期刊
ORGANOMETALLICS
卷 30, 期 5, 页码 965-973出版社
AMER CHEMICAL SOC
DOI: 10.1021/om101016s
关键词
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资金
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-PS02-08ER15944]
- Center for Catalytic Hydrocarbon Functionalization, CCHF [DE-SC0001298]
- Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences of the U.S. Department of Energy [DE-FG02-84ER13297]
The Ir precatalyst (3) contains both a Cp* and a kappa C-2(2),C-2'-1,3-diphenylimidazol-2-ylidene ligand, a C-C chelate, where one C donor is the NHC and the other is a cyclometalated N-phenyl wingtip group. The structure of 3 was confirmed by X-ray crystallography. Like our other recently described Cp*Ir catalysts, this compound is a precursor to a catalyst that can oxidize water to dioxygen. Electrochemical characterization of the new compound shows that it has a stable iridium(IV) oxidation state, [Cp*Ir-IV(NHC)Cl](+), in contrast with the unstable Ir(IV) state seen in our previous cyclometalated [Cp*Ir-III(2-pyridyl-2'-phenyl)Cl] catalyst. The new iridium(IV) species has been characterized by EPR spectroscopy and has a rhombic symmetry, a consequence of the ligand environment. These results both support previous studies which suggest that Cp*Ir catalysts can be advanced through the relevant catalytic cycle(s) in one-electron steps and help clarify the electrochemical behavior of this class of water-oxidation catalysts.
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