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Ceria-Supported Gold Nanoparticles as a Superior Catalyst for Nitrous Oxide Production via Ammonia Oxidation.

The production of nitrous oxide, N2O, via NH3 oxidation is not in practical scale due to the lack of a suitable catalyst. Instead, it is produced via thermal decomposition of NH4NO3, rendering N2O too costly and limiting its prospective uses. Herein, we report CeO2-supported Au nanoparticles (2-3 nm) as a highly selective catalyst for low-temperature NH3 oxidation to N2O, exhibiting two orders of magnitude higher space-time yield than the state-of-the-art Mn-Bi/α-Al2O3 and remarkable stability over 70 h on stream. The reaction proceeds via a Mars-Van Krevelen mechanism, with the density of interfacial Auδ+ species and the oxygen storage capacity of CeO2 identified as the key performance descriptors. The latter could be enhanced by cobalt doping, improving the catalytic activity and setting a new benchmark for N2O productivity. These findings establish NH3 oxidation as an efficient process for N2O manufacture and facilitate its broader utilization as a green and selective oxidant.