Thiolactomycin-based β-ketoacyl-AcpM synthase A (KasA) inhibitors: fragment-based inhibitor discovery using transient one-dimensional nuclear overhauser effect NMR spectroscopy

J Biol Chem. 2013 Mar 1;288(9):6045-52. doi: 10.1074/jbc.M112.414516. Epub 2013 Jan 10.

Abstract

Thiolactomycin (TLM) is a natural product inhibitor of KasA, the β-ketoacyl synthase A from Mycobacterium tuberculosis. To improve the affinity of TLM for KasA, a series of TLM analogs have been synthesized based on interligand NOEs between TLM and a pantetheine analog when both are bound simultaneously to the enzyme. Kinetic binding data reveal that position 3 of the thiolactone ring is a suitable position for elaboration of the TLM scaffold, and the structure-activity relationship studies provide information on the molecular features that govern time-dependent inhibition in this enzyme system. These experiments also exemplify the utility of transient one-dimensional NOE spectroscopy for obtaining interligand NOEs compared with traditional steady state two-dimensional NOESY spectroscopy.

Publication types

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

MeSH terms

  • 3-Oxoacyl-(Acyl-Carrier-Protein) Synthase / antagonists & inhibitors*
  • 3-Oxoacyl-(Acyl-Carrier-Protein) Synthase / genetics
  • 3-Oxoacyl-(Acyl-Carrier-Protein) Synthase / metabolism
  • Bacterial Proteins / antagonists & inhibitors*
  • Bacterial Proteins / genetics
  • Bacterial Proteins / metabolism
  • Enzyme Inhibitors / chemical synthesis
  • Enzyme Inhibitors / chemistry*
  • Mycobacterium smegmatis / enzymology
  • Mycobacterium smegmatis / genetics
  • Mycobacterium tuberculosis / enzymology*
  • Mycobacterium tuberculosis / genetics
  • Protein Binding
  • Structure-Activity Relationship
  • Thiophenes / chemical synthesis
  • Thiophenes / chemistry

Substances

  • Bacterial Proteins
  • Enzyme Inhibitors
  • Thiophenes
  • thiolactomycin
  • 3-Oxoacyl-(Acyl-Carrier-Protein) Synthase