An examination of active sites on Au-Ag bimetallic catalysts based on CO oxidation over Au/Ag2O and a comparison to Ag-contaminated Au powder

doi:10.1016/S1872-2067(16)62541-X

Chinese Journal of Catalysis ›› 2016, Vol. 37 ›› Issue (10): 1712-1720.DOI: 10.1016/S1872-2067(16)62541-X

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An examination of active sites on Au-Ag bimetallic catalysts based on CO oxidation over Au/Ag₂O and a comparison to Ag-contaminated Au powder

Yasuo Iizuka^a,b, Yasuhiro Hiragi^a, Hikaru Yakushiji^a, Takumi Miura^a

a Department of Chemistry and Materials Technology, Graduate School of Kyoto Institute of Technology, Matsugasaki, Sakyo-ku, Kyoto 606-8585, Japan;
b Research Institute for Ubiquitous Energy Division, National Institute of Advanced Industrial Science and Technology(AIST), Midorigaoka, Ikeda, Osaka 563-8577, Japan

Received:2016-04-15 Revised:2016-08-25 Online:2016-10-21 Published:2016-10-22
Contact: Yasuo Iizuka
Supported by:
This research was supported by CREST project (Catalyst Design of Gold Clusters through Junction Effect with Metal oxides, Carbons, and Polymers) sponsored by Japan Science and Technology Agency (JST).

Abstract

Abstract:

There are two theories regarding the origin of the remarkable synergistic effect observed in Au-Ag bimetallic catalysts when applied to various oxidative reactions. One is based on the importance of the contact interfaces between AgO_x regions and the surface of the bulk Au as active working sites, while the other holds that charge transfer from Ag to Au in a surface Au-Ag alloy causes the catalytic activity. One key point in examining these theories and determining the origin of the synergy involves determining whether or not Ag exists as an oxide or as a metallic alloy on the Au surface. To confirm that enhanced activity results from contact between Ag₂O and Au nanoparticles (NPs), a comparative study of catalytic CO oxidation over Au/Ag₂O and Ag₂O was performed in the present work, using a closed recirculation reaction system. A reaction mixture consisting of a stoichiometric composition of CO and O₂ (CO/O₂=2/1) was supplied to both catalysts and the resulting pressure decrease rates were tracked, from which the amounts of gas consumed as well as the quantity of CO₂ produced were determined. The steady state reactions of both Au/Ag₂O and Ag₂O did not lead to any meaningful difference in the rate of pressure decrease during the oxidation. The pressure decrease over both catalysts was attributed to the reduction of surface lattice O on Ag₂O by CO. The results obtained for Au/Ag₂O are in good agreement with previous data resulting from the use of Ag-contaminated Au powder (Ag/Au-b) having an oxidized surfaces. This finding suggests that the perimeters between AgO_x zones and the bulk Au surface may not function as active sites during CO oxidation. A review of previous results obtained with Ag/Au-b specimens having so-called steady state surfaces indicates that AgO_x species in such materials are reduced to the 0 state to form a Ag-Au alloy that provides the active sites.

Key words: Gold-silver bimetallic catalyst, Synergy effect, Carbon monoxide oxidation, Active site, Gold-silver alloy

Yasuo Iizuka, Yasuhiro Hiragi, Hikaru Yakushiji, Takumi Miura. An examination of active sites on Au-Ag bimetallic catalysts based on CO oxidation over Au/Ag₂O and a comparison to Ag-contaminated Au powder[J]. Chinese Journal of Catalysis, 2016, 37(10): 1712-1720.

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An examination of active sites on Au-Ag bimetallic catalysts based on CO oxidation over Au/Ag₂O and a comparison to Ag-contaminated Au powder

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