LAUSR

Ammonia is one of the most important fertilizer feedstock and chemical precursors besides a promising hydrogen carrier. However, the electrochemical reduction of nitrogen to ammonia is impeded by the low selectivity and high limiting potential of reported catalysts. Herein, the nitrogen reduction reaction (NRR) on Os-doped BN cluster supported on C 2 N (Os 1 B 11 N 12 /C 2 N) has been investigated systematically based on the density functional theory calculation. It is found that the adjustment of BN cluster on the upper d -band edge of Os atom enables the optimal adsorption strength for NRR intermediates. Consequently, Os 1 B 11 N 12 /C 2 N exhibits high catalytic activity for NRR with the limiting potential of -0.34 V and a remarkable suppressive effect on hydrogen evolution reaction (HER). This work not only benefits for understanding the mechanism of NRR, but also provides a fundamental guidance for rational design of catalysts for NRR.