Litcius/Paper detail

Reductive Catalytic Difluorocarbene Transfer via Palladium Catalysis

Xue‐Ying Zhang, Xue‐Ying Zhang, Shi‐Ping Sun, Yueqian Sang, Xiao‐Song Xue, Qiao‐Qiao Min, Xingang Zhang, Xingang Zhang

2023Angewandte Chemie International Edition43 citationsDOI

Abstract

Abstract A palladium‐catalyzed reductive difluorocarbene transfer reaction that tames difluorocarbene to couple with two electrophiles has been developed, representing a new mode of difluorocarbene transfer reaction. The approach uses low‐cost and bulk industrial chemical chlorodifluoromethane (ClCF 2 H) as the difluorocarbene precursor. It produces a variety of difluoromethylated (hetero)arenes from widely available aryl halides/triflates and proton sources, featuring high functional group tolerance and synthetic convenience without preparing organometallic reagents. Experimental mechanistic studies reveal that an unexpected Pd 0/II catalytic cycle is involved in this reductive reaction, wherein the oxidative addition of palladium(0) difluorocarbene ([Pd 0 (L n )]=CF 2 ) with aryl electrophile to generate the key intermediate aryldifluoromethylpalladium [ArCF 2 Pd(L n )X], followed by reaction with hydroquinone, is responsible for the reductive difluorocarbene transfer.

Topics & Concepts

DifluorocarbeneReductive eliminationElectrophilePalladiumCatalysisPhotochemistryChemistryArylReagentMedicinal chemistryOrganic chemistryAlkylFluorine in Organic ChemistryInorganic Fluorides and Related CompoundsCyclopropane Reaction Mechanisms