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  Enhanced organic photocatalysis in confined flow through a carbon nitride nanotube membrane with conversions in the millisecond regime

Zou, Y., Xiao, K., Qin, Q., Shi, J.-W., Heil, T., Markushyna, Y., et al. (2021). Enhanced organic photocatalysis in confined flow through a carbon nitride nanotube membrane with conversions in the millisecond regime. ACS Nano, 15(4), 6551-6561. doi:10.1021/acsnano.0c09661.

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 Creators:
Zou, Yajun1, Author              
Xiao, Kai2, Author              
Qin, Qing3, Author              
Shi, Jian-Wen, Author
Heil, Tobias4, Author              
Markushyna, Yevheniia1, Author              
Jiang, Lei, Author
Antonietti, Markus5, Author              
Savateev, Aleksandr1, Author              
Affiliations:
1Aleksandr Savateev, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_2421702              
2Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_1863288              
3Martin Oschatz, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_2364733              
4Nadezda V. Tarakina, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_2522693              
5Markus Antonietti, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_1863321              

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Free keywords: carbon nitride; nanotube; confined photocatalysis; nanometer flow reactors; enhanced flow
 Abstract: Bioinspired nanoconfined catalysis has developed to become an important tool for improving the performance of a wide range of chemical reactions. However, photocatalysis in a nanoconfined environment remains largely unexplored. Here, we report the application of a free-standing and flow-through carbon nitride nanotube (CNN) membrane with pore diameters of 40 nm for confined photocatalytic reactions where reactants are in contact with the catalyst for <65 ms, as calculated from the flow. Due to the well-defined tubular structure of the membrane, we are able to assess quantitatively the photocatalytic performance in each of the parallelized single carbon nitride nanotubes, which act as spatially isolated nanoreactors. In oxidation of benzylamine, the confined reaction shows an improved performance when compared to the corresponding bulk reaction, reaching a turnover frequency of (9.63 ± 1.87) × 105 s–1. Such high rates are otherwise only known for special enzymes and are clearly attributed to the confinement of the studied reactions within the one-dimensional nanochannels of the CNN membrane. Namely, a concave surface maintains the internal electric field induced by the polar surface of the carbon nitride inside the nanotube, which is essential for polarization of reagent molecules and extension of the lifetime of the photogenerated charge carriers. The enhanced flow rate upon confinement provides crucial insight on catalysis in such an environment from a physical chemistry perspective. This confinement strategy is envisioned not only to realize highly efficient reactions but also to gain a fundamental understanding of complex chemical processes.

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Language(s): eng - English
 Dates: 2021-04-062021
 Publication Status: Published in print
 Pages: -
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 Rev. Type: -
 Identifiers: DOI: 10.1021/acsnano.0c09661
BibTex Citekey: doi:10.1021/acsnano.0c09661
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Title: ACS Nano
  Other : ACS Nano
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: - Volume / Issue: 15 (4) Sequence Number: - Start / End Page: 6551 - 6561 Identifier: ISSN: 1936-0851