Articles producció científica> Química Física i Inorgànica

Tuning Photoinduced Electron Transfer in POM-Bodipy Hybrids by Controlling the Environment: Experiment and Theory

  • Datos identificativos

    Identificador: imarina:9162446
    Autores:
    Toupalas, GeorgiosKarlsson, JoshuaBlack, Fiona A.Masip-Sanchez, AlbertLopez, XavierBen M'Barek, YoussefBlanchard, SebastienProust, AnnaAlves, SandraChabera, PavelClark, Ian P.Pullerits, TonuPoblet, Josep M.Gibson, Elizabeth A.Izzet, Guillaume
    Resumen:
    The optical and electrochemical properties of a series of polyoxometalate (POM) oxoclusters decorated with two bodipy (boron-dipyrromethene) light-harvesting units were examined. Evaluated here in this polyanionic donor-acceptor system is the effect of the solvent and associated counterions on the intramolecular photoinduced electron transfer. The results show that both solvents and counterions have a major impact upon the energy of the charge-transfer state by modifying the solvation shell around the POMs. This modification leads to a significantly shorter charge separation time in the case of smaller counterion and slower charge recombination in a less polar solvent. These results were rationalized in terms of Marcus theory and show that solvent and counterion both affect the driving force for photoinduced electron transfer and the reorganization energy. This was corroborated with theoretical investigations combining DFT and molecular dynamics simulations.
  • Otros:

    Autor según el artículo: Toupalas, Georgios; Karlsson, Joshua; Black, Fiona A.; Masip-Sanchez, Albert; Lopez, Xavier; Ben M'Barek, Youssef; Blanchard, Sebastien; Proust, Anna; Alves, Sandra; Chabera, Pavel; Clark, Ian P.; Pullerits, Tonu; Poblet, Josep M.; Gibson, Elizabeth A.; Izzet, Guillaume;
    Departamento: Química Física i Inorgànica
    Autor/es de la URV: López Fernández, Javier / Masip Sánchez, Albert / Poblet Rius, Josep Maria
    Palabras clave: Zinc cytochrome-c Visible-light Redox potentials Polyoxometalates Polyoxometalate Noncovalent interactions Molecular dynamic simulations Kinetics Functionalization Energy Electron transfer Elaboration Donor-acceptor systems Charge-transfer Catalyst dyads
    Resumen: The optical and electrochemical properties of a series of polyoxometalate (POM) oxoclusters decorated with two bodipy (boron-dipyrromethene) light-harvesting units were examined. Evaluated here in this polyanionic donor-acceptor system is the effect of the solvent and associated counterions on the intramolecular photoinduced electron transfer. The results show that both solvents and counterions have a major impact upon the energy of the charge-transfer state by modifying the solvation shell around the POMs. This modification leads to a significantly shorter charge separation time in the case of smaller counterion and slower charge recombination in a less polar solvent. These results were rationalized in terms of Marcus theory and show that solvent and counterion both affect the driving force for photoinduced electron transfer and the reorganization energy. This was corroborated with theoretical investigations combining DFT and molecular dynamics simulations.
    Áreas temáticas: Química Medicina ii Medicina i Materiais Interdisciplinar General medicine General chemistry Farmacia Engenharias ii Ciências biológicas iii Ciências biológicas ii Ciências biológicas i Chemistry, multidisciplinary Chemistry (miscellaneous) Chemistry (all) Chemistry Catalysis Astronomia / física
    Acceso a la licencia de uso: https://creativecommons.org/licenses/by/3.0/es/
    Direcció de correo del autor: albert.masip@urv.cat albert.masip@urv.cat josepmaria.poblet@urv.cat javier.lopez@urv.cat
    Identificador del autor: 0000-0002-4533-0623 0000-0003-0322-6796
    Fecha de alta del registro: 2024-07-27
    Versión del articulo depositado: info:eu-repo/semantics/acceptedVersion
    Enlace a la fuente original: https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202014677
    URL Documento de licencia: https://repositori.urv.cat/ca/proteccio-de-dades/
    Referencia al articulo segun fuente origial: Angewandte Chemie (International Ed. Print). 60 (12): 6518-6525
    Referencia de l'ítem segons les normes APA: Toupalas, Georgios; Karlsson, Joshua; Black, Fiona A.; Masip-Sanchez, Albert; Lopez, Xavier; Ben M'Barek, Youssef; Blanchard, Sebastien; Proust, Anna; (2021). Tuning Photoinduced Electron Transfer in POM-Bodipy Hybrids by Controlling the Environment: Experiment and Theory. Angewandte Chemie (International Ed. Print), 60(12), 6518-6525. DOI: 10.1002/anie.202014677
    DOI del artículo: 10.1002/anie.202014677
    Entidad: Universitat Rovira i Virgili
    Año de publicación de la revista: 2021
    Tipo de publicación: Journal Publications
  • Palabras clave:

    Catalysis,Chemistry,Chemistry (Miscellaneous),Chemistry, Multidisciplinary
    Zinc cytochrome-c
    Visible-light
    Redox potentials
    Polyoxometalates
    Polyoxometalate
    Noncovalent interactions
    Molecular dynamic simulations
    Kinetics
    Functionalization
    Energy
    Electron transfer
    Elaboration
    Donor-acceptor systems
    Charge-transfer
    Catalyst dyads
    Química
    Medicina ii
    Medicina i
    Materiais
    Interdisciplinar
    General medicine
    General chemistry
    Farmacia
    Engenharias ii
    Ciências biológicas iii
    Ciências biológicas ii
    Ciências biológicas i
    Chemistry, multidisciplinary
    Chemistry (miscellaneous)
    Chemistry (all)
    Chemistry
    Catalysis
    Astronomia / física
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