High Oxidation State Iridium Mono-μ-oxo Dimers Related to Water Oxidation Catalysis

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. Oth...

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Published inJournal of the American Chemical Society Vol. 138; no. 49; pp. 15917 - 15926
Main Authors Sharninghausen, Liam S, Sinha, Shashi Bhushan, Shopov, Dimitar Y, Choi, Bonnie, Mercado, Brandon Q, Roy, Xavier, Balcells, David, Brudvig, Gary W, Crabtree, Robert H
Format Journal Article
LanguageEnglish
Published United States American Chemical Society 14.12.2016
American Chemical Society (ACS)
Subjects
catalysis (homogeneous), catalysis (heterogeneous), solar (photovoltaic), solar (fuels), photosynthesis (natural and artificial), bio-inspired, hydrogen and fuel cells, electrodes - solar, defects, charge transport, spin dynamics, membrane, materials and chemistry by design, optics, synthesis (novel materials), synthesis (self-assembly)
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Abstract 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 Ir­(IV,IV) mono-μ-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 μ-oxo Ir­(IV,IV) compounds without metal–carbon bonds.
AbstractList 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 Ir(IV,IV) mono-μ-oxo dimers, containing the closely related L Ir-O-IrL 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 ClL Ir-O-IrL Cl, 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 μ-oxo Ir(IV,IV) compounds without metal-carbon bonds.
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 Ir(IV,IV) mono-μ-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 μ-oxo Ir(IV,IV) compounds without metal-carbon bonds.
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 Ir­(IV,IV) mono-μ-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 μ-oxo Ir­(IV,IV) compounds without metal–carbon bonds.
Author Shopov, Dimitar Y
Mercado, Brandon Q
Sharninghausen, Liam S
Balcells, David
Choi, Bonnie
Sinha, Shashi Bhushan
Roy, Xavier
Brudvig, Gary W
Crabtree, Robert H
AuthorAffiliation Department of Chemistry
Centre of Excellence in Theoretical and Computational Chemistry, Department of Chemistry
Yale University
Columbia University
University of Oslo
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BackLink https://www.ncbi.nlm.nih.gov/pubmed/27960326$$D View this record in MEDLINE/PubMed
https://www.osti.gov/biblio/1388153$$D View this record in Osti.gov
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Snippet The highly active iridium “blue solution” chemical and electrochemical water oxidation catalyst obtained from Cp*IrL­(OH) precursors (L =...
The highly active iridium "blue solution" chemical and electrochemical water oxidation catalyst obtained from Cp*IrL(OH) precursors (L =...
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SubjectTerms catalysis (homogeneous), catalysis (heterogeneous), solar (photovoltaic), solar (fuels), photosynthesis (natural and artificial), bio-inspired, hydrogen and fuel cells, electrodes - solar, defects, charge transport, spin dynamics, membrane, materials and chemistry by design, optics, synthesis (novel materials), synthesis (self-assembly)
Title High Oxidation State Iridium Mono-μ-oxo Dimers Related to Water Oxidation Catalysis
URI http://dx.doi.org/10.1021/jacs.6b07716
https://www.ncbi.nlm.nih.gov/pubmed/27960326
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Volume 138
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