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Quantifying the dominant factors in Cu catalyst deactivation during glycerol hydrogenolysis
Tapas Rajkhowa,Guy B. Marin,Joris W. Thybaut 한국공업화학회 2017 Journal of Industrial and Engineering Chemistry Vol.54 No.-
Long term stability of a commercial Cu-based glycerol hydrogenolysis catalyst has been studied in an isothermal trickle-bed reactor at 473–503 K in the presence of impurities, such as S, Cl and glycerides. While glycerides have the least effect on the catalytic activity, the increase in the extent of deactivation with temperature as a consequence of thiophene indicates a kinetic rather than a thermodynamic adsorption effect. The threshold driven, ‘sudden’ manner in which deactivation manifests itself in case of Cl is indicative of sintering. A deactivation model accounting for the activity loss with changing concentration of impurities and temperature, was constructed.
Jonas Van Belleghem,Jia Yang,Pieter Janssens,Jeroen Poissonnier,De Chen,Guy B. Marin,Joris W. Thybaut 한국공업화학회 2022 Journal of Industrial and Engineering Chemistry Vol.105 No.-
A Single-Event MicroKinetic (SEMK) model has been extended towards the simulation of Steady StateIsotopic Transient Kinetic Analysis (SSITKA) data for Co catalyzed Fischer-Tropsch Synthesis (FTS). Theextended model considers two types of sites and both direct and H-assisted CO dissociation. Regression of the model parameters to the data obtained from 17 steady state and 11 SSITKA experimentsresulted in physicochemically meaningful estimates for the activation energies and atomic chemisorptionenthalpies. The application of the phenomenological UBI-QEP method allows to physically interpret thenature of the two site types considered in the model, i.e., terrace and step sites. A reaction path analysisshows that over 80 percent of the CO reacts on the step sites. Furthermore, chain growth exclusivelyoccurs on these sites. The terrace sites are less reactive for CO dissociation and are identified as responsiblefor methane production. A fraction of the alkenes, produced on the step sites, is hydrogenated toalkanes on the terrace sites. Based on model simulations, the metal particle size effect, i.e., a lowerTOF, higher methane selectivity and increasing alkane to alkene ratio with decreasing metal particle size,is attributed to an increasing relative importance of the terrace sites on the reaction kinetics.