Inhibition of S-ribosylhomocysteinase (LuxS) by substrate analogues modified at the ribosyl C-3 position

Bioorg Med Chem. 2009 Sep 15;17(18):6699-706. doi: 10.1016/j.bmc.2009.07.057. Epub 2009 Jul 26.

Abstract

S-ribosylhomocysteinase (LuxS) catalyzes the cleavage of the thioether bond of S-ribosylhomocysteine (SRH) to produce homocysteine and 4,5-dihydroxy-2,3-pentanedione (DPD), which is the precursor of type 2 autoinducer for bacterial cell-cell communication. In this work, we have synthesized several SRH analogues modified at the ribose C3 position as potential inhibitors of LuxS. While removal or methylation of the C3-OH resulted in simple competitive inhibitors of moderate potency, inversion of the C3 stereochemistry or substitution of fluorine for C3-OH resulted in slow-binding inhibitors of improved potency. The most potent inhibitor showed a K(I)(*) value of 0.43 microM.

Publication types

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

MeSH terms

  • Anti-Bacterial Agents / chemistry*
  • Anti-Bacterial Agents / pharmacology*
  • Bacillus subtilis / drug effects
  • Bacillus subtilis / metabolism
  • Bacterial Proteins / antagonists & inhibitors*
  • Bacterial Proteins / metabolism*
  • Carbon-Sulfur Lyases / antagonists & inhibitors*
  • Carbon-Sulfur Lyases / metabolism*
  • Homocysteine / analogs & derivatives*
  • Homocysteine / chemistry
  • Homocysteine / pharmacology
  • Ribose / chemistry
  • Structure-Activity Relationship

Substances

  • Anti-Bacterial Agents
  • Bacterial Proteins
  • S-ribosyl-L-homocysteine
  • Homocysteine
  • Ribose
  • Carbon-Sulfur Lyases
  • LuxS protein, Bacteria