4.8 Article

Electron Spin Catalysis with Graphene Belts

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 62, Issue 10, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202215295

Keywords

Electron Spin Resonance; Graphene Belts; Mechanism; Radical Coupling Reaction; Spin Catalysis

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In this study, kinetic studies were conducted on spin catalysis reactions using electron spin resonance spectroscopy. Graphene belts synthesized by radical coupling method were used as catalysts. The results showed that sigma-type free radical species played a dominant role in the catalytic activity through spin-spin interaction. The spin catalysis mechanism was found to be applicable in both the oxygen reduction reaction and organic synthesis. The graphene belt spin catalyst demonstrated excellent performance with high ORR half-wave potential and long-term stability, as well as high conversion and yield in benzylamine coupling with molecular oxygen to generate imine.
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 sigma-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 approximate to 97.7 % and an average yield of approximate to 97.9 %. This work opens up a new research direction for understanding aerobic processes in the field of spin catalysis.

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