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Complexed Semiconductor Cores Activate Hexaniobate Ligands as Nucleophilic Sites for Solar-Light Reduction of CO2 by Water

  • Datos identificativos

    Identificador: imarina:9282479
    Autores:
    Zhang GWang FTubul TBaranov MLeffler NNeyman APoblet JMWeinstock IA
    Resumen:
    Although pure and functionalized solid-state polyniobates such as layered perovskites and niobate nanosheets are photocatalysts for renewable-energy processes, analogous reactions by molecular polyoxoniobate cluster-anions are nearly absent from the literature. We now report that under simulated solar light, hexaniobate cluster-anion encapsulated 30-NiII-ion "fragments" of surface-protonated cubic-phase-like NiO cores activate the hexaniobate ligands towards CO2 reduction by water. Photoexcitation of the NiO cores promotes charge-transfer reduction of NbV to NbIV, increasing electron density at bridging oxo atoms of Nb-m-O-Nb linkages that bind and convert CO2 to CO. Photogenerated NiO "holes" simultaneously oxidize water to dioxygen. The findings point to molecular complexation of suitable semiconductor "fragments" as a general method for utilizing electron-dense polyoxoniobate anions as nucleophilic photocatalysts for solar-light driven activation and reduction of small molecules.© 2022 Wiley-VCH GmbH.
  • Otros:

    Autor según el artículo: Zhang G; Wang F; Tubul T; Baranov M; Leffler N; Neyman A; Poblet JM; Weinstock IA
    Departamento: Química Física i Inorgànica
    Autor/es de la URV: Poblet Rius, Josep Maria / Wang, Fei
    Palabras clave: Photocatalysis Oxide nanoparticles Nickel oxide Molecular complex Hexaniobate anion Co2 reduction Co reduction 2 temperature rhodium photoreduction mechanism photocatalytic properties photocatalysis oxidation niobate nio nickel oxide molecular complex mno metal-oxide hexaniobate anion
    Resumen: Although pure and functionalized solid-state polyniobates such as layered perovskites and niobate nanosheets are photocatalysts for renewable-energy processes, analogous reactions by molecular polyoxoniobate cluster-anions are nearly absent from the literature. We now report that under simulated solar light, hexaniobate cluster-anion encapsulated 30-NiII-ion "fragments" of surface-protonated cubic-phase-like NiO cores activate the hexaniobate ligands towards CO2 reduction by water. Photoexcitation of the NiO cores promotes charge-transfer reduction of NbV to NbIV, increasing electron density at bridging oxo atoms of Nb-m-O-Nb linkages that bind and convert CO2 to CO. Photogenerated NiO "holes" simultaneously oxidize water to dioxygen. The findings point to molecular complexation of suitable semiconductor "fragments" as a general method for utilizing electron-dense polyoxoniobate anions as nucleophilic photocatalysts for solar-light driven activation and reduction of small molecules.© 2022 Wiley-VCH GmbH.
    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: fei.wang@urv.cat josepmaria.poblet@urv.cat
    Identificador del autor: 0000-0001-5106-5793 0000-0002-4533-0623
    Fecha de alta del registro: 2024-09-07
    Versión del articulo depositado: info:eu-repo/semantics/publishedVersion
    URL Documento de licencia: https://repositori.urv.cat/ca/proteccio-de-dades/
    Referencia al articulo segun fuente origial: Angewandte Chemie (International Ed. Print). 61 (49): e202213162-
    Referencia de l'ítem segons les normes APA: Zhang G; Wang F; Tubul T; Baranov M; Leffler N; Neyman A; Poblet JM; Weinstock IA (2022). Complexed Semiconductor Cores Activate Hexaniobate Ligands as Nucleophilic Sites for Solar-Light Reduction of CO2 by Water. Angewandte Chemie (International Ed. Print), 61(49), e202213162-. DOI: 10.1002/anie.202213162
    Entidad: Universitat Rovira i Virgili
    Año de publicación de la revista: 2022
    Tipo de publicación: Journal Publications
  • Palabras clave:

    Catalysis,Chemistry,Chemistry (Miscellaneous),Chemistry, Multidisciplinary
    Photocatalysis
    Oxide nanoparticles
    Nickel oxide
    Molecular complex
    Hexaniobate anion
    Co2 reduction
    Co reduction 2
    temperature
    rhodium
    photoreduction mechanism
    photocatalytic properties
    photocatalysis
    oxidation
    niobate
    nio
    nickel oxide
    molecular complex
    mno
    metal-oxide
    hexaniobate anion
    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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