Low-Valent Iron Mono-Diazadiene Compounds: Electronic Structure and Catalytic Application
2015
A series of monodiazadiene diolefin iron compounds, [Fe(trop2dad)(L)] (4; L = neutral ligand), has been prepared by one-electron oxidation of the FeI species [NaFe(trop2dad)(thf)3] (dad = diazadiene; trop = 5H-dibenzo[a,d]cyclohepten-5-yl). The electronic structures of compounds 4 were investigated by NMR and Mossbauer spectroscopy, single-crystal X-ray diffraction, solid- and liquid-phase magnetic susceptibility measurements, and DFT calculations. Compounds of type 4 with labile ligands L were found to be active (pre)catalysts for the dehydrogenative coupling of (alkyl)amine–boranes. Remarkably high activities were observed, especially for the homogeneous dehydrogenative polymerization of methylamine–borane.
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