萤石型铱-基电催化剂的形貌与电子工程及酸性水氧化性能研究

基于可再生能源电力的质子交换膜电解水被认为是最具发展前景的零碳排放制氢技术，然而阳极析氧反应(OER)贵金属催化剂成本过高、稳定性欠佳，严重阻碍了该技术的商业化进程。因此，开发新型高性能、低成本的电催化剂至关重要。迄今为止，萤石型铱-基纳米材料用于电催化OER还鲜有报道，本项目拟通过“多尺度结构工程”和“电子结构优化”协同策略构筑新型的过渡金属掺杂的萤石型铱-基中空纳米催化剂。通过对催化剂的理性设计、可控制备及性能研究，探索组成、几何形貌、掺杂等对催化性能的影响规律；结合先进表征技术与理论模拟计算研究催化剂表面物种演化，揭示真实活性位点和活性起源，阐明OER稳定性机制，进而建立催化剂结构与性能的构-效关系。本项目将开发一个高性能、低成本酸性介质电催化OER新体系，丰富和发展高稳定性OER催化剂的基础理论和精准构筑策略，具有重要的理论意义和实际应用前景。

Proton exchange membrane water electrolysis based on renewable energy is considered as the most promising hydrogen production technology without CO2 emission. However, the high cost and poor stability of the noble metal electrocatalysts for the anodic oxygen evolution reaction (OER) has severely limited the commercialization of proton exchange membrane water electrolysis technology. Therefore, it is critically important to develop the high-performance and low-cost electrocatalysts for the OER. To the best of our knowledge, there are few reports on the fluorite-type iridium-based nanomaterials employed as the electrocatalysts to catalyze the OER in acidic media by far. In this project, the novel transition metal-doped fluorite-type iridium-based nano-catalysts with hollow structure are constructed through the synergistic strategy of “multi-scale structural engineering” and “electronic structure optimization”. The effect of components, geometric structure and doping on the catalytic performance will be explored by rational design and controllable synthesis of the catalysts, as well as the study of catalytic performance. Combining the advanced characterizations with theoretical calculations, the evolution of surface species during the OER process will be deeply investigated, and the real active sites, the origin of activities as well as the stability mechanisms will be intrinsically revealed. Finally, the relationship between structure and catalytic performance will be established. The purpose of this project is to develop a new electrocatalytic system featured with high efficiency as well as low cost by the morphology and electronic engineering. This project will enrich the basic theory and precise construction strategies for the durable OER electrocatalysts in acidic electrolytes, which has important theoretical significance and practical application prospect.