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Although extensive research has focused on stabilizing the carbon\u2010related intermediates, limited attention has been paid to investigating the local regulations of H\n                    <jats:sub>2<\/jats:sub>\n                    O molecules at molecular level. Considering the electrocatalytic interface, H\n                    <jats:sub>2<\/jats:sub>\n                    O is critical during CO\n                    <jats:sub>2<\/jats:sub>\n                    RR process, as H\n                    <jats:sub>2<\/jats:sub>\n                    O molecules are directly involved in CO\n                    <jats:sub>2<\/jats:sub>\n                    reduction process or indirectly modify the solid\u2013liquid interfacial structure, thereby impacting the reaction process. In this study, we use a model copper\u2010based catalyst containing palladium and indium dopants that have different hydrogen and oxygen adsorption capabilities to investigate the influence of H\n                    <jats:sub>2<\/jats:sub>\n                    O molecules on CO\n                    <jats:sub>2<\/jats:sub>\n                    electroreduction selectivity. We find, by enhancing the participation of isolated H\n                    <jats:sub>2<\/jats:sub>\n                    O molecules, instead of asymmetric H\u2010bonded H\n                    <jats:sub>2<\/jats:sub>\n                    O or ice\u2010like H\n                    <jats:sub>2<\/jats:sub>\n                    O, in the local electrocatalytic microenvironment during CO\n                    <jats:sub>2<\/jats:sub>\n                    reduction process, that the cathodic products remarkably change from 95% C\n                    <jats:sub>1<\/jats:sub>\n                    FE to 70% C\n                    <jats:sub>2<\/jats:sub>\n                    FE. We unveil, via in situ ATR\u2010SEIRAS measurement, that the H\n                    <jats:sub>2<\/jats:sub>\n                    O microenvironment regulation can promote the formation of key intermediates, thus tuning the CO\n                    <jats:sub>2<\/jats:sub>\n                    reduction pathways.\n                  <\/jats:p>","DOI":"10.1002\/anie.202508801","type":"journal-article","created":{"date-parts":[[2025,7,8]],"date-time":"2025-07-08T10:20:29Z","timestamp":1751970029000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":29,"title":["Molecular Scale Interfacial Water Management Switching Reaction Pathway of Carbon Dioxide Electroreduction"],"prefix":"10.1002","volume":"64","author":[{"given":"Zongying","family":"Li","sequence":"first","affiliation":[{"name":"Department of Chemical Engineering School of Chemistry and Chemical Engineering Shanghai Jiao Tong University  Shanghai 200240 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rongzhen","family":"Chen","sequence":"additional","affiliation":[{"name":"Key Laboratory for Ultrafine Materials of Ministry of Education Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering East China University of Science &amp; Technology  Shanghai 200237 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wangxin","family":"Ge","sequence":"additional","affiliation":[{"name":"Key Laboratory for Ultrafine Materials of Ministry of Education Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering East China University of Science &amp; Technology  Shanghai 200237 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kunchi","family":"Xie","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering East China University of Science &amp; Technology  Shanghai 200237 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yating","family":"Wang","sequence":"additional","affiliation":[{"name":"Key Laboratory for Ultrafine Materials of Ministry of Education Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering East China University of Science &amp; Technology  Shanghai 200237 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ling","family":"Zhang","sequence":"additional","affiliation":[{"name":"Key Laboratory for Ultrafine Materials of Ministry of Education Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering East China University of Science &amp; Technology  Shanghai 200237 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhen","family":"Song","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering East China University of Science &amp; Technology  Shanghai 200237 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fengwang","family":"Li","sequence":"additional","affiliation":[{"name":"School of Chemical and Biomolecular Engineering and The University of Sydney Nano Institute University of Sydney  Sydney New South Wales Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4086-0323","authenticated-orcid":false,"given":"Yuhang","family":"Li","sequence":"additional","affiliation":[{"name":"Department of Chemical Engineering School of Chemistry and Chemical Engineering Shanghai Jiao Tong University  Shanghai 200240 China"},{"name":"Key Laboratory for Ultrafine Materials of Ministry of Education Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering East China University of Science &amp; Technology  Shanghai 200237 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7897-5850","authenticated-orcid":false,"given":"Chunzhong","family":"Li","sequence":"additional","affiliation":[{"name":"Department of Chemical Engineering School of Chemistry and Chemical Engineering Shanghai Jiao Tong University  Shanghai 200240 China"},{"name":"School of Chemical Engineering East China University of Science &amp; Technology  Shanghai 200237 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