Photoassembly of the manganese cluster in mutants perturbed in the high affinity Mn-binding site of the H2O-oxidation complex of photosystem II

Biochemistry. 2007 Nov 27;46(47):13648-57. doi: 10.1021/bi700761v. Epub 2007 Nov 2.

Abstract

The light-driven, oxidative assembly of Mn2+ ions into the H2O-oxidation complex (WOC) of the photosystem II (PSII) reaction center is termed photoactivation and culminates in the formation of the oxygen-evolving (Mn4-Ca) center of the WOC. Initial binding and photooxidation of Mn2+ to the apoprotein is critically dependent upon aspartate 170 of the D1 protein (D1-D170) of the high affinity Mn site [Nixon and Diner (1992) Biochemistry 31, 942-948]. Three O2-evolving mutant strains of Synechocystis, D1-D170E, D1-D170H, and D1-D170V, were studied in terms of the kinetics of photoactivation under both continuous and flashing light. Photoactivation using single turnover flashes revealed D1-D170H and D1-D170V, but not D1-D170E, were prone to form substantial amounts ( approximately 40-50%) of inactive centers ascribed to photoligation of aberrant nonfunctional Mn based upon the reversibility of the inactivation and similarity to previous in vitro results [Chen, C., Kazimir, J., and Cheniae, G. M. (1995) Biochemistry 34, 13511-13526]. On the other hand, D1-D170E lowers the quantum efficiency of photoactivation compared to the wild-type by the largest amount (80% decrease) versus D1-D170H and D1-D170V, which do not produce measurable decreases in quantum efficiency. The low quantum efficiency of photoactivation in D1-D170E is due to the destabilization of photoactivation intermediates. Numerical analysis indicates that the PSII centers in D1-D170E are heterogeneous with respect to photoactivation kinetics and that the majority of centers are characterized by intermediates that decay approximately 10-fold more rapidly than the wild-type control. Additionally, the kinetics of O2 release during the S3-S0 transition was markedly retarded in D1-D170E, in contrast to D1-D170H and D1-D170V, which did not exhibit a discernible slow-down compared to the wild-type.

Publication types

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

MeSH terms

  • Binding Sites
  • Cells, Cultured
  • Hydroxylamine / pharmacology
  • Kinetics
  • Manganese / chemistry*
  • Manganese / metabolism
  • Mutagenesis, Site-Directed
  • Oxidation-Reduction
  • Photolysis
  • Photosystem II Protein Complex / chemistry*
  • Photosystem II Protein Complex / metabolism
  • Synechocystis / genetics
  • Water / chemistry*
  • Water / metabolism

Substances

  • Photosystem II Protein Complex
  • Water
  • Hydroxylamine
  • Manganese