Journal
ACS CATALYSIS
Volume 12, Issue 9, Pages 5595-5604Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.1c04467
Keywords
single-atom catalyst; nanoclusters; synergistic catalysis; singlet oxygen; oxidation of amines
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Funding
- National Natural Science Foundation of China [22078305, 22002178]
- Natural Science Foundation of Shandong Province [ZR2020KB016]
- Royal Society (UK) [NAF\R2\180695]
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The coexistence of Fe nanoclusters and Fe single atoms in N-doped porous carbon can significantly enhance the catalytic performance in the aerobic oxidation of primary amines to imines.
Tuning the geometric and electronic structure of the single-metal-atom catalysts via simultaneous presence of metal nanoparticles or nanoclusters (NCs) offers an alternative avenue to improving their catalytic performance. Herein, we demonstrate that the coexistence of Fe NCs in proximity to Fe single atoms on N-doped porous carbon can significantly improve the catalytic performance in aerobic oxidation of primary amines to imines using air as the oxidant. A broad spectrum of primary aromatic, heterocyclic, and aliphatic amines was efficiently and selectively oxidized into their corresponding imines in good to high yields. Experimental measurements and theoretical calculations reveal that the proximity of Fe NCs interacts with Fe single atoms, which not only benefits the adsorption of molecular O2 and amine substrates but also promotes the activation of O2 to selectively generate singlet oxygen (1O2) and then facilitates the key intermediate imine formation via H-atom abstraction with a lower energy barrier, thereby significantly boosting the reaction activity.
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