Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 5, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202112749
Keywords
gold nanoparticles; graphene; hot electrons; plasmon-induced photocatalysis; surface-enhanced Raman spectroscopy
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Funding
- National Key Research and Development Program of China [2019YFA0705400, 2020YFB1505800]
- National Natural Science Foundation of China (NSFC) [21972117, 21925404, 21902137, 21703180, 21991151, 22021001]
- Natural Science Foundation of Fujian Province [2019J01030]
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In this study, the transfer of hot electrons at the plasmonic metal-graphene interface was investigated using in situ SERS, revealing that hot electrons can directly penetrate graphene to trigger photocatalytic reactions. Furthermore, it was found that the efficiency of hot electron transfer rapidly decays with increasing graphene layers, and would be completely blocked after five layers of graphene. Additionally, the transfer of hot electrons can be modulated by applying an external electric field, and the efficiency is significantly improved in the presence of a monolayer of graphene under electrochemical conditions.
Plasmonic metals under photoexcitation can generate energetic hot electrons to directly induce chemical reactions. However, the capability and fundamental insights of the transportation of these hot electrons at plasmonic metal-2D material interfaces remain unclear. Herein, hot-electron transfer at Au-graphene interfaces has been in situ studied using surface-enhanced Raman spectroscopy (SERS) with atomic layer accuracy. Combining in situ SERS studies with density functional theory calculations, it is proved that hot electrons can be injected from plasmonic Au nanoparticles to graphene and directly penetrate graphene to trigger photocatalytic reactions. With increasing graphene layers, the transportation of hot electrons decays rapidly and would be completely blocked after five layers of graphene. Moreover, the transfer of hot electrons can be modulated by applying an external electric field, and the hot-electron transfer efficiency under electrochemical conditions is improved by over three times in the presence of a monolayer of graphene.
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