光催化技术在能源环境领域具有重大应用前景，但其过程复杂性使得阐明催化机理和调控活性面临诸多挑战。本项目拟选取Pt/TiO2、Pd/TiO2、Ni/TiO2、1T-MoS2/TiO2、2H-MoS2/TiO2五种结构迥异的代表性界面复合结构模型，借助从头算分子动力学、杂化泛函计算、微观动力学等理论方法，以光催化析氢反应（HER）为研究示例，（1）系统性考查复合催化剂多种几何/电子结构参数对于光催化HER各基元过程（光吸收、光电荷输运、表面催化析氢）的贡献权重，阐明影响光催化性能的关键物性参数和内在规律；（2）继而探究金属合金化、离子掺杂、构建空缺位、表面配体吸附等化学改性方法对关键物性参数的调变作用；（3）针对Ni/TiO2、MoS2/TiO2等廉价材料开展以关键物性参数为导向的光催化HER活性调控研究，提出优化的改性/调控方法组合策略，为高效光催化析氢催化剂的开发提供理论依据和方向。

Photocatalysis shows great potential applications in the fields of energy and environment. However, because of the complicated process, it remains challenging to clarify the catalytic nature and tailor the activity of photocatalytic reactions. In this project, we select five distinct composite structures (Pt/TiO2, Pd/TiO2, Ni/TiO2, 1T-MoS2/TiO2, 2H-MoS2/TiO2) as the representative models, take the photocatalytic hydrogen evolution reaction (HER) as the study case, and by resorting to various of theoretical methods such as the ab initio molecular dynamics, the hybrid functional calculations, and the microkinetic modeling, we focus on the following research contents: i) systematically examining the contribution weight of numbers of geometric/electronic parameters of composite catalysts on each elementary process in photocatalytic HER (the light absorption, photoelectric charge transport, surface catalytic hydrogen production), and illuminating the key physical parameters and inherent laws affecting the photocatalytic performance; ii) subsequently investigating the modulation effect of many chemical modification methods (such as the metal alloying, ion doping, construction of vacancy sites, surface ligand adsorption etc.) on the key parameters; iii) regulating the photocatalytic HER activity of cheap materials (e.g. Ni/TiO2、MoS2/TiO2) as guided by those key parameters, and attempting to propose optimized strategies (or combinations) of modification/regulation methods, and to provide theoretical support and direction for the development of highly efficient catalysts for photocatalytic hydrogen production.