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Kinetic Resolution of Azaarylethynyl Tertiary Alcohols by Chiral Brønsted Acid Catalysed Phosphine‐Mediated Deoxygenation

Guanghui Wang, Lulu Li, Yifeng Jiang, Xiaowei Zhao, Xu Ban, Tianju Shao, Yanli Yin, Zhiyong Jiang

2022Angewandte Chemie International Edition16 citationsDOI

Abstract

Abstract A chiral Brønsted acid catalysed phosphine‐mediated deoxygenation protocol is reported. This metal‐free method provides a precise kinetic resolution platform for azaarylethynyl tertiary alcohols, which are a broad category of biologically and synthetically important azaarene derivatives. In addition to providing an efficient method for the first asymmetric preparation of these tertiary alcohols, the strategy facilitates the construction of azaaryl‐functionalized allenes with good to excellent enantioselectivities. The high selectivity factors ( s up to 235), broad substrate scope, and ability to convert azaaryl compounds into both chiral tertiary alcohols and allenes robustly underscore the efficiency and promising utility of this method. The practicability is further validated by the successful synthesis of deuterated allenes with high ee values and substantial incorporation of deuterium using inexpensive D 2 O as the deuterium source.

Topics & Concepts

DeoxygenationChemistryKinetic resolutionPhosphineDeuteriumOrganic chemistryCatalysisBrønsted–Lowry acid–base theoryTertiary amineTertiary alcoholsAsymmetric hydrogenationCombinatorial chemistrySelectivityEnantioselective synthesisQuantum mechanicsPhysicsAsymmetric Hydrogenation and CatalysisAsymmetric Synthesis and CatalysisSynthesis and Catalytic Reactions