Combining energy and electron transfer in a supramolecular environment for the "green" generation and utilization of hydrated electrons through photoredox catalysis

Chemical Science
Christoph Kerzig, Martin Goez

Abstract

We present a new mechanism that sustainably produces hydrated electrons, i.e., extremely strong reductants, yet consumes only green photons (532 nm) and the bioavailable ascorbate as sacrificial donor. The mechanism couples an energy-transfer cycle, in which a light-harvesting ruthenium polypyridine complex absorbs a first photon and passes the excitation energy on to a pyrene-based redox catalyst, with an electron-transfer cycle, in which the resulting triplet is reductively quenched and the energy-rich aryl radical anion is finally ionized by a second photon. Thus separating the roles of primary and secondary absorber permitted choosing a redox catalyst with a nonabsorbing ground state but efficiently ionizable radical anion; the quantum yield of the ionization step in our complex mechanism surpasses that in a simple photoredox cycle featuring only the metal complex by a factor of four. We suppressed undesired cross reactions through the noncovalent interactions of an anionic micelle with the charges of the reactants, intermediates, and products: the cationic light-harvesting complex remains affixed to the micelle surface, which blocks the access of the negatively charged sacrificial donor, aryl radical anion and hydrated ele...Continue Reading

References

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Citations

Jan 27, 2019·Beilstein Journal of Organic Chemistry·Fabienne SpeckHans-Achim Wagenknecht
Jan 17, 2020·Angewandte Chemie·Felix GlaserOliver S Wenger
May 20, 2020·Chemistry : a European Journal·Fabian EisenreichAnja R A Palmans
Jun 27, 2020·Photochemical & Photobiological Sciences : Official Journal of the European Photochemistry Association and the European Society for Photobiology·Felix GlaserOliver S Wenger
Dec 15, 2016·Photochemical & Photobiological Sciences : Official Journal of the European Photochemistry Association and the European Society for Photobiology·Tim KohlmannMartin Goez
Dec 8, 2016·ChemSusChem·Mateo BertonMaría Elena González-Núñez
Mar 25, 2020·Chemical Science·Christoph Kerzig, Oliver S Wenger
Sep 20, 2017·Photochemical & Photobiological Sciences : Official Journal of the European Photochemistry Association and the European Society for Photobiology·Tim KohlmannMartin Goez
May 26, 2017·Angewandte Chemie·Indrajit GhoshBurkhard König
Jul 3, 2020·Chemistry : a European Journal·Maciej GiedykBurkhard König
Jan 6, 2017·Journal of the American Chemical Society·Laura A BüldtOliver S Wenger
Sep 24, 2019·Journal of the American Chemical Society·Timothy U ConnellPaul S Francis
Jan 13, 2021·Journal of the American Chemical Society·Jakob B BilgerOliver S Wenger

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