The density functional theory (DFT) calculations were performed to investigate the catalytic activities of Pd, Cu, and Pd_xCu_y alloy catalysts for N₂O reduction reaction (NRR). The activation and dissociation of N₂O on Pd_xCu_y catalysts were explored. The rate-determining step for the NRR was the dissociation of N₂O into N₂ and O. The electronic structure of Pd_xCu_y alloys was determined by both ligand and strain effects, but was not closely related to the catalytic activity for NRR because two kinds of surface Pd and Cu atoms are differently involved in active sites for molecular adsorption and dissociation. Owing to the different role of Pd and Cu in NRR, the PdCu catalyst had both strong N₂O adsorption strength and easier N₂O dissociation than did pure and Pd₃Cu catalysts, and therefore had the highest catalytic activity for NRR among the Pd_xCu_y alloy catalysts. These fundamental findings were further applied to predict the thermal and electrochemical NRR.

DOI: 10.1016/j.apsusc.2020.145349
Link: https://www.sciencedirect.com/science/article/pii/S0169433220301057