ArticleInorganic chemistry2013
Synthesis and ligand non-innocence of thiolate-ligated (N4S) Iron(II) and nickel(II) bis(imino)pyridine complexes.
Article in Inorganic chemistry, 2013. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 7 papers.
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7 citing papers in PubMed.
- Iminopyridonato Iridium Complexes:Inorganic chemistry · 2026Article
- Intramolecular Oxo Atom Migration to theJournal of the American Chemical Society · 2025Article
- A biradical oxo-molybdenum complex containing semiquinone andRSC advances · 2020Article
- How Do Ring Size and π-Donating Thiolate Ligands Affect Redox-Active, α-Imino-N-heterocycle Ligand Activation?Inorganic chemistry · 2018Article
- Metal-Assisted Oxo Atom Addition to an Fe(III) Thiolate.Journal of the American Chemical Society · 2017Article
- Synthesis, X-ray Structures, Electronic Properties, and OInorganic chemistry · 2016Article
- Facile hydrogen atom transfer to iron(iii) imido radical complexes supported by a dianionic pentadentate ligand.Chemical science · 2016Article
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Abstract
The known iron(II) complex [Fe(II)(LN3S)(OTf)] (1) was used as starting material to prepare the new biomimetic (N4S(thiolate)) iron(II) complexes [Fe(II)(LN3S)(py)](OTf) (2) and [Fe(II)(LN3S)(DMAP)](OTf) (3), where LN3S is a tetradentate bis(imino)pyridine (BIP) derivative with a covalently tethered phenylthiolate donor. These complexes were characterized by X-ray crystallography, ultraviolet-visible (UV-vis) spectroscopic analysis, (1)H nuclear magnetic resonance (NMR), and Mössbauer spectroscopy, as well as electrochemistry. A nickel(II) analogue, [Ni(II)(LN3S)](BF4) (5), was also synthesized and characterized by structural and spectroscopic methods. Cyclic voltammetric studies showed 1-3 and 5 undergo a single reduction process with E(1/2) between -0.9 V to -1.2 V versus Fc(+)/Fc. Treatment of 3 with 0.5% Na/Hg amalgam gave the monoreduced complex [Fe(LN3S)(DMAP)](0) (4), which was characterized by X-ray crystallography, UV-vis spectroscopic analysis, electron paramagnetic resonance (EPR) spectroscopy (g = [2.155, 2.057, 2.038]), and Mössbauer (δ = 0.33 mm s(-1); ΔE(Q) = 2.04 mm s(-1)) spectroscopy. Computational methods (DFT) were employed to model complexes 3-5. The combined experimental and computational studies show that 1-3 are 5-coordinate, high-spin (S = 2) Fe(II) complexes, whereas 4 is best described as a 5-coordinate, intermediate-spin (S = 1) Fe(II) complex antiferromagnetically coupled to a ligand radical. This unique electronic configuration leads to an overall doublet spin (S(total) = 1/2) ground state. Complexes 2 and 3 are shown to react with O2 to give S-oxygenated products, as previously reported for 1. In contrast, the monoreduced 4 appears to react with O2 to give a mixture of sulfur oxygenates and iron oxygenates. The nickel(II) complex 5 does not react with O2, and even when the monoreduced nickel complex is produced, it appears to undergo only outer-sphere oxidation with O2.
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