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Here, we report a dual\u2010confinement strategy for constructing a metal\u2013organic framework (MOF) based catalyst, MEC\u201088, by spatially confining triphenylphosphine (PPh\n                    <jats:sub>3<\/jats:sub>\n                    ) within the pores of MOF\u2010808 to anchor silver single\u2010atom sites. MEC\u201088 exhibits exceptional activity and pronounced substrate selectivity for the carboxylative cyclization of CO\n                    <jats:sub>2<\/jats:sub>\n                    with benzyl\u2010substituted propargylamines under mild, additive\u2010free aqueous conditions, achieving a turnover frequency up to 1051.3\u00a0\u00b1\u00a00.7\u00a0h\n                    <jats:sup>\u22121<\/jats:sup>\n                    . Moreover, PPh\n                    <jats:sub>3<\/jats:sub>\n                    , as a soft\u2010base ligand, provides robust coordination to silver atoms, effectively inhibiting their aggregation to endow the catalyst with good recyclability. Mechanistic studies reveal that the PPh\n                    <jats:sub>3<\/jats:sub>\n                    \u2010coordinated silver site synergizes with the Zr\n                    <jats:sub>6<\/jats:sub>\n                    O\n                    <jats:sub>8<\/jats:sub>\n                    cluster to activate both the alkyne substrate and CO\n                    <jats:sub>2<\/jats:sub>\n                    , substantially lowering the energy barriers for CO\n                    <jats:sub>2<\/jats:sub>\n                    insertion and cyclization. This work presents a molecule\u2010enhanced confinement approach for designing stable and efficient single\u2010atom catalysts with controllable substrate\u2010specificity.\n                  <\/jats:p>","DOI":"10.1002\/anie.2079917","type":"journal-article","created":{"date-parts":[[2026,3,17]],"date-time":"2026-03-17T10:47:29Z","timestamp":1773744449000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Stabilizing Silver Single\u2010Atom Site via A Pore\u2010Confined Triphenylphosphine for CO\n                    <sub>2<\/sub>\n                    Conversion With High Substrate\u2010Specificity"],"prefix":"10.1002","volume":"65","author":[{"given":"Jing","family":"Li","sequence":"first","affiliation":[{"name":"Key Lab of Fluorine and Silicon for Energy Materials and Chemistry\/College of Chemistry and Materials Jiangxi Normal University  Nanchang 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