Spectroscopic features and reactivity of CO adsorbed on different Au/CeO2 catalysts

被引:135
作者
Manzoli, Maela
Boccuzzi, Flora [1 ]
Chiorino, Anna
Vindigni, Floriana
Deng, Weiling
Flytzani-Stephanopoulos, Maria
机构
[1] Tufts Univ, Dept Biol & Chem Engn, Medford, MA 02155 USA
[2] Univ Turin, Dipartimento Chim, IFM, I-10125 Turin, Italy
[3] Univ Turin, NIS, Ctr Excellence, I-10125 Turin, Italy
基金
美国国家科学基金会;
关键词
gold-ceria catalysts; gold ions; FTIR; CO adsorption; CO oxidation; XPS; TPR;
D O I
10.1016/j.jcat.2006.10.021
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
An FTIR study of CO adsorption from 120 K up to room temperature on a series of Au-ceria samples is presented. Samples with low gold content (0.7 and 0.6 at%) were prepared by urea gelation/co-precipitation and by cyanide leaching of the high-gold content (5.8 at%) material prepared by deposition-precipitation on La-doped CeO2. The samples were subjected to different pretreatments to collect information on the surface composition under working conditions. An absorption band at 2130-2140 cm(-1), not reversible on outgassing and more resistant to oxidation than the usual carbonyl band on Au-0 sites, was present due to CO adsorbed on cationic gold clusters. This highly stable species is relevant for hydrogen gas upgrade by removing CO from reformate-type gases at low temperatures. In addition, a broad absorption band in the 2000-2100 cm(-1) range was observed after reduction in hydrogen, due to structural and electronic changes of gold. Interestingly, the reduced gold species in ceria. can be reoxidized at mild conditions. Light-off of the CO oxidation reaction took place below room temperature on the metallic gold-containing ceria but was delayed until 310 K on the ionic gold-containing sample. TPR and XPS analysis of the fresh and used catalysts corroborated the stability of ionic gold in ceria up to 393 K in the reaction gas mixture. (c) 2006 Elsevier Inc. All rights reserved.
引用
收藏
页码:308 / 315
页数:8
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