Catalytically active states of Ru(0001) catalyst in CO oxidation reaction

被引:80
作者
Blume, R
Hävecker, M
Zafeiratos, S
Teschner, D
Kleimenov, E
Knop-Gericke, A
Schlögl, R
Barinov, A
Dudin, P
Kiskinova, M
机构
[1] Sincrotrone Trieste, I-34012 Trieste, Italy
[2] Max Planck Gesell, Fritz Haber Inst, D-14195 Berlin, Germany
关键词
CO oxidation; Ru; high pressure XPS; catalytically active states;
D O I
10.1016/j.jcat.2006.02.019
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
Identifying the composition of the catalytically active state of metal catalysts under dynamic operating conditions is of particular importance for oxidation catalysis. Here we report new insights into the chemical identity of different catalytically active states formed on a Ru(0001) catalyst during CO oxidation at various reaction temperatures. The changes in the surface composition of the Ru catalyst and the CO2 yield under varying reaction conditions in the 10(-4)-10(-1) mbar pressure range were followed in situ by synchrotron-based high-pressure X-ray photoelectron spectroscopy and mass spectroscopy. The results reveal that the catalytic activity of a few layers thick surface oxide without well-defined stoichiometry and structure is comparable with that of the stoichiometric RuO2(110) phase. This surface oxide forms under reaction conditions when RuO2 formation is kinetically hindered and can coexist with RuO2 in wide temperature and pressure ranges. (c) 2006 Elsevier Inc. All rights reserved.
引用
收藏
页码:354 / 361
页数:8
相关论文
共 35 条
[1]   Methanol oxidation on a copper catalyst investigated using in situ X-ray photoelectron spectroscopy [J].
Bluhm, H ;
Hävecker, M ;
Knop-Gericke, A ;
Kleimenov, E ;
Schlögl, R ;
Teschner, D ;
Bukhtiyarov, VI ;
Ogletree, DF ;
Salmeron, M .
JOURNAL OF PHYSICAL CHEMISTRY B, 2004, 108 (38) :14340-14347
[2]   Identification of subsurface oxygen species created during oxidation of Ru(0001) [J].
Blume, R ;
Niehus, H ;
Conrad, H ;
Böttcher, A ;
Aballe, L ;
Gregoratti, L ;
Barinov, A ;
Kiskinova, M .
JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (29) :14052-14058
[3]   Surface-defect-mediated channel for oxygen incorporation into Ru(0001) [J].
Blume, R ;
Niehus, H ;
Conrad, H ;
Böttcher, A .
JOURNAL OF PHYSICAL CHEMISTRY B, 2004, 108 (38) :14332-14339
[4]   CO oxidation reaction over oxygen-rich Ru(0001) surfaces [J].
Böttcher, A ;
Niehus, H ;
Schwegmann, S ;
Over, H ;
Ertl, G .
JOURNAL OF PHYSICAL CHEMISTRY B, 1997, 101 (51) :11185-11191
[5]   Oxygen adsorbed on oxidized Ru(0001) [J].
Böttcher, A ;
Niehus, H .
PHYSICAL REVIEW B, 1999, 60 (20) :14396-14404
[6]   Mesoscopic-scale growth of oxygen-rich films on Ru(001) investigated by photoemission electron microscopy [J].
Böttcher, A ;
Krenzer, B ;
Conrad, H ;
Niehus, H .
SURFACE SCIENCE, 2002, 504 (1-3) :42-58
[7]   Spectral and spatial anisotropy of the oxide growth on Ru(0001) [J].
Böttcher, A ;
Starke, U ;
Conrad, H ;
Blume, R ;
Niehus, H ;
Gregoratti, L ;
Kaulich, B ;
Barinov, A ;
Kiskinova, M .
JOURNAL OF CHEMICAL PHYSICS, 2002, 117 (17) :8104-8109
[8]   Formation of subsurface oxygen at Ru(0001) [J].
Böttcher, A ;
Niehus, H .
JOURNAL OF CHEMICAL PHYSICS, 1999, 110 (06) :3186-3195
[9]   A systematic study of CO oxidation on metals and metal oxides: Density functional theory calculations [J].
Gong, XQ ;
Liu, ZP ;
Raval, R ;
Hu, P .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2004, 126 (01) :8-9
[10]   Atomic scale investigation of the oxidation of CO on RuO2(110) by scanning tunneling microscopy [J].
Kim, SH ;
Wintterlin, J .
JOURNAL OF PHYSICAL CHEMISTRY B, 2004, 108 (38) :14565-14569