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Size and composition dependence in CO oxidation reaction on small free gold, silver, and binary silver–gold cluster anions by Thorsten M. Bernhardt; Liana D. Socaciu-Siebert; Jan Hagen; Ludger Wöste is a Materials Science article available to read on EtoBox.

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Gas phase kinetics experiments with mass-selected gold, silver, and binary silver-gold cluster ions in a radio frequency (rf)-ion trap reactor are presented. For the catalytic CO combustion reaction, the adsorption of molecular oxygen onto the free clusters is identified as the first reaction step. A comparison of the measured O 2 adsorption reaction rate constants for the investigated Ag n Au m À (n + m = 1, 2, 3) clusters reveals a pronounced size and composition dependence. Favorable activation of the oxygen molecular bond is only expected in the case of Au 2 À . In the reaction of the gold dimer with O 2 and CO, a coadsorption complex is identified at cryogenic temperatures as decisive reaction intermediate in the observed CO oxidation reaction. Through detailed reaction kinetics measurements in combination with first-principles calculations, a comprehensive understanding of the molecular details of the catalytic reaction cycle emerges. The obtained data also permit the determination of the CO 2 formation rate and the catalytic turn-over-frequency in the rf-ion trap reactor. In contrast to gold, odd size silver cluster anions are found to adsorb two oxygen molecules. These Ag n

Who reads Size and composition dependence in CO oxidation reaction on small free gold, silver, and binary silver–gold cluster anions?

Author

Thorsten M. Bernhardt; Liana D. Socaciu-Siebert; Jan Hagen; Ludger Wöste

Publisher

Elsevier Science; Elsevier ; Elsevier BV (ISSN 0926-860X)

Published

2005

Language

EN

Field

Materials Science (Physical Sciences)