Design and synthesis of a dinucleating ligand system with varying terminal donor functions that provides no bridging donor and its application to the synthesis of a series of Fe(III)-μ-O-Fe(III) complexes

Dalton Transactions : an International Journal of Inorganic Chemistry
Julia B H StrautmannThorsten Glaser

Abstract

Based on a rational ligand design for stabilizing high-valent {Fe(μ-O)2Fe} cores, a new family of dinucleating bis(tetradentate) ligands with varying terminal donor functions has been developed: redox-inert biomimetic carboxylates in H4julia, pyridines in susan, and phenolates in H4hilde(Me2). Based on a retrosynthetic analysis, the ligands were synthesized and used for the preparation of their diferric complexes [(julia){Fe(OH2)(μ-O)Fe(OH2)}]·6H2O, [(julia){Fe(OH2)(μ-O)Fe(OH2)}]·7H2O, [(julia){Fe(DMSO)(μ-O)Fe(DMSO)}]·3DMSO, [(hilde(Me2)){Fe(μ-O)Fe}]·CH2Cl2, [(hilde(Me2)){FeCl}2]·2CH2Cl2, [(susan){FeCl(μ-O)FeCl}]Cl2·2H2O, [(susan){FeCl(μ-O)FeCl0.75(OCH3)0.25}](ClO4)2·0.5MeOH, and [(susan){FeCl(μ-O)FeCl}](ClO4)2·0.5EtOH, which were characterized by single-crystal X-ray diffraction, FTIR, UV-Vis-NIR, Mössbauer, magnetic, and electrochemical measurements. The strongly electron-donating phenolates afford five-coordination, while the carboxylates and pyridines lead to six-coordination. The analysis of the ligand conformations demonstrates a strong flexibility of the ligand backbone in the complexes. The different hydrogen-bonding in the secondary coordination sphere of [(julia){Fe(OH2)(μ-O)Fe(OH2)}] influences the C-O, C[double bond...Continue Reading

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Citations

Jan 28, 2017·Inorganic Chemistry·Susanne DammersThorsten Glaser
Oct 23, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Massinisa AyadDominique Mandon
Apr 11, 2018·Inorganic Chemistry·Thomas Philipp ZimmermannThorsten Glaser
Oct 22, 2020·Inorganic Chemistry·Thomas Philipp ZimmermannThorsten Glaser

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