Screening for electrocatalytic reduction of N2 by borophene supported bimetallic atoms

Ammonia (NH3), as a high energy density chemical and hydrogen energy storage medium, has garnered significant interest in the realms of energy storage and catalysis. In contrast to the traditional Haber-Bosch process, the electrocatalysis nitrogen reduction reaction (eNRR) can synthesize green ammonia under mild reaction conditions. Based on density functional theory (DFT), the potential of 2D borophene supported transition metals as bimetallic atomic catalysts (BACs) in eNRR was investigated. Progressive screening through energy-oriented screening mechanism, Sc2B12, Ti2B12, V2B12 and Zr2B12 were identified as potential eNRR catalysts. Their complete reaction pathways and Gibbs free energy (ΔG) were further explored, and corresponding overpotentials were obtained. The results showed that overpotentials of the potential determining steps (PDS) of these catalysts were 0.34, 0.40, 0.39 and 0.13 V, respectively, demonstrating excellent eNRR catalytic activity and good selectivity. Cu2B12 shows remarkable hydrogen evolution reaction (HER) catalytic activity with an overpotential (η) of only 0.05 V. The study also revealed that the catalytic activity of TM2B12 is derived from its excellent conductivity, and the charge transmission enhances the catalyst activity of eNRR. Consequently, this study provides significant theoretical guidance and support for the synthesis of novel eNRR catalysts, and promotes further advancement in the field of catalysis.