G‐C3N4/SnS2 van der Waals Heterostructures Enabling High‐Efficiency Photocatalytic Hydrogen Evolution

Abstract

AbstractVan der Waals (vdW) heterojunction has played an essential role in effectively utilizing solar energy for sustainable hydrogen production. Herein, a 2D/2D g‐C3N4/SnS2 photocatalyst with vdW heterojunction is developed by self‐assembly contacting SnS2 hexagonal nanoplates and g‐C3N4 nanosheets. A reasonable Type‐II charge transfer mechanism based on the vdW heterostructure is proposed and verified by hydroxyl radical generation test. Photocatalysts with vdW heterostructure enable high‐efficiency H2 production under the visible light illumination, of which the optimized rate is about seven times higher than that of SnS2. Experimental analysis and corresponding density functional theory simulation jointly identify that enhanced photocatalytic activity is ascribed to the optimized behavior of photogenerated carriers and promotional interaction between reactants with catalysts. Specifically, charge redistribution and staggered band structure of the heterojunction intrinsically facilitate the efficient interfacial charge migration and separation. Diminished free energy of surface hydrogen adsorption reveals the easier hydrogen adsorption‐desorption for a composite system from the viewpoint of thermodynamics. This work may be attractive for the implementation of rationally synthesizing catalysts for efficient photocatalytic water splitting.