Comprehensive kinetic study for pyridine hydrodenitrogenation on (Ni)WP/SiO2 catalysts

In this work the reaction kinetics for pyridine hydrodenitrogenation on (Ni)WP/SiO2 catalysts were determined. The experiments were conducted at 17.2 bar and between 573 K and 633 K for various flow rates of hydrogen and pyridine. Adding Ni to the WP/SiO2 catalyst enhanced the hydrogenation reaction and gave higher pentane and pentylamine yields. A trend in terms of selectivity was not evident on either catalyst. The results were fit to several models and a Bayesian approach was applied for parameter estimation and model discrimination. Adding Ni to the WP/SiO2 catalyst did not change the reaction mechanism - both catalysts favor the same Langmuir-Hinshelwood model with different active sites for hydrogenation and C-N bond cleavage. Ni did, however, influence the type of adsorbed species, the heat of adsorption and the activation energies. (C) 2012 Elsevier B.V. All rights reserved.