非贵金属氮化物/氧化物异质结构在碱性氢氧化反应中的应用研究

阴离子交换膜燃料电池（AEMFC）可以通过氢气和氧气反应直接将化学能转换成电能，是很有潜力的氢能利用技术。然而，其阳极的氢氧化反应（HOR）在碱性条件下进行缓慢，是其商业化应用的技术瓶颈。因此，设计制备高效、价格低廉的碱性HOR催化剂至关重要。传统的非贵金属催化剂HOR活性普遍较低，因其难以对反应中间体H*和OH*实现同时吸附。前期研究发现，异质结构催化剂界面处可以同时优化中间体的吸附过程，提升催化活性。本项目拟通过对复合金属前驱物进行煅烧和选择性氮化处理，利用不同金属氮化温度特异性，制备出特定的非贵金属氮化物/氧化物异质结构。利用某些氮化物的类Pt性质和异质结构中不同组分对H*和OH*中间体的吸附进行同步优化，提升其催化活性。同时拟利用先进的表征手段，结合密度泛函理论计算，探究异质结构界面组成和电子结构与HOR活性之间的“构-效关系”，为指导设计高效的非贵金属HOR催化剂提供新思路。

Alkaline exchange membrane fuel cells (AEMFC) can directly convert chemical energy into electricity through the reaction of hydrogen and oxygen, which is a promising hydrogen energy utilization technology. However, the sluggish anode hydrogen oxidation reaction (HOR) under alkaline conditions requires a large amount of precious metal catalyst, hindering the commercialization of alkaline exchange membrane fuel cells. Therefore, it is very important to design efficient and inexpensive HOR catalysts under alkaline condition. The traditional platinum group metal (PGM)-free HOR electrocatalysts is generally low in activity because they are difficult to achieve simultaneous adsorption of the reaction intermediates H * and OH *. Recent research found that the heterostructure interface can simultaneously optimize the adsorption process of intermediates and improve the catalytic activity. This project intends to prepare specific non-precious metal nitride/metal oxide heterostructures by calcining and selective nitriding of metal precursors, utilizing the characteristics of different metal ion nitriding temperatures. Utilizing the Pt-like properties of some metal nitrides and different components in the heterostructure, we planed to simultaneously optimize the adsorption of H* and OH* intermediates to improve their catalytic activity. Meanwhile, we planned to use advanced characterization methods, combined with density functional theoretical calculations, to explore the “structure-activity relationship” between heterostructure interface and HOR activity, providing new insight to design other efficient non-precious metal HOR catalysts.