Boosting Electrochemical Nitrogen Fixation via Regulating Surface Electronic Structure by CeO2 Hybridization

Abstract

AbstractElectrocatalytic nitrogen reduction reaction (NRR) paves a sustainable way to produce NH3 but suffering from the relatively low NH3 yield and poor selectivity. High‐performance NRR catalysts and a deep insight into the structure‐performance relationship are higher desired. Herein, a molten‐salt approach is developed to synthesize tiny CeO2 nanoparticles anchored by ultra‐thin MoN nanosheets as advanced catalysts for NRR. Specifically, a considerably high NH3 yield rate of 27.5 µg h−1 mg−1 with 17.2% Faradaic efficiency (FE) can be achieved at ‐0.3 V vs (RHE) under ambient conditions. Experimental and density functional theory (DFT) calculations further point out that the incorporation of MoN with CeO2 can promotes the enlargement of the electron deficient area of nitrogen vacancy site. The enlarged electron deficient area contributes to the accommodation of lone pair electrons of N2, which dramatically improves the N2 adsorption/activation and the key intermediates (*NNH and *NH3) generation, thus boosting the NRR performance.