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Synthesis and Electron-Transfer Processes in a New Family of Ligands for Coupled Ru−Mn2 Complexes

Authors

  • Dr. Erik A. Karlsson,

    1. Department of Organic Chemistry, Arrhenius Laboratory, Stockholm University, 106 91 Stockholm (Sweden)
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  • Dr. Bao-Lin Lee,

    1. Department of Organic Chemistry, Arrhenius Laboratory, Stockholm University, 106 91 Stockholm (Sweden)
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  • Dr. Rong-Zhen Liao,

    1. Department of Organic Chemistry, Arrhenius Laboratory, Stockholm University, 106 91 Stockholm (Sweden)
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  • Dr. Torbjörn Åkermark,

    1. Department of Organic Chemistry, Arrhenius Laboratory, Stockholm University, 106 91 Stockholm (Sweden)
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  • Dr. Markus D. Kärkäs,

    1. Department of Organic Chemistry, Arrhenius Laboratory, Stockholm University, 106 91 Stockholm (Sweden)
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  • Valeria Saavedra Becerril,

    1. Department of Chemical and Biological Engineering, Chalmers University of Technology, 412 96 Gothenburg (Sweden)
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  • Prof. Per E. M. Siegbahn,

    1. Department of Organic Chemistry, Arrhenius Laboratory, Stockholm University, 106 91 Stockholm (Sweden)
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  • Prof. Xiaodong Zou,

    1. Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, 106 91 Stockholm (Sweden)
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  • Prof. Maria Abrahamsson,

    Corresponding author
    1. Department of Chemical and Biological Engineering, Chalmers University of Technology, 412 96 Gothenburg (Sweden)
    • Maria Abrahamsson, Department of Chemical and Biological Engineering, Chalmers University of Technology, 412 96 Gothenburg (Sweden)

      Björn Åkermark, Department of Organic Chemistry, Arrhenius Laboratory, Stockholm University, 106 91 Stockholm (Sweden)

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  • Prof. Björn Åkermark

    Corresponding author
    1. Department of Organic Chemistry, Arrhenius Laboratory, Stockholm University, 106 91 Stockholm (Sweden)
    • Maria Abrahamsson, Department of Chemical and Biological Engineering, Chalmers University of Technology, 412 96 Gothenburg (Sweden)

      Björn Åkermark, Department of Organic Chemistry, Arrhenius Laboratory, Stockholm University, 106 91 Stockholm (Sweden)

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Abstract

A series of [Ru(bpy)3]2+-type (bpy=2,2′-bipyridine) photosensitisers have been coupled to a ligand for Mn, which is expected to give a dinuclear complex that is active as a water oxidation catalyst. Unexpectedly, photophysical studies showed that the assemblies had very short lived excited states and that the decay patterns were complex and strongly dependent on pH. One dyad was prepared that was capable of catalysing chemical water oxidation by using [Ru(bpy)3]3+ as an oxidant. However, photochemical water oxidation in the presence of an external electron acceptor failed, presumably because the short excited-state lifetime precluded initial electron transfer to the added acceptor. The photophysical behaviour could be explained by the presence of an intricate excited-state manifold, as also suggested by time-dependent DFT calculations.

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