Towards an artificial model for Photosystem II: a manganese(II,II) dimer covalently linked to ruthenium(II) tris-bipyridine via a tyrosine derivative

J Inorg Biochem. 2000 Jan 15;78(1):15-22. doi: 10.1016/s0162-0134(99)00200-7.

Abstract

In order to model the individual electron transfer steps from the manganese cluster to the photooxidized sensitizer P680+ in Photosystem II (PS II) in green plants, the supramolecular complex 4 has been synthesized. In this complex, a ruthenium(II) tris-bipyridine type photosensitizer has been linked to a manganese(II) dimer via a substituted L-tyrosine, which bridges the manganese ions. The trinuclear complex 4 was characterized by electron paramagnetic resonance (EPR) and electrospray ionization mass spectrometry (ESI-MS). The excited state lifetime of the ruthenium tris-bipyridine moiety in 4 was found to be about 110 ns in acetonitrile. Using flash photolysis in the presence of an electron acceptor (methylviologen), it was demonstrated that in the supramolecular complex 4 an electron was transferred from the excited state of the ruthenium tris-bipyridine moiety to methylviologen, forming a methylviologen radical and a ruthenium(III) tris-bipyridine moiety. Next, the Ru(III) species retrieved the electron from the manganese(II/II) dimer in an intramolecular electron transfer reaction with a rate constant kET > 1.0 x 10(7) s(-1), generating a manganese(II/III) oxidation state and regenerating the ruthenium(II) photosensitizer. This is the first example of intramolecular electron transfer in a supramolecular complex, in which a manganese dimer is covalently linked to a photosensitizer via a tyrosine unit, in a process which mimics the electron transfer on the donor side of PS II.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • 2,2'-Dipyridyl / analogs & derivatives
  • 2,2'-Dipyridyl / chemical synthesis
  • 2,2'-Dipyridyl / chemistry
  • 2,2'-Dipyridyl / metabolism
  • Coordination Complexes
  • Dimerization
  • Electron Spin Resonance Spectroscopy
  • Electrons
  • Gas Chromatography-Mass Spectrometry
  • Hydrogen Bonding
  • Indicators and Reagents / chemistry
  • Manganese / chemistry
  • Manganese / metabolism
  • Models, Molecular
  • Molecular Structure
  • Nuclear Magnetic Resonance, Biomolecular
  • Organometallic Compounds / chemical synthesis
  • Organometallic Compounds / chemistry
  • Organometallic Compounds / metabolism
  • Photolysis
  • Photosynthetic Reaction Center Complex Proteins / chemistry*
  • Photosystem II Protein Complex
  • Spectrometry, Mass, Fast Atom Bombardment
  • Tyrosine / chemical synthesis
  • Tyrosine / chemistry
  • Tyrosine / metabolism

Substances

  • Coordination Complexes
  • Indicators and Reagents
  • Organometallic Compounds
  • Photosynthetic Reaction Center Complex Proteins
  • Photosystem II Protein Complex
  • tris(2,2-bipyridine)-ruthenium(II)
  • Tyrosine
  • Manganese
  • 2,2'-Dipyridyl