Characterization of the aminocoumarin ligase SimL from the simocyclinone pathway and tandem incubation with NovM,P,N from the novobiocin pathway

Biochemistry. 2005 Mar 29;44(12):4949-56. doi: 10.1021/bi047303g.

Abstract

Simocyclinone D(8) consists of an anguicycline C-glycoside tethered by a tetraene diester linker to an aminocoumarin. Unlike the antibiotics novobiocin, clorobiocin, and coumermycin A(1), the phenolic hydroxyl group of the aminocoumarin in simocyclinone is not glycosylated with a decorated noviosyl moiety that is the pharmacophore for targeting bacterial DNA gyrase. We have expressed the Streptomyces antibioticus simocyclinone ligase SimL, purified it from Escherichia coli, and established its ATP-dependent amide bond forming activity with a variety of polyenoic acids including retinoic acid and fumagillin. We have then used the last three enzymes from the novobiocin pathway, NovM, NovP, and NovN, to convert a SimL product to a novel novobiocin analogue, in which the 3-prenyl-4-hydroxybenzoate of novobiocin is replaced with a tetraenoate moiety, to evaluate antibacterial activity.

Publication types

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

MeSH terms

  • Amide Synthases / biosynthesis
  • Amide Synthases / chemistry*
  • Amide Synthases / genetics
  • Amide Synthases / isolation & purification
  • Aminocoumarins
  • Anti-Bacterial Agents / pharmacology
  • Carboxylic Acids / chemistry
  • Carboxylic Acids / metabolism
  • Coumarins / chemistry*
  • Coumarins / metabolism*
  • Gene Expression Regulation, Bacterial
  • Glycosides / biosynthesis*
  • Glycosides / chemistry*
  • Novobiocin / analogs & derivatives*
  • Novobiocin / biosynthesis
  • Novobiocin / chemistry
  • Novobiocin / metabolism*
  • Streptomyces antibioticus / enzymology*
  • Streptomyces antibioticus / genetics
  • Substrate Specificity

Substances

  • Aminocoumarins
  • Anti-Bacterial Agents
  • Carboxylic Acids
  • Coumarins
  • Glycosides
  • simocyclinone D8
  • Novobiocin
  • clorobiocin
  • Amide Synthases
  • coumermycin