Radical cascade transformations of tris(o-aryleneethynylenes) into substituted benzo[a]indeno[2,1-c]fluorenes

J Am Chem Soc. 2008 Aug 27;130(34):11535-45. doi: 10.1021/ja8038213. Epub 2008 Aug 2.

Abstract

Oligomeric o-aryleneethynylenes with three triple bonds undergo cascade radical transformations in reaction with a Bu 3SnH/AIBN system. These cascades involve three consecutive cycle closures with the formation of substituted benzo[ a]indeno[2,1- c]fluorene or benzo[1,2]fluoreno[4,3- b]silole derivatives. The success of this sequence depends on regioselectivity of the initial attack of the Bu 3Sn radical at the central triple bond of the o-aryleneethynylene moiety. The cascade is propagated through the sequence of 5-exo-dig and 6-exo-dig cyclizations which is followed by either a radical attack at the terminal Ar substituent or radical transposition which involves H-abstraction from the terminal TMS group and 5-endo-trig cyclization. Overall, the transformation has potential to be developed into an approach to a new type of graphite ribbons.

Publication types

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

MeSH terms

  • Algorithms
  • Alkynes / chemistry*
  • Benzene Derivatives / chemistry*
  • Catalysis
  • Chemistry, Organic / methods*
  • Cyclization
  • Ethers / chemistry*
  • Fluorenes / chemical synthesis*
  • Free Radicals / chemistry*
  • Indenes / chemistry*
  • Magnetic Resonance Spectroscopy
  • Models, Chemical
  • Stereoisomerism
  • Thermodynamics

Substances

  • Alkynes
  • Benzene Derivatives
  • Ethers
  • Fluorenes
  • Free Radicals
  • Indenes
  • phenyleneethynylene