Synthesis of bivalent inhibitors of eucaryotic proteasomes

J Pept Sci. 2000 Jan;6(1):36-46. doi: 10.1002/(SICI)1099-1387(200001)6:1<36::AID-PSC232>3.0.CO;2-2.

Abstract

Based on the peculiar spatial array of the active sites in the internal chamber of the multicatalytic proteasome, as derived from the X-ray structure of yeast proteasome, homo- and heterobivalent inhibitors were designed and synthesized to exploit the principle of multivalency for enhancing inhibition potency. Peptidic bis-aldehyde compounds of the octapeptide size were synthesized to address adjacent active sites, whilst a PEG spacer with a statistical length distribution of 19-25 monomers was used to link two identical or different tripeptide aldehydes as binding heads. These bis-aldehyde compounds were synthesized applying both methods in solution and solid phase peptide synthesis. Bivalent binding was observed only for the PEG-spaced inhibitors suggesting that binding from the primed side prevents hemiacetal formation with the active site threonine residue.

MeSH terms

  • Chymases
  • Chymotrypsin / pharmacology
  • Cysteine Endopeptidases / chemistry
  • Cysteine Endopeptidases / metabolism*
  • Enzyme Inhibitors / chemical synthesis*
  • Eukaryotic Cells / ultrastructure
  • Fungal Proteins / chemistry
  • Inhibitory Concentration 50
  • Models, Chemical
  • Multienzyme Complexes / chemistry
  • Multienzyme Complexes / metabolism*
  • Peptides / chemical synthesis*
  • Polyethylene Glycols / chemistry
  • Proteasome Endopeptidase Complex
  • Saccharomyces cerevisiae / enzymology
  • Serine Endopeptidases / metabolism
  • Trypsin / pharmacology
  • Tryptases

Substances

  • Enzyme Inhibitors
  • Fungal Proteins
  • Multienzyme Complexes
  • Peptides
  • Polyethylene Glycols
  • Serine Endopeptidases
  • chymase 2
  • Chymotrypsin
  • Chymases
  • Trypsin
  • Tryptases
  • Cysteine Endopeptidases
  • Proteasome Endopeptidase Complex