Abstract

While the electrochemical nitrogen reduction reaction (NRR) represents a prospective blueprint for environmentally renewable ammonia generation, it has yet to overcome the limitations of weak activity and inferior selectivity. In this regard, surface modification tactic was constructed to markedly enhance the activity and selectivity via introducing Sn atoms into the surface of defective cerium oxide (denoted as Sn-CeO2−x) as the active and robust electrocatalyst for NRR under benign environment. The introduction of Sn atoms in CeO2−x can not only inhibit the HER activity of the catalyst but also modulate the electronic structure of ceria and optimize N-Ce interaction, thus enhancing NRR activity and selectivity. Outperforming all previous CeO2-based NRR catalysts, this catalyst has demonstrated an ammonia yield rate of 41.1 μg mgcat−1 h−1 and an exceptional Faradic efficiency of 35.3%. This work presents a viable approach for the development of advanced NRR electrocatalysts.

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