Electron Spin Catalysis with Graphene Belts

Here, we report kinetic studies using electron spin resonance spectroscopy on spin catalysis reactions caused by using graphene belts which were synthesized by a radical coupling method. The results show that σ‐type free radical species provide the dominant sites for catalytic activity through the s...

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Bibliographic Details
Published in:Angewandte Chemie International Edition 2023-03, Vol.62 (10), p.e202215295-n/a
Main Authors: Tian, Yulan, Cao, Huaqiang, Yang, Haijun, Yao, Wenqing, Wang, Jiaou, Qiao, Zirui, Cheetham, Anthony K.
Format: Article
Language:English
Subjects:
Aerobic processes
Belts
Catalysis
Catalysts
Catalytic activity
Chemical reduction
Chemical synthesis
Coupling (molecular)
Electron paramagnetic resonance
Electron spin
Electron Spin Resonance
Free radicals
Graphene
Graphene Belts
Mechanism
Oxygen reduction reactions
Radical Coupling Reaction
Spectroscopy
Spin Catalysis
Spin resonance
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Summary:Here, we report kinetic studies using electron spin resonance spectroscopy on spin catalysis reactions caused by using graphene belts which were synthesized by a radical coupling method. The results show that σ‐type free radical species provide the dominant sites for catalytic activity through the spin‐spin interaction, although there are some other influencing factors. The spin catalysis mechanism can be applied both in the oxygen reduction reaction (ORR) and in organic synthesis. The graphene belt spin catalyst shows excellent performance with a high ORR half‐wave potential of 0.81 V and long‐term stability with almost no loss of activity after 50 000 cycles in alkaline media. It also shows excellent performance in a benzylamine coupling with molecular oxygen to generate the corresponding imine at an average conversion of ≈97.7 % and an average yield of ≈97.9 %. This work opens up a new research direction for understanding aerobic processes in the field of spin catalysis. Graphene belts with high electron spin concentrations, which were synthesized by C (sp2)−C (sp2) radical coupling, act as aerobic spin catalysts for both the oxygen reduction reaction (ORR) and a benzylamine coupling with molecular oxygen to generate the corresponding imine; the catalytic mechanism has been studied by electron spin resonance spectroscopy.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202215295