金属离子诱生纳米组装结构双功能电催化材料的设计合成及构效关系

Metal-air batteries, whose advantages include relatively high energy density and very safe operational characteristics, are promising for applications in consumer electronics, electrified transportation, grid storage, and other fields. However, electrically rechargeable metal-air batteries have eluded widespread adoption due mainly to their mediocre power densities and poor cycling stability. To address these issues, a bifunctional oxygen electrocatalyst that can recharge the batteries more efficiently is required. The proposed research program aims to develop advanced bifunctional oxygen electrocatalysts by using nanostructures with novel three-dimensional (3D) hierarchical features. In this research, the relationship between microscopic composition characteristics, catalytic activity and stability will be systematically studied, and the morphology control and catalytic mechanism of the hierarchically nanostructured materials will also be investigated. Firstly, we will develop hierarchically nanostructured bifunctional oxygen electrocatalysts through the induction of different metal ions into the metal organic frameworks, wherein in-situ and ex-situ characterization techniques are used to dynamically study the effect of induced behavior of metallic ions on the morphology and properties of the bifunctional catalyst materials. Secondarily, through the combination of experimental research and theoretical simulation, the relationship between metallic ions and various active components and the nature of synergistic catalytic effect will be explored. By conducting each of these synergistic activities in a continuous feedback loop, lab-scale fundamental scientific knowledge of high-performance hierarchically nanostructured bifunctional oxygen electrocatalysts can be developed, and furthermore translated into device performance and commercial products for practical applications in metal-air batteries.

金属空气电池是极具应用前景的新一代绿色电源，双功能催化剂是可充式金属空气电池实现商业化的关键材料。本项目从可充式金属空气电池双功能催化剂面临的关键科学问题出发，基于金属离子诱生方法，在非煅烧MOFs衍生条件下设计合成形貌新颖的纳米组装结构材料，系统研究其微观组成特征与催化活性及稳定性的关系，明确纳米组装结构材料的形貌调控和催化性能机理。首先利用介入金属离子对MOFs的刻蚀和诱生作用，系统研究构筑纳米组装结构双功能催化材料的合成条件及影响因素，利用原位等现代表征技术，动态分析金属离子的诱生行为对材料形貌结构和双功能催化性能的影响规律；然后结合理论模拟，揭示金属离子与各活性组分间的作用关系和协同催化效应本质；最后明确非煅烧条件衍生合成纳米组装结构材料的微观调控机制，认识组成及形貌对纳米组装结构催化剂性能的影响本质，从而为创新金属空气电池双功能催化剂的合成方法及优化其催化性能提供科学依据。

本项目围绕可充式金属空气电池双功能催化剂面临的关键科学问题，基于金属离子诱生方法，系统研究了双功能催化剂的形貌调控和催化性能机理，取得了系列创新性成果：（1）利用介入金属离子对MOFs的刻蚀和诱生作用，创新了非煅烧制备纳米组装三维结构材料的合成方法；（2）揭示了金属离子与各活性组分间的作用关系和协同催化效应本质，为催化材料的优化设计提供了理论参考；（3）动态考察了金属离子的诱生行为对材料形貌结构和双功能催化性能的影响规律，为金属空气电池的应用研究提供科学借鉴。以第一或通讯作者在Angew. Chem. Int. Ed.、Adv Mater，Adv Energy Mater，Nano Energy等重要学术期刊发表SCI收录论文19篇（9篇为1区），研究成果受邀在Wiley等国际学术网站进行宣传。此外，项目组成员获授权国家发明专利1项，申报国家发明专利7项，参加国际和国内学术会议12个，作会议报告9次。