Malonyl carba(dethia)- and malonyl oxa(dethia)-coenzyme A as tools for trapping polyketide intermediates

Chembiochem. 2009 Jul 6;10(10):1714-23. doi: 10.1002/cbic.200900093.

Abstract

In order to study intermediates in polyketide biosynthesis two nonhydrolyzable malonyl coenzyme A analogues were synthesised by a chemoenzymatic route. In these analogues the sulfur atom of CoA was replaced either by a methylene group (carbadethia analogue) or by an oxygen atom (oxadethia analogue). These malonyl-CoA analogues were found to compete with the natural extender unit malonyl-CoA and to trap intermediates from stilbene synthase, a type III polyketide synthase (PKS). From the reaction of stilbene synthase with its natural phenylpropanoid substrates, diketide, triketide and tetraketide species were successfully off-loaded and characterised by LC-MS. Moreover, the reactivity of the nonhydrolyzable analogues offers insights into the flexibility of substrate alignment in the PKS active site for efficient malonyl decarboxylation and condensation.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Acyltransferases / metabolism*
  • Adenine Nucleotides / biosynthesis
  • Adenine Nucleotides / chemistry*
  • Adenine Nucleotides / pharmacology
  • Antioxidants / chemistry*
  • Biocatalysis
  • Chromatography, Liquid
  • Macrolides / chemistry*
  • Malonyl Coenzyme A / biosynthesis
  • Malonyl Coenzyme A / chemistry*
  • Malonyl Coenzyme A / pharmacology
  • Mass Spectrometry

Substances

  • Adenine Nucleotides
  • Antioxidants
  • Macrolides
  • malonylcarba(dethia)-coenzyme A
  • malonyloxa(dethia)-coenzyme A
  • Malonyl Coenzyme A
  • Acyltransferases
  • stilbene synthase