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Metal-free activation of molecular oxygen by covalent triazine frameworks for selective aerobic oxidation

Sara Abednatanzi, Parviz Gohari Derakhshandeh (UGent) , Karen Leus (UGent) , Henk Vrielinck (UGent) , Freddy Callens (UGent) , Johannes Schmidt, Aleksandr Savateev and Pascal Van Der Voort (UGent)
(2020) SCIENCE ADVANCES. 6(14).
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Abstract
Oxygen activation is a critical step in ubiquitous heterogeneous oxidative processes, most prominently in catalysis, electrolysis, and pharmaceutical applications. We present here our findings on metal-free O-2 activation on covalent triazine frameworks (CTFs) as an important class of N-rich materials. The O-2 activation process was studied for the formation of aldehydes, ketones and imines. A detailed mechanistic study of O-2 activation and the role of nitrogen heteroatoms were comprehensively investigated. The electron paramagnetic resonance (EPR) and control experiments provide strong evidence for the reaction mechanism proving the applicability of the CTFs to activate oxygen into superoxide species. This report highlights the importance of a self-templating procedure to introduce N functionalities for the development of metal-free catalytic materials. The presented findings reveal an important step toward the use of CTFs as inexpensive and high-performance alternatives to metal-based materials not only for catalysis but also for biorelated applications dealing with O-2 activation.
Keywords
Doped Carbon Nanosheets, Organic Frameworks, Porous Carbon, Free Catalyst, Nitrogen, Performance, Graphene, Nanoparticles, Evolution, Alcohols, CTF, General Environmental Science, Catalysis, COF, Oxidation, Aerobic, Metal-free, Sustainable, Green Chemistry

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MLA
Abednatanzi, Sara, et al. “Metal-Free Activation of Molecular Oxygen by Covalent Triazine Frameworks for Selective Aerobic Oxidation.” SCIENCE ADVANCES, vol. 6, no. 14, 2020, doi:10.1126/sciadv.aaz2310.
APA
Abednatanzi, S., Gohari Derakhshandeh, P., Leus, K., Vrielinck, H., Callens, F., Schmidt, J., … Van Der Voort, P. (2020). Metal-free activation of molecular oxygen by covalent triazine frameworks for selective aerobic oxidation. SCIENCE ADVANCES, 6(14). https://doi.org/10.1126/sciadv.aaz2310
Chicago author-date
Abednatanzi, Sara, Parviz Gohari Derakhshandeh, Karen Leus, Henk Vrielinck, Freddy Callens, Johannes Schmidt, Aleksandr Savateev, and Pascal Van Der Voort. 2020. “Metal-Free Activation of Molecular Oxygen by Covalent Triazine Frameworks for Selective Aerobic Oxidation.” SCIENCE ADVANCES 6 (14). https://doi.org/10.1126/sciadv.aaz2310.
Chicago author-date (all authors)
Abednatanzi, Sara, Parviz Gohari Derakhshandeh, Karen Leus, Henk Vrielinck, Freddy Callens, Johannes Schmidt, Aleksandr Savateev, and Pascal Van Der Voort. 2020. “Metal-Free Activation of Molecular Oxygen by Covalent Triazine Frameworks for Selective Aerobic Oxidation.” SCIENCE ADVANCES 6 (14). doi:10.1126/sciadv.aaz2310.
Vancouver
1.
Abednatanzi S, Gohari Derakhshandeh P, Leus K, Vrielinck H, Callens F, Schmidt J, et al. Metal-free activation of molecular oxygen by covalent triazine frameworks for selective aerobic oxidation. SCIENCE ADVANCES. 2020;6(14).
IEEE
[1]
S. Abednatanzi et al., “Metal-free activation of molecular oxygen by covalent triazine frameworks for selective aerobic oxidation,” SCIENCE ADVANCES, vol. 6, no. 14, 2020.
@article{8656324,
  abstract     = {{Oxygen activation is a critical step in ubiquitous heterogeneous oxidative processes, most prominently in catalysis, electrolysis, and pharmaceutical applications. We present here our findings on metal-free O-2 activation on covalent triazine frameworks (CTFs) as an important class of N-rich materials. The O-2 activation process was studied for the formation of aldehydes, ketones and imines. A detailed mechanistic study of O-2 activation and the role of nitrogen heteroatoms were comprehensively investigated. The electron paramagnetic resonance (EPR) and control experiments provide strong evidence for the reaction mechanism proving the applicability of the CTFs to activate oxygen into superoxide species. This report highlights the importance of a self-templating procedure to introduce N functionalities for the development of metal-free catalytic materials. The presented findings reveal an important step toward the use of CTFs as inexpensive and high-performance alternatives to metal-based materials not only for catalysis but also for biorelated applications dealing with O-2 activation.}},
  articleno    = {{eaaz2310}},
  author       = {{Abednatanzi, Sara and Gohari Derakhshandeh, Parviz and Leus, Karen and Vrielinck, Henk and Callens, Freddy and Schmidt, Johannes and Savateev, Aleksandr and Van Der Voort, Pascal}},
  issn         = {{2375-2548}},
  journal      = {{SCIENCE ADVANCES}},
  keywords     = {{Doped Carbon Nanosheets,Organic Frameworks,Porous Carbon,Free Catalyst,Nitrogen,Performance,Graphene,Nanoparticles,Evolution,Alcohols,CTF,General Environmental Science,Catalysis,COF,Oxidation,Aerobic,Metal-free,Sustainable,Green Chemistry}},
  language     = {{eng}},
  number       = {{14}},
  pages        = {{10}},
  title        = {{Metal-free activation of molecular oxygen by covalent triazine frameworks for selective aerobic oxidation}},
  url          = {{http://doi.org/10.1126/sciadv.aaz2310}},
  volume       = {{6}},
  year         = {{2020}},
}
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