Biosynthesis of a water-soluble lipid I analogue and a convenient assay for translocase I

Anal Biochem. 2014 Sep 15:461:36-45. doi: 10.1016/j.ab.2014.05.018. Epub 2014 Jun 2.

Abstract

Translocase I (MraY/MurX) is an essential enzyme in growth of the vast majority of bacteria that catalyzes the transformation from UDP-MurNAc-pentapeptide (Park's nucleotide) to prenyl-MurNAc-pentapeptide (lipid I), the first membrane-anchored peptidoglycan precursor. MurX has received considerable attention in the development of new tuberculosis (TB) drugs due to the fact that the MurX inhibitors kill exponentially growing Mycobacterium tuberculosis (Mtb) much faster than clinically used TB drugs. Lipid I isolated from Mtb contains the C50-prenyl unit that shows very poor water solubility; thus, this chemical characteristic of lipid I renders MurX enzyme assays impractical for screening and lacks reproducibility of the enzyme assays. We have established a scalable chemical synthesis of Park's nucleotide-N(ε)-dansylthiourea 2 that can be used as a MurX enzymatic substrate to form lipid I analogues. In our investigation of the minimum structure requirement of the prenyl phosphate in the MraY/MurX-catalyzed lipid I analogue synthesis with 2, we found that neryl phosphate (C10 phosphate) can be recognized by MraY/MurX to generate the water-soluble lipid I analogue in quantitative yield under the optimized conditions. Here, we report a rapid and robust analytical method for quantifying MraY/MurX inhibitory activity of library molecules.

Keywords: MraY; MurX; MurX inhibitors; Mycobacterium tuberculosis; Translocase I; Water-soluble lipid I.

Publication types

  • Research Support, N.I.H., Extramural
  • Research Support, Non-U.S. Gov't

MeSH terms

  • Anti-Bacterial Agents / chemistry
  • Anti-Bacterial Agents / pharmacology
  • Bacterial Proteins / antagonists & inhibitors
  • Bacterial Proteins / metabolism*
  • Enzyme Assays / methods*
  • Microbial Sensitivity Tests
  • Monosaccharides / biosynthesis*
  • Monosaccharides / chemistry*
  • Mycobacterium tuberculosis / drug effects
  • Mycobacterium tuberculosis / enzymology
  • Oligopeptides / biosynthesis*
  • Oligopeptides / chemistry*
  • Peptides / chemistry
  • Peptides / pharmacology
  • Solubility
  • Transferases (Other Substituted Phosphate Groups)
  • Transferases / antagonists & inhibitors
  • Transferases / metabolism*
  • Uridine / chemistry
  • Water / chemistry

Substances

  • Anti-Bacterial Agents
  • Bacterial Proteins
  • Monosaccharides
  • Oligopeptides
  • Peptides
  • lipid I
  • Water
  • Transferases
  • Transferases (Other Substituted Phosphate Groups)
  • mraY protein, Bacteria
  • Uridine