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Here, the surface roughness of Cu electrodes is introduced for the first time as the determinant to switch products from nitrones to imines owing to the controllable reduction of nitroarenes to hydroxylamines or amines on tailored Cu<jats:sup>I<\/jats:sup>\/Cu<jats:sup>0<\/jats:sup> interfaces. The roughness\u2010dependent selectivity, that is the decrease of nitrones and the increase of imines with enhanced roughness, is visible in the electro\u2010reductive coupling of nitrobenzene and furfural. Thus, the high selectivity of nitrone (98\u2009%) and imine (80\u2009%) can be achieved on a surface smooth Cu foil and the one electrochemically roughened in the presence of I<jats:sup>\u2212<\/jats:sup>, respectively. Such roughness\u2010dependence of nitrone\/imine selectivity on Cu electrodes is further verified in a wide substrate scope, highlighting the promise of surface\/interfacial engineering for electrochemical synthesis.<\/jats:p>","DOI":"10.1002\/cssc.202300180","type":"journal-article","created":{"date-parts":[[2023,3,29]],"date-time":"2023-03-29T09:40:29Z","timestamp":1680082829000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":11,"title":["Roughness\u2010Dependent Electro\u2010Reductive Coupling of Nitrobenzenes and Aldehydes on Copper Electrodes"],"prefix":"10.1002","volume":"16","author":[{"given":"Yinjian","family":"Zheng","sequence":"first","affiliation":[{"name":"College of Chemistry and Materials Science and Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications Jinan University  No. 601, Huangpu Avenue West Guangzhou 510632 P. R. 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