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Inspired by enzymatic compartmentalization, we report an aptamer\u2010functionalized Au\u2010Fe dual\u2010single\u2010atom catalyst (Apt\u2010Au\n                    <jats:sub>1<\/jats:sub>\n                    \u2010Fe\n                    <jats:sub>1<\/jats:sub>\n                    \/NC) that mimics nature's precision by integrating atomically dispersed Au\u2010Fe sites with a genetically engineered recognition element. This material design creates a \u201csmart reactive pocket\u201d featuring two synergistic interfaces: the Au\u2010Fe heteronuclear pair electronically modulates the\n                    <jats:italic>d<\/jats:italic>\n                    \u2010band center to lock the oxygen reduction reaction (ORR) into a highly selective 3\u2010electron pathway with a lowered energy barrier (0.424 eV), while the grafted aptamer acts as a molecular gatekeeper for substrate pre\u2010enrichment. The resulting architecture achieves exceptional selectivity (87.0%\u201392.6%) for specific targets while suppressing non\u2010specific mineralization to below 5.3%\u2014a stark contrast to conventional systems where selectivity is negligible and mineralization exceeds 90%. Mechanistically, the synergistic electronic interaction ensures localized \u00b7OH generation, while the aptamer enforces a strict \u201cproximity effect,\u201d confining these radicals within the nanoscale space for instantaneous consumption by captured substrates. By imposing biological recognition\u2010based spatial constraints on inorganic active centers, this work establishes a universal paradigm for decoupling activity from selectivity, enabling precision chemical conversion in complex matrices.\n                  <\/jats:p>","DOI":"10.1002\/adma.73645","type":"journal-article","created":{"date-parts":[[2026,6,9]],"date-time":"2026-06-09T08:21:11Z","timestamp":1780993271000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Dual\u2010Single\u2010Atom Catalyst with Aptamer\u2010Engineered Confined Reactive Milieu for Spatiotemporally Controlled Selective Conversion"],"prefix":"10.1002","volume":"38","author":[{"given":"Jingyan","family":"Liu","sequence":"first","affiliation":[{"name":"School of Chemical Science and Engineering Department of Thoracic Surgery Shanghai Tongji Hospital Tongji University  Shanghai P. R. 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