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However, navigating the intricate interactions inherent in ball\u2010milling conditions to fine\u2010tune reaction selectivity remains a formidable challenge. Herein, leveraging the dispersive and\/or trapping properties of cyclodextrins, an innovative mechanochemical approach is developed through the integration of cyclodextrins into a Fe\u2010catalyzed system, enabling a streamlined Wacker oxidation process from simple and\/or commercially available alkenes. Our efforts have yielded optimized mechanochemical conditions demonstrating exceptional reactivity and selectivity in generating a diverse array of ketone products, markedly enhancing catalytic efficiency compared to conventional batch methods. Mechanistic investigations have revealed a predominantly Markovnikov\u2010selective catalytic cycle, effectively minimizing undesired alcohol formation, hydrogenation, and the other competing pathways, boosting both reaction yield and selectivity.<\/jats:p>","DOI":"10.1002\/anie.202413901","type":"journal-article","created":{"date-parts":[[2024,9,2]],"date-time":"2024-09-02T09:30:45Z","timestamp":1725269445000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":11,"title":["Supramolecular Modulation for Selective Mechanochemical Iron\u2010Catalyzed Olefin Oxidation"],"prefix":"10.1002","volume":"64","author":[{"given":"Chuan","family":"Jiang","sequence":"first","affiliation":[{"name":"International Joint Laboratory on Resource Chemistry Shanghai Normal University  200234 Shanghai P.\u2005R. 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