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However, the current state of this technology is hindered by low selectivity and productivity, primarily due to a limited understanding of the atomic\u2010level active sites involved in ethanol formation. Herein, we identify that the interfacial oxygen vacancy\u2010neighboring Cu (O\n                    <jats:sub>v<\/jats:sub>\n                    \u2010Cu) pair sites are the active sites for CO\n                    <jats:sub>2<\/jats:sub>\n                    electroreduction to ethanol. A linear correlation between the density of O\n                    <jats:sub>v<\/jats:sub>\n                    \u2010Cu pair sites and ethanol productivity is experimentally evidenced. Moreover, a high Faradaic efficiency of 48.5\u2009% and a partial current density of 344.0\u2005mA\u2009cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    for ethanol production are achieved over the inverse CeO\n                    <jats:sub>2<\/jats:sub>\n                    \/Cu catalyst with a high density of O\n                    <jats:sub>v<\/jats:sub>\n                    \u2010Cu pair sites in acid. Mechanistic studies that combine density functional theory calculations and spectroscopic techniques propose an O\n                    <jats:sub>v<\/jats:sub>\n                    \u2010involved mechanism where interfacial O\n                    <jats:sub>v<\/jats:sub>\n                    sites directly activate and dissociate CO\n                    <jats:sub>2<\/jats:sub>\n                    into *CO in a thermodynamically spontaneous manner, thus favoring the subsequent *CHO formation and asymmetric CHO\u2010CO coupling. Besides, the asymmetric O\n                    <jats:sub>v<\/jats:sub>\n                    \u2010Cu pair sites could preferentially stabilize the *CH\n                    <jats:sub>2<\/jats:sub>\n                    CHOH intermediate, resulting in the favorable formation of ethanol over ethylene. Our findings provide new atomic\u2010level insights into CO\n                    <jats:sub>2<\/jats:sub>\n                    electroreduction to ethanol, paving the way for the rational design of future catalysts.\n                  <\/jats:p>","DOI":"10.1002\/anie.202424248","type":"journal-article","created":{"date-parts":[[2025,1,9]],"date-time":"2025-01-09T22:29:55Z","timestamp":1736461795000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":69,"title":["Interfacial Oxygen Vacancy\u2010Copper Pair Sites on Inverse CeO\n                    <sub>2<\/sub>\n                    \/Cu Catalyst Enable Efficient CO\n                    <sub>2<\/sub>\n                    Electroreduction to Ethanol in Acid"],"prefix":"10.1002","volume":"64","author":[{"given":"Yan","family":"Qiao","sequence":"first","affiliation":[{"name":"College of Materials Science and Engineering Hunan University  Changsha Hunan 410082 P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yangfan","family":"Lu","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering State Key Laboratory of Silicon and Advanced Semiconductor Materials Zhejiang University  Hangzhou Zhejiang 310027 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiong","family":"Li","sequence":"additional","affiliation":[{"name":"Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Chinese Academy of Sciences  Shanghai 201210 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jingjie","family":"Ge","sequence":"additional","affiliation":[{"name":"Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic University  Kowloon, Hong Kong 999077 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hsien\u2010Yi","family":"Hsu","sequence":"additional","affiliation":[{"name":"School of Energy and Environment Department of Materials Science and Engineering Centre for Functional Photonics (CFP) City University of Hong Kong  Kowloon, Hong Kong 999077 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yaqiong","family":"Su","sequence":"additional","affiliation":[{"name":"School of Chemistry Engineering Research Center of Energy Storage Materials and Devices of Ministry of Education National Innovation Platform (Center) for Industry-Education Integration of Energy Storage Technology Xi'an Jiaotong University  Xian Shanxi 710049 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Minhua","family":"Shao","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biological Engineering The Hong Kong University of Science and Technology  Kowloon, Hong Kong 999077 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zheng","family":"Hu","sequence":"additional","affiliation":[{"name":"Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Laboratory for Nanotechnology School of Chemistry and Chemical Engineering Nanjing University  Nanjing Jiangsu 210023 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3967-6182","authenticated-orcid":false,"given":"Hongwen","family":"Huang","sequence":"additional","affiliation":[{"name":"College of Materials Science and Engineering Hunan University  Changsha Hunan 410082 P. R. 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