CO adsorption on a Au/CeO2 (111) model catalyst

被引:56
作者
Weststrate, C. J. [1 ]
Resta, A. [1 ]
Westerstrom, R. [1 ]
Lundgren, E. [1 ]
Mikkelsen, A. [1 ]
Andersen, J. N. [1 ]
机构
[1] Lund Univ, Inst Phys, Natl Synchrotron Radiat Res, S-22100 Lund, Sweden
关键词
D O I
10.1021/jp7117482
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
We prepared a Au/CeO2 (111) model catalyst by depositing a thin cerium oxide film on a Ru(0001) surface and subsequently depositing gold. This model system was investigated using high-resolution photoemission spectroscopy. Gold forms metallic nanoparticles on CeO2 with an average particle size that depends on the Au dose. At 80 K adsorption of CO was observed on the supported Au particles, which induces a chemical shift of +0.9 eV in the An 4f level of the An atoms directly involved in the Au-CO bond. CO adsorption also induces an additional, particle-size-dependent shift, which affects all Au atoms in the particle; i.e., the whole Au particle is affected by CO adsorption. The fraction of surface atoms involved in CO bonding decreases with increasing gold particle size, from similar to 60-70% for small particles to 15-20% for large particles. It is concluded that CO only adsorbs on defects (low-coordinated Au atoms). The CO desorption temperature decreases with increasing particle size. This is explained as follows: on small particles the most abundant defects are corner atoms and kinks (6-coordinated), which interact strongly with CO. On large particles the most abundant defects are edges between two planes (7-coordinated), which interact less strongly with CO.
引用
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页码:6900 / 6906
页数:7
相关论文
共 38 条
[1]   TEM observation of gold nanoparticles deposited on cerium oxide [J].
Akita, T ;
Okumura, M ;
Tanaka, K ;
Kohyama, M ;
Haruta, M .
JOURNAL OF MATERIALS SCIENCE, 2005, 40 (12) :3101-3106
[2]   Substrate and morphology effects on photoemission from core-levels in gold clusters [J].
Dalacu, D ;
Klernberg-Sapieha, JE ;
Martinu, L .
SURFACE SCIENCE, 2001, 472 (1-2) :33-40
[3]   Growth and thermal properties of ultrathin cerium oxide layers on Rh(111) [J].
Eck, S ;
Castellarin-Cudia, C ;
Surnev, S ;
Ramsey, MG ;
Netzer, FP .
SURFACE SCIENCE, 2002, 520 (03) :173-185
[4]   Electron localization determines defect formation on ceria substrates [J].
Esch, F ;
Fabris, S ;
Zhou, L ;
Montini, T ;
Africh, C ;
Fornasiero, P ;
Comelli, G ;
Rosei, R .
SCIENCE, 2005, 309 (5735) :752-755
[5]   Nanostructured Au-CeO2 catalysts for low-temperature water-gas shift [J].
Fu, Q ;
Weber, A ;
Flytzani-Stephanopoulos, M .
CATALYSIS LETTERS, 2001, 77 (1-3) :87-95
[6]   Active nonmetallic Au and Pt species on ceria-based water-gas shift catalysts [J].
Fu, Q ;
Saltsburg, H ;
Flytzani-Stephanopoulos, M .
SCIENCE, 2003, 301 (5635) :935-938
[7]   The beneficial effect of the addition of base metal oxides to gold catalysts on reactions relevant to air pollution abatement [J].
Gluhoi, AC ;
Lin, SD ;
Nieuwenhuys, BE .
CATALYSIS TODAY, 2004, 90 (3-4) :175-181
[8]   Spectroscopic evidence for the supply of reactive oxygen during CO oxidation catalyzed by gold supported on nanocrystalline CeO2 [J].
Guzman, J ;
Carrettin, S ;
Corma, A .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2005, 127 (10) :3286-3287
[9]   CO oxidation catalyzed by supported gold: Cooperation between gold and nanocrystalline rare-earth supports forms reactive surface superoxide and peroxide species [J].
Guzman, J ;
Carrettin, S ;
Fierro-Gonzalez, JC ;
Hao, YL ;
Gates, BC ;
Corma, A .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2005, 44 (30) :4778-4781
[10]   NOVEL GOLD CATALYSTS FOR THE OXIDATION OF CARBON-MONOXIDE AT A TEMPERATURE FAR BELOW 0-DEGREES-C [J].
HARUTA, M ;
KOBAYASHI, T ;
SANO, H ;
YAMADA, N .
CHEMISTRY LETTERS, 1987, (02) :405-408