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Evolution of atomically dispersed co-catalysts during solar or UV photocatalysis for efficient and sustained H2 production

2025-02Journal article Open access
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datacite.subject.fosCiências Naturais::Ciências Químicas
datacite.subject.fosEngenharia e Tecnologia::Outras Engenharias e Tecnologias
datacite.subject.sdg07:Energias Renováveis e Acessíveis
datacite.subject.sdg12:Produção e Consumo Sustentáveis
dc.contributor.authorCapelo, Anabela
dc.contributor.authorFattoruso, Domenico
dc.contributor.authorValencia-Valero, Laura
dc.contributor.authorEsteves, M. Alexandra
dc.contributor.authorRangel, Carmen M.
dc.contributor.authorPuga, Alberto
dc.date.accessioned2025-03-24T17:17:31Z
dc.date.available2025-03-24T17:17:31Z
dc.date.issued2025-02
dc.description.abstractABSTRACT: 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.por
dc.identifier.citationCapelo, 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
dc.identifier.doi10.1016/j.ijhydene.2025.01.203
dc.identifier.issn0360-3199
dc.identifier.urihttp://hdl.handle.net/10400.9/5618
dc.language.isoeng
dc.peerreviewedyes
dc.publisherElsevier
dc.relationSolar Facilities for the European Research Area - Third Phase
dc.relation.hasversionhttps://www.sciencedirect.com/journal/international-journal-of-hydrogen-energy
dc.rights.urihttp://creativecommons.org/licenses/by/4.0/
dc.subjectHydrogen production
dc.subjectGreen hydrogen
dc.subjectEthanol
dc.subjectAdsorption
dc.subjectCatalysts
dc.titleEvolution of atomically dispersed co-catalysts during solar or UV photocatalysis for efficient and sustained H2 productioneng
dc.typejournal article
dspace.entity.typePublication
oaire.awardTitleSolar Facilities for the European Research Area - Third Phase
oaire.awardURIinfo:eu-repo/grantAgreement/EC/H2020/823802/EU
oaire.citation.endPage658
oaire.citation.startPage645
oaire.citation.titleInternational Journal of Hydrogen Energy
oaire.citation.volume103
oaire.fundingStreamH2020
oaire.versionhttp://purl.org/coar/version/c_970fb48d4fbd8a85
person.familyNameCapelo
person.familyNameEsteves
person.familyNameRangel
person.givenNameAnabela
person.givenNameM. Alexandra
person.givenNameCarmen M.
person.identifier.ciencia-id8D1A-97AE-F411
person.identifier.ciencia-idAA13-FF7C-9E29
person.identifier.orcid0000-0002-6034-8565
person.identifier.orcid0000-0002-7010-605X
person.identifier.orcid0000-0001-7996-8142
person.identifier.ridH-2971-2017
person.identifier.ridD-5477-2011
person.identifier.scopus-author-id35581297200
person.identifier.scopus-author-id7006108156
project.funder.identifierhttp://doi.org/10.13039/501100008530
project.funder.nameEuropean Commission
relation.isAuthorOfPublicationd4e2ab37-019b-4af4-890f-ed965806ccf2
relation.isAuthorOfPublication341c4414-3fe7-4a05-99d5-8577bfdd05c8
relation.isAuthorOfPublication804e595a-d539-46a2-ae78-6cadc8ca9457
relation.isAuthorOfPublication.latestForDiscoveryd4e2ab37-019b-4af4-890f-ed965806ccf2
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