Applied Catalysis2022，Vol.30411.DOI:10.1016/j.apcatb.2021.120965

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. Lopez-Salas, Nieves Savateev, Aleksandr Ribeiro, Caue Kuhne, Thomas D. Antonietti, Markus Teixeira, Ivo F.
Applied Catalysis2022，Vol.30411.DOI:10.1016/j.apcatb.2021.120965
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  • NSTL
  • Elsevier

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

da Silva, Marcos A. R. 1Silva, Ingrid F. 2Xue, Qi 3Lo, Benedict T. W. 3Tarakina, Nadezda, V 4Nunes, Barbara N. 5Adler, Peter 6Sahoo, Sudhir K. 7Bahnemann, Detlef W. 5Lopez-Salas, Nieves 4Savateev, Aleksandr 4Ribeiro, Caue 8Kuhne, Thomas D. 7Antonietti, Markus 4Teixeira, Ivo F.1
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作者信息

  • 1. Fed Univ Sao Carlo
  • 2. Univ Fed Minas Gerais
  • 3. Hong Kong Polytech Univ
  • 4. Max Planck Inst Colloids & Interfaces
  • 5. Leibniz Univ Hannover
  • 6. Max Planck Inst Chem Phys Solids
  • 7. Univ Paderborn
  • 8. Brazilian Agr Res Corp Embrapa
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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.

Key words

Single-atom catalysis/Photooxidation/Benzene Oxidation/Iron/Poly (heptazine imide)/TOTAL-ENERGY CALCULATIONS/SELECTIVE OXIDATION/HYDROGEN-PEROXIDE/CARBON NITRIDE/ACTIVE-SITES/BENZENE/PHENOL/NANOPARTICLES/HYDROXYLATION/ACTIVATION

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出版年

2022
Applied Catalysis

Applied Catalysis

ISSN：0926-3373
被引量30
参考文献量76
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