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Here, we present a rational ligand\u2010effect\u2010oriented microenvironment design for the de novo construction of multifunctional COFs that integrate N\n                    <jats:sup>+<\/jats:sup>\n                    \/Br\n                    <jats:sup>\u2212<\/jats:sup>\n                    ion\u2010pairs and imine\u2010anchored atomically dispersed copper sites. A key innovation lies in the precise control of the COFs microenvironment, enabling a seamless three\u2010component cascade reaction of CO\n                    <jats:sub>2<\/jats:sub>\n                    (1\u00a0bar), epoxides, and anilines to afford 2\u2010oxazolidinones under mild and precious\u2010metal\u2010free conditions. The optimized catalyst, Cu@PD\u2010iCOF, delivers up to 99% yield, exhibits broad functional\u2010group compatibility, and retains &gt;96% activity over nine cycles. This work shows that combining ion\u2010pairs and single\u2010atom sites reprograms the COFs microenvironment for efficient CO\n                    <jats:sub>2<\/jats:sub>\n                    utilization.\n                  <\/jats:p>","DOI":"10.1002\/anie.4841198","type":"journal-article","created":{"date-parts":[[2026,9,16]],"date-time":"2026-09-16T03:04:58Z","timestamp":1789527898000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Ligand\u2010Mediated Microenvironment in COFs Incorporating Ion\u2010Pair Motifs and Atomically Dispersed Copper Sites for Cascade CO\n                    <sub>2<\/sub>\n                    Conversion"],"prefix":"10.1002","author":[{"given":"Ping","family":"Liu","sequence":"first","affiliation":[{"name":"Guizhou Provincial Key Laboratory of Green Catalysis and Materials for Resource Conversion School of Chemistry and Chemical Engineering Guizhou University  Guiyang P. R. 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