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Here, we demonstrate that an adaptive hybrid ionomer interface steers proton-coupled pathways to achieve highly selective ethanol electrosynthesis. Through surface-limited oxidative reconstruction, the interphase evolves into a robust hydrogen-bonding network paired with an intact cationic sublayer. This architecture limits solvated proton diffusion, effectively suppressing the disruptive Eley\u2013Rideal (ER) pathway toward ethylene. Instead, it dynamically shifts the reaction toward the Langmuir\u2013Hinshelwood (LH) mechanism, optimizing surface-bound *H availability within a fixed mildly alkaline microenvironment (pH \u2248 10.5). Consequently, our membrane electrode assembly achieves &amp;gt;64% ethanol Faradaic efficiency at 200 mA cm\u20132 with &amp;gt;350 h of stability in pH = 1 electrolyte. This elucidates the pivotal role of interfacial hydrogen-bond networks in dictating proton-coupling mechanisms, offering a paradigm for pathway-specific acidic electrosynthesis.<\/jats:p>","DOI":"10.1021\/jacs.6c06774","type":"journal-article","created":{"date-parts":[[2026,7,23]],"date-time":"2026-07-23T09:45:12Z","timestamp":1784799912000},"page":"32053-32064","source":"Crossref","is-referenced-by-count":2,"title":["Hybrid\nHydrogen-Bond Networks Steer Proton-Coupled\nPathway for Acidic CO2-To-Ethanol Electrosynthesis"],"prefix":"10.1021","volume":"148","author":[{"given":"Fuqing","family":"Yu","sequence":"first","affiliation":[{"name":"Huazhong University of Science and Technology , , ,","place":["Wuhan, China, 430074"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiwen","family":"Chen","sequence":"additional","affiliation":[{"name":"Huazhong University of Science and Technology , , ,","place":["Wuhan, China, 430074"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2207-8015","authenticated-orcid":true,"given":"Hongming","family":"Wang","sequence":"additional","affiliation":[{"name":"Nanchang University , , ,","place":["Nanchang, China, 330031"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6408-7796","authenticated-orcid":true,"given":"Fei","family":"Song","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Shanghai, China, 201800"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2054-908X","authenticated-orcid":true,"given":"Bao Yu","family":"Xia","sequence":"additional","affiliation":[{"name":"Huazhong University of Science and Technology , , ,","place":["Wuhan, China, 430074"]},{"name":"Chinese Academy of Sciences , , ,","place":["Dalian, China, 116023"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,23]]},"reference":[{"issue":"9","key":"2026080511132529500_cit1","doi-asserted-by":"publisher","first-page":"763","DOI":"10.1038\/s41929-023-01003-5","article-title":"Cationic-group-functionalized electrocatalysts\nenable stable acidic CO2 electrolysis","volume":"6","author":"Fan","year":"2023","journal-title":"Nat. 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