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However, achieving high efficiency remains challenging due to insufficient control over intermediate adsorption and reaction pathways. In this work, we reveal that the coordination number (CN) of Cu inversely regulates the adsorption strength of *CO and *NO, while C\u2500N coupling activity follows a volcano\u2010type relationship with CN. Alloying Cu with intrinsically inert Ga atoms lowers the CN of Cu, upshifts\n                    <jats:italic>d<\/jats:italic>\n                    \u2010band center, and finely tunes intermediate adsorption, thereby facilitating the formation of the key *ONCO. The optimized Cu\n                    <jats:sub>0.875<\/jats:sub>\n                    Ga\n                    <jats:sub>0.115<\/jats:sub>\n                    catalyst, with a moderate CN of 9.3 situated between its counterparts (6.0 and 12.0), balances adsorption and coupling activity, delivering a desirable urea yield rate of 575.6\u00a0mmol h\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u00a0g\n                    <jats:sup>\u22121<\/jats:sup>\n                    and a Faradaic efficiency of 30.4% at \u22121.4\u00a0V versus RHE. This work underscores coordination engineering as an effective strategy for guiding efficient C\u2500N coupling toward urea synthesis.\n                  <\/jats:p>","DOI":"10.1002\/anie.6998509","type":"journal-article","created":{"date-parts":[[2026,3,31]],"date-time":"2026-03-31T06:01:42Z","timestamp":1774936902000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["Moderate Intermediate Adsorption Boosts Electrocatalytic C\u2500N Coupling via Coordination Engineering"],"prefix":"10.1002","volume":"65","author":[{"given":"Kefan","family":"Zhang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Chemo and Biosensing College of Chemistry and Chemical Engineering International Joint Lab of Energy Electrochemistry of the Ministry of Education Hunan University  Changsha 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State Key Laboratory of Space Power\u2010Sources School of Chemistry and Chemical Engineering Harbin Institute of Technology  Harbin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mingming","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemo and Biosensing College of Chemistry and Chemical Engineering International Joint Lab of Energy Electrochemistry of the Ministry of Education Hunan University  Changsha China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0964-1037","authenticated-orcid":false,"given":"Chade","family":"Lv","sequence":"additional","affiliation":[{"name":"MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage State Key Laboratory of Space Power\u2010Sources School of Chemistry and Chemical Engineering Harbin Institute of Technology  Harbin 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