高效铜催化剂在一氧化氮电还原产氨中的应用  

Highly Efficient Cu-based Electrocatalysts Convert Nitric Oxide to Ammonia

作　　者：赵斯文 朱晨远 常明伟 华炎波 张黎明 ZHAO Siwen;ZHU Chenyuan;CHANG Mingwei;HUA Yanbo;ZHANG Liming(Department of Chemistry,Fudan University,Shanghai 200438,China)

机构地区：[1]复旦大学化学系,上海200438

出　　处：《复旦学报（自然科学版）》2023年第6期741-746,I0001,共7页Journal of Fudan University：Natural Science

基　　金：上海市科委创新行动计划基础类项目(18JC1411700)。

摘　　要：利用可再生能源如太阳能、海洋能等驱动产生的电能将大气污染物一氧化氮(NO)转化为具有经济价值的氨(NH _(3))有重要意义。一方面可以缓解氮氧化物过度累积所引发的氮循环失衡问题,另一方面其是一种高效生产氨的理想手段,具有广泛的应用前景。然而,目前,电化学NO还原(NOR)仍存在诸多挑战,高效产氨催化剂有待进一步发展,且对反应机理的认识不足。基于此,我们首先建立了电化学NOR的基准研究范式,以非贵金属铜为催化剂,实现了高选择性的产氨,其法拉第效率达到84.7%,并结合原位电化学红外光谱实验追踪了反应过程中间体,加深对反应机制的理解,为催化剂的理性设计提供指导。To convert one of pollutant gas—Nitric Oxide(NO)into value-added chemical products via electricity generated by reversible energy such as solar and ocean energy has great significance and application prospects,which can not only balance the disturbed nitrogen-cycle and ameliorate environmental problems including acid rain,greenhouse effect,but serve as an effective way to produce NH _(3).However,NO Electroreduction(NOR)suffers from low Faradaic Efficiency(FE)and poor mechanistic understanding.Here,we report a protocol for establishing a reaction system by excluding the influence of oxygen.We engaged non-noble metal copper as an electrocatalyst,on which the selectivity towards NH_(3) reaches to 84.7%.Combining with in-situ electrochemical infrared spectroscopy,we observed the absorption of NO on the surface of Cu at 1522 cm^(-1) and the major product NH_(3) at 1628 cm^(-1).In summary,our work establishes a paradigm to design NO electroreduction experiment and guides the rational design of NO reduction electrocatalysts by providing deep insights to understand the reaction mechanism.

关 键 词：NO电还原 铜催化剂 原位红外光谱测试 

分 类 号：O643[理学—物理化学]