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

Da Silva MAR, Silva IF, Xue Q, Lo BTW, Tarakina N, Nunes BN, Adler P, Sahoo SK, Bahnemann DW, Lopez-Salas N, Savateev A, Ribeiro C, Kühne TD, Antonietti M, Teixeira IF (2022)

Publication Type: Journal article

Publication year: 2022

Journal

Applied Catalysis B-Environmental Elsevier

Book Volume: 304

Article Number: 120965

DOI: 10.1016/j.apcatb.2021.120965

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.

Involved external institutions

Universidade Federal de São Carlos (UFSCar) / Federal University of São Carlos BR Brazil (BR) Universidade Federal de Minas Gerais (UFMG) BR Brazil (BR) Hong Kong Polytechnic University (PolyU) CN China (CN) Max-Planck-Institut für Kolloid- und Grenzflächenforschung / Max Planck Institute of Colloids and Interfaces DE Germany (DE) Gottfried Wilhelm Leibniz Universität Hannover DE Germany (DE) Max-Planck-Institut für Chemische Physik fester Stoffe (MPI CPfS) / Max Planck Institute for Chemical Physics of Solids DE Germany (DE) Universität Paderborn DE Germany (DE) Brazilian Agricultural Research Corporation / Empresa Brasileira de Pesquisa Agropecuária (Embrapa) BR Brazil (BR)

How to cite

APA:

Da Silva, M.A.R., Silva, I.F., Xue, Q., Lo, B.T.W., Tarakina, N., Nunes, B.N.,... Teixeira, I.F. (2022). Sustainable oxidation catalysis supported by light: Fe-poly (heptazine imide) as a heterogeneous single-atom photocatalyst. Applied Catalysis B-Environmental, 304. https://dx.doi.org/10.1016/j.apcatb.2021.120965

MLA:

Da Silva, Marcos A. R., et al. "Sustainable oxidation catalysis supported by light: Fe-poly (heptazine imide) as a heterogeneous single-atom photocatalyst." Applied Catalysis B-Environmental 304 (2022).

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