Computational Insight into Transition Metal Atoms Anchored on B2c3p As Single-Atom Electrocatalysts for Nitrogen Reduction Reaction

Abstract

NH3 is not only an important chemical raw material, but also a high energy storage chemical with zero carbon. Electrocatalytic nitrogen reduction reaction (NRR), which can be driven by clean electric energy under ambient conditions, have become a promising technology for NH3 synthesis due to their environmentally friendly properties. Due to the limitations of low yield and high overpotential, efficient catalysts are urgently needed to solve this problem. In this study, based on density functional theory method and high throughput screening strategy, the NRR was investigated on transition metal single atom anchored to two-dimensional B2C3P surface (TM@B2C3P) as single-atom catalysts (SACs). The results showed that V@B2C3P and Ti@B2C3P have good catalytic properties, and the limiting potentials via the enzymatic pathway were −0.10 and −0.24 V, respectively. Furthermore, the charge density difference and crystal orbital Hamilton population calculations demonstrated that the high catalytic activity can be attributed to the obvious charge transfer between TM@B2C3P and the adsorption intermediates. It is hoped that our work will facilitate experimental and theoretical studies of SACs to explore the potential of SACs in the NRR and other electrocatalytic reactions.

Keywords: NH3 synthesis, single-atom electrocatalyst, DFT calculations, nitrogen reduction reaction, B2C3P