Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 138, Issue 49, Pages 15917-15926Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.6b07716
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Funding
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences of the Argonne-Northwestern Solar Energy Research (ANSER) Energy Frontier Research Center [DE-SC0001059, DEFG02-07ER15909]
- NSF [DGE 11-44155]
- Research Council of Norway through the Centre of Excellence for Theoretical and Computational Chemistry (CTCC) [179568/V30]
- Norwegian Metacenter for Computational Science (NOTUR) [nn4654k]
- EU REA for a Marie Curie Fellowship [CompuWOC/618303]
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The highly active iridium blue solution chemical and electrochemical water oxidation catalyst obtained from Cp*IrL(OH) precursors (L = 2-pyridyl-2-propanoate) has been difficult to characterize as no crystal structure can be obtained because of the multiplicity of geometrical isomers present. Other data suggest complete loss of the Cp* ligand and the formation of a LIr-O-IrL unit. We have now developed a route to a series of well-defined mono-mu-oxo dimers, containing the closely related L2Ir-O-IrL2 unit. Unlike the catalyst, these model compounds are separable by silica gel chromatography and readily form single crystals. We report three stereoisomers with the formula ClL2Ir-O-IrL2Cl, which are fully characterized, including by X-ray crystallography, and are compared to the blue solution. To the best of our knowledge, these species represent the first examples of structurally characterized dinuclear mu-oxo Ir(IV,IV) compounds without metal-carbon bonds.
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