| Summary: | Water vapor has generally been recognized as an inhibitor of catalysts in nitrous oxide (N<sub>2</sub>O) decomposition because it limits the lifetime of catalytic reactors. Oxygen produced in reactions also deactivates the catalytic performance of bulk surface catalysts. Herein, we propose a potential catalyst that is tolerant of water and oxygen in the process of N<sub>2</sub>O decomposition. By applying density functional theory calculations, we investigated the reaction mechanism of N<sub>2</sub>O decomposition into N<sub>2</sub> and O<sub>2</sub> catalyzed by oxotitanium(IV) porphyrin (TiO-por) with interfacially bonded water. The activation energies of reaction Path A and B are compared under thermal and photo-assisted conditions. The obtained calculation results show that the photo-assisted reaction in Path B is highly exothermic and proceeds smoothly with the low activation barrier of 27.57 kcal/mol at the rate determining step. The produced O<sub>2</sub> is easily desorbed from the surface of the catalyst, requiring only 4.96 kcal/mol, indicating the suppression of catalyst deactivation. Therefore, TiO-por is theoretically proved to have the potential to be a desirable catalyst for N<sub>2</sub>O decomposition with photo-irradiation because of its low activation barrier, water resistance, and ease of regeneration.
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