Journal
APPLIED CATALYSIS A-GENERAL
Volume 455, Issue -, Pages 219-226Publisher
ELSEVIER
DOI: 10.1016/j.apcata.2013.02.003
Keywords
Dimethyl carbonate; High pressure reaction; CeO2
Categories
Funding
- Fundacao para a Ciencia e a Tecnologia (Portugal) [SFRH/BD/68470/2010, SFRH/BPD/71358/2010, PTDC/EQU-EQU/100564/2008]
- Fundação para a Ciência e a Tecnologia [PTDC/EQU-EQU/100564/2008, SFRH/BD/68470/2010] Funding Source: FCT
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The kinetics for the direct synthesis of dimethyl carbonate was studied over CeO2 at high pressure conditions in a batch reactor. Langmuir-Hinshelwood and Eley-Rideal mechanisms were proposed and compared by the performance of the respective reaction rate expression in fitting to the experimental kinetic data. The reactions were held at different temperatures (378-408 K), CO2/methanol molar ratios (1.1-4.0) and pressures (15-20 MPa) in order to adjust the kinetic parameters. An activation energy of 106 kJ mol(-1), as well as the standard enthalpy and Gibbs energy of reaction (-20.10 and 31.50 kJ mol(-1)) were calculated from experiments. Furthermore, the changes in pressure revealed an effect on the kinetic constant, with an activation volume equal to -0.208 cm(3) mol(-1). (c) 2013 Elsevier B.V. All rights reserved.
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