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 Au0 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.

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

MANZOLI, Maela;BOCCUZZI, Flora;CHIORINO, Anna;VINDIGNI, FLORIANA;
2007-01-01

Abstract

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 Au0 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.
2007
245
308
315
http://dx.doi.org/10.1016/j.jcat.2006.10.021
M. MANZOLI; F. BOCCUZZI; A. CHIORINO; F. VINDIGNI; W. DENG; M. FLYTZANI-STEPHANOPOULOS
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/2318/38305
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