Promoting nitric oxide electroreduction to ammonia over electron-rich Cu modulated by Ru doping

作     者：Jiangwei Shi Changhong Wang Rong Yang Fanpeng Chen Nannan Meng Yifu Yu Bin Zhang Jiangwei Shi;Changhong Wang;Rong Yang;Fanpeng Chen;Nannan Meng;Yifu Yu;Bin Zhang

作者机构：Department of Catalysis Science and EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China Institute of Molecular PlusSchool of ScienceTianjin UniversityTianjin300072China 

出 版 物：《Science China Chemistry》 (中国科学（化学英文版）)

年 卷 期：2021年第64卷第9期

页      面：1493-1497页

核心收录：

学科分类：083002[工学-环境工程] 0830[工学-环境科学与工程（可授工学、理学、农学学位）] 081702[工学-化学工艺] 08[工学] 0817[工学-化学工程与技术] 0805[工学-材料科学与工程（可授工学、理学学位）] 080502[工学-材料学] 0703[理学-化学] 

基　　金：financially supported by the National Natural Science Foundation of China(22071173) the Natural Science Foundation of Tianjin City(20JCJQJC00050,17JCJQJC44700)。 

主　　题：Electrocatalysis NO ammonia synthesis in situ characterizations Ru-doped Cu 

摘      要：Electrocatalytic nitric oxide(NO)reduction is a promising strategy to produce ammonia.Developing a facile approach to synthesize efficient catalysts with enhanced NO electroreduction performance is highly desirable.Here,a series of Ru-doped Cu materials are constructed through in situ electroreduction of corresponding metal hydroxides.The optimized Ru_(0.05)Cu_(0.95)exhibits superior electrocatalytic performance for ammonia synthesis by using NO/Ar(1/4,n/n)as the feedstocks(Faradaic efficiency:64.9%,yield rate:17.68μmol cm^(-2)h^(-1)),obviously outperforming Cu counterpart(Faradaic efficiency:33.0%,yield rate:5.73μmol cm^(-2)h^(-1)).Electrochemical in situ Fourier transform infrared(FTIR)spectroscopy and online differential electrochemical mass spectrometry(DEMS)are adopted to detect intermediates and unveil the possible reaction pathway.The downshift of the Cu d-band center induced by Ru doping facilitates the rate-limiting hydrogenation step and decreases the desorption energy of NH_(3),leading to high Faradaic efficiency and yield of ammonia.