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

da Silva, Marcos A. R.; Silva, Ingrid F.; Xue, Qi; Lo, Benedict T. W.; Tarakina, Nadezda V.; Nunes, Barbara N.; Adler, Peter; Sahoo, Sudhir K.; Bahnemann, Detlef W.; López-Salas, Nieves; Savateev, Aleksandr; Ribeiro, Caue; Kühne, Thomas D.; Antonietti, Markus; Teixeira, Ivo F.

doi:10.1016/j.apcatb.2021.120965

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

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Adler, Peter
Peter Adler, Inorganic Chemistry, Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Citation

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.

Cite as: https://hdl.handle.net/21.11116/0000-0009-C01A-1

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.