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Here, we resolve this dilemma by establishing interfacial water orientation that directly couples H\n                    <jats:sub>2<\/jats:sub>\n                    O polarization with reaction pathway bifurcation. Using electrocatalytic CO\n                    <jats:sub>2<\/jats:sub>\n                    reduction as a typical platform, we demonstrate that precisely engineered H\u2010down water alignment, achieved via adaptive subsurface tuning (AST) strategy of Ga\u2010doped Cu catalysts, dynamically regulates proton transfer directionality and intermediate stabilization. The optimized Ga\/Cu catalyst achieved a Faradaic efficiency (FE) of 68.8% for ethylene at 800\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , surpassing ethanol production by 8.2\u2010fold, and the current density was among the highest reported for catalysts with high ethylene FE. Detailed experimental studies and theoretical calculations corroborate that H\u2010down alignment enhanced *H availability, directing protons to selectively cleave the C\u2500O bond of *CHCOH intermediates over hydrogenation pathways, yielding high ethylene FE and current density. These findings establish interfacial water orientation as a pivotal descriptor for steering C\u2500C coupling selectivity in electrocatalysis, offering a rational design principle for efficient electroreduction systems.\n                  <\/jats:p>","DOI":"10.1002\/anie.202520546","type":"journal-article","created":{"date-parts":[[2026,2,5]],"date-time":"2026-02-05T06:11:28Z","timestamp":1770271888000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":23,"title":["Steering Ethylene Electrosynthesis by Controlling Interfacial Water Orientation"],"prefix":"10.1002","volume":"65","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 Chemistry Institute of Chemistry, Chinese Academy of Sciences  Beijing China"},{"name":"School of Chemical Sciences University of Chinese Academy of Sciences  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Libing","family":"Zhang","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 China"},{"name":"School of Chemical Sciences University of Chinese Academy of Sciences  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaodong","family":"Ma","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, 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Chemistry Institute of Chemistry, Chinese Academy of Sciences  Beijing China"},{"name":"School of Chemical Sciences University of Chinese Academy of Sciences  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Weixiang","family":"Li","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 China"},{"name":"School of Chemical Sciences University of Chinese Academy of Sciences  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chaofeng","family":"Zheng","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 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