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- Title
Photocatalytic Water Oxidation by a Mixed-Valent Mn<sup>III</sup><sub>3</sub>Mn<sup>IV</sup>O<sub>3</sub> Manganese Oxo Core that Mimics the Natural Oxygen-Evolving Center.
- Authors
Al ‐ Oweini, Rami; Sartorel, Andrea; Bassil, Bassem S.; Natali, Mirco; Berardi, Serena; Scandola, Franco; Kortz, Ulrich; Bonchio, Marcella
- Abstract
The functional core of oxygenic photosynthesis is in charge of catalytic water oxidation by a multi-redox MnIII/MnIV manifold that evolves through five electronic states (S i , where i=0-4). The synthetic model system of this catalytic cycle and of its S0→S4 intermediates is the expected turning point for artificial photosynthesis. The tetramanganese-substituted tungstosilicate [MnIII3MnIVO3(CH3COO)3(A-α-SiW9O34)]6− (Mn4POM) offers an unprecedented mimicry of the natural system in its reduced S0 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 S0→S1 transition within milliseconds and multiple-hole-accumulating properties were studied. Photocatalytic oxygen evolution is achieved in a buffered medium (pH 5) with a quantum efficiency of 1.7 %.
- Subjects
PHOTOCATALYTIC oxidation; POLYOXOTUNGSTATES; OXIDATION of water; MANGANESE catalysts; SUBSTITUENTS (Chemistry); TURNOVER frequency (Catalysis)
- Publication
Angewandte Chemie, 2014, Vol 126, Issue 42, p11364
- ISSN
0044-8249
- Publication type
Article
- DOI
10.1002/ange.201404664