Plasmon-Generated Solvated Electrons for Chemical Transformations.

Autor: Solti D; Laboratory for Nanophotonics, Rice University, Houston, Texas 77005, United States.; Department of Chemistry, Rice University, Houston, Texas 77005, United States., Chapkin KD; Laboratory for Nanophotonics, Rice University, Houston, Texas 77005, United States.; Department of Electrical and Computer Engineering, Rice University, Houston, Texas 77005, United States.; Applied Physics Graduate Program, Smalley-Curl Institute, Rice University, Houston, Texas 77005, United States., Renard D; Laboratory for Nanophotonics, Rice University, Houston, Texas 77005, United States.; Department of Chemistry, Rice University, Houston, Texas 77005, United States., Bayles A; Laboratory for Nanophotonics, Rice University, Houston, Texas 77005, United States.; Department of Chemistry, Rice University, Houston, Texas 77005, United States., Clark BD; Laboratory for Nanophotonics, Rice University, Houston, Texas 77005, United States.; Department of Chemistry, Rice University, Houston, Texas 77005, United States., Wu G; Department of Internal Medicine, The University of Texas McGovern Medical School, Houston, Texas 77030, United States., Zhou J; Laboratory for Nanophotonics, Rice University, Houston, Texas 77005, United States.; Department of Materials Science and Nanoengineering, Rice University, Houston, Texas 77005, United States., Tsai AL; Department of Internal Medicine, The University of Texas McGovern Medical School, Houston, Texas 77030, United States., Kürti L; Department of Chemistry, Rice University, Houston, Texas 77005, United States., Nordlander P; Laboratory for Nanophotonics, Rice University, Houston, Texas 77005, United States.; Department of Electrical and Computer Engineering, Rice University, Houston, Texas 77005, United States.; Department of Materials Science and Nanoengineering, Rice University, Houston, Texas 77005, United States.; Department of Physics and Astronomy, Rice University, Houston, Texas 77005, United States., Halas NJ; Laboratory for Nanophotonics, Rice University, Houston, Texas 77005, United States.; Department of Chemistry, Rice University, Houston, Texas 77005, United States.; Department of Electrical and Computer Engineering, Rice University, Houston, Texas 77005, United States.; Department of Materials Science and Nanoengineering, Rice University, Houston, Texas 77005, United States.; Department of Physics and Astronomy, Rice University, Houston, Texas 77005, United States.
Jazyk: angličtina
Zdroj: Journal of the American Chemical Society [J Am Chem Soc] 2022 Nov 09; Vol. 144 (44), pp. 20183-20189. Date of Electronic Publication: 2022 Oct 28.
DOI: 10.1021/jacs.2c07768
Abstrakt: Methods for generating solvated electrons─free electrons in solution─have focused primarily on alkali metal ionization or high-energy electrons or photons. Here we report the generation of solvated electrons by exciting the plasmon resonance of Al nanocrystals suspended in solution with visible light. Two chemical reactions were performed: a radical-addition reaction with the spin-trap 2-methyl-2-nitrosopropane, and a model cyclization reaction with the radical clock 6-bromohex-1-ene. A quantum efficiency of at least ∼1.1% for plasmon absorbed photon to solvated electron generation can be inferred from the measured radical clock reaction concentration. This study demonstrates a simple way to generate solvated electrons for driving reductive organic chemical reactions in a quantifiable and controlled manner.
Databáze: MEDLINE