A nanoflower-on-nanowire heterogeneous electrocatalyst for enhanced interfacial water activation in nitrate reduction reaction  

作　　者：Jingwen Yu Yunliang Liu Cunhao Fan Naiyun Liu Jingya Yin Yaxi Li Yuanyuan Cheng Xinya Yuan Xinyue Zhang Yixian Liu Sanjun Fan Lei Xu Haitao Li 

机构地区：[1]Institute for Energy Research,School of Chemistry and Chemical Engineering,Jiangsu University,Zhenjiang 212013,China [2]Qingdao Municipal Center for Disease Control and Prevention,Qingdao 266033,China [3]Department of Chemistry and Biochemistry,The Ohio State University,Columbus,Ohio 43210,USA [4]Jiangsu Engineering Technology Research Center of Biomass Composites and Addictive Manufacturing,Institute of Agricultural Facilities and Equipment,Jiangsu Academy of Agricultural Sciences,Nanjing 210014,China [5]Key Laboratory for Protected Agricultural Engineering in the Middle and Lower Reaches of Yangtze River,Ministry of Agriculture and Rural Affairs,Nanjing 210014,China

出　　处：《Nano Research》2025年第2期173-183,共11页纳米研究(英文版)

基　　金：This work was supported by the National Natural Science Foundation of China(Nos.52072152 and 51802126);the Jiangsu University Jinshan Professor Fund,the Jiangsu Specially-Appointed Professor Fund,Open Fund from Guangxi Key Laboratory of Electrochemical Energy Materials,Zhenjiang“Jinshan Talents”Project 2021,China Post Doctoral Science Foundation(No.2022M721372);“Doctor of Entrepreneurship and Innovation”in Jiangsu Province(No.JSSCBS20221197);the Postgraduate Research&Practice Innovation Program of Jiangsu Province(Nos.KYCX22_3645 and KYCX24_3964);Student Research Project of Jiangsu University(Nos.23A586 and 23A804).

摘　　要：Electrocatalytic nitrate reduction reaction(NitRR)is an efficient route for simultaneous wastewater treatment and ammonia production,but the conversion of NO_(3)–to NH_(3) involves multiple electron and proton transfer processes and diverse by-products.Therefore,developing ammonia catalysts with superior catalytic activity and selectivity is an urgent task.The distinctive electronic structure of Cu enhances the adsorption of nitrogen-containing intermediates,but the insufficient activation capability of Cu for interfacial water restricts the generation of reactive hydrogen and inhibits the hydrogenation process.In this work,a Ce-doped CuO catalyst(Ce_(10)/CuO)was synthesized by in situ oxidative etching and annealing.The redox of Ce^(3+)/Ce^(4+)enables the optimization of the electronic structure of the catalyst,and the presence of Ce^(3+)as a defect indicator introduces more oxygen vacancies.The results demonstrate that Ce10/CuO provides an impressive ammonia yield of 3.88±0.14 mmol·cm^(–2)·h^(–1) at 0.4 V vs.reversible hydrogen electrode(RHE)with an increase of 1.04 mmol·cm^(–2)·h^(–1) compared to that of pure CuO,and the Faradaic efficiencies(FE)reaches 93.2%±3.4%.In situ characterization confirms the doping of Ce facilitates the activation and dissociation of interfacial water,which promotes the production of active hydrogen and thus enhances the ammonia production efficiency.

关 键 词：active hydrogen electron transfer NITRATE AMMONIA 

分 类 号：O64[理学—物理化学]