Sulfur-deficient In2S3 Photocatalyst for High-efficiency Hydrogen Evolution via Water Splitting
Defect engineering is considered as one of the key strategies to enhance the photocatalyst performance for water splitting hydrogen production.However,it is still unclear how defects induce changes in the electronic structure of semiconductor materials and enhance the photogenerated carrier transfer.In this study,we successfully synthesized In2S3 photocatalyst with abundant sulfur defects(Vs-In2S3)by a simple one-step hydrothermal method.It exhibits a photocatalytic hydrogen production performance of 221.18 pmol·g 1 h 1,and nearly one order magnitude higher than that of In2S3(P-In2S3).Furthermore,employing self-developed in situ X-ray photoelectron spectroscopy(SI-XPS)combined with density functional theory(DFT)calculations confirmed that sulfur defects induce the exposure of highly reducible low-valence state In(In(3-x)+),thereby enhancing the adsorption and activation capability of In sites towards H2O.Consequently,sulfur-defective In2S3 exhibits significantly enhanced photocatalytic hydrogen evolution activity.Additionally,the proton reduction of H2O molecules to OH has been visualized during the water splitting hydrogen production process under illumination conditions.This work provides new insights into defect-engineered photocatalyst design and the mechanism of photocatalytic water splitting reaction processes.