Iodoarene-Catalyzed Stereospecific Intramolecular sp(3) C-H Amination: Reaction Development and Mechanistic Insights

J Am Chem Soc. 2015 Jun 24;137(24):7564-7. doi: 10.1021/jacs.5b03488. Epub 2015 Jun 11.

Abstract

A new strategy is reported for intramolecular sp(3) C-H amination under mild reaction conditions using iodoarene as catalyst and m-CPBA as oxidant. This C-H functionalization involving iodine(III) reagents generated in situ occurs readily at sterically hindered tertiary C-H bonds. DFT (M06-2X) calculations show that the preferred pathway involves an iodonium cation intermediate and proceeds via an energetically concerted transition state, through hydride transfer followed by the spontaneous C-N bond formation. This leads to the experimentally observed amination at a chiral center without loss of stereochemical information.

Publication types

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

MeSH terms

  • Amination
  • Catalysis
  • Chlorobenzoates / chemistry*
  • Hydrocarbons, Aromatic / chemistry*
  • Iodine / chemistry*
  • Models, Molecular
  • Oxidants / chemistry*

Substances

  • Chlorobenzoates
  • Hydrocarbons, Aromatic
  • Oxidants
  • Iodine
  • 3-chloroperbenzoic acid