Carbonyl compounds are abundant in nature and represent a substantial portion of biomass resources.Despite significant recent progress in homo-coupling of carbonyl compounds,achieving their deoxyfunctionalization homo...Carbonyl compounds are abundant in nature and represent a substantial portion of biomass resources.Despite significant recent progress in homo-coupling of carbonyl compounds,achieving their deoxyfunctionalization homo-coupling remains a highly intricate challenge.Herein,we report an entirely novel reaction paradigm:the trifluoromethylative homo-coupling of carbonyl compounds via hydrazones,which enables the formation of three C(sp^(3))-C(sp^(3))bonds in a single step.This method provides a new pathway for synthesizing trifluoromethylative coupling product which has unique applications in both fields of medical and material sciences.Mechanistic investigations have unveiled that the formation of a trifluoromethyl-substituted benzyl radical plays a pivotal role as a key intermediate in this reaction.展开更多
基金National Natural Science Foundation of China(NSFC,No.21971093)the Fundamental Research Funds for the Central Universities(No.lzujbky-2021-sp53)+2 种基金the International Joint Research centre for Green Catalysis and Synthesis(No.2016B01017)The Science and Technology Major Program of Gansu Province of China(No.22ZD6FA006)the 111 project for support of our research.We also thank the Canada Research Chair(Tier I)foundation,the E.B。
文摘Carbonyl compounds are abundant in nature and represent a substantial portion of biomass resources.Despite significant recent progress in homo-coupling of carbonyl compounds,achieving their deoxyfunctionalization homo-coupling remains a highly intricate challenge.Herein,we report an entirely novel reaction paradigm:the trifluoromethylative homo-coupling of carbonyl compounds via hydrazones,which enables the formation of three C(sp^(3))-C(sp^(3))bonds in a single step.This method provides a new pathway for synthesizing trifluoromethylative coupling product which has unique applications in both fields of medical and material sciences.Mechanistic investigations have unveiled that the formation of a trifluoromethyl-substituted benzyl radical plays a pivotal role as a key intermediate in this reaction.