Efficient Photocatalytic Selective Oxidation of Benzylamines over Cobalt Molecular Catalyst Covalently Bonded to Carboxyl Functionalized Carbon Nitride

Photocatalysis is accepted as a promising method for selective oxidative coupling of amine to imine. However, owing to the rapid dehydrogenation of the generated imine intermediate of α‐amino hydrogen to butyronitrile, it remains a huge challenge to fabricate an exquisite catalyst with enhanced conv...

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Bibliographic Details
Published in:Advanced energy and sustainability research 2023-11, Vol.4 (11), p.n/a
Main Authors: Wang, Chuntao, Li, Haixia, Guo, Yingxin, Zhao, Hui, Dong, Yuming, Zhu, Yongfa
Format: Article
Language:English
Subjects:
Amines
benzylamine
Carbon
Carbon nitride
carbon nitrides
Catalysts
Chemical bonds
Cobalt
Coupling (molecular)
covalent bonding
Dehydrogenation
Fourier transforms
Imines
Microscopy
molecule catalysts
Oxidation
Oxygen
Photocatalysis
photocatalytic selective oxidation
Selectivity
Substrates
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Summary:Photocatalysis is accepted as a promising method for selective oxidative coupling of amine to imine. However, owing to the rapid dehydrogenation of the generated imine intermediate of α‐amino hydrogen to butyronitrile, it remains a huge challenge to fabricate an exquisite catalyst with enhanced conversion and selectivity. Herein, a novel heterogeneous catalyst (Bpy‐CoCl 2 /CNCOOH) is developed, where carboxyl functionalized carbon nitride (CNCOOH) serves as a substrate material and couples with highly efficient cobalt‐aminopyridine (Bpy‐CoCl 2 ) molecular catalyst through covalent bonding. The catalyst not only effectively facilitates the transfer of photogenerated charges, but also generates mildly oxidatively active species of superoxide radicals, which can effectively oxidize various functionalized benzylamines to corresponding imines in the presence of oxygen with at least 78.5% conversion and >99% selectivity using O 2 as oxygen source, especially for the unmodified benzylamine with >99% conversion and >99% selectivity. This unique combination of a selective molecular catalyst and a simple and robust semiconducting material open new avenues for the selective oxidative coupling of amines.
ISSN:2699-9412
2699-9412
DOI:10.1002/aesr.202300114