Single transition metal atom modified MoSe2 as a promising electrocatalyst for nitrogen Fixation: A first-principles study

Highlights: • W/MoSe₂ possesses an excellent thermodynamic stability. • W/MoSe₂ exhibits low potential barrier of the determining step (0.21 eV). • The increased TM atoms can strengthen E(*N₂) and decrease limiting potential. Single atom electrocatalysts show great potential to nitrogen reduction reaction (NRR). Here, we studied transition metals (V, Cr, Nb, Mo, Ta, W) doped on MoSe₂ as single atom electrocatalysts by first-principles theory. We investigated different NRR pathways and its corresponding Gibbs free energy. It is found that W/MoSe₂ has a better NRR catalytic activity than others due to the larger charge composition with N₂ molecule. Furthermore, the limiting potential has a quasi-linear relationship with the N₂ adsorption energy, which is also related to the changes of charge composition. The result highlights a new family of efficient TM/MoSe₂ catalysts for NRR.