Os 1 B 11 N 12 /C 2 N as an Efficient Electrocatalyst for Nitrogen Reduction Reaction.

Ammonia is one of the most important fertilizer feedstocks and chemical precursor 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) was investigated systematically based on density functional theory calculations. It was found that the adjustment of BN cluster on the upper d-band edge of Os atom enabled the optimal adsorption strength for NRR intermediates. Consequently, Os 1 B 11 N 12 /C 2 N exhibited high catalytic activity for NRR with the limiting potential of -0.34 V and a remarkable suppressive effect on the hydrogen evolution reaction. This work is not only beneficial for understanding the mechanism of NRR but also provides a fundamental guidance for rational design of catalysts for NRR.