Type-2 isopentenyl diphosphate isomerase. Mechanistic studies with cyclopropyl and epoxy analogues

J Am Chem Soc. 2007 Jun 27;129(25):7740-1. doi: 10.1021/ja072501r. Epub 2007 Jun 5.

Abstract

Type-2 isopentenyl diphosphate isomerase, which catalyzes the interconversion if isopentenyl diphosphate and dimethylallyl diphosphate, contains a tightly bound molecule of FMN. Incubation of the active enzyme•FMNH2 complex with an analog of isopentenyl diphosphate, where the methyl group has been replaced with a cyclopropane ring, results in isomerization of the analog to the corresponding allylic isomer without inactivation of the enzyme. In contrast, the related epoxide analog is a potent irreversible inhibitor that covalently modifies the flavin cofactor in a proton-initiated reaction. These results suggest that the mechanism for isomerization by the type-2 isopentenyl diphosphate isomerase may be similar to the protonation-deprotonation sequence of the type-1 enzyme and places limits on the lifetimes of radical intermediates in an alternative hydrogen atom addition/abstraction mechanism.

Publication types

  • Research Support, N.I.H., Extramural

MeSH terms

  • Carbon-Carbon Double Bond Isomerases / chemistry*
  • Carbon-Carbon Double Bond Isomerases / metabolism*
  • Catalysis
  • Hemiterpenes / chemistry
  • Hemiterpenes / metabolism
  • Molecular Structure
  • Organophosphorus Compounds / chemistry
  • Organophosphorus Compounds / metabolism
  • Protein Conformation

Substances

  • Hemiterpenes
  • Organophosphorus Compounds
  • 3,3-dimethylallyl pyrophosphate
  • Carbon-Carbon Double Bond Isomerases
  • isopentenyldiphosphate delta-isomerase