Biosynthesis of the phenazine antibiotics, the saphenamycins and esmeraldins, in Streptomyces antibioticus

The Journal of Organic Chemistry
1993.0

Abstract

The biosynthesis of the phenazine antibiotics, the esmeraldins and the related saphenamycins, was studied by feeding radioactive and stable isotope-labeled precursors to Streptomyces antibioticus, strain TU 2706. After purification, the labeled antibiotics were degraded to the diastereomeric esmeraldic acid dimethyl esters 3 and 4 and racemic saphenic acid methyl ester (51, respectively. The 'H- and W-NMR spectra of these were assigned by single and multiple bond correlation experiments. Although 1%- and 13C-labeled shikimic acid was not incorporated, W-NMR analysis of the samples biosynthesized from [U-W3]-, [ lI3J3C2]-, and [2-'3Clglycerol provided evidence that these phenazine antibiotics are derived from the shikimic acid pathway and display the same head-to-tail coupling pattern of monomer units seen in other phenazine antibiotics. The extra methyl group attached to the carbon corresponding to the shikimate carboxyl group originates from C-2 of acetate. Radiolabeled saphenic acid was incorporated into the diphenazine ring system of the esmeraldins. Mechanistic aspects of the formation of the phenazine and diphenazine ring systems are discussed.

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