Palladium/PC-Phos-Catalyzed Asymmetric Heck/Tsuji-Trost Reactions of Amino-Tethered 1,3-Cyclohexadiene with Aryl and Alkenyl Halides

Angew Chem Int Ed Engl. 2023 Jan 2;62(1):e202215407. doi: 10.1002/anie.202215407. Epub 2022 Dec 1.

Abstract

Chiral perhydroindoles are found in a number of natural products and biologically active compounds. Therefore, the development of new asymmetric methodology for rapid access to this core is of high importance. Herein, we reported a highly regio- and diastereo-selective palladium/PC-Phos-catalyzed asymmetric Heck/Tsuji-Trost reactions of readily available amino tethered 1,3-cyclohexadienes with aryl and alkenyl halides, delivering various functionalized chiral hexahydroindoles in good yields with high enantioselectivity. The application of this reaction to the concise synthesis of (-)-α-Lycorane was demonstrated. DFT computation results indicate that the difference in ΔEdis of two migration insertion transition states determines the enantioselectivity of the reaction.

Keywords: 1,3-Cyclohexadiene; Carboamination; Chiral Hexahydroindoles; Heck/Tsuji-Trost Reactions; Palladium.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Catalysis
  • Cyclohexenes*
  • Molecular Structure
  • Palladium*

Substances

  • Palladium
  • 1,3-cyclohexadiene
  • Cyclohexenes
  • 1,4-cyclohexadiene