Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 22, Issue 20, Pages 6740-+Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201600875
Keywords
donor flexibility; iridium; N-donor ligands; water oxidation; zwitterion
Categories
Funding
- European Research Council [CoG 615653]
- Swiss National Science Foundation [200021_162868, 206021_128724]
- Science Foundation Ireland [RC/1074]
- U.S. National Science Foundation [CHE-1362629]
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1362629] Funding Source: National Science Foundation
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A pyridylideneamide ligand with variable donor properties owing to a pronounced zwitterionic and a neutral diene-type resonance structure was used as a dynamic ligand at a Cp* iridium center to facilitate water oxidation catalysis, a reaction that requires the stabilization of a variety of different iridium oxidation states and that is key for developing an efficient solar fuel device. The ligand imparts high activity (nearly three-fold increase of turnover frequency compared to benchmark systems), and exceptionally high turnover numbers, which indicate a robust catalytic cycle and little catalyst degradation.
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