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Extent of carbon nitride photocharging controls energetics of hydrogen transfer in photochemical cascade processes

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  • Oleksandr Savateev

    (Max Planck Institute of Colloids and Interfaces
    The Chinese University of Hong Kong, Shatin, New Territories)

  • Karlo Nolkemper

    (Max Planck Institute of Colloids and Interfaces
    University of Paderborn)

  • Thomas D. Kühne

    (University of Paderborn
    Center for Advanced Systems Understanding (CASUS) and Helmholtz-Zentrum Dresden-Rossendorf
    Technische Universität Dresden)

  • Vitaliy Shvalagin

    (Max Planck Institute of Colloids and Interfaces)

  • Yevheniia Markushyna

    (Max Planck Institute of Colloids and Interfaces)

  • Markus Antonietti

    (Max Planck Institute of Colloids and Interfaces)

Abstract

Graphitic carbon nitride is widely studied in organic photoredox catalysis. Reductive quenching of carbon nitride excited state is postulated in many photocatalytic transformations. However, the reactivity of this species in the turn over step is less explored. In this work, we investigate electron and proton transfer from carbon nitride that is photocharged to a various extent, while the negative charge is compensated either by protons or ammonium cations. Strong stabilization of electrons by ammonium cations makes proton-coupled electron transfer uphill, and affords air-stable persistent carbon nitride radicals. In carbon nitrides, which are photocharged to a smaller extent, protons do not stabilize electrons, which results in spontaneous charge transfer to oxidants. Facile proton-coupled electron transfer is a key step in the photocatalytic oxidative-reductive cascade – tetramerization of benzylic amines. The feasibility of proton-coupled electron transfer is modulated by adjusting the extent of carbon nitride photocharging, type of counterion and temperature.

Suggested Citation

  • Oleksandr Savateev & Karlo Nolkemper & Thomas D. Kühne & Vitaliy Shvalagin & Yevheniia Markushyna & Markus Antonietti, 2023. "Extent of carbon nitride photocharging controls energetics of hydrogen transfer in photochemical cascade processes," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-43328-6
    DOI: 10.1038/s41467-023-43328-6
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    References listed on IDEAS

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    1. Stefano Mazzanti & Bogdan Kurpil & Bartholomäus Pieber & Markus Antonietti & Aleksandr Savateev, 2020. "Dichloromethylation of enones by carbon nitride photocatalysis," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
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