Structural Revision and Elucidation of the Biosynthesis of Hypodoratoxide by (13) C,(13) C COSY NMR Spectroscopy

Angew Chem Int Ed Engl. 2015 May 26;54(22):6637-40. doi: 10.1002/anie.201501765. Epub 2015 Apr 15.

Abstract

Feeding of (2,3,4,5,6-(13) C5 )mevalonolactone to the fungus Hypomyces odoratus resulted in a completely labeled sesquiterpene ether. The connectivity of the carbon atoms was easily deduced from a (13) C,(13) C COSY spectrum, revealing a structure that was different from the previously reported structure of hypodoratoxide, even though the reported (13) C NMR data matched. A structural revision of hypodoratoxide is thus presented. Its absolute configuration was tentatively assigned from its co-metabolite cis-dihydroagarofuran. Its biosynthesis was investigated by feeding of (3-(13) C)- and (4,6-(13) C2 )mevalonolactone, which gave insights into the complex rearrangement of the carbon skeleton during terpene cyclization by analysis of the (13) C,(13) C couplings.

Keywords: NMR spectroscopy; biosynthesis; isotopic labeling; structure elucidation; terpenoids.

MeSH terms

  • Ascomycota / metabolism
  • Carbon Isotopes / chemistry
  • Magnetic Resonance Spectroscopy
  • Mevalonic Acid / analogs & derivatives
  • Mevalonic Acid / chemistry
  • Mevalonic Acid / metabolism
  • Molecular Conformation
  • Sesquiterpenes / chemistry
  • Sesquiterpenes / metabolism*

Substances

  • Carbon Isotopes
  • Sesquiterpenes
  • hypodoratoxide
  • mevalonolactone
  • Mevalonic Acid