Dienophile twisting and substituent effects influence reaction rates of intramolecular Diels-Alder cycloadditions: a DFT study

J Am Chem Soc. 2005 Mar 23;127(11):3688-9. doi: 10.1021/ja050135a.

Abstract

Intramolecular cycloadditions of 5-vinyl-1,3-cyclohexadienes were studied with B3LYP/6-31G(d) density functional calculations. The one-atom tether dictates that the Z substituent becomes exo and the E substituent becomes endo in the TS. The geometry of the cycloaddition TS is typical of a pericyclic transformation except unusual twisting of the dienophile places the endo substituent in a relatively steric-free position and the exo substituent in a highly crowded position. The experimental rate differences between isomeric pairs of vinylcyclohexadienes can be explained by comparing reactant destabilization when a bulky group occupies the Z position of the starting alkene and transition state stabilization when a bulky group is endo in the cycloaddition TS.

Publication types

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

MeSH terms

  • Cyclohexanes / chemistry*
  • Cyclohexenes
  • Models, Molecular
  • Structure-Activity Relationship
  • Thermodynamics
  • Vinyl Compounds / chemistry*

Substances

  • Cyclohexanes
  • Cyclohexenes
  • Vinyl Compounds
  • 1,4-cyclohexadiene