基于非贵金属的多酸-配合物双金属催化剂的设计、合成及其电解水析氧催化性能研究

The crisis of energy and pollution are fatal problems for the world. The oxidative half reaction is a bottleneck restricting hydrogen production from electrolyzed water because of its high overpotential. The synthesis of efficient, inexpensive, and stable electrolytic water oxygen evolution catalysts has become the key to breaking through this bottleneck. In order to solve the key problems of poor stability, low efficiency, difficult recovery, and expensive noble metal based polyoxometalate catalysts, the project will use the nano-size and easy-modification structural characteristics of polyoxometalates to synthesize polyoxometalate-coordination complex bimetallic hybrid material. We will study its catalytic performance in oxygen evolution. The emphasis will be placed on the influence of the assembly mode of polyoxometalates-coordination complex on the stability of the catalyst. The synergistic effect of the combination of polyoxometalates-coordination complex on the catalytic efficiency of the catalysts will be clarified. The catalytic mechanism of the catalysts in the process of electrolysis of oxygen will be illustrated. We will also summarize the law that can enhance the stability and catalytic efficiency of the polyoxometalates-coordination complex catalysts. The development of inexpensive, efficient and stable electrolytic water oxygen evolution catalysts with independent intellectual property will promote the practical application of electrocatalytic decomposition of water.

能源和环境危机是当今世界共同面对的重要难题，电解水制氢气被认为是解决该难题的重要方法之一，但水氧化半反应因其电势过高而成为制约电解水制氢的瓶颈。合成高效、廉价、稳定的电解水析氧催化剂成为突破该瓶颈的关键。为了解决多酸电解水析氧催化剂稳定性差、效率低、回收难，以及基于贵金属的多酸催化剂价格昂贵的关键问题，本项目拟利用多酸的纳米尺寸以及易修饰的结构特点，合成基于非贵金属的多酸-配合物双金属固体催化剂，研究其电解水析氧催化性能。重点探索多酸与配合物的组装方式对提高催化剂稳定性的影响，多酸与配合物组装后产生的协同作用对提高催化剂的催化效率的影响，阐明催化剂在电解水析氧过程中的催化机理，总结可增强多酸-配合物催化剂的稳定性和催化效率的规律。开发具有自主知识产权的廉价、高效、稳定的电解水析氧催化剂。本项目的研究结果将多酸材料在电解水制氢领域的应用提供坚实的理论和实验依据，推动电催化分解水的实际应用。

采用水热法合成了20种无机有机杂化化合物。通过单晶X射线衍射、元素分析、粉末X射线衍射、红外光谱和热重分析对其结构进行了表征。研究了它们的循环伏安行为和电催化性能。探讨了化合物对有机染料污染物的去除行为。此外，还研究了抗菌/抗真菌活性，光致发光性能和电催化析氧反应（OER）性能。