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.
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).
