Intramolecular "hydroiminiumation and -amidiniumation" of alkenes: a convenient, flexible, and scalable route to cyclic iminium and imidazolinium salts

J Org Chem. 2007 Apr 27;72(9):3492-9. doi: 10.1021/jo0703909. Epub 2007 Apr 5.

Abstract

Addition of a stoichiometric amount of HCl to alkenylaldimines, -formamidines, and -amidines results in the protonation of the sp2-nitrogen atom. The resulting alkenylaldiminium, -formamidinium, and -amidinium salts can be isolated and fully characterized, including single-crystal X-ray diffraction studies. Heating solutions of these salts induces ring closure cleanly and regioselectively via formal "exo" addition of the nitrogen-hydrogen bond to the pendent carbon-carbon double bond, affording the corresponding cyclic aldiminium, dihydroisoquinolinium, and imidazolinium salts. Of special interest, novel 4,4-disubstituted imidazolinium salts are accessible via this synthetic route. Similarly, addition of phosgene to alkenyl ureas and alkenyl amides, followed by gentle heating, cleanly affords C-chloro imidazolinium, and cyclic C-chloro iminium salts, respectively. Treatment of the latter with tetrakis(triphenylphosphine)palladium allows for the preparation of the first transition-metal complex bearing a cyclic arylaminocarbene as ligand. Deuterium labeling experiments suggest that the mechanism of the hydroiminiumation and -amidiniumation reactions involves an intramolecular proton transfer to the double bond in the rate-determining step. This novel synthetic methodology gives access to a variety of N-heterocyclic carbene (NHC) and cyclic alkyl- and arylaminocarbene (CAAC) precursors.

Publication types

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

MeSH terms

  • Alkenes / chemistry*
  • Amidines / chemistry
  • Chemistry, Organic / methods*
  • Crystallography, X-Ray
  • Hydrocarbons, Cyclic / chemistry
  • Imidazoles / chemical synthesis
  • Imidazoles / chemistry*
  • Imines / chemistry
  • Molecular Structure
  • Salts / chemistry

Substances

  • Alkenes
  • Amidines
  • Hydrocarbons, Cyclic
  • Imidazoles
  • Imines
  • Salts