| Summary: | The single gold atom doped aluminum oxide clusters AuAlO, AuAlO, and AuAlO have been prepared and mass-selected to react with CO, O, and mixtures of CO and O in an ion trap reactor under thermal collision conditions. The reactions have been characterized by mass spectrometry with isotopic substitution (O → O) and density functional theory calculations. The AuAlO cluster can oxidize two CO molecules consecutively to form AuAlO and then AuAlO, the latter of which can react with one O molecule to regenerate AuAlO. The AuAlO ions interact with a mixture of CO and O to produce the fully substituted O species AuAlO, which firmly identifies a catalytic cycle for CO oxidation by O. The oxidation catalysis is driven by electron cycling primarily through making and breaking a gold–aluminum chemical bond. To the best of our knowledge, this is the first identification of catalytic CO oxidation by O mediated with gas-phase cluster catalysts with single-noble-metal atoms, which serves as an important step to understand single-atom catalysis at strictly a molecular level.
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