Hydrogen adsorption and coadsorption with CO on well-defined bimetallic PtRu surfaces - a model study on the CO tolerance of bimetallic PtRu anode catalysts in low temperature polymer electrolyte fuel cells

被引:68
作者
Diemant, T [1 ]
Hager, T [1 ]
Hoster, HE [1 ]
Rauscher, H [1 ]
Behm, RJ [1 ]
机构
[1] Univ Ulm, Abt Oberflachenchem & Katalyse, D-89069 Ulm, Germany
关键词
adsorption kinetics; metallic surfaces; surface electronic phenomena (work function; surface potential; surface states; etc.); surface stress; alloys; ruthenium; platinum; thermal desorption; scanning tunneling microscopy; hydrogen molecule; deuterium; carbon monoxide;
D O I
10.1016/S0039-6028(03)00915-4
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
The influence of PtRu surface alloy formation and of coadsorbed CO on the adsorption/desorption characteristics of hydrogen on bimetallic PtRu surfaces was investigated by temperature programmed desorption, using a 40% Pt containing PtRu surface alloy pseudomorphic on a Ru(0001) surface with an almost statistical distribution of Pt surface atoms as substrate. Alloy formation leads to a significant broadening of the desorption peak compared to pure Ru, together with a considerable down-shift in the onset of desorption. This trend is even more pronounced in the presence of coadsorbed CO. The weakening of the hydrogen adsorption bond is attributed mainly to strain effects, imposed by the considerable compression of the pseudomorphic Pt as compared to bulk Pt(111). Finally we discuss the implications of these results for the mechanistic understanding of the improved performance of PtRu anode catalysts in reformate operated polymer electrolyte fuel cells. (C) 2003 Elsevier B.V. All rights reserved.
引用
收藏
页码:137 / 146
页数:10
相关论文
共 42 条
[1]   Spatially resolved chemistry on bimetallic surfaces [J].
Behm, RJ .
ACTA PHYSICA POLONICA A, 1998, 93 (02) :259-272
[2]   THEORETICAL-STUDY OF HYDROGEN ADSORPTION ON RU(0001) - POSSIBLE SURFACE AND SUBSURFACE OCCUPATION SITES [J].
CHOU, MY ;
CHELIKOWSKY, JR .
PHYSICAL REVIEW B, 1989, 39 (09) :5623-5631
[3]   ADSORPTION OF HYDROGEN ON A PT(111) SURFACE [J].
CHRISTMANN, K ;
ERTL, G ;
PIGNET, T .
SURFACE SCIENCE, 1976, 54 (02) :365-392
[4]   Anode materials for low-temperature fuel cells: A density functional theory study [J].
Christoffersen, E ;
Liu, P ;
Ruban, A ;
Skriver, HL ;
Norskov, JK .
JOURNAL OF CATALYSIS, 2001, 199 (01) :123-131
[5]   ADSORPTION OF HYDROGEN AND DEUTERIUM ON RU(001) [J].
CONRAD, H ;
SCALA, R ;
STENZEL, W ;
UNWIN, R .
JOURNAL OF CHEMICAL PHYSICS, 1984, 81 (12) :6371-6378
[6]   ADSORPTION AND DESORPTION OF AMMONIA, HYDROGEN, AND NITROGEN ON RUTHENIUM (0001) [J].
DANIELSON, LR ;
DRESSER, MJ ;
DONALDSON, EE ;
DICKINSON, JT .
SURFACE SCIENCE, 1978, 71 (03) :599-614
[7]  
DAVIS LE, 1978, HDB AUGER ELECT SPEC
[8]   CO adsorption and oxidation on bimetallic Pt/Ru(0001) surfaces - a combined STM and TPD/TPR study [J].
de Mongeot, FB ;
Scherer, M ;
Gleich, B ;
Kopatzki, E ;
Behm, RJ .
SURFACE SCIENCE, 1998, 411 (03) :249-262
[9]   THE ADSORPTION OF HYDROGEN ON RUTHENIUM (001) - ADSORPTION STATES, DIPOLE-MOMENTS AND KINETICS OF ADSORPTION AND DESORPTION [J].
FEULNER, P ;
MENZEL, D .
SURFACE SCIENCE, 1985, 154 (2-3) :465-488
[10]   H-2 AND CO ELECTROOXIDATION ON WELL-CHARACTERIZED PT, RU, AND PT-RU .1. ROTATING-DISK ELECTRODE STUDIES OF THE PURE GASES INCLUDING TEMPERATURE EFFECTS [J].
GASTEIGER, HA ;
MARKOVIC, NM ;
ROSS, PN .
JOURNAL OF PHYSICAL CHEMISTRY, 1995, 99 (20) :8290-8301