Charge-Modulated VS2 Monolayer for Effective Hydrogen Evolution Reaction

Controlling the electronic structure of the basal plane of transition metal dichalcogenides (TMDs) is essential to develop effective catalysts for hydrogen evolution reaction (HER). In this work, we engineer the surface structure of VS2 by doping 3d transition metal (TM = Ti–Ni) atoms aiming to improve its catalytic activity. Our results indicate that the HER performances of these TM@VS2s are much better than that of pristine VS2 due to the charge modulation in S sites. Particularly, three systems of TM@VS2s (TM = Ti, Mn, Co) are found to be perfect catalysts for HER with ideal ΔGH ∼ 0 eV, even superior to that of Pt. Moreover, the HER performances of TM@VS2s are revealed to depend strongly on the choice of TM elements as well as their doping concentrations. Our study provides a promising way to design effective electrocatalysts for energy conversion in the future.