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Enantioselective Nickel-Catalyzed Alkyne–Azide Cycloaddition by Dynamic Kinetic Resolution

En-Chih Liu, Joseph J. Topczewski

2021Journal of the American Chemical Society53 citationsDOI

Abstract

The triazole heterocycle has been widely adopted as an isostere for the amide bond. Many native amides are α-chiral, being derived from amino acids. This makes α- N -chiral triazoles attractive building blocks. This report describes the first enantioselective triazole synthesis that proceeds via nickel-catalyzed alkyne–azide cycloaddition (NiAAC). This dynamic kinetic resolution is enabled by a spontaneous [3,3]-sigmatropic rearrangement of the allylic azide. The 1,4,5-trisubstituted triazole products, derived from internal alkynes, are complementary to those commonly obtained by the related CuAAC reaction. Initial mechanistic experiments indicate that the NiAAC reaction proceeds through a monometallic Ni complex, which is distinct from the CuAAC manifold.

Topics & Concepts

ChemistryCycloadditionEnantioselective synthesisKinetic resolutionAzideAlkyneCombinatorial chemistryAllylic rearrangementTriazoleCatalysisAmideIsostereStereochemistryOrganic chemistryClick Chemistry and ApplicationsChemical Synthesis and AnalysisCyclopropane Reaction Mechanisms
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