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  Sustainable oxidation catalysis supported by light : Fe-poly (heptazine imide) as a heterogeneous single-atom photocatalyst

da Silva, M. A., Silva, I. F., Xue, Q., Lo, B. T., Tarakina, N. V., Nunes, B. N., et al. (2022). Sustainable oxidation catalysis supported by light: Fe-poly (heptazine imide) as a heterogeneous single-atom photocatalyst. Applied Catalysis B: Environmental, 304: 120965. doi:10.1016/j.apcatb.2021.120965.

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 Creators:
da Silva, Marcos A.R., Author
Silva, Ingrid F.1, Author              
Xue, Qi, Author
Lo, Benedict T.W., Author
Tarakina, Nadezda V.2, Author              
Nunes, Barbara N., Author
Adler, Peter, Author
Sahoo, Sudhir K., Author
Bahnemann, Detlef W., Author
López-Salas, Nieves3, Author              
Savateev, Aleksandr4, Author              
Ribeiro, Caue, Author
Kühne, Thomas D., Author
Antonietti, Markus1, Author              
Teixeira, Ivo1, Author              
Affiliations:
1Markus Antonietti, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_1863321              
2Nadezda V. Tarakina, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_2522693              
3Nieves Lopez Salas, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_3029702              
4Aleksandr Savateev, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_2421702              

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Free keywords: Single-atom catalysis, Photooxidation, Benzene Oxidation, Iron, Poly (heptazine imide)
 Abstract: Fe-N-C materials, when prepared as single-atom catalysts (SAC), display excellent activities in oxidation reactions. The systematic investigation of the iron coordination mode revealed that Fe-N4C catalysts are the most active for C-H bond oxidation. However, many of these catalysts are synthesized through pyrolysis, which is characterized by a lack of control and structures with heterogeneous composition, rarely presenting only atomically dispersed Fe−N − C as active sites. Herein, an alternative, reliable and easily reproducible method to obtain highly active Fe SACs (atomically dispersed) with Fe-N4 sites is presented, which is based on ion exchange of sodium from high crystalline sodium poly(heptazine imide) (Na-PHI) by other ions. The obtained catalyst can photocatalytically oxidize C-H bonds selectively toward ketones using only dioxygen. Detailed mechanism investigations indicate that the active species in the C-H bond oxidation are highly valent Fe(IV)/Fe(V)-oxo species, which are further activated by the holes generated at the PHI support under light irradiation.

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Language(s): eng - English
 Dates: 2021-11-272022
 Publication Status: Published in print
 Pages: -
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 Table of Contents: -
 Rev. Type: -
 Identifiers: DOI: 10.1016/j.apcatb.2021.120965
BibTex Citekey: DASILVA2022120965
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Title: Applied Catalysis B: Environmental
  Abbreviation : Appl. Catal. B Environ.
Source Genre: Journal
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Publ. Info: Amsterdam : Elsevier
Pages: - Volume / Issue: 304 Sequence Number: 120965 Start / End Page: - Identifier: ISSN: 0926-3373