Autor según el artículo: Capelo, Anabela; Fattoruso, Domenico; Valencia-Valero, Laura Carolina; Esteves, M Alexandra; Rangel, Carmen M; Puga, Alberto
Departamento: Enginyeria Química
Autor/es de la URV: Puga Vaca, Alberto
Palabras clave: Water Tio2 Pt/tio2 Particle-size Hydrogen-production Generation Ethanol Catalyst Adsorption Acetic-acid
Resumen: The evolution of metal/titania photocatalysts during photocatalytic H-2 evolution is herein studied. Samples containing atomically dispersed Pt co-catalysts (single atoms, clusters and sub-nanoparticles) formed after calcination were compared to pre-reduced analogues mostly having metallic nanoparticles (diameters >1 nm) during ethanol photoreforming under either UV-rich irradiation or natural sunlight. Aggregation of ultra-dispersed oxidised platinum entities (Pt delta+) with concomitant reduction into Pt-0 nanoparticles (1-2 nm) was observed after UV irradiation by transmission electron microscopy (TEM), and diffuse reflectance UV-visible (DRUV-vis) and X-ray photoelectron (XPS) spectroscopies. A parallel, albeit slower, evolution trend was evidenced during solar photocatalysis. Conversely, atomically dispersed Cu co-catalyst species did not grow and became in-situ reduced into sub-nanometric Cu-0 under irradiation. Hydrogen production rates were remarkably high during initial stages of UV irradiation, and then declined to a sustained regime (approximate to 50 and 8 mmol g(-1) h(-1) for Pt/TiO2 or Cu/TiO2, respectively, for up to 24 h of irradiation). Steadier solar photoreforming was observed in experiments performed in a compound parabolic collector tubular reactor (approximate to 7.6 and 1.7 mmol g(-1) h(-1) for Pt/TiO2 or Cu/TiO2, respectively). Despite the non-negligible effect of co-catalyst rearrangement on activity rationalised herein, attenuated total reflectance Fourier-transform infrared (ATR-FTIR) spectroscopy measurements pre- and post-photocatalysis suggest that accumulation of strongly adsorbed degradation intermediates, chiefly acetate, is a major cause for rate decreases. Notwithstanding, this phenomenon did not result in total deactivation, so that sustained hydrogen production upon long-term irradiation was not compromised.
Áreas temáticas: Renewable energy, sustainability and the environment Química Physics, atomic, molecular & chemical Medicina ii Medicina i Materiais Interdisciplinar Geociências Fuel technology Farmacia Environmental sciences Engenharias iv Engenharias iii Engenharias ii Engenharias i Energy engineering and power technology Energy & fuels Electrochemistry Economia Condensed matter physics Ciências biológicas ii Ciências biológicas i Ciências ambientais Ciências agrárias i Ciência de alimentos Ciência da computação Chemistry, physical Biotecnología Astronomia / física
Acceso a la licencia de uso: https://creativecommons.org/licenses/by/3.0/es/
Direcció de correo del autor: alberto.puga@urv.cat
Identificador del autor: 0000-0003-4201-2635
Fecha de alta del registro: 2025-03-03
Versión del articulo depositado: info:eu-repo/semantics/publishedVersion
Referencia al articulo segun fuente origial: International Journal Of Hydrogen Energy. 103 645-658
Referencia de l'ítem segons les normes APA: Capelo, Anabela; Fattoruso, Domenico; Valencia-Valero, Laura Carolina; Esteves, M Alexandra; Rangel, Carmen M; Puga, Alberto (2025). Evolution of atomically dispersed co-catalysts during solar or UV photocatalysis for efficient and sustained H2 production. International Journal Of Hydrogen Energy, 103(), 645-658. DOI: 10.1016/j.ijhydene.2025.01.203
URL Documento de licencia: https://repositori.urv.cat/ca/proteccio-de-dades/
Entidad: Universitat Rovira i Virgili
Año de publicación de la revista: 2025
Tipo de publicación: Journal Publications
Repositori URV