过渡或主族金属硒化物/ZnIn2S4直接或双直接Z型二维异质结可见光解水产氢催化剂的设计与构建及其性能和机理研究

直接Z型光催化剂既可实现光生载流子的有效分离，又可保持光生电子的高还原活性，是一种非常有前途的产氢光催化剂。然而，要成功构建Z型光催化剂就需解决两大关键问题：如何选择材料体系以使材料间的能级相匹配；如何构建不同材料间的良好界面接触以保证载流子的高效分离。本项目针对上述问题，分别选用具有二维结构的过渡（Mo/W）或主族（In/Sn）两类金属硒化物与富缺陷ZnIn2S4复合，构建出系列直接或双直接Z型二维异质结可见光解水产氢催化剂，并揭示这类光催化剂的构建规律。主要研究内容：1）构建富缺陷ZnIn2S4及系列过渡（Mo/W）或主族（In/Sn）金属硒化物/ZnIn2S4二维异质结可见光催化剂，并揭示其生长机理；2）系统研究所构建的系列直接或双直接Z型二维异质结可见光催化剂的本征电子结构、能级匹配及光生载流子的迁移及复合动力学，揭示催化剂产氢性能的提升机理，并阐明其构建与产氢性能之间的构效关系。

Direct Z-scheme photocatalyst can not only achieve the efficient separation of the photocarriers, but also retain the prominent reduction activity of the photogenerated electrons, which has been considered as a promising photocatalyst for hydrogen evolution. However, how to select material system to obtain the energy level matching between materials, and how to build a fine interface contact among the different materials to ensure the efficient separation of the carriers, these two pivotal problems need to be solved to construct the Z-scheme photocatalyst successfully. Aiming at the above mentioned key issues, two-dimensional transition (Mo/W) or main-group (In/Sn) metal selenides and defect-rich ZnIn2S4 were selected to construct a series of the direct or dual direct Z-scheme two-dimensional heterojunction visible-light water-splitting photocatalyst for hydrogen production, and the basic constructing laws for such photocatalysts were revealed. Main research contents are as follows: 1)The defect-rich ZnIn2S4 and series transition (Mo/W) or main-group (In/Sn) metal selenides/ZnIn2S4 two-dimensional heterojunction visible photocatalysts are synthesized, and their growth mechanisms are disclosed; 2) The intrinsic electronic structure, energy level matching, photocarriers migration and recombination dynamics of the fabricated direct or dual direct Z-scheme two-dimensional heterojunction visible photocatalysts are systematically studied. The mechanisms of the enhancing hydrogen production performance for the photocatalysts are unveiled, and elucidating the structure-activity relationship between the constructed the visible-light photocatalyst and the hydrogen production performance.