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Multiple CO Oxidation Promoted by Au 2 Dimers in Au 2 TiO 4 − Cluster Anions
Author(s) -
Li XiaoNa,
Li ZiYu,
Li HaiFang,
He ShengGui
Publication year - 2016
Publication title -
chemistry – a european journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.687
H-Index - 242
eISSN - 1521-3765
pISSN - 0947-6539
DOI - 10.1002/chem.201600451
Subject(s) - chemistry , dimer , dissociation (chemistry) , molecule , photochemistry , cluster (spacecraft) , oxygen , ion , peroxide , mass spectrometry , photodissociation , inorganic chemistry , organic chemistry , chromatography , computer science , programming language
Time‐of‐flight mass spectrometry experiments demonstrated that laser ablation generated and mass selected Au 2 TiO 4 − cluster anions can unexpectedly oxidize three CO molecules in an ion trap reactor. This is an improvement on the more commonly observed oxidation of at most two CO molecules by a doped cluster. Quantum chemistry calculations were performed to rationalize the reactions. The lowest energy isomer of Au 2 TiO 4 − contains a superoxide unit, the participation of which in CO oxidation can be promoted by the Au 2 dimer. The Au 2 dimer functions as a rather flexible electron reservoir in each CO oxidation step in terms of the release and storage of electrons to drive the dissociation of superoxide to peroxide and then to lattice oxygen atoms, which can be removed by reaction with CO molecules. This gas‐phase study enriches our understanding toward the nature of reactive oxygen species involved in gold‐catalyzed oxidation reactions.