High-throughput screening of single metal atom anchored on N-doped boron phosphide for N₂ reduction

Developing eco-friendly and highly-efficient catalysts for the electrochemical nitrogen reduction reaction (NRR) under ambient conditions to replace the energy-intensive and environment-polluting Haber-Bosch process is of great significance, while remaining a long-standing challenge in the field of energy conversion today. Herein, through the first principles high-throughput screening, we systematically investigated the catalytic activity of a series of single metal atom immobilized on N-doped boron phosphide (N₃-BP) for N₂ reduction, denoted as MN₃-BP. In particular, a "four-step" screening strategy, involving the structural stability, N₂ chemisorption, low energy cost, as well as good selectivity, was adopted for the stringent screening of the promising MN₃-BP candidates for NRR. Our results unveil that among these candidates, MoN₃-BP eventually stands out, benefiting from its high selectivity and activity, as well as accompanying a considerably favorable limiting potential of -0.25 V for NRR. More impressively, the NRR activity origin of various candidates was revealed by the descriptor φ and ICOHP. Overall, our work not only accelerates the discovery of SACs for converting N₂ into sustainable NH₃ but also provides an exciting impetus for the rational design of NRR catalysts with high stability, high activity, and high selectivity.