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Precatalyst‐Enabled Selectivity: Enantioselective NiH‐Catalyzed <i>anti</i>‐Hydrometalative Cyclization of Alkynones to <i>Endo</i>‐ and Heterocyclic Allylic Alcohols

Xiaowen Zhang, Minghui Zhu, Hai‐Xiang Zeng, Qi‐Yang Li, Wen‐Bo Liu

2021Angewandte Chemie International Edition36 citationsDOI

Abstract

Abstract A highly enantioselective NiH‐catalyzed hydrocyclization of alkynones with unparalleled anti ‐ and endocyclic selectivities is described. The choice of the precatalysts has significant influence in tuning the regio‐ and enantioselectivity. Using Ni(OTs) 2 /Phox as a precatalyst and (EtO) 2 MeSiH as a hydride source, an array of enantioenriched O‐, N‐, and S‐containing heterocyclic tertiary allylic alcohols are obtained in 24–81 % yields with 80:20–99:1 er. Mechanistic investigations and synthetic application are also carried out. This study represents an efficient access to a set of allylic alcohols that are unable to access by the state‐of‐the‐art coupling reactions.

Topics & Concepts

Allylic rearrangementEnantioselective synthesisChemistryCatalysisSelectivityHydrideCombinatorial chemistryOrganic chemistryHydrogenCatalytic C–H Functionalization MethodsCatalytic Alkyne ReactionsAsymmetric Hydrogenation and Catalysis
Precatalyst‐Enabled Selectivity: Enantioselective NiH‐Catalyzed <i>anti</i>‐Hydrometalative Cyclization of Alkynones to <i>Endo</i>‐ and Heterocyclic Allylic Alcohols | Litcius