Pathways and populations: stereoelectronic insights into the exocyclic torsion of 5-(hydroxymethyl)tetrahydropyran

J Am Chem Soc. 2008 May 21;130(20):6345-7. doi: 10.1021/ja077633z. Epub 2008 Apr 29.

Abstract

High level ab initio computations in vacuum and with the IEFPCM implicit solvent model are carried out on 5-(hydroxymethyl)tetrahydropyran to investigate the effects of water on the exocyclic torsional surface. Rotamer populations evaluated from the omega(C-C-C-O), theta(C-C-C-O) solvent surface agree almost quantitatively with experimental values for the closely related methyl 4-deoxy-alpha-D-xylohexopyranoside. Potentials of mean force obtained from the two surfaces show substantial solvent stabilization of the TG (omega = 180 +/- 60 degrees) rotamer and the barriers at omega= 120 and 240 degrees but solvent destabilization at the cis barrier (omega = 0 degrees). Natural bond orbital analyses indicate that energetics of these effects are largely explained by overstabilization of the vacuum GT (omega= 60 +/- 60 degrees) and GG (omega = 300 +/- 60 degrees) rotamers. Solvent stabilization of theta conformations provides entropic stabilization.

Publication types

  • Research Support, N.I.H., Intramural

MeSH terms

  • Glycosides / chemistry*
  • Models, Molecular
  • Molecular Conformation
  • Pyrans / chemistry*
  • Stereoisomerism
  • Surface Properties
  • Thermodynamics
  • Vacuum
  • Water / chemistry

Substances

  • Glycosides
  • Pyrans
  • Water