), superior to a commercial Pt/Al2O3 system. The selectivity, though steadily decreasing with temperature, is remarkably high, 85% at low temperatures around 0-20 degreesC, and even at 120 degreesC it is, at 45%, still higher than that of standard Pt catalysts. The observation that CO desorption is not rate limiting and that the selectivity decreases with increasing temperature, can be explained in a mechanistic model involving separation of the reactant adsorption sites (bifunctional surface), with competing CO and hydrogen adsorption on Pt sites/areas and oxygen adsorption predominantly on Sn sites and SnOx islands on/adjacent to the active PtSn particles. The reaction takes place in a bifunctional way at the perimeter of these islands or by invoking a spill-over process. This model is supported by CO temperature-programmed desorption (TPD), in situ diffuse reflectance IR Fourier transform spectroscopy (DRIFTS), and x-ray photon spectroscopy (XPS) measurements, which indicate that under reaction conditions the surface CO coverage on the metallic particles is high, but decreases with temperature, and that only part of the Sn is reduced, included in PtSn alloy particles, while another part is in an oxidic state, forming SnOx islands on and presumably also beside the active particles. Its excellent performance makes PtSn an interesting catalyst for fuel gas purification in low temperature polymer electrolyte membrane fuel cell technology (PEM-FC).
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页码:1123 / 1131
页数:9
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