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Evolution of atomically dispersed co-catalysts during solar or UV photocatalysis for efficient and sustained H2 production
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Abstract(s)
ABSTRACT: 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.
Description
Keywords
Hydrogen production Green hydrogen Ethanol Adsorption Catalysts
Citation
Capelo, A., Fattoruso, D., Valencia-Valero, L., Esteves, M.A., Rangel, C.M. & Puga, A. (2025) Evolution of atomically dispersed co-catalysts during solar or UV photocatalysis for efficient and sustained H2 production. In: International Journal of Hydrogen Energy, 2025, vol. 103, p. 645–658. https://doi.org/10.1016/j.ijhydene.2025.01.203
Publisher
Elsevier