{1,1′-(Dimethylsilylene)bis[methanechalcogenolato]}diiron Complexes [2Fe2E(Si)] (E=S, Se, Te) – [FeFe] Hydrogenase Models

Authors

  • Ulf-Peter Apfel,

    1. Institut für Anorganische und Analytische Chemie, Friedrich-Schiller-Universität Jena, Humboldtstrasse 8, D-07743 Jena
    2. Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA, 02139, USA
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  • Helmar Görls,

    1. Institut für Anorganische und Analytische Chemie, Friedrich-Schiller-Universität Jena, Humboldtstrasse 8, D-07743 Jena
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  • Greg A. N. Felton,

    1. Department of Chemistry and Biochemistry, The University of Arizona, Tucson, AZ, 85721, USA
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  • Dennis H. Evans,

    Corresponding author
    1. Department of Chemistry, Purdue University, West Lafayette, IN, 47907, USA
    • Dennis H. Evans, Department of Chemistry, Purdue University, West Lafayette, IN, 47907, USA

      Richard S. Glass, Department of Chemistry and Biochemistry, The University of Arizona, Tucson, AZ, 85721, USA

      Dennis L. Lichtenberger, Department of Chemistry and Biochemistry, The University of Arizona, Tucson, AZ, 85721, USA

      Wolfgang Weigand, Institut für Anorganische und Analytische Chemie, Friedrich-Schiller-Universität Jena, Humboldtstrasse 8, D-07743 Jena

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  • Richard S. Glass,

    Corresponding author
    1. Department of Chemistry and Biochemistry, The University of Arizona, Tucson, AZ, 85721, USA
    • Dennis H. Evans, Department of Chemistry, Purdue University, West Lafayette, IN, 47907, USA

      Richard S. Glass, Department of Chemistry and Biochemistry, The University of Arizona, Tucson, AZ, 85721, USA

      Dennis L. Lichtenberger, Department of Chemistry and Biochemistry, The University of Arizona, Tucson, AZ, 85721, USA

      Wolfgang Weigand, Institut für Anorganische und Analytische Chemie, Friedrich-Schiller-Universität Jena, Humboldtstrasse 8, D-07743 Jena

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  • Dennis L. Lichtenberger,

    Corresponding author
    1. Department of Chemistry and Biochemistry, The University of Arizona, Tucson, AZ, 85721, USA
    • Dennis H. Evans, Department of Chemistry, Purdue University, West Lafayette, IN, 47907, USA

      Richard S. Glass, Department of Chemistry and Biochemistry, The University of Arizona, Tucson, AZ, 85721, USA

      Dennis L. Lichtenberger, Department of Chemistry and Biochemistry, The University of Arizona, Tucson, AZ, 85721, USA

      Wolfgang Weigand, Institut für Anorganische und Analytische Chemie, Friedrich-Schiller-Universität Jena, Humboldtstrasse 8, D-07743 Jena

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  • Wolfgang Weigand

    Corresponding author
    1. Institut für Anorganische und Analytische Chemie, Friedrich-Schiller-Universität Jena, Humboldtstrasse 8, D-07743 Jena
    • Dennis H. Evans, Department of Chemistry, Purdue University, West Lafayette, IN, 47907, USA

      Richard S. Glass, Department of Chemistry and Biochemistry, The University of Arizona, Tucson, AZ, 85721, USA

      Dennis L. Lichtenberger, Department of Chemistry and Biochemistry, The University of Arizona, Tucson, AZ, 85721, USA

      Wolfgang Weigand, Institut für Anorganische und Analytische Chemie, Friedrich-Schiller-Universität Jena, Humboldtstrasse 8, D-07743 Jena

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Abstract

(Bis-selenolato) and (bis-tellurolato)diiron complexes [2Fe2E(Si)] were prepared and compared with the known (bis-thiolato)diiron complex A to assess their ability to produce hydrogen from protons. Treatment of [Fe3(CO)12] with 4,4-dimethyl-1,2,4-diselenasilolane (1) in boiling toluene afforded hexacarbonyl{μ-{[1,1′-(dimethylsilylene)bis[methaneselenolato-κSe : κSe]](2 −)}}diiron(Fe[BOND]Fe) (2). The analog bis-tellurolato complex hexacarbonyl{μ-{[1,1′-(dimethylsilylene)bis[methanetellurolato-κTe : κTe]](2 −)}}diiron(Fe[BOND]Fe) (3) was obtained by treatment of [Fe3(CO)12] with dimethylbis(tellurocyanatomethyl)dimethylsilane, which was prepared in situ. All compounds were characterized by NMR, IR spectroscopy, mass spectrometry, elemental analysis and single-crystal X-ray analysis. The electrocatalytic properties of the [2Fe2X(Si)] (X=S, Se, Te) model complexes A, 1, and 2 towards hydrogen formation were evaluated.

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