Kinetics of the solvent-free hydrogenation of 2-methyl-3-butyn-2-ol over a structured Pd-based catalyst |
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Authors: | Micaela Crespo-Quesada Martin Grasemann Natalia Semagina Albert Renken Lioubov Kiwi-Minsker |
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Affiliation: | aGroup of Catalytic Reaction Engineering, Ecole Polytechnique Fédérale de Lausanne, EPFL-SB-ISIC-GGRC, Station 6, CH-1015 Lausanne, Switzerland |
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Abstract: | The solvent-free selective hydrogenation of 2-methyl-3-butyn-2-ol (MBY) to 2-methyl-3-buten-2-ol (MBE) was studied over a Pd/ZnO structured catalyst and compared to its behavior in water-assisted conditions. The catalytic behavior was correlated with the surface properties of the catalysts which were characterized by X-ray diffraction and X-ray photoelectron spectroscopy. The catalyst showed high selectivity and stability with the performance being superior to that of the industrial Lindlar catalyst (50%). The addition of a sulphur-containing modifier in the reaction mixture was found to affect the activity and to hinder the over-hydrogenation reaction. The MBE yield of 97% was attained at MBY conversion >99%. The reuse of the catalyst showed that it deactivated by a 38% and that its selectivity slightly increased (0.5%) over 10 runs. The reaction kinetics was modeled using a Langmuir–Hinshelwood mechanism considering competitive adsorption for the organic species and dissociative adsorption for hydrogen. The kinetic experiments were planned and the results analyzed following a design of experiments (DOE) methodology. This approach led not only to a robust model that predicts the reaction rate in a wide range of reaction conditions but also to the determination of its kinetic parameters. |
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Keywords: | Hydrogenation Kinetics modeling Palladium Structured catalyst Design of experiments 2-Methyl-3-butyn-2-ol |
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