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See detailExperimental procedure and statistical data treatment for the kinetic study of selective hydrodechlorination of 1,2-dichloroethane into ethylene over a Pd-Ag sol–gel catalyst
Pirard, Sophie ULg; Pirard, Jean-Paul ULg; Heyen, Georges ULg et al

in Chemical Engineering Journal (2011), 173(3), 801-812

The kinetics of selective hydrodechlorination of 1,2-dichloroethane into ethylene over a Pd- Ag/SiO2 catalyst was studied using an a priori experimental design with five independent variables—temperature ... [more ▼]

The kinetics of selective hydrodechlorination of 1,2-dichloroethane into ethylene over a Pd- Ag/SiO2 catalyst was studied using an a priori experimental design with five independent variables—temperature and partial pressures of 1,2-dichloroethane, hydrogen, ethylene and hydrogen chloride. A Langmuir–Hinshelwood model including two types of active site and the 1,2-dichloroethane adsorption as the rate-determining step was found to fit correctly with experimental data, according to the analysis of variance and the analysis of pondered residuals. The study allowed for catalytic deactivation. The rigorous experimental and statistical approach followed to carry out such a kinetic study is explained in detail. [less ▲]

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See detailPalladium-silver sol-gel catalysts for selective hydrodechlorination of 1,2-dichloroethane into ethylene - IV. Deactivation mechanism and regeneration
Heinrichs, Benoît ULg; Noville, Francis ULg; Schoebrechts, Jean-Paul ULg et al

in Journal of Catalysis (2003), 220(1), 215-225

The activity and selectivity of a 1.9% Pd-3.7% Ag/SiO2 catalyst during selective hydrodechlorination of 1,2-dichloroethane into ethylene have been followed in the course of time. The deactivation curves ... [more ▼]

The activity and selectivity of a 1.9% Pd-3.7% Ag/SiO2 catalyst during selective hydrodechlorination of 1,2-dichloroethane into ethylene have been followed in the course of time. The deactivation curves show two distinct periods: an initial period at the very beginning of catalyst operation, that is, during the first 20 operating hours, characterized by a sharp decrease of the rates of both reactions involved in the process (1,2-dichloroethane hydrodechlorination and undesired ethylene hydrogenation) and a second period, after the first 20 operating hours and investigated for more than 600 h, characterized by a clearly slower deactivation. During the initial period, the hydrodechlorination rate decreases less quickly than the hydrogenation rate and this results in a fast increase of ethylene selectivity which reaches a maximum at the end of this period. After the initial period, the hydrodechlorination rate decreases faster than the hydrogenation rate and this results in a slow decrease of ethylene selectivity. A comparison between the physico-chemical properties of the fresh catalyst and of the deactivated one suggests a deactivation mechanism by poisoning or coking of silver sites at the surface of the active Pd-Ag alloy particles whereas palladium sites would remain intact. The selectivity evolution during the second period, that is, after the very first operating hours, is in agreement with such a mechanism. However, the sharp ethylene selectivity increase during the initial operating hours suggests, in addition to the deactivation by silver sites disappearance, the presence of a further nonidentified phenomenon. The characterization of the catalyst after a regeneration treatment including an oxidation step followed by a reduction step shows that this treatment allows restoration near to the physico-chemical properties of the fresh catalyst. (C) 2003 Elsevier Inc. All rights reserved. [less ▲]

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