Theoretical Investigations of Electrochemical Nitrogen Reduction on Single Transition Metal Atom Catalysts Supported by 1T-MoSe₂

The search for stable and efficient single-atom catalysts (SACs) for the electrocatalytic nitrogen reduction reaction (eNRR) has garnered significant theoretical interest. In this study, we evaluate the eNRR performance of eighteen two-dimensional 1T-MoSe₂-supported transition metal single-atom catalysts (TM@1T-MoSe₂, TM=V, Cr, Mn, Fe, Co, Ni, Nb, Mo, Tc, Ru, Rh, Pd, Ta, W, Re, Os, Ir, and Pt) using density functional theory calculations. We assess the stability of each TM@1T-MoSe₂, as well as the limiting potential of eNRR and the ammonia selectivity on each stable TM@1T-MoSe₂. Our results show that W@1T-MoSe₂ is the most promising single-atom catalyst for eNRR, with a limiting potential of −0.23 V via the distal pathway starting from three co-adsorbed nitrogen molecules. Furthermore, the multi-adsorption of N₂ on W@1T-MoSe₂ effectively suppress the hydrogen evolution reaction, thus enhancing the selectivity of the eNRR. This research provides a promising avenue for the development of a new class of 1T-MoSe₂-based single-atom catalysts for electrocatalytic ammonia synthesis.