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In this context, a ligand-centered redox-controlled zinc amide system is disclosed herein that enables highly selective defluoroetherification of aryl fluorides, irrespective of their electronic nature, with diverse alcohols under mild conditions (70\u201380 \u00b0C, 4\u20138 h), for the first time. Comprehensive mechanistic studies, including radical-trapping experiments, EPR spectroscopy, HRMS analysis, and various control experiments, support a radical-mediated C(sp2)\u2013O cross-coupling driven by unique intramolecular electron transfer within the Zn(II)\u2013amide framework. Intriguingly, the protocol could engage both electron-neutral and -rich aryl fluorides that are typically unreactive under conventional SNAr conditions and display excellent functional-group tolerance. Accordingly, selective C\u2013F bond activation delivers F-containing aryl ethers of pharmaceutical relevance with high chemoselectivity over readily reducible, e.g., CN, NO2, C\u2550O, and C\u2261C, functional groups. Moreover, many types of alcohols (primary, secondary, aliphatic, and benzylic) are efficiently transformed within a unified manifold. The mildness and breadth of the method further enable late-stage diversification of complex, bioactive molecules, providing streamlined access to structurally convoluted ether architectures including drug derivatives. Overall, this work establishes a mechanistically distinct, operationally simple, and sustainable platform for selective aryl C\u2013F bond functionalization that expands the toolbox of C\u2013O bond generation.<\/jats:p>","DOI":"10.1021\/jacsau.6c00750","type":"journal-article","created":{"date-parts":[[2026,7,8]],"date-time":"2026-07-08T17:05:08Z","timestamp":1783530308000},"page":"4269-4282","source":"Crossref","is-referenced-by-count":0,"title":["Adaptive Zinc-Amide\nCatalysis Enables C(sp2)\u2013O Cross-Coupling of Aryl\nFluorides with Alcohols"],"prefix":"10.1021","volume":"6","author":[{"given":"Subarna","family":"Manna","sequence":"first","affiliation":[{"name":"Indian Institute of Technology Madras , , ,","place":["Chennai, India, 600036"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Navya Shenny","family":"Kavil","sequence":"additional","affiliation":[{"name":"Indian Institute of Technology Madras , , ,","place":["Chennai, India, 600036"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0224-8387","authenticated-orcid":true,"given":"Arnab","family":"Rit","sequence":"additional","affiliation":[{"name":"Indian Institute of Technology Madras , , ,","place":["Chennai, India, 600036"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,8]]},"reference":[{"key":"2026072709074273500_cit1b","doi-asserted-by":"publisher","first-page":"3054","DOI":"10.1021\/cr8002505","article-title":"Copper-Mediated Coupling\nReactions and Their Applications in Natural Products and Designed\nBiomolecules Synthesis","volume":"108","author":"Evano","year":"2008","journal-title":"Chem. 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