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Self-Assembly of a Diferrous Triple-Stranded Helicate with Bis(2,2‘-Bipyridine) Ligands: Thermodynamic and Kinetic Intermediates

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    Self-Assembly of a Diferrous Triple-Stranded Helicate with Bis(2,2‘-Bipyridine) Ligands: Thermodynamic and Kinetic Intermediates
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    Laboratoire de Physico-Chimie Bioinorganique, UMR 7509 du CNRS, Faculté de Chimie, 1 rue Blaise Pascal, 67000 Strasbourg, France, Laboratoire de Spectrométrie de Masse Bioorganique, UMR 7509 du CNRS, Faculté de Chimie, 1 rue Blaise Pascal, 67000 Strasbourg, France, and Laboratoire de Chimie Biomimétique, UMR 5616 du CNRS, 301 rue de la Chimie, 38041 Grenoble, France
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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2000, 39, 25, 5771–5778
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    https://doi.org/10.1021/ic000229f
    Published November 15, 2000
    Copyright © 2000 American Chemical Society
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    Abstract

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    The protonation and iron(II) coordination properties of a bis(2,2‘-bipyridine) ligand L were investigated in methanol. The protonated forms showed allosteric effects due to the flexibility of the strand. Speciation studies of the corresponding ferrous complexes were carried out as a function of pH and iron(II) concentrations. A combination of electrospray mass spectroscopy, potentiometry, and spectrophotometry allowed the determination in solution of three ferrous complexes, one mononuclear (L2Fe2+) and two dinuclear (L2Fe24+ and L3Fe24+) species. Their structure was deduced from the metal spin state and confirmed by 1H NMR measurements and molecular modeling. The dissociation process of the triple-stranded diferrous helicate L3Fe24+ by OH- revealed two rate-limiting steps. The former leads to the formation of a monoferrous triple-stranded compound via a classical mechanism, which involves hydroxy−ferrous complexes. A similar process was observed in the latter step for the release of the ferrous cation from the mononuclear intermediate. Taking into account the structural, thermodynamic, and kinetic features provided by the present study, we could propose a self-assembling mechanism of the triple-stranded diferrous helicate.

    Copyright © 2000 American Chemical Society

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    †

     Laboratoire de Physico-Chimie Bioinorganique.

    §

     Laboratoire de Spectrométrie de Masse Bioorganique.

    ‡

     Laboratoire de Chimie Biomimétique.

    *

     To whom correspondence should be addressed. E-mail:  [email protected].

    Supporting Information Available

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    Tables of the 1H NMR data for L3Fe24+ in CD3CN, ESMS data for ferrous complexes, and figures of the absorption spectra of ligand L versus pH, of the dissociation kinetics of the diferrous helicate and of time-resolved spectra during the basic dissociation process of L3Fe24+. This material is available free of charge via the Internet at http://pubs.acs.org.

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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2000, 39, 25, 5771–5778
    Click to copy citationCitation copied!
    https://doi.org/10.1021/ic000229f
    Published November 15, 2000
    Copyright © 2000 American Chemical Society
    Request reuse permissions

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