Oxidation of CO into CO2 is a major solution to reduce CO emission into the atmosphere and to remove CO in fuel gas cleanup. Furthermore, CO oxidation serves as a prototypical reaction for heterogeneous catalysis. This review provides an overview and an update on how to study catalytic CO oxidation at a strictly molecular level by performing well-controlled gas-phase experiments in combination with quantum chemistry calculations. The advances in the unique catalytic reactivity of single-atom cluster catalysts are emphasized. The catalytically active sites and various mechanistic aspects in the redox couples N2O/CO and O2/CO for the seemingly simple oxidation reaction are described.
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