The position of a key tyrosine in dTDP-4-Keto-6-deoxy-D-glucose-5-epimerase (EvaD) alters the substrate profile for this RmlC-like enzyme

J Biol Chem. 2004 Jul 30;279(31):32684-91. doi: 10.1074/jbc.M404091200. Epub 2004 May 24.

Abstract

Vancomycin, the last line of defense antibiotic, depends upon the attachment of the carbohydrate vancosamine to an aglycone skeleton for antibacterial activity. Vancomycin is a naturally occurring secondary metabolite that can be produced by bacterial fermentation. To combat emerging resistance, it has been proposed to genetically engineer bacteria to produce analogues of vancomycin. This requires a detailed understanding of the biochemical steps in the synthesis of vancomycin. Here we report the 1.4 A structure and biochemical characterization of EvaD, an RmlC-like protein that is required for the C-5' epimerization during synthesis of dTDP-epivancosamine. EvaD, although clearly belonging to the RmlC class of enzymes, displays very low activity in the archetypal RmlC reaction (double epimerization of dTDP-6-deoxy-4-keto-D-glucose at C-3' and C-5'). The high resolution structure of EvaD compared with the structures of authentic RmlC enzymes indicates that a subtle change in the enzyme active site repositions a key catalytic Tyr residue. A mutant designed to re-establish the normal position of the Tyr increases the RmlC-like activity of EvaD.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Amino Acid Sequence
  • Anti-Bacterial Agents / pharmacology*
  • Carbohydrate Epimerases / chemistry*
  • Carbohydrate Sequence
  • Carbohydrates
  • Catalysis
  • Circular Dichroism
  • Crystallography, X-Ray
  • Kinetics
  • Mass Spectrometry
  • Models, Chemical
  • Models, Molecular
  • Molecular Sequence Data
  • Mutagenesis
  • Mutagenesis, Site-Directed
  • Protein Conformation
  • Protein Structure, Secondary
  • Salmonella enterica / metabolism
  • Sequence Homology, Amino Acid
  • Structure-Activity Relationship
  • Substrate Specificity
  • Tyrosine / chemistry*
  • Vancomycin / chemistry
  • Vancomycin / pharmacology*

Substances

  • Anti-Bacterial Agents
  • Carbohydrates
  • Tyrosine
  • Vancomycin
  • Carbohydrate Epimerases
  • dTDP-4-keto-6-deoxyglucose-5-epimerase
  • dTDP-4-ketorhamnose 3,5-epimerase

Associated data

  • PDB/1OFN
  • PDB/1OI6