Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 53, Issue 42, Pages 11182-11185Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201404664
Keywords
flash photolysis; manganese; oxygen evolution; polyoxometalates; water oxidation
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Funding
- Italian MIUR (FIRB NanoSolar) [RBAP11C58Y]
- Italian MIUR (PRIN Hi-Phuture) [2010N3T9M4_001]
- Fondazione Cariparo (Nanomode, progetti di eccellenza)
- EU COST Action program [CM1003, CM1203, CM1205]
- German Science Foundation (DFG) [KO-2288/20-1]
- Jacobs University
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The functional core of oxygenic photosynthesis is in charge of catalytic water oxidation by a multi-redox Mn-III/Mn-IV manifold that evolves through five electronic states (S-i, where i=0-4). The synthetic model system of this catalytic cycle and of its S0S4 intermediates is the expected turning point for artificial photosynthesis. The tetramanganese-substituted tungstosilicate [(Mn3MnO3)-Mn-III-O-IV(CH3COO)(3)(A--SiW9O34)](6-) (Mn4POM) offers an unprecedented mimicry of the natural system in its reduced S(0)state; it features a hybrid organic-inorganic coordination sphere and is anchored on a polyoxotungstate. Evidence for its photosynthetic properties when combined with [Ru(bpy)(3)](2+) and S2O82- is obtained by nanosecond laser flash photolysis; its S0S1 transition within milliseconds and multiple-hole-accumulating properties were studied. Photocatalytic oxygen evolution is achieved in a buffered medium (pH5) with a quantum efficiency of 1.7%.
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