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Herein, this challenge is addressed through sulfur\u2010induced electronic modulation of Ag\u2010based catalysts, steering the CO\n                    <jats:sub>2<\/jats:sub>\n                    reduction pathway toward ethanol production. By constructing atomically engineered Ag\/Ag\n                    <jats:sub>2<\/jats:sub>\n                    S nanowires (NWs) via a controlled sulfurization strategy, a remarkable Faradaic efficiency (FE) of 75% for ethanol at \u22120.95\u00a0V, along with exceptional stability over 14 h of high\u2010performance metrics surpassing most reported Ag\u2010based systems is achieved. Operando electrochemical surface\u2010enhanced Raman spectroscopy\u00a0(EC\u2010SERS) and density functional theory (DFT) calculations unveil that the Ag\/Ag\n                    <jats:sub>2<\/jats:sub>\n                    S heterointerface synergistically regulates interfacial water networks and stabilizes key\n                    <jats:sup>*<\/jats:sup>\n                    CO intermediates, thereby accelerating CO\n                    <jats:sub>2<\/jats:sub>\n                    activation, proton\u2010coupled electron transfer, and asymmetric C\u2010C coupling. Furthermore, sulfurization\u2010induced dual effects\u2010optimized hydrogen\u2010bond interactions and enriched K\u207a confinement are identified as critical drivers for tailoring the local microenvironment to favor ethanol selectivity. This work not only demonstrates a rational atomic interface design for C\n                    <jats:sub>2<\/jats:sub>\n                    product orientation but also deciphers the dynamic interplay between catalyst electronic structure and interfacial species, offering a molecular\u2010level roadmap for advanced CO\n                    <jats:sub>2<\/jats:sub>\n                    conversion systems.\n                  <\/jats:p>","DOI":"10.1002\/adma.202503010","type":"journal-article","created":{"date-parts":[[2025,5,30]],"date-time":"2025-05-30T05:13:21Z","timestamp":1748582001000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":32,"title":["Interfacial Water on Ag\/Ag\n                    <sub>2<\/sub>\n                    S Nanowires Enhancing the Ethanol Selectivity for CO\n                    <sub>2<\/sub>\n                    Electroreduction"],"prefix":"10.1002","volume":"37","author":[{"given":"Can\u2010Jun","family":"Zou","sequence":"first","affiliation":[{"name":"School of Advanced Energy Sun Yat\u2010Sen University (Shenzhen)  Shenzhen 518107 China"},{"name":"School of Chemistry Sun Yat\u2010Sen University  Guangzhou 510275 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zi\u2010Yu","family":"Du","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Physical Chemistry of Solid Surfaces iChEM College of Chemistry and Chemical Engineering College of Energy College of Materials Xiamen University  Xiamen 361005 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wei","family":"Tang","sequence":"additional","affiliation":[{"name":"School of Chemistry Sun Yat\u2010Sen University  Guangzhou 510275 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qiong","family":"Liu","sequence":"additional","affiliation":[{"name":"School of Chemistry Sun Yat\u2010Sen University  Guangzhou 510275 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xing\u2010Biao","family":"Liu","sequence":"additional","affiliation":[{"name":"School of Chemistry Sun Yat\u2010Sen University  Guangzhou 510275 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jin\u2010Chao","family":"Dong","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Physical Chemistry of Solid Surfaces iChEM College of Chemistry and Chemical Engineering College of Energy College of Materials Xiamen University  Xiamen 361005 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ping\u2010Ping","family":"Fang","sequence":"additional","affiliation":[{"name":"School of Advanced Energy Sun Yat\u2010Sen University (Shenzhen)  Shenzhen 518107 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1598-6856","authenticated-orcid":false,"given":"Jian\u2010Feng","family":"Li","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Physical Chemistry of Solid Surfaces iChEM College of Chemistry and Chemical Engineering College of Energy College of Materials Xiamen University  Xiamen 361005 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,5,30]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aav3506"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.9b02945"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41893-021-00739-x"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.3c04143"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202313646"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1007\/s11426-022-1460-7"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1002\/adsu.202100256"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.1802256115"},{"key":"e_1_2_7_9_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41560-024-01633-4"},{"key":"e_1_2_7_10_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.3c12321"},{"key":"e_1_2_7_11_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.3c05880"},{"key":"e_1_2_7_12_1","volume":"62","author":"Liu Z.","year":"2023","journal-title":"Angew. 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