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Ammonia binding to ...
Ammonia binding to the oxygen-evolving complex of photosystem II identifies the solvent-exchangeable oxygen bridge (µ-oxo) of the manganese tetramer
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- Navarro, Montserrat Perez (författare)
- Max Planck Inst Chem Energiekonvers, D-45470 Mulheim, Germany.
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- Ames, William M. (författare)
- Max Planck Inst Chem Energiekonvers, D-45470 Mulheim, Germany.
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- Nilsson, Håkan (författare)
- Umeå universitet,Kemiska institutionen,Umea Univ, Chem Biol Ctr, Dept Chem, S-90187 Umea, Sweden.
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- Lohmiller, Thomas (författare)
- Max Planck Inst Chem Energiekonvers, D-45470 Mulheim, Germany.
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- Pantazis, Dimitrios A. (författare)
- Max Planck Inst Chem Energiekonvers, D-45470 Mulheim, Germany.
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- Rapatskiy, Leonid (författare)
- Max Planck Inst Chem Energiekonvers, D-45470 Mulheim, Germany.
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- Nowaczyk, Marc M. (författare)
- Ruhr Univ Bochum, D-44780 Bochum, Germany.
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- Neese, Frank (författare)
- Max Planck Inst Chem Energiekonvers, D-45470 Mulheim, Germany.
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- Boussac, Alain (författare)
- CEA Saclay, CNRS, iBiTec S, UMR 8221, F-91191 Gif Sur Yvette, France.
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- Messinger, Johannes (författare)
- Umeå universitet,Kemiska institutionen,Umea Univ, Chem Biol Ctr, Dept Chem, S-90187 Umea, Sweden.
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- Lubitz, Wolfgang (författare)
- Max Planck Inst Chem Energiekonvers, D-45470 Mulheim, Germany.
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- Cox, Nicholas (författare)
- Max Planck Inst Chem Energiekonvers, D-45470 Mulheim, Germany.
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Max Planck Inst Chem Energiekonvers, D-45470 Mulheim, Germany Kemiska institutionen (creator_code:org_t)
- 2013-09-10
- 2013
- Engelska.
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Ingår i: Proceedings of the National Academy of Sciences of the United States of America. - : Proceedings of the National Academy of Sciences. - 0027-8424 .- 1091-6490. ; 110:39, s. 15561-15566
- Relaterad länk:
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https://www.pnas.org...
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https://urn.kb.se/re...
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https://doi.org/10.1...
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https://urn.kb.se/re...
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Abstract
Ämnesord
Stäng
- The assignment of the two substrate water sites of the tetramanganese penta-oxygen calcium (Mn4O5Ca) cluster of photosystem II is essential for the elucidation of the mechanism of biological O-O bond formation and the subsequent design of bio-inspired water-splitting catalysts. We recently demonstrated using pulsed EPR spectroscopy that one of the five oxygen bridges (mu-oxo) exchanges unusually rapidly with bulk water and is thus a likely candidate for one of the substrates. Ammonia, a water analog, was previously shown to bind to the Mn4O5Ca cluster, potentially displacing a water/substrate ligand [Britt RD, et al. (1989) J Am Chem Soc 111(10):3522-3532]. Here we show by a combination of EPR and time-resolved membrane inlet mass spectrometry that the binding of ammonia perturbs the exchangeable mu-oxo bridge without drastically altering the binding/exchange kinetics of the two substrates. In combination with broken-symmetry density functional theory, our results show that (i) the exchangable mu-oxo bridge is O5 {using the labeling of the current crystal structure [Umena Y, et al. (2011) Nature 473(7345):55-60]}; (ii) ammonia displaces a water ligand to the outer manganese (Mn-A4-W1); and (iii) as W1 is trans to O5, ammonia binding elongates the Mn-A4-O5 bond, leading to the perturbation of the mu-oxo bridge resonance and to a small change in the water exchange rates. These experimental results support O-O bond formation between O5 and possibly an oxyl radical as proposed by Siegbahn and exclude W1 as the second substrate water.
Ämnesord
- TEKNIK OCH TEKNOLOGIER -- Kemiteknik (hsv//swe)
- ENGINEERING AND TECHNOLOGY -- Chemical Engineering (hsv//eng)
- NATURVETENSKAP -- Biologi -- Biokemi och molekylärbiologi (hsv//swe)
- NATURAL SCIENCES -- Biological Sciences -- Biochemistry and Molecular Biology (hsv//eng)
Nyckelord
- PSII
- OEC
- water oxidizing complex
- water-oxidation
- Mn cluster
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Navarro, Montser ...
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Ames, William M.
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Nilsson, Håkan
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Lohmiller, Thoma ...
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Pantazis, Dimitr ...
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Rapatskiy, Leoni ...
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Nowaczyk, Marc M ...
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Neese, Frank
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Boussac, Alain
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Messinger, Johan ...
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Lubitz, Wolfgang
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Cox, Nicholas
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