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While previous strategies primarily focused on modulating electrolyte compositions or pH to tune the EDL, tailoring the interfacial water structure through catalyst design remains underexplored. Herein, we report a composite catalyst comprising atomically dispersed cobalt sites (Co\n                    <jats:sub>SA<\/jats:sub>\n                    ) embedded in a N\u2010doped carbon matrix and palladium nanoparticles (PdCo\n                    <jats:sub>NP<\/jats:sub>\n                    @Co\n                    <jats:sub>SA<\/jats:sub>\n                    NC), which exhibits enhanced oxygen reduction reaction (ORR).\u00a0In situ\u00a0spectroscopy and density functional theory calculations reveal that Co\n                    <jats:sub>SA<\/jats:sub>\n                    \u00a0incorporation induces a negative shift in the potential of zero charge (\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>PZC<\/jats:sub>\n                    ), causing more positively charged surface under working conditions compared to the Co\u2010free analogue (Pd\n                    <jats:sub>NP<\/jats:sub>\n                    @NC). This charge redistribution reorients interfacial water from H\u2010down to O\u2010down configuration, promoting *OH hydrogenation by strengthening electrostatic interaction with the OH\n                    <jats:sub>sol<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    product. Consequently, PdCo\n                    <jats:sub>NP<\/jats:sub>\n                    @Co\n                    <jats:sub>SA<\/jats:sub>\n                    NC achieves an outstanding half\u2010wave potential of 0.937\u00a0V and a mass activity of 2.58\u00a0 A mg\n                    <jats:sub>Pd<\/jats:sub>\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u00a0for ORR, along with 6.15\u00a0 A mg\n                    <jats:sub>Pd<\/jats:sub>\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u00a0for methanol oxidation reaction (MOR), outperforming Pd\n                    <jats:sub>NP<\/jats:sub>\n                    @NC and commercial Pd\/C. Leveraging its bifunctional ORR\/MOR activity, we construct carbonate\u2010free Zn\u2013methanol\u2013air battery with decent kinetics up to 100\u00a0mA\u00a0cm\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>2<\/jats:sup>\n                    \u00a0and stable operation over 2500\u00a0h with an energy efficiency of 70%.\n                  <\/jats:p>","DOI":"10.1002\/anie.202523272","type":"journal-article","created":{"date-parts":[[2026,1,19]],"date-time":"2026-01-19T10:04:13Z","timestamp":1768817053000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":14,"title":["Reoriented Interfacial Water Structure Around Pd Enhances Oxygen Reduction Kinetics in Zn\u2013Methanol\u2013Air Batteries"],"prefix":"10.1002","volume":"65","author":[{"given":"Lulu","family":"Lyu","sequence":"first","affiliation":[{"name":"Department of Materials Science and Engineering Korea University  Seoul 02841 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xu","family":"Hu","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Institute of New Energy Material Chemistry Renewable Energy Conversion and Storage Center (ReCast) Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Nankai University  Tianjin 300350 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bing","family":"Shao","sequence":"additional","affiliation":[{"name":"Department of Chemistry Southern University of Science and Technology  Shenzhen 518055 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qichen","family":"Wang","sequence":"additional","affiliation":[{"name":"Frontiers Science Center for Flexible Electronics Xi'an Institute of Flexible Electronics Northwestern Polytechnical University  Xi'an 710072 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Gonglei","family":"Shao","sequence":"additional","affiliation":[{"name":"Interdisciplinary Research Center for Sustainable Energy Science and Engineering (IRC4SE<sup>2<\/sup>) School of Chemical Engineering Zhengzhou University  Zhengzhou Henan 450001 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiacong","family":"Lei","sequence":"additional","affiliation":[{"name":"Interdisciplinary Research Center for Sustainable Energy Science and Engineering (IRC4SE<sup>2<\/sup>) School of Chemical Engineering Zhengzhou University  Zhengzhou Henan 450001 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenqi","family":"Fan","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering Korea University  Seoul 02841 Republic of 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