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Redox Interconversion between Cobalt(III) Thiolate and Cobalt(II) Disulfide Compounds.

Feng Jiang1, Maxime A Siegler2, Xiaobo Sun3

  • 1Leiden Institute of Chemistry, Gorlaeus Laboratories , Leiden University , P.O. Box 9502, 2300 RA Leiden , The Netherlands.

Inorganic Chemistry
|July 20, 2018
PubMed
Summary
This summary is machine-generated.

This study demonstrates the reversible redox transformation between cobalt(II) disulfide and cobalt(III) thiolate complexes, influenced by anion exchange. This provides an unprecedented example of anion-triggered redox interconversion in cobalt chemistry.

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Area of Science:

  • Coordination Chemistry
  • Organometallic Chemistry
  • Bioinorganic Chemistry

Background:

  • Cobalt complexes with disulfide and thiolate ligands are crucial in various catalytic processes.
  • Understanding the redox behavior of cobalt is essential for designing new catalysts and understanding biological systems.

Purpose of the Study:

  • To investigate the redox interconversion between cobalt(III) thiolate and cobalt(II) disulfide compounds.
  • To explore the influence of anion exchange on this redox process.
  • To compare the reactivity of cobalt with iron in similar ligand systems.

Main Methods:

  • Experimental synthesis and characterization of cobalt and iron complexes.
  • UV-vis spectroscopy for monitoring redox reactions.
  • X-ray crystallography for structural determination.
  • Computational studies (DFT) to analyze electronic structure changes.

Main Results:

  • Formation of high-spin cobalt(II) disulfide [CoII2(L1SSL1)Cl4] and low-spin cobalt(III) thiolate [CoIII(L1S)(MeCN)2](BF4)2 complexes.
  • Anion exchange (Cl- or NCS-) triggers reversible redox interconversion between Co(II) and Co(III) states.
  • Computational analysis reveals changes in metal d-orbital and sulfur p-orbital contributions upon anion exchange.
  • Structural differences observed between analogous dinuclear iron(II) and cobalt(II) disulfide compounds.
  • Iron complexes did not yield the expected Fe(III) thiolate compound under similar conditions.

Conclusions:

  • Demonstrated an unprecedented anion-triggered redox interconversion between high-spin Co(II) disulfide and low-spin Co(III) thiolate compounds.
  • Highlighted the significant role of the counter-anion in modulating cobalt's redox state and electronic properties.
  • Showcased distinct reactivity patterns between cobalt and iron with the disulfide ligand, suggesting unique coordination preferences.