Hydrogen evolution with hot electrons on a plasmonic-molecular catalyst hybrid system

Ananta Dey, Amal Mendalz, Anna Wach, Robert Bericat Vadell, Vitor R. Silveira, Paul Maurice Leidinger, Thomas Huthwelker, Vitalii Shtender, Zbynek Novotny, Luca Artiglia and Jacinto Sá ()
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Ananta Dey: Uppsala University
Amal Mendalz: Uppsala University
Anna Wach: Paul Scherrer Institut
Robert Bericat Vadell: Uppsala University
Vitor R. Silveira: Uppsala University
Paul Maurice Leidinger: Paul Scherrer Institut
Thomas Huthwelker: Paul Scherrer Institut
Vitalii Shtender: Uppsala University
Zbynek Novotny: Paul Scherrer Institut
Luca Artiglia: Paul Scherrer Institut
Jacinto Sá: Uppsala University

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract 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.

Date: 2024
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DOI: 10.1038/s41467-024-44752-y

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