Alternative mechanisms for O2 release and O-O bond formation in the oxygen evolving complex of photosystem II

Phys Chem Chem Phys. 2015 May 14;17(18):12168-74. doi: 10.1039/c5cp00138b.

Abstract

In a previous detailed study of all the steps of water oxidation in photosystem II, it was surprisingly found that O2 release is as critical for the rate as O-O bond formation. A new mechanism for O2 release has now been found, which can be described as an opening followed by a closing of the interior of the oxygen evolving complex. A transition state for peroxide rotation forming a superoxide radical, missed in the previous study, and a structural change around the outside manganese are two key steps in the new mechanism. However, O2 release may still remain rate-limiting. Additionally, for the step forming the O-O bond, an alternative, experimentally suggested, mechanism was investigated. The new model calculations can rule out the precise use of that mechanism. However, a variant with a rotation of the ligands around the outer manganese by about 30° will give a low barrier, competitive with the old DFT mechanism. Both these mechanisms use an oxyl-oxo mechanism for O-O bond formation involving the same two manganese atoms and the central oxo group (O5).

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Manganese / chemistry
  • Manganese / metabolism
  • Models, Molecular
  • Oxidation-Reduction
  • Oxygen / chemistry
  • Oxygen / metabolism*
  • Photosystem II Protein Complex / chemistry
  • Photosystem II Protein Complex / metabolism*
  • Quantum Theory
  • Thermodynamics
  • Water / metabolism*

Substances

  • Photosystem II Protein Complex
  • Water
  • Manganese
  • Oxygen