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New Core-Substituted Naphtalenediimides anchored on BiVO4 for Visible Light-Driven Water Splitting


In this work, a novel catalytic system for the sunlight-driven water splitting, 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 naphtalenediimides (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 NDIs 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 opens new perspectives for the utilization of this new series of core-substituted NDIs, which are able to improve photocatalysts activity 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.

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Publication details

The article was received on 12 Jan 2017, accepted on 18 Apr 2017 and first published on 18 Apr 2017

Article type: Paper
DOI: 10.1039/C7GC00125H
Citation: Green Chem., 2017, Accepted Manuscript
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    New Core-Substituted Naphtalenediimides anchored on BiVO4 for Visible Light-Driven Water Splitting

    S. Hernandez, C. Ottone, S. Proto, K. Tolod, M. Díaz de los Bernardos, A. Solé-Daura, J. J. Carbó, C. Godard, S. Castillón, N. Russo, G. Saracco and C. Claver, Green Chem., 2017, Accepted Manuscript , DOI: 10.1039/C7GC00125H

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