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Herein, we constructed an organic\u2013inorganic cooperative FLP catalyst (C\u00b7\u00b7\u00b7CuSA FLP) within ordered confined space through anchoring Cu single atoms at N-heterocyclic olefin (NHO) sites in a robust metal\u2013organic framework. The C\u00b7\u00b7\u00b7CuSA FLP catalyzes the carboxylative cyclization of propargylamines with CO2 to yield 2-oxazolidinones, achieving a record turnover frequency of 1548 h\u20131 among non-noble catalysts, and retaining impressive activities of 816 h\u20131 (simulated flue gas, 15 vol % CO2), 291 h\u20131 (simulated breath-level gas, 5 vol % CO2), and 5.0 h\u20131 (indoor air, \u223c450 ppm of CO2). Combined operando spectroscopic experiments and density functional theory calculations elucidate that the electron-rich in situ generated NHO as a Lewis base activates CO2 to form a reversible NHO\u2013CO2 adduct, enabling the subsequent kinetically favorable electrophilic addition. Meanwhile, the electron-deficient CuSA serves as a Lewis acid to activate the C\u2261C bond for promoting the nucleophilic attack step as well as triggering the intramolecular cyclization. These findings establish atomically precise solid FLP architectures as a transformative paradigm for highly efficient activation and conversion of CO2 from ambient air.<\/jats:p>","DOI":"10.1021\/jacs.6c07709","type":"journal-article","created":{"date-parts":[[2026,9,1]],"date-time":"2026-09-01T04:23:21Z","timestamp":1788236601000},"page":"37799-37808","source":"Crossref","is-referenced-by-count":0,"title":["Engineering\nAtomic Copper-Based Solid Frustrated Lewis-Pair\nSites toward Dilute CO2 Activation and Transformation"],"prefix":"10.1021","volume":"148","author":[{"given":"Jie","family":"Chen","sequence":"first","affiliation":[{"name":"Gannan Normal University , , ,","place":["Ganzhou, China, 341000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jing","family":"Li","sequence":"additional","affiliation":[{"name":"Gannan Normal University , , ,","place":["Ganzhou, China, 341000"]},{"name":"Jiangxi Normal University , , ,","place":["Nanchang, China, 330022"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qinggang","family":"Zhang","sequence":"additional","affiliation":[{"name":"Gannan Normal University , , ,","place":["Ganzhou, China, 341000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huihua","family":"Deng","sequence":"additional","affiliation":[{"name":"Gannan Normal University , , ,","place":["Ganzhou, China, 341000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hao","family":"Liu","sequence":"additional","affiliation":[{"name":"Gannan Normal University , , ,","place":["Ganzhou, China, 341000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0003-2374","authenticated-orcid":true,"given":"Zhonggao","family":"Zhou","sequence":"additional","affiliation":[{"name":"Gannan Normal University , , ,","place":["Ganzhou, China, 341000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4709-7623","authenticated-orcid":true,"given":"Yun","family":"Bai","sequence":"additional","affiliation":[{"name":"Gannan Normal University , , ,","place":["Ganzhou, China, 341000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0009-7693","authenticated-orcid":true,"given":"Yiwang","family":"Chen","sequence":"additional","affiliation":[{"name":"Gannan Normal University , , ,","place":["Ganzhou, China, 341000"]},{"name":"Jiangxi Normal University , , ,","place":["Nanchang, China, 330022"]},{"name":"Nanchang University , , ,","place":["Nanchang, China, 330022"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chun-Ting","family":"He","sequence":"additional","affiliation":[{"name":"Jiangxi Normal University , , ,","place":["Nanchang, China, 330022"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,25]]},"reference":[{"issue":"7","key":"2026090910092299000_cit1","doi-asserted-by":"publisher","first-page":"1520","DOI":"10.1016\/j.chempr.2020.05.007","article-title":"Catalysis,\nFLPs, and Beyond","volume":"6","author":"Stephan","year":"2020","journal-title":"Chem"},{"issue":"14","key":"2026090910092299000_cit2","doi-asserted-by":"publisher","first-page":"4632","DOI":"10.1039\/D3CS00294B","article-title":"Frustrated\nLewis pair chemistry of CO","volume":"52","author":"Stephan","year":"2023","journal-title":"Chem. 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