Journal
JOURNAL OF CATALYSIS
Volume 234, Issue 2, Pages 385-400Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2005.06.028
Keywords
H-ZSM-5; propene methylation; butene methylation; methanol-to-hydrocarbons; propene; linear butenes; isobutene; isotopic labeling
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The co-reaction of propene or n-butene and methanol over an H-ZSM-5 acidic zeolite catalyst has been investigated using isotopically labeled reagents. The main objective has been to obtain kinetic data for the methylation of the propene and n-butene. This study is an extension of our previous investigation of the co-reaction of ethene and methanol [S. Svelle, P.O. Ronning, S. Kolboe, J. Catal. 224 (2004) 115]. At the very high feed rates employed here, the methylation products are dominating, and the isotopic composition is in accord with a methylation formation mechanism. Arrhenius plots have been constructed, and the activation energies, when corrected for the appropriate heats of alkene adsorption, were similar to 110 kJ/mol for the methylation of propene and similar to 90 kJ/mol for the methylation of n-butene. The results are compared with recent computational studies of the methylation of alkenes. The origin of the products not formed via methylation is briefly discussed. A short survey of the reactivity of propene and n-butene without methanol co-feed is presented. It has been found that alkene interconversion reactions are strongly suppressed by the presence of methanol. (c) 2005 Elsevier Inc. All rights reserved.
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