硼-多元金属-氧复合原子簇的协同产氧催化机制研究

产氧反应是电解型储能技术框架中的重要半反应，但因其动力学极其缓慢，限制了电能向化学能的转换效率。本项目将以申请人在界面电催化，以及复合催化剂微结构调控等方面的研究成果为基础，基于金属-非金属复合协同策略，采用理论与实验相结合的研究方法，开展以下研究内容：构建原子簇催化模型体系，在其表面优化催化反应历程和关键参数，预测不同位点硼原子、氧原子和多元金属间协同作用对催化活性及稳定性的影响规律；可控合成一批配位结构和电子结构可调的基于硼-多元金属-氧原子簇的复合催化剂材料；通过原位谱学研究手段，揭示硼-金属-氧原子簇对活性中心微观电子结构及配位结构的影响规律，结合理论研究结果，建立较为可靠的协同稳定及催化作用机制。基于以上研究成果的实现，开发一批高催化活性、高稳定性、低成本的中性产氧电催化材料，提升基于水氧化的电解水产氢和二氧化碳电还原系统的能量转化效率。

Oxygen evolution reaction is an important half-reaction in the technical framework of electrolysis energy storage, but due to the extremely sluggish kinetics, it limits the conversion efficiency of electric energy to chemical energy. Based on the successful research of interface electrocatalysis, microstructural and coordination modulations in composite catalyst and so on, we will apply the metal and nonmetal synergistic strategy, and adopt the combined theoretical and experimental research methods, to do the research items as follow. Firstly, we will build atomic cluster model of catalytic system, optimize surface catalytic reaction pathway and the key parameters, and predict synergistic effect of boron atom, oxygen atom and multiple metal atoms at different sites on catalytic activity and stability. Secondly, a series of composite catalyst materials based on boron-multimetal-oxygen cluster with rich coordination structures and electronic structures will be designed and controllably synthesized. By in-situ spectroscopy research methods, the modulation effects of boron-multimetal-oxygen cluster on the coordination and electronic structures of active sites will be measured and revealed. Combining with the theoretical research results, we propose to establish a more reliable synergistic stabilization and catalytic mechanism. Based on the above obtained research results, we will explore a batch of highly efficient, highly stable and low cost neutral oxygen-evolution catalysts, and improve the energy conversion efficiency of water splitting and electroreduction of carbon dioxide.