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Hydrogen evolution with hot electrons on a plasmonic-molecular catalyst hybrid system
Ananta Dey1, Amal Mendalz1, Anna Wach2,3
1Department of Chemistry-Ångström, Physical Chemistry division, Uppsala University, Box 532, 751 20, Uppsala, Sweden.
Nature Communications
|January 10, 2024
Summary
This study shows plasmon hot electrons directly drive hydrogen evolution using visible light. A special nanohybrid system design minimizes heat, proving hot carriers are key to this catalytic process.
Area of Science:
- Materials Science
- Photocatalysis
- Nanotechnology
Background:
- Plasmonic systems convert light to electrical charges and heat, aiding catalysis.
- The role of hot carriers versus thermal effects in plasmon-mediated catalysis is debated.
Purpose of the Study:
- To demonstrate the direct use of plasmon hot electrons in visible-light-driven hydrogen evolution.
- To elucidate the mechanism of hot carrier involvement in catalysis.
Main Methods:
- Assembly of a NiO/Au/[Co(1,10-Phenanthrolin-5-amine)2(H2O)2] plasmonic nanohybrid system.
- Utilisation of photoelectrocatalysis and in situ spectroscopies.
- Design of a system unstable at high temperatures to isolate hot carrier effects.
Main Results:
- Demonstrated direct utilisation of plasmon hot electrons for hydrogen evolution.
- Substantiated a mechanism where hot electrons transfer to phenanthroline ligands.
- Facilitated rapid, concerted proton-electron transfer for hydrogen generation.
- Observed a catalytic response consistent with hot carrier mediation, with minor thermal contribution.
Conclusions:
- Plasmon-induced hot electrons are the primary drivers of hydrogen evolution in this system.
- The designed nanohybrid effectively isolates and demonstrates the hot carrier catalytic mechanism.
- This work clarifies the role of hot carriers in plasmon-driven catalysis.
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