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Hydrogen evolution with hot electrons on a plasmonic-molecular catalyst hybrid system
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.
Paul Scherrer Inst, CH-5232 Villigen, Switzerland.;Jagiellonian Univ, SOLARIS Natl Synchrotron Radiat Ctr, Krakow, Poland..ORCID iD: 0000-0003-3112-2759
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
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2024 (English)In: Nature Communications, E-ISSN 2041-1723, Vol. 15, article id 445Article in journal (Refereed) Published
Abstract [en]

Plasmonic systems convert light into electrical charges and heat, mediating catalytic transformations. However, there is ongoing controversy regarding the involvement of hot carriers in the catalytic process. In this study, we demonstrate the direct utilisation of plasmon hot electrons in the hydrogen evolution reaction with visible light. We intentionally assemble a plasmonic nanohybrid system comprising NiO/Au/[Co(1,10-Phenanthrolin-5-amine)2(H2O)2], which is unstable at water thermolysis temperatures. This assembly limits the plasmon thermal contribution while ensuring that hot carriers are the primary contributors to the catalytic process. By combining photoelectrocatalysis with advanced in situ spectroscopies, we can substantiate a reaction mechanism in which plasmon-induced hot electrons play a crucial role. These plasmonic hot electrons are directed into phenanthroline ligands, facilitating the rapid, concerted proton-electron transfer steps essential for hydrogen generation. The catalytic response to light modulation aligns with the distinctive profile of a hot carrier-mediated process, featuring a positive, though non-essential, heat contribution. Direct participation of plasmon-induced hot electrons in the photoelectrocatalytic synthesis of hydrogen. This report solves a long-lasting contentious issue surrounding plasmonic materials on catalytic applications.

Place, publisher, year, edition, pages
Springer Nature, 2024. Vol. 15, article id 445
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Chemical Process Engineering
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URN: urn:nbn:se:uu:diva-522503DOI: 10.1038/s41467-024-44752-yISI: 001141040600006PubMedID: 38200016OAI: oai:DiVA.org:uu-522503DiVA, id: diva2:1835714
Funder
Olle Engkvists stiftelse, 210-0007Knut and Alice Wallenberg Foundation, 2019-0071Swedish Research Council, 2019-03597Available from: 2024-02-07 Created: 2024-02-07 Last updated: 2024-02-07Bibliographically approved

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Dey, AnantaVadell, Robert BericatSilveira, VitorShtender, VitaliiSá, Jacinto

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