Potassium Poly(Heptazine Imide): Transition Metal-Free Solid-State Triplet Sensitizer in Cascade Energy Transfer and [3+2]-cycloadditions.
carbon nitrides
organic photocatalysis
potassium poly(heptazine imide)
singlet oxygen
solid-state sensitizer
Journal
Angewandte Chemie (International ed. in English)
ISSN: 1521-3773
Titre abrégé: Angew Chem Int Ed Engl
Pays: Germany
ID NLM: 0370543
Informations de publication
Date de publication:
24 Aug 2020
24 Aug 2020
Historique:
received:
01
04
2020
revised:
06
05
2020
pubmed:
16
5
2020
medline:
16
5
2020
entrez:
16
5
2020
Statut:
ppublish
Résumé
Polymeric carbon nitride materials have been 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 (DOS) 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, in addition to 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 (
Identifiants
pubmed: 32412175
doi: 10.1002/anie.202004747
pmc: PMC7496904
doi:
Types de publication
Journal Article
Langues
eng
Sous-ensembles de citation
IM
Pagination
15061-15068Subventions
Organisme : Deutsche Forschungsgemeinschaft
ID : DFG-An 156 13-1
Organisme : Australian Research Council
ID : FT170100373
Organisme : Ural Branch, Russian Academy of Sciences
ID : 0397-2019-0003
Informations de copyright
© 2020 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
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