Litcius/Paper detail

A Catalytic Asymmetric Hydrolactonization

Rajat Maji, Santanu Ghosh, Oleg Grossmann, Pinglu Zhang, Markus Leutzsch, Nobuya Tsuji, Benjamin List

2023Journal of the American Chemical Society50 citationsDOIOpen Access PDF

Abstract

Despite recent advancements in the development of catalytic asymmetric electrophile induced lactonization reactions of olefinic carboxylic acids, the archetypical hydrolactonization has long remained an unsolved and well-recognized challenge. Here, we report the realization of a catalytic asymmetric hydrolactonization using a confined imidodiphosphorimidate (IDPi) Brønsted acid catalyst. The method is operationally simple, scalable, and compatible with a wide variety of substrates. Its potential is showcased with concise syntheses of the sesquiterpenes (-)-boivinianin A and (+)-gossonorol. Through in-depth physicochemical and DFT analyses, we derive a nuanced picture of the mechanism and enantioselectivity of this reaction.

Topics & Concepts

ChemistryElectrophileCatalysisCombinatorial chemistryRealization (probability)Brønsted–Lowry acid–base theoryMechanism (biology)Enantioselective synthesisCarboxylic acidOrganic chemistryComputational chemistryNanotechnologyMathematicsStatisticsPhilosophyMaterials scienceEpistemologyAsymmetric Synthesis and CatalysisVanadium and Halogenation ChemistryTraditional and Medicinal Uses of Annonaceae