Design, synthesis, and evaluation of Phe-Gly mimetics: heterocyclic building blocks for pseudopeptides

J Med Chem. 1999 Oct 21;42(21):4331-42. doi: 10.1021/jm990197+.

Abstract

Enantiopure heterocyclic Boc-protected Phe-Gly dipeptidomimetics containing 1,3,4-oxadiazole, 1,2,4-oxadiazole, and 1,2,4-triazole ring systems have been synthesized as building blocks in the synthesis of pseudopeptides. Three derivatives (1-3) have the carboxylic acid function directly bound to the heterocyclic ring, and three derivatives (4-6) have an extra methylene group between the heterocyclic ring and the acid function to allow for an increased conformational flexibility. The mimetics were used as Phe-Gly replacements in the biologically active peptides dermorphin (Tyr-D-Ala-Phe-Gly-Tyr-Pro-Ser-NH(2)) and substance P (Arg-Pro-Lys-Pro-Gln-Gln-Phe-Phe-Gly-Leu-MetNH(2), SP). The pseudopeptide synthesis was performed using solid-phase methodology on a MBHA-resin using Boc-chemistry. The biological evaluation was performed by testing the micro- and delta-opioid receptor affinities of the dermorphin pseudopeptides and the NK(1) receptor affinities of the SP pseudopeptides. The results showed that all mimetics except 3 were excellent replacements of Phe-Gly in dermorphin since they displayed affinities for the micro-receptor (IC(50) = 12-31 nM) in the same range as dermorphin itself (IC(50) = 6.2 nM). The agonist activity of three pseudopeptides at human micro-receptors was also evaluated. It was shown that the tested compounds retained their agonist activity. The SP pseudopeptides showed considerably lower affinities (IC(50) > 1 microM) for the NK(1) receptor than SP itself (IC(50) = 1.5 nM) indicating that the Phe-Gly replacements prevent the pseudopeptides from adopting bioactive conformations.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Animals
  • Brain / metabolism
  • Cell Line
  • Dipeptides / chemistry*
  • Drug Design
  • Humans
  • In Vitro Techniques
  • Models, Molecular
  • Molecular Conformation
  • Molecular Mimicry
  • Oligopeptides / chemical synthesis*
  • Oligopeptides / chemistry
  • Oligopeptides / metabolism
  • Oxadiazoles / chemical synthesis*
  • Oxadiazoles / chemistry
  • Oxadiazoles / metabolism
  • Radioligand Assay
  • Rats
  • Receptors, Neurokinin-1 / metabolism
  • Receptors, Opioid, delta / metabolism
  • Receptors, Opioid, mu / metabolism
  • Triazoles / chemical synthesis*
  • Triazoles / chemistry
  • Triazoles / metabolism

Substances

  • Dipeptides
  • Oligopeptides
  • Oxadiazoles
  • Receptors, Neurokinin-1
  • Receptors, Opioid, delta
  • Receptors, Opioid, mu
  • Triazoles
  • phenylalanylglycine