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Identification and Characterization of the “Super-Reduced” State of the H-Cluster in [FeFe] Hydrogenase: A New Building Block for the Catalytic Cycle?

Authors

  • Agnieszka Adamska,

    1. Max-Planck-Institut für Chemische Energiekonversion, Stiftstrasse 34–36, 45470 Mülheim an der Ruhr (Germany)
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  • Dr. Alexey Silakov,

    Corresponding author
    1. Max-Planck-Institut für Chemische Energiekonversion, Stiftstrasse 34–36, 45470 Mülheim an der Ruhr (Germany)
    • Max-Planck-Institut für Chemische Energiekonversion, Stiftstrasse 34–36, 45470 Mülheim an der Ruhr (Germany)
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  • Dr. Camilla Lambertz,

    1. Lehrstuhl Biochemie der Pflanzen, AG Photobiotechnologie, Ruhr Universität Bochum, Universitätsstrasse 150, 44801 Bochum (Germany)
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  • Dr. Olaf Rüdiger,

    1. Max-Planck-Institut für Chemische Energiekonversion, Stiftstrasse 34–36, 45470 Mülheim an der Ruhr (Germany)
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  • Prof. Thomas Happe,

    1. Lehrstuhl Biochemie der Pflanzen, AG Photobiotechnologie, Ruhr Universität Bochum, Universitätsstrasse 150, 44801 Bochum (Germany)
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  • Dr. Edward Reijerse,

    Corresponding author
    1. Max-Planck-Institut für Chemische Energiekonversion, Stiftstrasse 34–36, 45470 Mülheim an der Ruhr (Germany)
    • Max-Planck-Institut für Chemische Energiekonversion, Stiftstrasse 34–36, 45470 Mülheim an der Ruhr (Germany)
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  • Prof. Wolfgang Lubitz

    Corresponding author
    1. Max-Planck-Institut für Chemische Energiekonversion, Stiftstrasse 34–36, 45470 Mülheim an der Ruhr (Germany)
    • Max-Planck-Institut für Chemische Energiekonversion, Stiftstrasse 34–36, 45470 Mülheim an der Ruhr (Germany)
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  • Gudrun Klihm and Leslie Currell are gratefully acknowledged for their technical support in the EPR and FTIR experiments. Financial Support from the Max Planck Society and the EU (FP7 Energy 212508 “SOLAR H2”) is gratefully acknowledged.

Abstract

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Super-reduced and super-active: A new redox state in the active site of algal [FeFe] hydrogenases has been identified and characterized by EPR and FTIR spectroscopy. Electrochemical and in vitro essays show that this species is highly active in hydrogen production and suggest that it is a key intermediate in the catalytic cycle of all [FeFe] hydrogenases.

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