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作 者:Wenjie Xue Hongxia Liu Xinqing Chen Xiaoju Yang Ruoou Yang Youwen Liu Minghao Li Xuan Yang Bao Yu Xia Bo You
机构地区:[1]Key Laboratory of Material Chemistry for Energy Conversion and Storage,Ministry of Education,Hubei Key Laboratory of Material Chemistry and Service Failure,School of Chemistry and Chemical Engineering,Huazhong University of Science and Technology,Wuhan 430074,China [2]School of Chemistry and Chemical Engineering,Wuhan Textile University,Wuhan 430200,China [3]Shanghai Advanced Research Institute,Chinese Academy of Sciences,Shanghai 201210,China [4]State Key Laboratory of Materials Processing and Die&Mold Technology,and School of Materials Science and Engineering Huazhong University of Science and Technology,Wuhan 430074,China
出 处:《Science China Chemistry》2023年第6期1834-1843,共10页中国科学(化学英文版)
基 金:financially supported by The National Key Research and Development Program of China(2021YFA1600800);the Start-up Funding of the Huazhong University of Science and Technology(HUST);the Program for HUST Academic Frontier Youth Team;the National Natural Science Foundation of China(22075092);the National 1000 Young Talents Program of China and The Innovation and Talent Recruitment Base of New Energy Chemistry and Device(B21003)。
摘 要:Cu-based electrocatalysts with favorable facets and Cu^(+)can boost CO_(2) reduction to valuable multicarbon products.However,the inevitable Cu^(+)reduction and the phase evolution usually result in poor performance.Herein,we fabricate CuI nanodots with favorable(220)facets and a stable Cu^(+)state,accomplished by operando reconstruction of Cu(OH)_(2) under CO_(2)-and I--containing electrolytes for enhanced CO_(2)-to-C_(2)H_(4) conversion.Synchrotron X-ray absorption spectroscopy(XAS),in-situ Raman spectroscopy and thermodynamic potential analysis reveal the preferred formation of CuI.Vacuum gas electroresponse and density functional theory(DFT)calculations reveal that CO_(2)-related species induce the exposure of the(220)plane of Cu I.Moreover,the small size of nanodots enables the adequate contact with I^(-),which guarantees the rapid formation of Cu I instead of the electroreduction to Cu^(0).As a result,the resulting catalysts exhibit a high C2H4 Faradaic efficiency of 72.4%at a large current density of 800 m A cm^(-2) and robust stability for 12 h in a flow cell.Combined in-situ ATR-SEIRS spectroscopic characterizations and DFT calculations indicate that the(220)facets and stable Cu^(+) in CuI nanodots synergistically facilitate CO_(2)/*CO adsorption and*CO dimerization.
关 键 词:CO_(2)reduction reaction cuprous iodide favorable facets halogen electrolyte RECONSTRUCTION
分 类 号:TQ221.211[化学工程—有机化工] TQ426[环境科学与工程—环境工程] X701
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