Journal
CATALYSIS TODAY
Volume 105, Issue 1, Pages 93-105Publisher
ELSEVIER
DOI: 10.1016/j.cattod.2005.04.005
Keywords
ab initio; Car-Parrinello molecular dynamics; C-C bond; chabazite; constrained molecular dynamics; coupling; methanol; reaction; transition path sampling; zeolite
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We describe the application of transition path sampling methods to the methanol coupling reaction in the zeolite chabazite; these methods have only been recently applied to complex chemical systems. Using these methods, we have found a new mechanism for the formation of the first C-C bond. In our mechanism, the reaction, at 400 degrees C, proceeds via a two-step process: (1) the breaking of the C-O bond of the chemisorbed methoxonium cation, followed by the transfer of a hydride ion from the remaining methanol molecule to the methyl cation, resulting in the formation of H2O, CH4, and CH2OH+ and (2) a simultaneous proton transfer from methane to water, and direct C-C bond formation between the methyl anion and CH2OH+, resulting in the formation of ethanol. The C-C bond forming process has the higher barrier, with an activation energy of about 100.49 kJ/mol. (c) 2005 Elsevier B.V. All rights reserved.
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