ACS Catalysis p. 8396 - 8405 (2018)
Update date:2022-08-11
Topics:
Li, Guoqiang
Yang, Huanhuan
Zhang, Haifu
Qi, Zhiyuan
Chen, Minda
Hu, Wei
Tian, Lihong
Nie, Renfeng
Huang, Wenyu
Ordered mesoporous N-doped carbon (OMNC) encapsulating Co nanoparticles (NPs) have been prepared under direct polymerization between [Co(NH2CH2CH2NH2)2]Cl2 and carbon tetrachloride through a hard template method. The catalysts (Co@OMNC) are pyrolyzed at various temperatures and characterized by elemental analysis, Brunauer-Emmett-Teller (BET), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and transmission electron microscopy (TEM). In the quinoline transfer hydrogenation with formic acid (FA) as the hydrogen source under a base-free condition, the encapsulated Co NPs are physically isolated from the acidic reaction solution, which prevents them from poisoning or leaching. The rich mesopores and N dopants afford enhanced adsorption of quinoline. Co@OMNC-700 (pyrolyzed at 700 °C) gives the best activity (98.8% conversion) as well as >99% 1,2,3,4-tetrahydroquinoline (THQ) selectivity at 140 °C for 4 h, exhibiting significantly improved performance compared to using H2 as the hydrogenation source. Moreover, Co@OMNC-700 is stable for recycling and exhibits high efficiency in FA dehydrogenation. Co@OMNC-700 is also a high-performance catalyst in the transfer hydrogenation of various unsaturated hydrocarbons. On the contrary, without the protection of OMNC, the exposed Co NPs in a control catalyst, Co/OMNC-700, lead to obvious Co leaching and low efficiency for the transfer hydrogenation of quinoline with FA.
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