Hybrids of Deep HOMO Organic Cyanoacrylic Acid Dyes and Graphene Nanomaterials for Water Splitting Photoanodes

Ansón-Casaos, Alejandro ; Benito, Ana M. ; Maser, Wolfgang K. ; Orduna, Jesús ; Villacampa, Belén (Universidad de Zaragoza) ; Blesa, María-Jesús (Universidad de Zaragoza)

Resumen: Dye-sensitization is a promising strategy to improve the light absorption and photoactivity abilities of wide-bandgap semiconductors, like TiO2. For effective water-splitting photoanodes with no sacrificial agents, the electrochemical potential of the dye must exceed the thermodynamic threshold needed for the oxygen evolution reaction. This study investigates two promising organic cyanoacrylic dyes, designed to meet that criterion by means of theoretical calculations. Both yellow-colored dyes were synthesized and characterized by optical and photoelectrochemical techniques, demonstrating strong light absorption in the visible region, suitable experimental reduction potentials, and adsorption from the organic solvent onto mesoporous TiO2 layers. In addition, to promote immobilization in aqueous electrolytes, the dyes were hybridized with graphene oxide or multi-walled carbon nanotubes. Photoelectrochemical analysis of the dye-sensitized photoelectrodes demonstrated efficient charge transfer from the dyes to the TiO2 photoanode under simulated solar light. While the starting photocurrent notably surpassed the blank TiO2, a subsequent decay points to kinetic obstacles that still need to be overcome.

Idioma: Inglés

DOI: 10.3390/ma18020463

Año: 2025

Publicado en: Materials 18, 2 (2025), 463 [9 pp.]
ISSN: 1996-1944

Financiación: info:eu-repo/grantAgreement/ES/AEI/CEX2023-001286-S
Financiación: info:eu-repo/grantAgreement/ES/DGA/E47-23R
Financiación: info:eu-repo/grantAgreement/ES/DGA/T03-23R
Financiación: info:eu-repo/grantAgreement/ES/MICINN/PID2022-139671OB-I00
Financiación: info:eu-repo/grantAgreement/ES/UZ/UZ2023-CIE-01

Tipo y forma: Artículo (Versión definitiva)

Área (Departamento): Área Química Orgánica (Dpto. Química Orgánica)
Área (Departamento): Área Física Materia Condensada (Dpto. Física Materia Condensa.)