4.8 Article

Quantifying Hot Electron Energy Contributions in Plasmonic Photocatalysis Using Electrochemical Surface-Enhanced Raman Spectroscopy

期刊

JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 13, 期 24, 页码 5495-5500

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.2c01213

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资金

  1. National Key RD Program [2021YFB4000600]
  2. National Natural Science Foundation of China [22022406]
  3. Natural Science Foundation of Tianjin [20JCJQJC00110, 20JCYBJC00590]
  4. 111 project [B12015]
  5. Haihe Laboratory of Sustainable Chemical Transformations

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Due to the challenges in measuring hot electron energy under reaction conditions, there are very few studies that focus on the experimental determination of hot carrier energy. In this study, we adjust the energy state of free electrons in Au nanoparticles to quantify the hot electron energy in plasmonic photocatalysis. By comparing the voltage required to achieve the same conversion of photo- and electro-reaction pathways, we calibrate the maximum energy efficiency of hot electrons in 4-NTP reduction to be 0.32 eV, which is much lower than the excitation photon energy of 1.96 eV. This work provides insight into the energy distribution of hot electrons and will be helpful for the rational design of highly efficient plasmon-mediated chemical reactions.
Due to the challenge in measuring hot electron energy under reaction conditions, very few studies focus on experimental determination of hot carrier energy. Here, we adjust the energy state of free electrons in Au nanoparticles to quantify the hot electron energy in plasmonic photocatalysis. Reactant molecules with different reduction potentials such as 4-nitrothiophenol (4-NTP), 4-iodothiophenol (4-ITP), etc. are chosen as molecular probes to investigate the reducing ability of hot electrons. By comparing the voltage required to achieve the same conversion of photo- and electro-reaction pathways, we calibrate the maximum energy efficiency of hot electrons in 4-NTP reduction to be 0.32 eV, which is much lower than the excitation photon energy of 1.96 eV. Our work provides insight into the energy distribution of hot electrons and will be helpful for rational design of highly efficient plasmon-mediated chemical reactions.

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