An Eight-Atom Iridium-Aluminum Oxide Cluster IrAlO 6 + Catalytically Oxidizes Six CO Molecules

Fundamental understanding regarding oxygen storage capacity involving how and why an active site can buffer a large number of oxygen atoms in redox processes is vital to the design of advanced oxygen storage materials, while it is challenging because of the complexity of heterogeneous catalysis. Her...

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Bibliographic Details
Published in:The journal of physical chemistry letters 2019-12, Vol.10 (24), p.7850-7855
Main Authors: Li, Xiao-Na, Jiang, Li-Xue, Wang, Li Na, Ou, Shu-Hua, Zhang, Mei-Qi, Yang, Yuan, Ma, Tong-Mei, He, Sheng-Gui
Format: Article
Language:English
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Summary:Fundamental understanding regarding oxygen storage capacity involving how and why an active site can buffer a large number of oxygen atoms in redox processes is vital to the design of advanced oxygen storage materials, while it is challenging because of the complexity of heterogeneous catalysis. Herein, we identified that an eight-atom iridium-aluminum oxide cluster IrAlO can transfer all the oxygen atoms to catalytically oxidize six CO molecules. This finding represents a breakthrough in cluster catalysis where at most three oxygen atoms from a heteronuclear metal oxide cluster can be catalytically involved in CO oxidation. We found that oxygen prefers to be stored on aluminum to form an O radical in the energetically unfavorable IrAlO isomer and generate the low-coordinated iridium that is pivotal to capturing CO and triggering the catalysis. The powerful electron cycling capability of iridium and the cooperative iridium-aluminum interplay are emphasized to drive the oxygen atom-transfer behavior.
ISSN:1948-7185
1948-7185
DOI:10.1021/acs.jpclett.9b03056