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Rhodium(II)-catalyzed multicomponent assembly of α,α,α-trisubstituted esters via formal insertion of O–C(sp3)–C(sp2) into C–C bonds

Dan Ba, Si Wen, Qingyu Tian, Yanhui Chen, Weiwei Lv, Guolin Cheng

2020Nature Communications31 citationsDOIOpen Access PDF

Abstract

Abstract The direct cleavage of C(CO)−C single bonds, delivering otherwise inaccessible compounds, is a significant challenge. Although the transition metal-catalyzed insertion of functional groups into C(CO)−C bonds has been studied, strained ketone substrates or chelating assistance were commonly required. In this article, we describe a rhodium(II)-catalyzed three-component reaction of 1,3-diones, diazoesters, and N,N -dimethylformamide (DMF), leading to an unusual formal insertion of O–C(sp 3 )–C(sp 2 ) into unstrained C(CO)−C bonds. This procedure provides a rapid entry to a gamut of otherwise inaccessible α,α,α-trisubstituted esters/amide from relatively simple substrates in a straightforward manner. 55 examples of highly decorated products demonstrate the broad functional group tolerance and substrate scope. The combination of control experiments and isotope-labeling reactions support that O, C(sp 3 ), and C(sp 2 ) units derive from 1,3-diones, diazoesters, and DMF, respectively.

Topics & Concepts

RhodiumChemistryInsertion reactionCatalysisFunctional groupAmideCombinatorial chemistryKetoneBond cleavageStereochemistrySubstrate (aquarium)DimethylformamideMedicinal chemistryOrganic chemistrySolventGeologyPolymerOceanographyCyclopropane Reaction MechanismsCatalytic C–H Functionalization MethodsCatalytic Cross-Coupling Reactions