Synthesis of regio- and stereoselectively deuterium-labelled derivatives of L-glutamate semialdehyde for studies on carbapenem biosynthesis

Org Biomol Chem. 2009 Jul 7;7(13):2770-9. doi: 10.1039/b903312b. Epub 2009 May 11.

Abstract

L-glutamate semialdehyde (L-GSA) is an intermediate in biosynthetic pathways including those leading to the carbapenem antibiotics. We describe studies on asymmetric deuteration or hydrogenation of appropriate didehydro-amino acid precursors for the stereoselective synthesis of C-2- and/or C-3-[2H]-labelled L-GSA suitable for use in mechanistic studies. Regioselective deuterium incorporation into the 5-position of L-GSA was achieved using a labelled form of the Schwartz reagent (Cp2Zr2HCl). 4,4-Dideuterated and fully backbone deuterated L-GSAs were prepared. The application of the labelled L-GSA derivatives to biosynthetic studies was exemplified by the chemo-enzymatic preparation of selectively deuterated trans-carboxymethylprolines using two different carboxymethylproline synthases (CarB and ThnE), enzymes that catalyse early steps in the biosynthesis of two carbapenems: (5R)-carbapenem-3-carboxylate and thienamycin, respectively.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Carbapenems / biosynthesis*
  • Carbapenems / chemistry
  • Deuterium / chemistry*
  • Glutamates / chemical synthesis*
  • Glutamates / chemistry
  • Glutamates / metabolism
  • Hydrogenation
  • Isotope Labeling
  • Molecular Conformation
  • Stereoisomerism

Substances

  • Carbapenems
  • Glutamates
  • glutamic acid gamma-semialdehyde
  • Deuterium