Journal
MICROPOROUS AND MESOPOROUS MATERIALS
Volume 256, Issue -, Pages 10-17Publisher
ELSEVIER SCIENCE BV
DOI: 10.1016/j.micromeso.2017.07.048
Keywords
Ordered mesoporous N-doped carbon; Ruthenium; Selective hydrogenation; Adsorption; Quinoline
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Funding
- National Natural Science Foundation of China [21603066, 21673069, 21503074, 21571055]
- Natural Science Fund of Hubei Province [2015CFB232]
- Natural Science Fund of the Education Department of Hubei Province [Q2015009]
- Natural Science Fund for Creative Research Groups of Hubei Province of China [2014CFA015]
- Sci-tech Support Project of the Science and Technology Department of Hubei Province of China [2014BAA098]
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Ordered mesoporous N-doped carbon (OMNC) is prepared via a facile nanocasting approach using ethylenediamine (EDA) and carbon tetrachloride (CTC) as precursors, for which the pore structure, Ndopants and basicity are strongly dependent on the pyrolysis temperature (500-800 degrees C). After supporting 2.5% Ru by incipient wetness impregnation, the imitate interaction of N-dopants with Ru has a strong influence on the activity and selectivity of quinoline hydrogenation, as disclosed by XPS and H2TPR studies. It is found that Ru/OMNC-700 obtained at 700 degrees C shows superior substrate adsorption and catalytic activity under mild conditions (40 degrees C and 1 MPa H-2). The turnover frequency (TOF) and activation energy of Ru/OMNC-700 for the hydrogenation of quinoline are 71.0 h(-1) and 31.37 kJ/mol. In particular, this catalyst retains 98.3% of the initial catalytic activity after 5 recycles and shows high compatibility with various N-heterocycles with good conversion and high selectivity, attributed to the strong electron donation from OMNC-700 to Ru and the enhanced adsorption of pyridine ring with high selectivity over OMNC-700. This strategy for the preparation of the supported Ru catalysts opens a new possibility of designing highly efficient heterogeneous catalysts in the future. (C) 2017 Published by Elsevier Inc.
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