Origins of Stereoselectivity of Enamine-Iminium-Activated Nazarov Cyclizations by Vicinal Diamines

J Org Chem. 2017 Aug 4;82(15):8186-8190. doi: 10.1021/acs.joc.7b01606. Epub 2017 Jul 21.

Abstract

The mechanism and sources of asymmetric induction in Nazarov reactions reported by Tius and co-workers have been determined with quantum chemical calculations. A chiral vicinal diamine forms an enamine-iminium adduct with α-ketoenones, and this undergoes a cationic conrotatory electrocyclization. The chiral diamine imparts stereocontrol in the enamine-iminium complex by forming a six-membered ring that favors one helicity of the electrocyclization transition state.

Publication types

  • Research Support, N.I.H., Extramural
  • Research Support, U.S. Gov't, Non-P.H.S.

MeSH terms

  • Amines / chemistry*
  • Cyclization
  • Imines / chemistry*
  • Ketones / chemistry*
  • Molecular Conformation
  • Quantum Theory
  • Stereoisomerism
  • Thermodynamics

Substances

  • Amines
  • Imines
  • Ketones