Atomic Plane-Vacancy Engineering of Transition Metal Dichalcogenides with Enhanced Hydrogen Evolution Capability

Introducing anion vacancies on 2D transition-metal dichalcogenides (TMDs) would significantly improve their catalytic activity but still lack an industrially viable approach. In this work, we proposed a general solid phase reduction (SPR) strategy, simultaneously achieving scalable exfoliation and controllable generation of chalcogen vacancies on TMDs. Consecutive sulfur vacancies were successfully created on the basal plane of the bulk MoS2 and WS2, and their interlamellar distances were distinctly expanded after the SPR treatment (about 16%), which can be conveniently exfoliated by only gentle shaking within several seconds. The S-vacancy significantly increases the hydrogen evolution reaction activity of the MoS2 and WS2 nanosheets (NSs), with overpotential of -238 and -241 mV at 10 mA cm-2, respectively. We anticipate our SPR strategy will supply a general platform for the development of TMD-based electrocatalysts for industrial water splitting and hydrogen production in the near future.