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Conventional approaches primarily focus on the bulk electronic modulation of the electrocatalyst while neglecting interfacial water dynamics. Here, we propose a dual\u2010functional sulfur\u2010doping strategy in Co\n                    <jats:sub>3<\/jats:sub>\n                    O\n                    <jats:sub>4<\/jats:sub>\n                    (S\u2010Co\n                    <jats:sub>3<\/jats:sub>\n                    O\n                    <jats:sub>4<\/jats:sub>\n                    ) to simultaneously enhance bulk conductivity and optimize interfacial proton transfer. Through innovative benzene sulfonyl chloride blocking experiment, in situ spectroscopic analyses, and kinetic isotope effect studies, we reveal that sulfur doping narrows the bandgap of Co\n                    <jats:sub>3<\/jats:sub>\n                    O\n                    <jats:sub>4<\/jats:sub>\n                    to enhance bulk charge transport while disrupting rigid hydrogen\u2010bond network of water in the electric double layer; the weakly hydrogen\u2010bonded H\n                    <jats:sub>2<\/jats:sub>\n                    O reduces the dissociation barrier and facilitates proton supply for nitrate hydrogenation. The proposed \u201celectronic\u2010interfacial synergy\u201d strategy establishes a transformative paradigm for designing electrocatalysts in PCET\u2010driven reactions, advancing sustainable energy conversion and environmental applications.\n                  <\/jats:p>","DOI":"10.1002\/anie.202504815","type":"journal-article","created":{"date-parts":[[2025,6,3]],"date-time":"2025-06-03T03:25:02Z","timestamp":1748921102000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":34,"title":["Beyond Conventional Doping: Sulfur\u2010Induced Electronic and Interfacial Dynamics for Advanced Nitrate Reduction"],"prefix":"10.1002","volume":"64","author":[{"given":"Qinghao","family":"Zhang","sequence":"first","affiliation":[{"name":"Graphene Composite Research Centre College of Chemistry and Environmental Engineering, Shenzhen University  Shenzhen 518060 P.R. 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