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In this work, we propose a strategy to boost efficient and durable urea synthesis by coupling the electrochemical and chemical steps. Utilizing fullerene (C\n                    <jats:sub>60<\/jats:sub>\n                    ) as a redox\u2010active electron mediator during the electrochemical reduction process, we effectively inhibit the irreversible reduction deactivation of positively charged copper (Cu\n                    <jats:sup>\u03b4+<\/jats:sup>\n                    ) active sites. The electron\u2010accepting fullerene form ions (C\n                    <jats:sub>60<\/jats:sub>\n                    <jats:sup>n\u2013<\/jats:sup>\n                    ) that engage in a spontaneous chemical redox reaction with nitrate ions, producing nitrite ions and regenerating neutral C\n                    <jats:sub>60<\/jats:sub>\n                    (C\n                    <jats:sub>60<\/jats:sub>\n                    <jats:sup>n\u2013<\/jats:sup>\n                    + NO\n                    <jats:sub>3<\/jats:sub>\n                    <jats:sup>\u2013<\/jats:sup>\n                    \u2192 C\n                    <jats:sub>60<\/jats:sub>\n                    \u00a0+\u00a0NO\n                    <jats:sub>2<\/jats:sub>\n                    <jats:sup>\u2013<\/jats:sup>\n                    ). This recycling mechanism closes the electron transfer loop while optimizing the overall reaction pathway. The urea yield rate is dramatically increased to 385.9\u00a0mmol h\n                    <jats:sup>\u22121<\/jats:sup>\n                    g\n                    <jats:sup>\u22121<\/jats:sup>\n                    , accompanied by long\u2010term durability. Our findings provide a valuable framework for designing highly efficient electrocatalyst for coupling reactions, advancing the field of sustainable urea synthesis.\n                  <\/jats:p>","DOI":"10.1002\/anie.202517450","type":"journal-article","created":{"date-parts":[[2025,10,21]],"date-time":"2025-10-21T04:30:07Z","timestamp":1761021007000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":11,"title":["Closing Electron Transfer Loop to Boost Electrocatalytic Urea Synthesis"],"prefix":"10.1002","volume":"64","author":[{"given":"Ruping","family":"Miao","sequence":"first","affiliation":[{"name":"State Key Laboratory of Chemo and Biosensing College of Chemistry and Chemical Engineering Advanced Catalytic Engineering Research Center of the Ministry of Education Hunan University  Changsha 410082 P.R. 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