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Synthesis, Spectroscopy, and Electrochemistry of (?-Diimine)M(CO)3Br, M = Mn, Re, Complexes: Ligands Isoelectronic to Bipyridyl Show Differences in CO2 Reduction.


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-(?-diimine)M(CO)3Br (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)5Br in refluxing ethanol. Despite the electronic similarity of DAB to 2,2'-bipyridyl, the complexes described herein were poor mediators of electrochemical CO2 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 CO2 reduction, by EPR and single-crystal X-ray analysis is described.

SUBMITTER: Vollmer MV 

PROVIDER: S-EPMC4399245 | biostudies-literature | 2014 Sep

REPOSITORIES: biostudies-literature

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

Vollmer Matthew V MV   Machan Charles W CW   Clark Melissa L ML   Antholine William E WE   Agarwal Jay J   Schaefer Henry F HF   Kubiak Clifford P CP   Walensky Justin R JR  

Organometallics 20140901 1


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 <i>fac</i>-(α-diimine)M(CO)<sub>3</sub>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)<sub>5</sub>Br in refluxing ethanol. Despite the electronic similarity of DAB to 2,2'-bipyridyl, the complexes described herein were poor media  ...[more]

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