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Efficient Water Oxidation Catalyzed by Mononuclear Ruthenium(II) Complexes Incorporating Schiff Base Ligands
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Update time: 2014-06-12
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Proposed mechanism for water oxidation catalyzed by WOCs
Photochemical water splitting is a promising strategy to convert solar energy into chemical energy to meet rising global energy demands.Four new charge-neutral ruthenium(II) complexes containing dianionic Schiff base and isoquinoline or 4-picoline ligands were synthesized and characterized by NMR and ESI-MS spectroscopies, elemental analysis, and X-ray diffraction. The complexes exhibited excellent chemical water oxidation activity and high stability under acidic conditions (pH 1.0) using (NH4)2Ce(NO3)6 as a sacrificial electron acceptor. The high catalytic activities of these complexes for water oxidation were sustained for more than 10 h at low concentrations. High turnover numbers of up to 3200 were achieved. A water nucleophilic attack mechanism was proposed. A RuV[DOUBLE BOND]O intermediate was detected during the catalytic cycle by high-resolution mass spectrometry.
Chemistry - A European Journal, 2014
 
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