Elucidation of the natural artemisinin decomposition route upon iron interaction: a fine electronic redistribution promotes reactivity

Phys Chem Chem Phys. 2008 Sep 1;10(33):5083-93. doi: 10.1039/b804516j. Epub 2008 Jun 25.

Abstract

The conformational analysis of artemisinin by molecular dynamics and quantum chemistry calculations revealed the existence of seven energy minima with specific interconversion pathways. Among the seven conformers, only , and were able to undergo bond rearrangements upon Fe(2+) interaction. These rearrangements were due to a peculiar puckering of the trioxane ring that brings its three oxygen atoms in an ideal geometrical position for interacting with Fe(2+) ions, promoting an electronic redistribution in the molecule. A rapid molecule rearrangement led to a stable energy minimum structure with an additional ring that is similar to a plant metabolite. Our results suggest an alternative pathway for generating toxic radical chemical species for the malaria parasite, where artemisinin is not toxic by itself but rather is an intermediate for molecular partners that generate radical structures deleterious for the parasite proteins, after electron transfers from the Fe(2+)/artemisinin complex.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Antimalarials / chemistry*
  • Artemisinins / chemistry*
  • Circular Dichroism
  • Iron / chemistry*
  • Magnetic Resonance Spectroscopy
  • Models, Molecular
  • Spectrophotometry, Infrared

Substances

  • Antimalarials
  • Artemisinins
  • artemisinin
  • Iron