中性析氢反应中界面水结构调控机制研究

在中性析氢反应过程中，水分子吸附解离过程作为主要限速步骤，其动力学过程受到界面水分子结构的显著影响。在分子层面揭示界面水结构与催化性能之间的关系具有重要的科学意义。目前，由于缺少具有代表性的中性析氢模型催化材料，导致在中性条件下系统地研究界面水结构调控手段以及界面水结构与析氢性能之间的构效关系面临巨大的挑战。本项目拟以具有界面水结构响应能力的钌纳米颗粒作为研究对象，将不同非金属杂原子可控配位在钌纳米颗粒表面，通过表面结构的精细控制，针对性调控表面的物理化学性质（表面功函/表面非共价相互作用/表面电荷）从而进一步诱导调节界面水分子结构，完成结构明确且活性主要受界面水结构影响的模型催化材料制备。在此基础上结合分子动力学模拟、原位表面增强红外、原位同步辐射技术，通过材料合成、理论模拟、原位表征的有机结合对中性析氢反应中界面水调控的物理化学本质进行基础研究，以期为高效电催化剂设计奠定理论基础。

In the neutral hydrogen evolution reaction process, the adsorption and dissociation process of water molecules is the main rate-limiting step, and its kinetic process is significantly affected by the structure of the interface water molecules. It is of great scientific significance to reveal the relationship between interface water structure and catalytic performance at the molecular level. At present, due to the lack of representative neutral hydrogen evolution model catalytic materials, it is a huge challenge to systematically study the interface water structure regulation method and the structure-activity relationship between the interface water structure and hydrogen evolution performance under neutral conditions. In this project, we intend to use ruthenium nanoparticles with interfacial water structure response capability as the research object, and introduce non-metallic elements on the surface of ruthenium nanoparticles. Through the control of the surface structure, the physical and chemical properties of the surface (surface work function/surface non-covalent interaction/surface charge) can be adjusted to change of the molecular structure of the interface water for preparation model catalytic materials. Material synthesis, ab initio molecular dynamics simulation, in-situ surface enhanced infrared characterization, and in-situ x-ray absorption spectroscopy are organically combined for studying the physical and chemical nature of interface water to contribute to the design and application of efficient electrocatalysts.