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Nickel‐Catalyzed Intramolecular 1,2‐Aryl Migration of Mesoionic Carbenes (iMICs)

Arne Merschel, Timo Glodde, Beate Neumann, Hans‐Georg Stammler, Rajendra S. Ghadwal

2020Angewandte Chemie International Edition29 citationsDOIOpen Access PDF

Abstract

Abstract Intramolecular 1,2‐Dipp migration of seven mesoionic carbenes (iMIC Ar ) 2 a – g (iMIC Ar =ArC{N(Dipp)} 2 CHC; Ar=aryl; Dipp=2,6‐iPr 2 C 6 H 3 ) under nickel catalysis to give 1,3‐imidazoles (IMD Ar ) 3 a – g (IMD Ar =ArC{N(Dipp)CHC(Dipp)N}) has been reported. The formation of 3 indicates the cleavage of an N−C Dipp bond and the subsequent formation of a C−C Dipp bond in 2 , which is unprecedented in NHC chemistry. The use of 3 in accessing super‐iMICs ( 5 ) (S‐iMIC=ArC{N(Dipp)N(Me)C(Dipp)}C) has been shown with selenium ( 6 ), gold ( 7 ), and palladium ( 8 ) compounds. The quantification of the stereoelectronic properties reveals the superior σ‐donor strength of 5 compared to that of classical NHCs. Remarkably, the percentage buried volume of 5 (%V bur =45) is the largest known amongst thus far reported iMICs. Catalytic studies show a remarkable activity of 5 , which is consistent with their auspicious stereoelectronic features.

Topics & Concepts

MesoionicIntramolecular forceChemistryArylCatalysisMedicinal chemistryBond cleavageNickelPalladiumStereochemistryOrganic chemistryAlkylN-Heterocyclic Carbenes in Organic and Inorganic ChemistryCatalytic Cross-Coupling ReactionsCyclopropane Reaction Mechanisms
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