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Achieving highly selective electrochemical CO_(2) reduction to C_(2)H_(4) on cu nanosheets

Journal of Energy Chemistry 2023年第4期79卷 312-320页

作者： Huan Xie Ruikuan Xie Zhiyuan Zhang Yongyu Pang Yuting Luo Jiong Li Bilu Liu Maria-Magdalena Titirici Guoliang Chai State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002FujianChina Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources International Innovation Center for Forest Chemicals and MaterialsCollege of Materials Science and EngineeringNanjing Forestry UniversityNanjing 210037JiangsuChina Shenzhen Geim Graphene Center(SGC) Tsinghua-Berkeley Shenzhen Institute(TBSI)and Tsinghua Shenzhen International Graduate School(TSIGS)Tsinghua UniversityShenzhen 518055GuangdongChina School of Chemical Science University of Chinese Academy of SciencesBeijing 100049China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Chinese Academy of SciencesShanghai 201210China Department of Chemical Engineering Imperial College LondonSW72AZUK

The conversion of CO_(2)into value-added chemicals coupled with the storage of intermittent renewable electricity is *** nanosheets with an average size and thickness of~30 and~20 nm have been developed,which are in situ reduced into cu nanosheets during electrochemical CO_(2)reduction reaction(ECO_(2)RR).The derived cu nanosheets demonstrate much higher selectivity for C2H4production than commercial cuO derived cu powder,with an optimum Faradaic efficiency of 56.2%and a partial current density of C_(2)H_(4)as large as 171.0 mA cm^(-2)in a gas diffusion flow *** operando attenuated total reflectance-Fourier transform infrared spectra measurements and density functional theory simulations illustrate that the high activity and selectivity of cu nanosheets originate from the edge sites on cu nanosheets with a coordinate number around 5(4–6),which facilitates the formation of^(*)CHO rather than^(*)COH intermediate,meanwhile boosting the C-C coupling reaction of^(*)CO and^(*)CHO intermediates,which are the critical steps for C_(2)H_(4)formation.

关键词： Electrochemical CO_(2)reduction cu nanosheets C_(2)H_(4) High selectivity Coordination number

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