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Mechanism for plasmon-generated solvated electrons

Solvated electrons are powerful reducing agents capable of driving some of the most energetically expensive reduction reactions. Their generation under mild and sustainable conditions remains challenging though. Using near-ultraviolet irradiation under low-intensity one-photon conditions coupled wit...

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Detalles Bibliográficos
Autores principales: Al-Zubeidi, Alexander, Ostovar, Behnaz, Carlin, Claire C., Li, Boxi Cam, Lee, Stephen A., Chiang, Wei-Yi, Gross, Niklas, Dutta, Sukanya, Misiura, Anastasiia, Searles, Emily K., Chakraborty, Amrita, Roberts, Sean T., Dionne, Jennifer A., Rossky, Peter J., Landes, Christy F., Link, Stephan
Formato: Online Artículo Texto
Lenguaje:English
Publicado: National Academy of Sciences 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9934022/
https://www.ncbi.nlm.nih.gov/pubmed/36626548
http://dx.doi.org/10.1073/pnas.2217035120
Descripción
Sumario:Solvated electrons are powerful reducing agents capable of driving some of the most energetically expensive reduction reactions. Their generation under mild and sustainable conditions remains challenging though. Using near-ultraviolet irradiation under low-intensity one-photon conditions coupled with electrochemical and optical detection, we show that the yield of solvated electrons in water is increased more than 10 times for nanoparticle-decorated electrodes compared to smooth silver electrodes. Based on the simulations of electric fields and hot carrier distributions, we determine that hot electrons generated by plasmons are injected into water to form solvated electrons. Both yield enhancement and hot carrier production spectrally follow the plasmonic near-field. The ability to enhance solvated electron yields in a controlled manner by tailoring nanoparticle plasmons opens up a promising strategy for exploiting solvated electrons in chemical reactions.