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Catalytic CO Oxidation by O 2 Mediated with Single Gold Atom Doped Titanium Oxide Cluster Anions AuTi 2 O 4–6 −
Author(s) -
Wang SiDun,
Chen JiaoJiao,
Li XiaoNa,
Ma TongMei,
He ShengGui
Publication year - 2020
Publication title -
chemphyschem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.016
H-Index - 140
eISSN - 1439-7641
pISSN - 1439-4235
DOI - 10.1002/cphc.202000755
Subject(s) - catalysis , heteronuclear molecule , chemistry , reactivity (psychology) , moiety , titanium oxide , cluster (spacecraft) , oxide , dissociation (chemistry) , crystallography , metal , density functional theory , gold cluster , inorganic chemistry , stereochemistry , computational chemistry , nuclear magnetic resonance spectroscopy , organic chemistry , medicine , alternative medicine , pathology , computer science , programming language
Gas‐phase studies on catalytic CO oxidation by O 2 mediated with gold‐containing heteronuclear metal oxide clusters are vital to obtain the structure−reactivity relationship of supported gold catalysts, while it is challenging to trigger the reactivity of clusters with closed‐shell electronic structure in O 2 activation. Herein, we identified that CO oxidation by O 2 can be catalyzed by the AuTi 2 O 4–6 − clusters, among which AuTi 2 O 4 − with closed‐shell electronic structure can effectively activate O 2 . The reactions were characterized by mass spectrometry and quantum chemical calculations. Theoretical calculations showed that in the initial stage of O 2 activation, the Ti 2 O 4 moiety in AuTi 2 O 4 − contributes dominantly to activate O 2 into superoxide (O 2 − ⋅) without participation of the Au atom. In subsequent steps, the intimate charge transfer interaction between Au and the Ti 2 O 4 moiety drives the direct dissociation of the O 2 − ⋅ unit.