高效水相电催化制氢硫族化物-金属复合纳米结构的合成、组装与机理研究

Hydrogen evolution reaction (HER), as a kind of important means to develop clean and efficient energy, has broad application prospects. It is crucial to design, synthesize and assemble high-efficiency catalysts for HER applications. Metal chalcogenide with HER activity, has become research hotspot, due to its lower price relative to noble metal; however, it still remains challenging to further improve the structural selectivity and catalytic activity. This research project will be focused on the nanostructures of noble metals (including Pt, Pd, Rh, Ru and their alloys, with high HER activities), metal chalcogenides (namely MX2 or AaMXb）and their hybrid nanostructures, mainly based on synthetic methodology for nanomaterials. We will tailor the chemical compositions, sizes, surface facets and active sites of the nanocatalysts via material design, synthesis, doping and assembly, and implement them to study and optimize their catalytic activity, stability and selectivity in HER. It enables to further understand the key construction factors, evolutionary mechanism, catalytic mechanism and structure-activity relationship of the nanocatalysts in HER system, through a series of experimental characterizations and theoretical simulations. We aim to develop several kinds of high-performance and low-cost catalysts for HER, and sort out some key parameters to the synthetic design, structural assembly and performance optimization of HER nanocatalysts, contributing to China's energy development and environmental protection.

氢析出反应（HER）作为清洁高效能源的一种重要开发手段，具有广阔的应用前景。设计、制备与组装高效的HER催化剂至为关键。金属硫族化物具有一定的HER活性且比贵金属便宜，开始成为研究热点，然而其结构选择性和催化活性尚需调控和优化。本项目将基于纳米材料的合成方法学，以HER性能优良的Pt、Pd、Rh、Ru等贵金属及其合金纳米结构、MX2或AaMXb金属硫族化物及其复合纳米材料为研究重点。通过对可控合成、元素掺杂和负载组装过程的调控，获得不同化学组成、形貌结构、厚度尺寸、表面晶面、位点分布的纳米结构，将它们应用于电催化HER，考察并优化其催化HER的活性、稳定性及选择性等。通过一系列的实验调控表征和理论计算模拟，阐释纳米材料的演化机制、构建关键、催化机制和构效关系，开发出几种高性能低成本的HER催化剂，总结出催化剂的合成设计、复合构建及性能优化的关键参数，为中国能源开发和环境保护做出贡献。

燃料电池技术是解决能源和环境问题的重要手段，制约其应用的瓶颈是催化剂的开发。本项目聚焦金属及其合金、过渡金属硫族化合物（包括含硫金属纳米团簇）、非金属元素掺杂金属基-材料等纳米结构及其复合纳米结构，并将其应用于氢析出（HER）等相关化催化反应体系（如氧还原ORR、氧析出OER和甲酸氧化FAO等）及相关性能研究，取得了较好的研究成果和发现。本项目着力对可控合成、元素掺杂和负载组装过程的合理设计和精细调控，开展催化剂化学组成、形貌结构、厚度尺寸、表界面、活性位点、电子结构、吸附脱附等研究，阐释纳米结构的演化进程、构建关键、构效关系乃至反应机制，开发出多种低成本高性能催化剂，获得了一些有用经验，有望为合理设计理想纳米结构和多种特定功能应用提供新的启示。