The functional core of oxygenic photosynthesis is in charge of catalytic water oxidation by a multi-redoxMnIII/MnIV manifold that evolves through five electronic states (Si , 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 [MnIII 3MnIVO3(CH3COO)3(A-a-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 S2O8 2 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%.

Photo-catalytic Water Oxidation by a Mixed-Valent MnIII3MnIVO3 Manganese-Oxo-Core mimicking the Natural Oxygen Evolving Center

NATALI, Mirco;SCANDOLA, Franco;
2014

Abstract

The functional core of oxygenic photosynthesis is in charge of catalytic water oxidation by a multi-redoxMnIII/MnIV manifold that evolves through five electronic states (Si , 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 [MnIII 3MnIVO3(CH3COO)3(A-a-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 S2O8 2 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%.
2014
R., Al Oweini; A., Sartorel; B. S., Bassil; Natali, Mirco; S., Berardi; Scandola, Franco; U., Kortz; M., Bonchio
File in questo prodotto:
Non ci sono file associati a questo prodotto.

I documenti in SFERA sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.

Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/11392/2142412
 Attenzione

Attenzione! I dati visualizzati non sono stati sottoposti a validazione da parte dell'ateneo

Citazioni
  • ???jsp.display-item.citation.pmc??? ND
  • Scopus 176
  • ???jsp.display-item.citation.isi??? 161
social impact