Clorobiocin biosynthesis in Streptomyces: identification of the halogenase and generation of structural analogs

Chem Biol. 2003 Mar;10(3):279-88. doi: 10.1016/s1074-5521(03)00051-6.

Abstract

Clorobiocin (clo) and novobiocin (nov) are potent inhibitors of bacterial DNA gyrase. The two substances differ in the substitution pattern at C-8' of the aminocoumarin ring, carrying a chlorine atom or a methyl group, respectively. By gene inactivation, clo-hal was identified as the gene of the halogenase responsible for the introduction of the chlorine atom of clorobiocin. Inactivation of cloZ did not affect clorobiocin formation, showing that this ORF is not essential for clorobiocin biosynthesis. Expression of the methyltransferase gene novO in the clo-hal(-) mutant led to the very efficient formation of a hybrid antibiotic containing a methyl group instead of a chlorine atom at C-8'. Comparison of the antibacterial activity of clorobiocin analogs with -Cl, -H, or -CH(3) at C-8' showed that chlorine leads to 8-fold higher activity than hydrogen and to 2-fold higher activity than a methyl group.

Publication types

  • Comparative Study
  • Research Support, Non-U.S. Gov't

MeSH terms

  • Anti-Bacterial Agents / biosynthesis*
  • Anti-Bacterial Agents / chemistry
  • Methyltransferases / biosynthesis
  • Mutation
  • Novobiocin / analogs & derivatives*
  • Novobiocin / biosynthesis*
  • Novobiocin / chemistry
  • Oxidoreductases / genetics
  • Oxidoreductases / metabolism*
  • Streptomyces / enzymology
  • Streptomyces / metabolism*
  • Structure-Activity Relationship

Substances

  • Anti-Bacterial Agents
  • novclobiocin 101
  • novclobiocin 102
  • Novobiocin
  • clorobiocin
  • Oxidoreductases
  • Methyltransferases