XANES evidence against a manganyl species in the S3 state of the oxygen-evolving complex

J Am Chem Soc. 2004 Jul 7;126(26):8070-1. doi: 10.1021/ja0494104.

Abstract

Manganyl Mn=O species have been suggested as possible intermediates in photosynthetic water oxidation and as the reactive species in asymmetric olefin epoxidation. The first X-ray absorption spectrum for a MnV=O complex is reported. Comparison of the EXAFS data for Na[MnV=O(HMPAB) with those for lower-valent Mn complexes suggests that EXAFS measurements and edge-energy measurements are unlikely to have sufficient sensitivity to reliably reflect the presence of Mn=O species. In contrast, the preedge transition for Na[MnV=O(HMPAB) is 4-fold more intense than the most intense preedge transition observed for nonmanganyl complexes. This increase in intensity is shown to be sufficiently sensitive to allow detection of a manganyl species if it is formed. These data together with published data for the photosynthetic oxygen-evolving complex provide strong evidence against the presence of manganyl Mn=O species in the oxygen-evolving complex through the S3 state.

Publication types

  • Research Support, U.S. Gov't, Non-P.H.S.
  • Research Support, U.S. Gov't, P.H.S.

MeSH terms

  • Manganese / chemistry*
  • Oxidation-Reduction
  • Oxygen / chemistry*
  • Photosystem II Protein Complex / chemistry*
  • Spectrometry, X-Ray Emission

Substances

  • Photosystem II Protein Complex
  • Manganese
  • Oxygen