Modular polyketide synthases and cis double bond formation: establishment of activated cis-3-cyclohexylpropenoic acid as the diketide intermediate in phoslactomycin biosynthesis

J Am Chem Soc. 2007 Feb 21;129(7):1910-1. doi: 10.1021/ja068818t. Epub 2007 Jan 27.

Abstract

The majority of modular polyketide synthase (PKS) systems which generate unsaturated products do so with trans double bonds. Phoslactomycin B (PLM B) presents a class of antitumor and antiviral natural polyketide products that have unique structural features, including a linear unsaturated backbone with one trans and three cis double bonds. There is substantial evidence that trans double bonds are established by ketoreductase-dehydratase (KR-DH) didomains within a PKS module. In cases where modules containing these didomains appear to generate product containing a cis double bond there is no experimental evidence to determine if they do so directly, or if they also form a trans double bond with a subsequent isomerization step. A critical step in addressing this issue is establishing the stereochemistry of the polyketide intermediate which passes to the subsequent module. Herein, we demonstrate through a series of experiments that an activated cis-3-cyclohexylpropenoic acid is the diketide intermediate which passes from module 1 to module 2 of the PLM PKS. The trans isomer of the diketide intermediate could not be processed directly into PLM B by module 2, but could be converted to PLM B by degradation to cyclohexanecarboxylic acid and elongation by the entire PLM PKS. These observations indicate not only that module 1 with a DH-KR didomain is responsible for establishing C14–C15 cis double bond of PLM B, but that the subsequent modules of the PKS clearly discriminate between the cis and trans-diketide intermediate and do not contain domains capable of catalyzing double bond isomerization.

Publication types

  • Research Support, N.I.H., Extramural

MeSH terms

  • Caprylates / metabolism
  • Lactones / metabolism
  • Organophosphorus Compounds / metabolism
  • Polyketide Synthases / genetics
  • Polyketide Synthases / metabolism*
  • Propionates / metabolism*
  • Stereoisomerism
  • Streptomyces / genetics
  • Streptomyces / metabolism

Substances

  • Caprylates
  • Lactones
  • N-(8-(2-hydroxybenzoyl)amino)caprylate
  • Organophosphorus Compounds
  • Propionates
  • phoslactomycin B
  • Polyketide Synthases