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However, the kinetics mismatching between CO\n 2<\/jats:sub>\n reduction and NO\n 3<\/jats:sub>\n \u2212<\/jats:sup>\n reduction, as well as the difficulty of C\u2500N coupling, are major challenges in urea electrosynthesis. Herein, we first calculated the free energy of *CO, *OCNO, and *NOH formation over defect\u2010rich Fe\n 2<\/jats:sub>\n O\n 3<\/jats:sub>\n catalysts with different metal dopants, which showed that Zn dopant was a promising candidate. Based on the theoretical study, we developed Zn\u2010doped defect\u2010rich Fe\n 2<\/jats:sub>\n O\n 3<\/jats:sub>\n catalysts (Zn\u2013Fe\n 2<\/jats:sub>\n O\n 3<\/jats:sub>\n \/O\n V<\/jats:sub>\n ) containing asymmetric Zn\u2013O\n V<\/jats:sub>\n \u2013Fe sites. It exhibited an outstanding urea faradaic efficiency of 62.4% and the remarkable recycling stability. The production rate of urea was as high as 7.48\u00a0mg h\n \u22121<\/jats:sup>\n mg\n cat<\/jats:sub>\n \u22121<\/jats:sup>\n , which is higher than most of the reported works to date. Detailed control experiments and in situ spectroscopy analyses identified *OCNO as a crucial intermediate for C\u2500N coupling. The Zn\u2013Fe\n 2<\/jats:sub>\n O\n 3<\/jats:sub>\n \/O\n V<\/jats:sub>\n catalyst with asymmetric Zn\u2013O\n V<\/jats:sub>\n \u2013Fe sites showed enhanced *CO coverage and promoted *OCNO formation, leading to high efficiency toward urea production.\n <\/jats:p>","DOI":"10.1002\/anie.202501830","type":"journal-article","created":{"date-parts":[[2025,5,6]],"date-time":"2025-05-06T03:49:45Z","timestamp":1746503385000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":53,"title":["Boosting Urea Electrosynthesis via Asymmetric Oxygen Vacancies in Zn\u2010Doped Fe\n 2<\/sub>\n O\n 3<\/sub>\n Catalysts"],"prefix":"10.1002","volume":"64","author":[{"given":"Xinning","family":"Song","sequence":"first","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences CAS Laboratory of Colloid and Interface and Thermodynamics CAS Research\/Education Center for Excellence in Molecular Sciences Center for Carbon Neutral 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Laboratory of Colloid and Interface and Thermodynamics CAS Research\/Education Center for Excellence in Molecular Sciences Center for Carbon Neutral Chemistry Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China"},{"name":"School of Chemical Sciences University of Chinese Academy of Sciences Beijing 100049 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xing","family":"Tong","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences CAS Laboratory of Colloid and Interface and Thermodynamics CAS Research\/Education Center for Excellence in Molecular Sciences Center for Carbon Neutral Chemistry Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China"},{"name":"School of Chemical Sciences University of Chinese Academy of Sciences Beijing 100049 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ziwei","family":"Zhao","sequence":"additional","affiliation":[{"name":"Beijing 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100190 China"},{"name":"School of Chemical Sciences University of Chinese Academy of Sciences Beijing 100049 China"},{"name":"Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular Engineering East China Normal University Shanghai 200062 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