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Herein, we propose a hierarchical core\u2010shell catalyst, SiO\n                    <jats:sub>2<\/jats:sub>\n                    @C\/Sn. Mesoporous silicon dioxide (SiO\n                    <jats:sub>2<\/jats:sub>\n                    ) serves as a rigid confinement scaffold to effectively suppress the migration and aggregation of Sn nanoparticles. Simultaneously, a conductive carbon layer was in\u2010situ formed on the SiO\n                    <jats:sub>2<\/jats:sub>\n                    surface, markedly enhancing interfacial charge transport. Importantly, the interfacial electronic structure of the Sn nanoparticles is moderately tuned by the combined effect of SiO\n                    <jats:sub>2<\/jats:sub>\n                    confinement and the continuous electronic interface provided by the carbon layer, thereby maintaining an optimal adsorption\u2010desorption balance for the *OOH intermediate and significantly improving selectivity toward the 2e\n                    <jats:sup>\u2212<\/jats:sup>\n                    pathway. SiO\n                    <jats:sub>2<\/jats:sub>\n                    @C\/Sn achieves H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    selectivity exceeding 97% and a production rate of 16.15 mol\u00b7g\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    \u00b7h\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    in alkaline media, while 80% selectivity with a yield of 8.13 mol\u00b7g\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    \u00b7h\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    in neutral media. The catalytic activity shows almost no decay after 100\u00a0h of continuous operation. In\u2010situ spectroscopies combined with DFT calculations further reveal that polarization coupling at the SiO\n                    <jats:sub>2<\/jats:sub>\n                    \u2010carbon interface induces electronic redistribution that optimizes the electronic states of Sn sites and thereby stabilizes the 2e\n                    <jats:sup>\u2212<\/jats:sup>\n                    reaction pathway.\n                  <\/jats:p>","DOI":"10.1002\/smll.74494","type":"journal-article","created":{"date-parts":[[2026,7,20]],"date-time":"2026-07-20T04:52:08Z","timestamp":1784523128000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Rigid Confinement and Interfacial Electronic Polarization Enable Highly Selective SiO\n                    <sub>2<\/sub>\n                    @C\/Sn Catalysts for Two\u2010Electron Oxygen Reduction Toward Efficient H\n                    <sub>2<\/sub>\n                    O\n                    <sub>2<\/sub>\n                    Production"],"prefix":"10.1002","volume":"22","author":[{"given":"Qian","family":"Ning","sequence":"first","affiliation":[{"name":"School of Chemistry and Chemical Engineering University Engineering Research Center of Green Chemical New Materials Guangxi University  Nanning Guangxi China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chengcheng","family":"He","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering University Engineering Research Center of Green Chemical New Materials Guangxi University  Nanning Guangxi China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaolin","family":"Xue","sequence":"additional","affiliation":[{"name":"National Key Laboratory of Advanced Polymer Materials Polymer Research Institute Sichuan University  Chengdu 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