Imidazole and imidazolate iron complexes: on the way for tuning 3D-structural characteristics and reactivity. Redox interconversions controlled by protonation state

Inorganic Chemistry
François LambertLouis Nadjo

Abstract

X-ray structures for six Fe(II) and Fe(III) complexes from two closely heptadentate N-tripodal ligands, L1H(3) = tris[(imidazol-4-yl)-3-aza-3-butenyl]amine and L2H(3) = tris[(imidazol-2-yl)-3-aza-3-butenyl]amine, are described: three complexes in the L1 series (namely, [Fe(II)(L1H(3))](2+) and [Fe(III)(L1H(3))](3+) at low pH and [Fe(III)(L1)](0) at high pH) and three complexes in the L2 series (namely, [Fe(II)(L2H(3))](2+) at low pH and [Fe(II)(L2H)](0) and [Fe(III)(L2)](0) at high pH). Most of these complexes are stable in both Fe(II) and Fe(III) redox states and with the ligand in various protonation states. In the solid state, hydrogen bonds networks were obtained. Structural differences induced by 2- or 4-imidazole substitution are described and discussed. In solution, interconversions between different forms, with regard to oxidation and protonation states, were investigated by UV-visible spectroscopy, cyclic voltammetry, and potentiometry. The deprotonation pattern of these polyimidazole iron(II) and iron(III) complexes is described in detail. pK(a)s of the imidazolate/imidazole moieties in MeOH/H(2)O are reported. Two new species, namely, [Fe(II)(L1)](-) and [Fe(II)(L2)](-), were shown to be obtained in DMSO upon strong ...Continue Reading

Citations

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