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Core-substituted naphthalenediimides anchored on BiVO4 for visible light-driven water splitting 

  • Dades identificatives

    Identificador: PC:3116
    Handle: https://hdl.handle.net/20.500.11797/PC3116
    Autors:
    Carbó, J.Hernández, S.Ottone, C.Proto, S.Tolod, K.Díaz de los Bernardos, M.Solé-Daura, A.Godard, C.Castillón, S.Russo, N.Saracco, G.Claver, C.
    Resum:
    In this work, a novel catalytic system for the sunlight-driven water splitting reaction, which exploits the photocatalytic ability of BiVO4 coupled to a new kind of noble-metal-free organic dye molecules, is proposed. Hence, mono- and di-substituted naphthalenediimides (NDIs) were designed to have different functional groups that provide to them both tunable optical properties and adjustable HOMO/LUMO levels, and were selectively prepared (starting from 1,4,5,8-naphthalenetetracarboxylic acid) achieving yields >69%. Smart anchoring groups (i.e. carboxylates or aromatic amines) were added to the dyes in order to allow them to covalently bond to acidic –OH groups present on the BiVO4 surface. An easy and low-cost room temperature dip-coating technique was used to dye-sensitize both BiVO4 powders and thin films. NMR, MS, FT-IR, TG, FESEM, XRD, XPS and optical analyses confirmed the successful organic synthetic routes and good dyes/BiVO4 linkages. Photochemical and photoelectrochemical water oxidation reaction tests, together with DFT calculations, demonstrated that a proper alignment of the semiconductor/NDI-based dye energy levels is fundamental for enhancing the photocatalyst performance through a Z-scheme mechanism. The ability of the NDI organic molecules to delocalize the electronic charges was also a key factor for minimizing recombination processes and achieving more than a ten-fold increase in the photocurrent density of a 6 cm2 BiVO4 photo-electrode. The here reported results open new perspectives for the utilization of this new series of core-substituted NDIs, which are able to improve the activity of photocatalysts for different sunlight-driven applications, e.g. waste water treatment and organic contaminants’ degradation, other than the production of sola

  • Altres:

    Autor segons l'article: Carbó, J. ; Hernández, S. ; Ottone, C. ; Proto, S.; Tolod, K.; Díaz de los Bernardos, M. ; Solé-Daura, A. ; Godard, C.; Castillón, S. ; Russo, N. ; Saracco, G. ; Claver, C.
    Departament: Química Física i Inorgànica Química Analítica i Química Orgànica
    Autor/s de la URV: CARBÓ MARTIN, JORGE JUAN; Hernández, S. ; Ottone, C. ; Proto, S.; Tolod, K.; Díaz de los Bernardos, M. ; Solé-Daura, A. ; GODARD , CYRIL; CASTILLÓN MIRANDA, SERGIO; Russo, N. ; Saracco, G. ; CLAVER CABRERO, MARIA DEL CARMEN OROSIA
    Paraules clau: naphthalenediimides water splitting mechanisms Photocatalysis
    Resum: In this work, a novel catalytic system for the sunlight-driven water splitting reaction, which exploits the photocatalytic ability of BiVO4 coupled to a new kind of noble-metal-free organic dye molecules, is proposed. Hence, mono- and di-substituted naphthalenediimides (NDIs) were designed to have different functional groups that provide to them both tunable optical properties and adjustable HOMO/LUMO levels, and were selectively prepared (starting from 1,4,5,8-naphthalenetetracarboxylic acid) achieving yields >69%. Smart anchoring groups (i.e. carboxylates or aromatic amines) were added to the dyes in order to allow them to covalently bond to acidic –OH groups present on the BiVO4 surface. An easy and low-cost room temperature dip-coating technique was used to dye-sensitize both BiVO4 powders and thin films. NMR, MS, FT-IR, TG, FESEM, XRD, XPS and optical analyses confirmed the successful organic synthetic routes and good dyes/BiVO4 linkages. Photochemical and photoelectrochemical water oxidation reaction tests, together with DFT calculations, demonstrated that a proper alignment of the semiconductor/NDI-based dye energy levels is fundamental for enhancing the photocatalyst performance through a Z-scheme mechanism. The ability of the NDI organic molecules to delocalize the electronic charges was also a key factor for minimizing recombination processes and achieving more than a ten-fold increase in the photocurrent density of a 6 cm2 BiVO4 photo-electrode. The here reported results open new perspectives for the utilization of this new series of core-substituted NDIs, which are able to improve the activity of photocatalysts for different sunlight-driven applications, e.g. waste water treatment and organic contaminants’ degradation, other than the production of solar fuels by water splitting mechanisms.
    Grup de recerca: Organometàl.lics i Catàlisi Homogènia Química Quàntica Síntesis Orgànica Estereoselectiva
    Àrees temàtiques: Química Química Chemistry
    Accès a la llicència d'ús: https://creativecommons.org/licenses/by/3.0/es/
    ISSN: 1463-9262
    Identificador de l'autor: 0000-0002-3945-6721; ; ; ; ; ; ; 0000-0001-5762-4904; 0000-0002-0690-7549; ; ; 0000-0002-2518-7401
    Data d'alta del registre: 2018-02-21
    Pàgina final: 2462
    Volum de revista: 19
    Versió de l'article dipositat: info:eu-repo/semantics/acceptedVersion
    Enllaç font original: https://pubs.rsc.org/en/content/articlelanding/2017/gc/c7gc00125h#!divAbstract
    Programa de finançament: european; NMP-2012; Eco2CO2; 309701 plan; Excelencia; CTQ2014-52774-P plan; Retos; CTQ2013-43438-R altres; Grupos consolidados; 2014SGR199 altres; Grupos consolidados; 2014SGR670
    URL Document de llicència: https://repositori.urv.cat/ca/proteccio-de-dades/
    DOI de l'article: 10.1039/C7GC00125H
    Entitat: Universitat Rovira i Virgili
    Any de publicació de la revista: 2017
    Pàgina inicial: 2448
    Tipus de publicació: Article Artículo Article

  • Paraules clau:

    Fotocatàlisi
    naphthalenediimides
    water splitting mechanisms
    Photocatalysis
    Química
    Química
    Chemistry
    1463-9262

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