Doping P atom with a lone pair: an effective strategy to realize high HER catalytic activity and avoid deactivation under wide H* coverage on 2D silicene and germanene by increasing the structural rigidity

Abstract

, N, P, As, Sb and Bi) heteroatoms with different electronegativity under detailed DFT calculations. It is revealed that the doped P atoms and almost all the Si/Ge atoms can uniformly serve as highly active sites. Especially, in view of the existence of the lone pair, doping P effectively prevents hydrogenation (even under full H* coverage) by increasing the structural rigidity. Moreover, the P-doping concentration also plays a crucial role in obtaining high HER activity. The relevant mechanisms have been analyzed in detail. Clearly, all these fascinating findings are beneficial for realizing new HER electrocatalysts based on the excellent silicene or germanene nanomaterials, and even other Si/Ge-related materials in the near future.