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  Potassium poly(heptazine imide) – transition metal-free solid state triplet sensitizer in cascade energy transfer and [3+2]-cycloadditions

Savateev, A., Tarakina, N. V., Strauß, V., Hussain, T., ten Brummelhuis, K., Vadillo, S., et al. (2020). Potassium poly(heptazine imide) – transition metal-free solid state triplet sensitizer in cascade energy transfer and [3+2]-cycloadditions. Angewandte Chemie International Edition. doi:10.1002/anie.202004747.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0006-6C81-F Version Permalink: http://hdl.handle.net/21.11116/0000-0006-6C82-E
Genre: Journal Article

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 Creators:
Savateev, Aleksandr1, Author              
Tarakina, Nadezda V.2, Author              
Strauß, Volker3, Author              
Hussain, Tanveer, Author
ten Brummelhuis, Katharina4, Author              
Vadillo, Sánchez, Author
Manuel, José, Author
Markushyna, Yevheniia1, Author              
Mazzanti, Stefano1, Author              
Tyutyunnik, Alexander P., Author
Walczak, Ralf5, Author              
Oschatz, Martin5, Author              
Guldi, Dirk, Author
Karton, Amir, Author
Antonietti, Markus6, Author              
Affiliations:
1Aleksandr Savateev, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_2421702              
2Nadezda V. Tarakina, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_2522693              
3Volker Strauß, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_3025555              
4Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_1863288              
5Martin Oschatz, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_2364733              
6Markus Antonietti, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_1863321              

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Free keywords: carbon nitride, potassium poly(heptazine imide), solid state sensitizer, Singlet oxygen, organic photocatalysis
 Abstract: Polymeric carbon nitride materials have been successfully used in numerous light-to-energy conversion applications ranging from photocatalysis to optoelectronics. For a new application and modelling, we first refined the crystal structure of potassium poly(heptazine imide) (K-PHI) – a benchmark carbon nitride material in photocatalysis – by means of X-ray powder diffraction and transmission electron microscopy. Using the crystal structure of K-PHI, periodic DFT calculations were performed to calculate the density-of-states and localize intra band states (IBS). IBS were found to be responsible for the enhanced K-PHI absorption in the near IR region, to serve as electron traps, and to be useful in energy transfer reactions. Once excited with visible light, carbon nitrides, beside the direct recombination, can also undergo singlet-triplet intersystem crossing. We utilized the K-PHI centered triplet excited states to trigger a cascade of energy transfer reactions and, in turn, to sensitize, for example, singlet oxygen (1O2) as a starting point to synthesis up to 25 different N-rich heterocycles.

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Language(s): eng - English
 Dates: 2020-05-15
 Publication Status: Published online
 Pages: -
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 Table of Contents: -
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Title: Angewandte Chemie International Edition
  Abbreviation : Angew. Chem., Int. Ed.
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: - Volume / Issue: - Sequence Number: - Start / End Page: - Identifier: ISSN: 1433-7851

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Title: Angewandte Chemie
  Abbreviation : Angew. Chem.
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: - Volume / Issue: - Sequence Number: - Start / End Page: - Identifier: ISSN: 0044-8249