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Here the local microenvironment of three\u2013phase interface is successfully regulated to boost the CO\n                    <jats:sub>2<\/jats:sub>\n                    RR performance of Ni species in the universal pH range by introducing the highly electronegative F. The optimized Ni\/FC achieves high\u2013performance in converting CO\n                    <jats:sub>2<\/jats:sub>\n                    to CO with Faraday efficiencies (FEs) over 90% in pH\u2013universal conditions, while the main product of Ni\/C is H\n                    <jats:sub>2<\/jats:sub>\n                    , especially under acidic conditions. Significantly, it can steadily operate at a high current density of 200\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    for over 3000\u00a0h in a broad pH range, outperforming most recently reported CO\n                    <jats:sub>2<\/jats:sub>\n                    RR electrocatalysts. Detail in situ experiments and density functional theory calculations reveal that the presence of highly electronegative F will cause the formation of a positive C\n                    <jats:sup>\u03b4+<\/jats:sup>\n                    center, which inhibits the adsorption of hydrogen and increases the dissociation energy barrier of interfacial water, thereby suppressing the competitive hydrogen evolution reaction (HER). This work highlights the importance of regulating the local microenvironment of interfacial water, providing a new perspective in the field of electrocatalysis for suppressing competitive HER.\n                  <\/jats:p>","DOI":"10.1002\/adma.202509720","type":"journal-article","created":{"date-parts":[[2025,6,13]],"date-time":"2025-06-13T01:55:27Z","timestamp":1749779727000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":41,"title":["Fluorine\u2013Mediated Interfacial Microenvironment for Boosting pH\u2013Universal CO\n                    <sub>2<\/sub>\n                    Reduction"],"prefix":"10.1002","volume":"37","author":[{"given":"Tingjie","family":"Mao","sequence":"first","affiliation":[{"name":"Wenzhou Key Lab of Advanced Energy Storage and Conversion Zhejiang Province Key Lab of Leather Engineering College of Chemistry and Materials Engineering Wenzhou University  Wenzhou Zhejiang 325035 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