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Water-Soluble Polymeric Carbon Nitride Colloidal Nanoparticles for Highly Selective Quasi-Homogeneous Photocatalysis

preprint
submitted on 19.09.2019 and posted on 24.09.2019 by Igor Krivtsov, Dariusz Mitoraj, Marina Ilkaeva, Mariana Sardo, Luís Mafra, Christof Neumann, Andrey Turchanin, Chunyu Li, Benjamin Dietzek, Robert Leiter, Johannes Biskupek, Ute Kaiser, Changbin Im, Björn Kirchhoff, Timo Jacob, Radim Beranek
Heptazine-based polymeric carbon nitrides (PCN) are well established as promising photocatalysts for light-driven redox transformations. However, the activity of these materials is hampered by their low surface area translating into low concentration of active sites accessible for reactants. Herein, we report, for the first time, a bottom-up preparation of PCN nanoparticles with a narrow size distribution (~10±3 nm), which are fully soluble in water showing no gelation or precipitation over several months, and allow carrying out photocatalysis under quasi-homogeneous conditions. The rate of selective (up to 100%) photooxidation of 4-methoxybenzyl alcohol to 4-methoxybenzaldehyde was enhanced by the factor of 6.5 as compared to conventional solid PCN and was accompanied by simultaneous H2O2 production via reduction of oxygen. The dissolved photocatalyst can be easily recovered and re-dissolved by simple modulation of the ionic strength of the medium, without any loss of activity and selectivity. This work thus establishes a new paradigm of easily operable quasi-homogeneous photocatalysis with PCN, and opens up a route for other applications in which liquid aqueous operation or processing of PCN is required.

History

Email Address of Submitting Author

radim.beranek@uni-ulm.de

Institution

Ulm University

Country

Germany

ORCID For Submitting Author

0000-0002-7926-0774

Declaration of Conflict of Interest

The authors declare no competing interests.

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