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Copper-catalyzed carbo-difluoromethylation of alkenes via radical relay

Aijie Cai, Wenhao Yan, Xiaojun Zeng, Samson B. Zacate, Tzu‐Hsuan Chao, Jeanette A. Krause, Mu‐Jeng Cheng, Wei Liu

2021Nature Communications55 citationsDOIOpen Access PDF

Abstract

Abstract Organic molecules that contain alkyl-difluoromethyl moieties have received increased attention in medicinal chemistry, but their synthesis in a modular and late-stage fashion remains challenging. We report herein an efficient copper-catalyzed radical relay approach for the carbo-difluoromethylation of alkenes. This approach simultaneously introduces CF 2 H groups along with complex alkyl or aryl groups into alkenes with regioselectivity opposite to traditional CF 2 H radical addition. We demonstrate a broad substrate scope and a wide functional group compatibility. This scalable protocol is applied to the late-stage functionalization of complex molecules and the synthesis of CF 2 H analogues of bioactive molecules. Mechanistic studies and density functional theory calculations suggest a unique ligand effect on the reactivity of the Cu-CF 2 H species.

Topics & Concepts

RegioselectivityChemistryCombinatorial chemistryMoleculeCatalysisFunctional groupAlkylArylDensity functional theoryReactivity (psychology)RadicalSurface modificationOrganic chemistryComputational chemistryPhysical chemistryMedicineAlternative medicinePathologyPolymerFluorine in Organic Chemistry
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