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Working the other way around: Photocatalytic water oxidation triggered by reductive quenching of the photoexcited chromophore
- Publication Year :
- 2015
- Publisher :
- American Chemical Society, 2015.
-
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.
- Subjects :
- MECHANISM
chemistry.chemical_element
Photochemistry
Coatings and Films
Electronic
ELECTRON-TRANSFER
Photosensitizer
Optical and Magnetic Materials
Physical and Theoretical Chemistry
chemistry.chemical_classification
CATALYST
COMPLEX
Quenching (fluorescence)
PHOTOCHEMISTRY
ELECTRON-TRANSFER, VIBRATIONAL-RELAXATION, ENERGY-TRANSFER, COMPLEX, MECHANISM, CATALYST, PHOTOCHEMISTRY, SYSTEM
VIBRATIONAL-RELAXATION
Electron acceptor
Chromophore
Persulfate
Surfaces, Coatings and Films
Electronic, Optical and Magnetic Materials
Ruthenium
Surfaces
General Energy
Energy (all)
chemistry
Polyoxometalate
Photocatalysis
ENERGY-TRANSFER
SYSTEM
Subjects
Details
- Language :
- English
- Database :
- OpenAIRE
- Accession number :
- edsair.doi.dedup.....34632108a5ab5cb87ea2a2709774e22e