Photoelectrochemical hole injection revealed in polyoxotitanate nanocrystals functionalized with organic adsorbates

We find that crystallographically resolved Ti17O24(OPri)20 nanoparticles, functionalized by covalent attachment of 4-nitrophenyl-acetylacetonate or coumarin 343 adsorbates, exhibit hole injection into surface states when photoexcited with visible light (λ = 400–680 nm). Our findings are supported by...

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Detalles Bibliográficos
Autores: Negre, Christian Francisco Andres, Young, Karin J., Oviedo, María Belén, Allen, Laura J., Sanchez, Cristian Gabriel, Jarzembska , Katarzyna N., Benedict, Jason B., Crabtree, Robert H., Coppens, Philip, Brudvig, Gary W., Batista, Víctor S.
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2014
País:Argentina
Institución:Consejo Nacional de Investigaciones Científicas y Técnicas
Repositorio:CONICET Digital (CONICET)
Idioma:inglés
OAI Identifier:oai:ri.conicet.gov.ar:11336/31537
Acceso en línea:http://hdl.handle.net/11336/31537
Access Level:acceso abierto
Palabra clave:Photoinduced Electron Transfer
Dye Sensitized Solar Cells
Electron Paramagnetic Ressonance
Quantum Dynamics
https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
Descripción
Sumario:We find that crystallographically resolved Ti17O24(OPri)20 nanoparticles, functionalized by covalent attachment of 4-nitrophenyl-acetylacetonate or coumarin 343 adsorbates, exhibit hole injection into surface states when photoexcited with visible light (λ = 400–680 nm). Our findings are supported by photoelectrochemical measurements, EPR spectroscopy, and quantum dynamics simulations of interfacial charge transfer. The underlying mechanism is consistent with measurements of photocathodic currents generated with visible light for thin layers of functionalized polyoxotitanate nanocrystals deposited on FTO working electrodes. The reported experimental and theoretical analysis demonstrates for the first time the feasibility of p-type sensitization of TiO2 solely based on covalent binding of organic adsorbates.