Syntheses and pyrolyses of furan analogues of α-oxo-o-quinodimethanes. Formation of methylenecyclobutenone and 1-buten-3-yne via a vinylcarbene-cyclopropene rearrangement

J Org Chem. 2011 Oct 21;76(20):8440-6. doi: 10.1021/jo201743h. Epub 2011 Sep 27.

Abstract

Flash vacuum pyrolyses (FVP) of benzoic 2-methyl-3-furoic anhydride (12) and benzoic 3-methyl-2-furoic anhydride (13) at 550 °C and ca. 10(-2) Torr both give methylenecyclobutenone (16) and 1-buten-3-yne (17) as the main products. A mechanism involving generation of furan analogues of α-oxo-o-quinodimethane, 10 and 11, from FVP of 12 and 13, respectively, followed by elimination of a CO molecule to give the respective carbenes 34 and 36 is proposed. Carbenes 34 and 36 are interconvertible via a cyclopropene intermediate 35. A ring contraction from 36 will give 16, whereas a ring-opening of 34 followed by elimination of a CO molecule then leads to 17. The proposed mechanism is supported by substituent- and deuterium-labeling study on FVP of the derivatives of 12.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Anhydrides / chemistry
  • Chemistry, Organic / methods*
  • Cyclobutanes / chemical synthesis*
  • Cyclopropanes / chemistry
  • Furans / chemical synthesis*
  • Magnetic Resonance Spectroscopy
  • Methane / analogs & derivatives
  • Methane / chemistry*
  • Molecular Structure
  • Vinyl Compounds / chemistry

Substances

  • Anhydrides
  • Cyclobutanes
  • Cyclopropanes
  • Furans
  • Vinyl Compounds
  • cyclobutenone
  • vinylcarbene
  • cyclopropene
  • Methane
  • furan