Electron-transfer-mediated synthesis of phenanthridines by intramolecular arylation of anions from N-(ortho-halobenzyl)arylamines: regiochemical and mechanistic analysis

J Org Chem. 2010 Apr 2;75(7):2206-18. doi: 10.1021/jo9025918.

Abstract

The synthesis of a series of substituted phenanthridines by photostimulated C-C cyclization of anions from N-(ortho-halobenzyl)arylamines has been found to proceed in very good to excellent yields (79-95%) in liquid ammonia and in DMSO. The N-(ortho-halobenzyl)arylamines are obtained in good to very good isolated yields (44-85%) by nucleophilic substitution of ortho-halobenzylchlorides with different arylamines. The reaction of the anions of a diverse set of N-(ortho-halobenzyl)arylamines was studied, and the methodology was extended to the synthesis of trispheridine, a natural product, in very good yield. In order to explain the regiochemical outcome of these reactions, a theoretical analysis was performed with DFT methods and the B3LYP functional.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Amines / chemistry*
  • Ammonia / chemistry
  • Anions / chemistry*
  • Benzylamines / chemistry*
  • Combinatorial Chemistry Techniques
  • Cyclization
  • Hydrocarbons, Halogenated / chemistry*
  • Magnetic Resonance Spectroscopy
  • Molecular Structure
  • Phenanthridines / chemical synthesis*
  • Phenanthridines / chemistry
  • Solutions / chemistry

Substances

  • Amines
  • Anions
  • Benzylamines
  • Hydrocarbons, Halogenated
  • Phenanthridines
  • Solutions
  • Ammonia