14-helical folding in a cyclobutane-containing beta-tetrapeptide

J Org Chem. 2004 Jul 23;69(15):5093-9. doi: 10.1021/jo0497555.

Abstract

The efficient synthesis of tetrapeptide 5 containing, in alternation, cyclobutane and beta-alanine residues is described. NMR experiments both at low temperature in CDCl(3) and at 298 K in DMSO-d(6) solutions show the contribution of a strong hydrogen bond in the folded major conformation of 5. Temperature coefficients and diffusion times point out a hydrogen bond involving the NH proton from the cyclobutane residue 1 whereas NOEs manifest the high rigidity of the central fragment of the molecule and are compatible with a 14-membered macrocycle. Theoretical calculations predict a most stable folded conformation corresponding to a 14-helix stabilized by a hydrogen bond between NH(10) in the first residue and OC(25) in the third residue. This structure remains unaltered during the molecular dynamics simulation at 298 K in chloroform. All these results provide evidence for a 14-helical folding and reveal the ability of cis-2-aminocyclobutane carboxylic acid residues to promote folded conformations when incorporated into beta-peptides.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Cyclobutanes / chemistry*
  • Hydrogen Bonding
  • Magnetic Resonance Spectroscopy
  • Models, Molecular
  • Oligopeptides / chemical synthesis*
  • Oligopeptides / chemistry*
  • Protein Conformation
  • Protein Folding*

Substances

  • Cyclobutanes
  • Oligopeptides