Comparative metabolomics and structural characterizations illuminate colibactin pathway-dependent small molecules

J Am Chem Soc. 2014 Jul 2;136(26):9244-7. doi: 10.1021/ja503450q. Epub 2014 Jun 20.

Abstract

The gene cluster responsible for synthesis of the unknown molecule "colibactin" has been identified in mutualistic and pathogenic Escherichia coli. The pathway endows its producer with a long-term persistence phenotype in the human bowel, a probiotic activity used in the treatment of ulcerative colitis, and a carcinogenic activity under host inflammatory conditions. To date, functional small molecules from this pathway have not been reported. Here we implemented a comparative metabolomics and targeted structural network analyses approach to identify a catalog of small molecules dependent on the colibactin pathway from the meningitis isolate E. coli IHE3034 and the probiotic E. coli Nissle 1917. The structures of 10 pathway-dependent small molecules are proposed based on structural characterizations and network relationships. The network will provide a roadmap for the structural and functional elucidation of a variety of other small molecules encoded by the pathway. From the characterized small molecule set, in vitro bacterial growth inhibitory and mammalian CNS receptor antagonist activities are presented.

Publication types

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

MeSH terms

  • Algorithms
  • Bacillus subtilis / drug effects
  • Dopamine Antagonists / pharmacology
  • Drug Evaluation, Preclinical / methods
  • Escherichia coli / isolation & purification
  • Escherichia coli / metabolism*
  • Escherichia coli / pathogenicity
  • HeLa Cells / drug effects
  • Humans
  • Magnetic Resonance Spectroscopy
  • Meningitis, Escherichia coli / microbiology
  • Metabolic Networks and Pathways
  • Metabolomics / methods*
  • Molecular Structure
  • Peptides / genetics
  • Peptides / metabolism*
  • Polyketides / metabolism*
  • Probiotics
  • Small Molecule Libraries / chemistry*
  • Small Molecule Libraries / metabolism*
  • Small Molecule Libraries / pharmacology

Substances

  • Dopamine Antagonists
  • Peptides
  • Polyketides
  • Small Molecule Libraries
  • colibactin