Please use this identifier to cite or link to this item: https://doi.org/10.1016/j.jcat.2005.09.019
Title: First-principles based kinetic model for the hydrogenation of toluene
Authors: Saeys, M. 
Reyniers, M.-F.
Thybaut, J.W.
Neurock, M.
Marin, G.B.
Keywords: Benzene
First-principles modeling
Hydrogenation
Kinetic modeling
Toluene
Issue Date: 15-Nov-2005
Source: Saeys, M., Reyniers, M.-F., Thybaut, J.W., Neurock, M., Marin, G.B. (2005-11-15). First-principles based kinetic model for the hydrogenation of toluene. Journal of Catalysis 236 (1) : 129-138. ScholarBank@NUS Repository. https://doi.org/10.1016/j.jcat.2005.09.019
Abstract: A fundamental kinetic model for the hydrogenation of toluene over platinum has been constructed, based on detailed first-principles density functional theory calculations for the hydrogenation of benzene over Pt(111). A Langmuir-Hinshelwood-Hougen-Watson (LHHW) kinetic model was derived based on an ab initio reaction path analysis [M. Saeys, M.-F. Reyniers, M. Neurock, G.B. Marin, J. Phys. Chem. B 109 (2005) 2064], enabling easy interpretation and evaluation of the parameters appearing in the rate equation. The activation energy, adsorption, and reaction enthalpies in the model were obtained from the first-principles calculations. The pre-exponential factors were calculated from statistical mechanics, using assumptions derived from the first-principles results. The coverage-dependent hydrogen chemisorption enthalpy was optimized to accurately model lab-scale experimental data for the gas phase hydrogenation of toluene over a 0.5 wt% Pt/ZSM-22 catalyst. The resulting hydrogen chemisorption enthalpy of -54.0±1.0 kJ/mol falls between the high and low coverage values, consistent with a simulated average hydrogen surface coverage of 61%. The LHHW model based on the ab initio calculations captures the main trends in the reaction rates. The reaction model predicts reaction orders for the inlet partial pressure of hydrogen and toluene ranging from 1.6 to 2.2 and from -0.4 to 0.7, respectively. This is in reasonable agreement with experimental values, which range from 1.3 to 1.8 and from -0.3 to 0.3, respectively. © 2005 Elsevier Inc. All rights reserved.
Source Title: Journal of Catalysis
URI: http://scholarbank.nus.edu.sg/handle/10635/63925
ISSN: 00219517
DOI: 10.1016/j.jcat.2005.09.019
Appears in Collections:Staff Publications

Show full item record
Files in This Item:
There are no files associated with this item.

SCOPUSTM   
Citations

49
checked on Dec 13, 2017

WEB OF SCIENCETM
Citations

46
checked on Nov 16, 2017

Page view(s)

67
checked on Dec 10, 2017

Google ScholarTM

Check

Altmetric


Items in DSpace are protected by copyright, with all rights reserved, unless otherwise indicated.