期刊
APPLIED CATALYSIS A-GENERAL
卷 530, 期 -, 页码 132-144出版社
ELSEVIER SCIENCE BV
DOI: 10.1016/j.apcata.2016.11.015
关键词
Hydrodenitrogenation; Quinoline; Kinetics; NiMo(P) catalysts; Support; Acidity; Silica-alumina; Liquid-vapor mass transfer
资金
- IFP Energies Nouvelles
- CNRS, France
A detailed kinetic study of the hydrodenitrogenation (HDN) network of quinoline was carried out over Ni-promoted MoS2 catalysts supported either on gamma-Al2O3 or on amorphous silica alumina (ASA), the objective is to identify the role of the support acidity in HDN reactions. The kinetic data obtained from catalytic tests in a batch reactor were analyzed by a model including the liquid-vapor mass transfer. The adsorption constants of all intermediates and the kinetic constants of all elementary steps were estimated. We found that the NiMo(P)/ASA exhibited a higher rate constant in the hydrogenation of tetrahydroquinoline, which was the rate determining step of the main reaction pathway, and in exocyclic carbon-nitrogen bond cleavage reactions, than the NiMo(P)/Al2O3. Characterization data by Infra-Red spectroscopy of CO suggested that this result might be related to the modification of the electronic properties of promoted NiMoS phase due to higher acidity of ASA. However, the stronger self-inhibiting effect due to stronger adsorption of nitrogen compounds over NiMo(P)/ASA and its lower content of NiMoS phase decreased its global catalytic activity. (C) 2016 Elsevier B.V. All rights reserved.
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