Low-Valent Iron Mono-Diazadiene Compounds: Electronic Structure and Catalytic Application

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• 作者：Crispin Lichtenberg ; Mario Adelhardt ; Thomas L. Gianetti ; Karsten Meyer ; Bas de Bruin ; Hansj枚rg Gr眉tzmacher
• 刊名：ACS Catalysis
• 出版年：2015
• 出版时间：October 2, 2015
• 年：2015
• 卷：5
• 期：10
• 页码：6230-6240
• 全文大小：430K
• ISSN：2155-5435

文摘

A series of monodiazadiene diolefin iron compounds, [Fe(trop₂dad)(L)] (4; L = neutral ligand), has been prepared by one-electron oxidation of the Fe^I 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 M枚ssbauer 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鈥揵oranes. Remarkably high activities were observed, especially for the homogeneous dehydrogenative polymerization of methylamine鈥揵orane.