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

da Silva, M. A. R., Silva, I. F., Xue, Q., Lo, B. T. W., 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, pp. 1-11. doi:10.1016/j.apcatb.2021.120965.

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 Creators:
da Silva, Marcos A. R.1, Author
Silva, Ingrid F.1, Author
Xue, Qi1, Author
Lo, Benedict T. W.1, Author
Tarakina, Nadezda V.1, Author
Nunes, Barbara N.1, Author
Adler, Peter2, Author              
Sahoo, Sudhir K.1, Author
Bahnemann, Detlef W.1, Author
López-Salas, Nieves1, Author
Savateev, Aleksandr1, Author
Ribeiro, Caue1, Author
Kühne, Thomas D.1, Author
Antonietti, Markus1, Author
Teixeira, Ivo F.1, Author
Affiliations:
1External Organizations, ou_persistent22              
2Peter Adler, Inorganic Chemistry, Max Planck Institute for Chemical Physics of Solids, Max Planck Society, ou_1863435              

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Free keywords: Atoms; Catalyst activity; Ion exchange; Iron compounds; Ketones; Photooxidation; Sodium, Benzene oxidation; C-H bond oxidations; Coordination modes; Oxidation catalysis; Oxidation reactions; Poly (heptazine imide); Single-atom catalyse; Single-atoms; Synthesised; ]+ catalyst, Catalysis
 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. © 2021 Elsevier B.V.

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Language(s): eng - English
 Dates: 2022-01-032022-01-03
 Publication Status: Published in print
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: -
 Identifiers: DOI: 10.1016/j.apcatb.2021.120965
BibTex Citekey: daSilva2022
 Degree: -

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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: 1 - 11 Identifier: ISSN: 0926-3373
CoNE: https://pure.mpg.de/cone/journals/resource/954928540173