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Exploiting hot electrons from a plasmon nanohybrid system for the photoelectroreduction of CO2
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.ORCID iD: 0000-0002-7208-0092
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Condensed Matter Physics of Energy Materials.ORCID iD: 0000-0002-9188-9604
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2024 (English)In: Communications Chemistry, E-ISSN 2399-3669, Vol. 7, no 1, article id 59Article in journal (Refereed) Published
Abstract [en]

Plasmonic materials convert light into hot carriers and heat to mediate catalytic transformation. The participation of hot carriers (photocatalysis) remains a subject of vigorous debate, often argued on the basis that carriers have ultrashort lifetime incompatible with drive photochemical processes. This study utilises plasmon hot electrons directly in the photoelectrocatalytic reduction of CO2 to CO via a Ppasmonic nanohybrid. Through the deliberate construction of a plasmonic nanohybrid system comprising NiO/Au/ReI(phen-NH2)(CO)3Cl (phen-NH2 = 1,10-Phenanthrolin-5-amine) that is unstable above 580 K; it was possible to demonstrate hot electrons are the main culprit in CO2 reduction. The engagement of hot electrons in the catalytic process is derived from many approaches that cover the processes in real-time, from ultrafast charge generation and separation to catalysis occurring on the minute scale. Unbiased in situ FTIR spectroscopy confirmed the stepwise reduction of the catalytic system. This, coupled with the low thermal stability of the ReI(phen-NH2)(CO)3Cl complex, explicitly establishes plasmonic hot carriers as the primary contributors to the process. Therefore, mediating catalytic reactions by plasmon hot carriers is feasible and holds promise for further exploration. Plasmonic nanohybrid systems can leverage plasmon’s unique photophysics and capabilities because they expedite the carrier’s lifetime.

Place, publisher, year, edition, pages
Springer Nature, 2024. Vol. 7, no 1, article id 59
National Category
Physical Chemistry Atom and Molecular Physics and Optics
Identifiers
URN: urn:nbn:se:uu:diva-526189DOI: 10.1038/s42004-024-01149-8ISI: 001190547400001PubMedID: 38509134OAI: oai:DiVA.org:uu-526189DiVA, id: diva2:1849290
Part of project
Light-driven nitrogen reduction catalysed by gold plasmonic nano-hybrid photo-systems , Swedish Research Council
Funder
Olle Engkvists stiftelse, 210-0007Swedish Research Council, 2019-03597Knut and Alice Wallenberg Foundation, 2019-0071Uppsala UniversityWallenberg Foundations, WISE, LiU-2023-00139
Note

De två första författarna delar förstaförfattarskapet

Available from: 2024-04-05 Created: 2024-04-05 Last updated: 2024-04-05Bibliographically approved

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Dey, AnantaSilveira, Vitor R.Bericat Vadell, RobertLindblad, AndreasLindblad, RebeckaShtender, VitaliiGörlin, MikaelaSá, Jacinto

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