Citation: HU Jian-Ping, WANG Jun, TANG Dian-Yong, FU Qin-Chao, ZHANG Yuan-Qin. Reaction Mechanisms of CO Oxidation Catalyzed by Binary Copper Group Cluster Anions[J]. Acta Physico-Chimica Sinica, ;2011, 27(02): 329-336. doi: 10.3866/PKU.WHXB20110226 shu

Reaction Mechanisms of CO Oxidation Catalyzed by Binary Copper Group Cluster Anions

1.
1. Molecular Design Center, College of Chemistry and Life Science, Leshan Normal University, Leshan 614000, Sichuan Province, P. R. China;
2. Neurology Department, Chengdu Military General Hospital, Chengdu 610083, P. R. China

Received Date: 25 August 2010
Available Online: 5 January 2011
Fund Project: 教育部科学技术研究重点项目(210189) (210189) 四川省自然科学基金(2008JY0119) (2008JY0119)四川省教育厅(07ZA158)资助 (07ZA158)

The detailed mechanisms of CO oxidation catalyzed by AuAg^-, AuCu^-, and AgCu^- were investigated using density functional theory at the B3LYP level. The computational results indicate that the adsorption site of CO onto the mixed clusters decreases as follows: Cu>Au>Ag. Copper is the preferred adsorption site for O₂ on the binary clusters. The adsorption of O₂ onto ld was found to be the weakest. Three reaction pathways exist for CO oxidation catalyzed by AuAg^-, AuCu^-, and AgCu^-. The most feasible pathway for CO oxidation catalyzed by AuAg^- is CO insertion into the Ag―O bond of AuA ₂^- to produce the [Au―AgC(O―O)O]^- intermediate, which then decomposes into CO₂ and AuA ^-, or another CO molecule attacks [Au―AgC(O―O)O]^- to form two CO₂ molecules and AuAg^- anion. A feasible pathway for CO oxidation catalyzed by AuCu^- or AgCu^- is initiated by the co-absorption of CO and O₂ onto the clusters followed by the formation of a four-membered ring intermediate to produce the corresponding products. The cooperation effect of the second CO is very weak. The catalytic activities of AuAg^- and AuCu^- toward CO oxidation are stronger than that of Au₂^- . Doping the Au clusters with Ag and Cu increases the catalytic activity. These results are in agreement with the previous experimental results.
- Density functional theory,
- CO oxidation,
- Binary copper group cluster anion,
- Reaction mechanism
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