Liquid-phase hydrogenation of 1-alkenes over Rh/AlPO4 and Rh/sepiolite catalysts |
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| Affiliation: | 1. Instituto de Catálisis y Petroleoquímica, ICP-CSIC, C/Marie Curie 2, 28049, Cantoblanco, Madrid, Spain;2. Institute of Chemistry, University of Campinas, Rua Monteiro Lobato, 270, 13084-861 Campinas, SP, Brazil;3. Laboratory of Crystallography, ETH Zürich, CH-8093 Zürich, Switzerland;1. School of Chemistry and Chemical Engineering, Queen′s University Belfast, Stranmillis Road, Belfast BT9 5AG, UK;2. School of Mathematics and Physics, Queen''s University Belfast, University Road, Belfast BT7 1NN, UK;1. Jerzy Haber Institute of Catalysis and Surface Chemistry, Polish Academy of Sciences, Niezapominajek 8, 30-239, Krakow, Poland;2. Institute of Metallurgy and Materials Science, Polish Academy of Sciences, Reymonta 25, 30-059, Krakow, Poland;3. AGH University of Science and Technology, Faculty of Geology, Geophysics and Environmental Protection, al. Mickiewicza 30, 30-059, Krakow, Poland;1. Materials Science Centre, Department of Nuclear Physics, University of Madras, Guindy Campus, Chennai 600025, India;2. Department of Inorganic Chemistry, University of Madras, Guindy Campus, Chennai 600025, India;1. Otto von Guericke University, Institute of Process Engineering, Magdeburg, Germany;2. Max Planck Institute for Dynamics of Complex Technical Systems, Molecular Simulations and Design Group, Sandtorstrasse 1, 39106 Magdeburg, Germany;3. Anhalt University of Applied Sciences, Department of Bioscience and Process Engineering, Köthen, Germany;1. State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences Lanzhou 730000, China;2. University of Chinese Academy of Sciences, Beijing 100049, China |
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| Abstract: | The catalytic activity of Rh (1 wt.%) catalysts supported on AlPO4 and sepiolite has been studied in the liquid-phase hydrogenation of linear 1-alkenes. The reaction orders with respect to 1-alkene concentration are negative but are first order with respect to hydrogen, indicating that 1-alkene adsorbs very strongly on Rh sites and alkene and H2, compete for adsorption sites on the surface. The initial hydrogenation rates increase in the order 1-hexene < 1-heptene < 1-octene, and furthermore, on going from 1-hexene to 1-octene the steric effects (through ΔS≠) are activating, while electronic effects (from ΔH≠) deactivate the reaction process. A cis-concerted mechanism taking place in a single step on a Rh site with three coordinative unsaturations which can simultaneously adsorb hydrogen and a π-bonded alkene is suggested. |
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