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Herein, we report the synthesis of a class of electrocatalysts using carbon\u2010micropore confinement with adjacent isolated oxophilic Ga sites to stabilize Os ACs and decouple these conflicting interfacial adsorption demands. We demonstrate that carbon aerogel micropores kinetically lock ultrasmall Os clusters against migration and coalescence, while Ga sites polarize spatially proximate Os clusters through support\u2010mediated charge redistribution, downshifting the Os\n                    <jats:italic>d<\/jats:italic>\n                    \u2010band center and weakening H* and CO* binding. Meanwhile, Lewis\u2010acidic oxophilic Ga centers capture and activate H\n                    <jats:sub>2<\/jats:sub>\n                    O\/OH* species, establishing an oxygenated\u2010intermediate relay that lowers the barrier for the sluggish Volmer step. Os AC\/Ga\n                    <jats:sub>1<\/jats:sub>\n                    @pCA delivers exceptional mass activities for hydrogen evolution (2185.5 A g\n                    <jats:sub>Os<\/jats:sub>\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 100 mV) and hydrogen oxidation (7.29 A mg\n                    <jats:sub>Os<\/jats:sub>\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 50 mV), together with outstanding CO tolerance. In an anion\u2010exchange\u2010membrane water\u2010electrolyzer, it achieves a PGM\u2010price\u2010normalized activity of 370.7 A dollar\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 1.8 V and operates stably at 500 mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    for over 300 h with a degradation rate of mere \u223c48.6 \u00b5V h\n                    <jats:sup>\u22121<\/jats:sup>\n                    .\n                  <\/jats:p>","DOI":"10.1002\/anie.2044894","type":"journal-article","created":{"date-parts":[[2026,8,12]],"date-time":"2026-08-12T17:00:36Z","timestamp":1786554036000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Oxophilic Gallium Single\u2010Atom Regulating Micropore\u2010Confined Os Atomic Clusters Enables Efficient Alkaline Hydrogen Electrocatalysis"],"prefix":"10.1002","volume":"65","author":[{"given":"Mengyang","family":"Yang","sequence":"first","affiliation":[{"name":"School of Chemistry National Innovation Platform (Center) for Industry\u2010Education Integration of Energy Storage Technology Engineering Research Center of Energy Storage Materials and Devices of Ministry of Education Xi'an Jiaotong University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ling","family":"Li","sequence":"additional","affiliation":[{"name":"School of Chemistry National Innovation Platform (Center) for Industry\u2010Education Integration of Energy Storage Technology Engineering Research Center of Energy Storage Materials and Devices of Ministry of Education Xi'an Jiaotong University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuheng","family":"He","sequence":"additional","affiliation":[{"name":"School of Chemistry National Innovation Platform (Center) for 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