Autor según el artículo: 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.

Departamento: Química Física i Inorgànica Química Analítica i Química Orgànica

Autor/es 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

Palabras clave: naphthalenediimides water splitting mechanisms Photocatalysis

Resumen: 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.

Grupo de investigación: Organometàl.lics i Catàlisi Homogènia Química Quàntica Síntesis Orgànica Estereoselectiva

Áreas temáticas: Química Química Chemistry

Acceso a la licencia de uso: https://creativecommons.org/licenses/by/3.0/es/

ISSN: 1463-9262

Identificador del autor: 0000-0002-3945-6721; ; ; ; ; ; ; 0000-0001-5762-4904; 0000-0002-0690-7549; ; ; 0000-0002-2518-7401

Fecha de alta del registro: 2018-02-21

Página final: 2462

Volumen de revista: 19

Versión del articulo depositado: info:eu-repo/semantics/acceptedVersion

Enlace a la fuente original: https://pubs.rsc.org/en/content/articlelanding/2017/gc/c7gc00125h#!divAbstract

Programa de financiación: european; NMP-2012; Eco2CO2; 309701 plan; Excelencia; CTQ2014-52774-P plan; Retos; CTQ2013-43438-R altres; Grupos consolidados; 2014SGR199 altres; Grupos consolidados; 2014SGR670

DOI del artículo: 10.1039/C7GC00125H

Entidad: Universitat Rovira i Virgili

Año de publicación de la revista: 2017

Página inicial: 2448

Tipo de publicación: Article Artículo Article