Diastereo- and Enantioselective Synthesis of Bisbenzannulated Spiroketals and Spiroaminals by Ir/Ag/Acid Ternary Catalysis

Angew Chem Int Ed Engl. 2022 Oct 17;61(42):e202210207. doi: 10.1002/anie.202210207. Epub 2022 Aug 19.

Abstract

We reported herein an iridium/silver/acid ternary catalytic system to access bisbenzannulated [6,6]-spiroketals in high efficiency with generally high diastereo- and enantioselectivities (up to >20 : 1 dr, >99 % ee). In this procedure, readily available o-alkynylacetophenones undergo cycloisomerization to generate isochromenes in situ that participate in stereoselective allylation/spiroketalization sequence with 2-(1-hydroxyallyl)phenols. Meanwhile, 2-(1-hydroxyallyl)anilines were also compatible in this cascade reaction, furnishing structurally novel bisbenzannulated [6,6]-spiroaminals with good diastereoselectivities (8 : 1-12 : 1 dr) and excellent enantioselectivities (98 %->99 % ee). Moreover, experimental studies and theoretical calculations were performed to illustrate the reaction mechanism and stereochemistry.

Keywords: Allylation; Asymmetric Synthesis; Iridium; Spiroketals; Ternary Catalysis.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Aniline Compounds
  • Catalysis
  • Furans
  • Iridium*
  • Phenols
  • Silver*
  • Spiro Compounds
  • Stereoisomerism

Substances

  • Aniline Compounds
  • Furans
  • Phenols
  • Spiro Compounds
  • spiroketal
  • Silver
  • Iridium