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EnglishA detailed photophysical investigation of the photocatalytic water oxidation system based on the tetraruthenium polyoxometalate [Ru₄(μ-O)₄(μ−OH)₂(H₂O)₄(γ-SiW₁₀O₃₆)₂]¹⁰⁻ (1) as the catalyst, the tetranuclear ruthenium dendrimer [Ru{(μ-2,3-dpp)Ru(bpy)₂}₃]⁸⁺ (2) as the light-harvesting photosensitizer, and persulfate (S₂O₈²⁻) as the sacrificial electron acceptor has shown that the water oxidation mechanism proceeds through an unusual, “anti-biomimetic” pathway: The first photochemical event is indeed a reductive quenching of the excited photosensitizer by the catalyst, followed by electron scavenging by the sacrificial electron acceptor, both occurring on the picosecond time scale within ion-paired species. As an unprecedented photoreaction mechanism for molecular water oxidation systems, these results suggest a new way to combine photosensitizers and catalysts, taking advantage of suitable chemical interactions and alternative photoinduced processes for the construction of efficient water-splitting devices.
| Titolo: | Working the other way around: photocatalytic water oxidation triggered by reductive quenching of the photoexcited chromophore | |
| Autori: | PUNTORIERO, Fausto (Secondo) | |
| Data di pubblicazione: | 2015 | |
| Rivista: | ||
| Abstract: | A detailed photophysical investigation of the photocatalytic water oxidation system based on the tetraruthenium polyoxometalate [Ru₄(μ-O)₄(μ−OH)₂(H₂O)₄(γ-SiW₁₀O₃₆)₂]¹⁰⁻ (1) as the catalyst, the tetranuclear ruthenium dendrimer [Ru{(μ-2,3-dpp)Ru(bpy)₂}₃]⁸⁺ (2) as the light-harvesting photosensitizer, and persulfate (S₂O₈²⁻) as the sacrificial electron acceptor has shown that the water oxidation mechanism proceeds through an unusual, “anti-biomimetic” pathway: The first photochemical event is indeed a reductive quenching of the excited photosensitizer by the catalyst, followed by electron scavenging by the sacrificial electron acceptor, both occurring on the picosecond time scale within ion-paired species. As an unprecedented photoreaction mechanism for molecular water oxidation systems, these results suggest a new way to combine photosensitizers and catalysts, taking advantage of suitable chemical interactions and alternative photoinduced processes for the construction of efficient water-splitting devices. | |
| Handle: | http://hdl.handle.net/11570/3056578 | |
| Appare nelle tipologie: | 14.a.1 Articolo su rivista |
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| 3056578.pdf | Working the Other Way Around: Photocatalytic Water Oxidation Triggered by Reductive Quenching of the Photoexcited Chromophore | Versione Editoriale (PDF) | Tutti i diritti riservati (All rights reserved) | Utenti riconosciuti Richiedi una copia |
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http://hdl.handle.net/11570/3056578
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