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 CN bond cleavage. Ni did, however, influence the type of adsorbed species, the heat of adsorption and the activation energies.

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► Adding Ni to WP/SiO2 increases pyridine conversion and pentane yields.
► Adding Ni to WP/SiO2 does not change the HDN reaction mechanism.
► Hydrogenation and CN bond cleavage reactions occur on different active sites.
► Adding Ni to WP/SiO2 does change the type of adsorbed species on both sites.