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

Zhenchen TangIvan SurinAsbjörn RasmussenFrank KrumeichEvgenii V KondratenkoVita A KondratenkoJavier Pérez-Ramírez
Published in: Angewandte Chemie (International ed. in English) (2022)
The production of nitrous oxide, N 2 O, via NH 3 oxidation is not on a practical scale due to the lack of a suitable catalyst. Instead, it is produced via thermal decomposition of NH 4 NO 3 , rendering N 2 O too costly and limiting its prospective uses. Herein, we report CeO 2 -supported Au nanoparticles (2-3 nm) as a highly selective catalyst for low-temperature NH 3 oxidation to N 2 O, exhibiting two orders of magnitude higher space-time yield than the state-of-the-art Mn-Bi/α-Al 2 O 3 and remarkable stability over 70 h on stream. The reaction proceeds via a Mars-van Krevelen mechanism, with the density of interfacial Au δ+ species and the oxygen storage capacity of CeO 2 identified as the key performance descriptors. The latter could be enhanced by cobalt doping, improving the catalytic activity and setting a new benchmark for N 2 O productivity. These findings establish NH 3 oxidation as an efficient process for N 2 O manufacture and facilitate its broader utilization in selective oxidations.
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