Synthesis, Spectroscopy, and Electrochemistry of (α-Diimine)M(CO)(3)Br, M = Mn, Re, Complexes: Ligands Isoelectronic to Bipyridyl Show Differences in CO(2) Reduction

(α-二亚胺)M(CO)₃Br,M = Mn,Re配合物的合成、光谱和电化学性质:与联吡啶等电子的配体在CO₂还原方面表现出差异

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Abstract

The synthesis and characterization of new Mn(I)- and Re(I)-centered organometallic complexes fashioned with 1,4-diazabutadiene (DAB) ligands is reported. Ten compounds of the type fac-(α-diimine)M(CO)(3)Br (M = Mn, Re) were obtained in moderate to excellent yield (35-80%) and high purity from the coordination of the five ligands with M(CO)(5)Br in refluxing ethanol. Despite the electronic similarity of DAB to 2,2'-bipyridyl, the complexes described herein were poor mediators of electrochemical CO(2) conversion to CO, but provide insight into the role of redox-active ligands in catalysis. Additional characterization of the one-electron reduced rhenium compounds, relevant intermediates in CO(2) reduction, by EPR and single-crystal X-ray analysis is described.

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