Journal
JOURNAL OF CATALYSIS
Volume 355, Issue -, Pages 53-62Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2017.09.007
Keywords
Co@N-doped graphene shells; Bifunctional catalysts; Oxidative dehydrogenation; Hydrogenation; Active sites
Categories
Funding
- Chinese Academy of Sciences
- National Natural Science Foundation of China [21503242, 21522309, 21603244, 21773271]
- Suzhou Science and Technology Projects [SYG201518, SYG201519]
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Low-cost, active and stable catalysts, with a bifunctional capability if possible, are required to achieve the chemical transformations between saturated and unsaturated N-heterocycles. In this work, Co@N-doped graphene shells (Co@NGS) was used as a bifunctional catalyst with high activity and stability for the oxidative dehydrogenation (ODH) and hydrogenation (HYD) of quinolines. The excellent performance can be attributed to the synergetic effect of N-doped graphene, underlying Co nanoparticles, and the encapsulation structure in which carbon shells protect Co from leaching and aggregation. Poisoning tests with KSCN and spectroscopic analysis clearly unveil that the active sites for ODH and HYD are quite different: N-doped graphene shells modified by Co NPs via electron transfer serve as active sites for the O-2 activation in ODH, while the underlying Co NPs promoted by N dopants favor the H-2 activation in HYD. This finding challenges the previous concept of N-doped carbon sites as active sites for both ODH and HYD. The bifunctional property is due to the access of both N-doped graphene and Co sites to small molecules in our one-pot pyrolyzed Co@NGS catalysts. (C) 2017 Elsevier Inc. All rights reserved.
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