Precursor-directed biosynthesis: biochemical basis of the remarkable selectivity of the erythromycin polyketide synthase toward unsaturated triketides

Chem Biol. 2002 Jan;9(1):131-42. doi: 10.1016/s1074-5521(02)00089-3.

Abstract

The structural basis for the striking stereochemical discrimination among triketide analogs has been investigated by incubating a series of N-acetyl cysteamine (-SNAC) esters of unsaturated triketides with DEBS module 2+TE. The triketide analogs were first screened under a standard set of short-term incubation conditions in the presence of the extender substrate methylmalonyl-CoA and NADPH. For those triketide analogs that served as substrates for module 2+TE, the relative specificity, represented by the k(cat)/K(M) values, was quantitated. Triketide diastereomers that were converted in precursor-directed biosynthesis experiments to unsaturated 16-membered ring macrolides by DEBS(KS1(0)) were good to excellent substrates for DEBS module 2+TE, whereas analogs that were converted to the 14-membered ring analogs of 10,11-dehydro-6-deoxyerythronolide B by DEBS(KS1(0)) were not turned over at all by module 2+TE.

Publication types

  • Research Support, U.S. Gov't, P.H.S.

MeSH terms

  • Binding, Competitive
  • Erythromycin / biosynthesis*
  • Kinetics
  • Multienzyme Complexes / chemistry*
  • Multienzyme Complexes / metabolism
  • Protein Precursors / biosynthesis
  • Protein Precursors / metabolism
  • Saccharopolyspora / metabolism
  • Substrate Specificity

Substances

  • Multienzyme Complexes
  • Protein Precursors
  • Erythromycin