Spontaneous Enhanced Visible-Light-Driven Photocatalytic Water Splitting on Novel Type-II GaSe/CN and Ga2SSe/CN vdW Heterostructures.

With the aggravation of environmental pollution and the energy crisis, it is particularly important to develop and design environment-friendly and efficient spontaneous enhanced visible-light-driven photocatalysts for water splitting. Herein novel type-II van der Waals (vdW) GaSe/CN and Ga2SSe/CN heterostructures are proposed through first-principles calculations. Their electronic properties and photocatalytic performance are theoretically analyzed. In particular, their appropriate band gap and band-edge position meet the requirements of the oxygen evolution reaction, and the reaction is thermodynamically feasible in most pH ranges. The unique band alignment of these heterostructured photocatalysts leads to high solar-to-hydrogen energy conversion efficiencies up to 15.11%, which has a good commercial application prospect. More excitingly, with the application of 2% biaxial strain, the smooth progress of the water-splitting reaction of the GaSe/CN and Ga2SSe/CN heterostructures can still be maintained, and the carrier mobility and optical absorption characteristics can be effectively improved. Consequently, these findings suggest that the GaSe/CN and Ga2SSe/CN vdW heterostructures have promising potentials as photocatalysts for water splitting. This work may provide a promising clue for the design of efficient and stable photocatalytic water-splitting catalysts under visible spectroscopy.