Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 57, Issue 35, Pages 11247-11251Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201805244
Keywords
electrochemical catalysis; ruthenium complexes; supramolecular chemistry; water oxidation
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Funding
- University of Amsterdam
- European Research Council (ERC) [339786-NAT_CAT]
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Oxygen formation through water oxidation catalysis is a key reaction in the context of fuel generation from renewable energies. The number of homogeneous catalysts that catalyze water oxidation at high rate with low overpotential is limited. Ruthenium complexes can be particularly active, especially if they facilitate a dinuclear pathway for oxygen bond formation step. A supramolecular encapsulation strategy is reported that involves preorganization of dilute solutions (10(-5)m) of ruthenium complexes to yield high local catalyst concentrations (up to 0.54m). The preorganization strategy enhances the water oxidation rate by two-orders of magnitude to 125s(-1), as it facilitates the diffusion-controlled rate-limiting dinuclear coupling step. Moreover, it modulates reaction rates, enabling comprehensive elucidation of electrocatalytic reaction mechanisms.
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