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Herein, we report a supercritical carbon dioxide (SC CO\n                    <jats:sub>2<\/jats:sub>\n                    ) modulation strategy to synergistically engineer surface amorphization and oxygen vacancy (O\n                    <jats:sub>V<\/jats:sub>\n                    ) defects in orthorhombic CaSnO\n                    <jats:sub>3<\/jats:sub>\n                    . Under an optimal SC CO\n                    <jats:sub>2<\/jats:sub>\n                    pressure of 16\u00a0MPa, the treated CaSnO\n                    <jats:sub>3<\/jats:sub>\n                    exhibits a partially amorphized surface, abundant O\n                    <jats:sub>V<\/jats:sub>\n                    , and concomitant Sn\n                    <jats:sup>3+<\/jats:sup>\n                    defects. These features collectively increase unsaturated coordination sites, accelerate interfacial charge transfer, and lower the reaction overpotential. Consequently, the optimal catalyst achieves a H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    production rate of 26.6\u00a0\u00b5mol cm\u2212\n                    <jats:sup>2<\/jats:sup>\n                    min\n                    <jats:sup>\u22121<\/jats:sup>\n                    , a Faradaic efficiency (FE) of 82% at 2.9\u00a0V versus RHE, and a cumulative yield over 300 min approximately eight times that of pristine CaSnO\n                    <jats:sub>3<\/jats:sub>\n                    , with stable operation for 24 h. This work demonstrates that SC CO\n                    <jats:sub>2<\/jats:sub>\n                    treatment is an effective tool to construct defect coupled surface amorphous regions, providing a new paradigm for designing high \u2010 performance 2e\u2010WOR electrocatalysts for green H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    synthesis.\n                  <\/jats:p>","DOI":"10.1002\/anie.7663698","type":"journal-article","created":{"date-parts":[[2026,7,30]],"date-time":"2026-07-30T12:39:32Z","timestamp":1785415172000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Supercritical CO\n                    <sub>2<\/sub>\n                    \u2010Modulated Surface Amorphization and O\n                    <sub>V<\/sub>\n                    Defect in CaSnO\n                    <sub>3<\/sub>\n                    for High\u2010Efficiency Electrocatalytic H\n                    <sub>2<\/sub>\n                    O\n                    <sub>2<\/sub>\n                    Production"],"prefix":"10.1002","volume":"65","author":[{"given":"Lei","family":"Xu","sequence":"first","affiliation":[{"name":"Henan Institute of Advanced Technology Zhengzhou University  Zhengzhou P.R. 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