Boosting Electrochemical Nitrogen Fixation via Regulating Surface Electronic Structure by CeO 2 Hybridization

Electrocatalytic 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.