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

Oleksandr Savateev (), Karlo Nolkemper, Thomas D. Kühne, Vitaliy Shvalagin, Yevheniia Markushyna and Markus Antonietti
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Oleksandr Savateev: Max Planck Institute of Colloids and Interfaces
Karlo Nolkemper: Max Planck Institute of Colloids and Interfaces
Thomas D. Kühne: University of Paderborn
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

Nature Communications, 2023, vol. 14, issue 1, 1-12

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-43328-6

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