Determination of kinetics and equilibria of heterogeneously catalyzed gas-phase reactions in gradientless autoclave reactors by using the total pressure method: Methanol synthesis

A1 Journal article (refereed)


Internal Authors/Editors


Publication Details

List of Authors: Tapio Salmi, Kari Eränen, Pasi Tolvanen, J.-P. Mikkola, Vincenzo Russo
Publication year: 2019
Journal: Chemical Engineering Science
Journal acronym: Chem. Eng. Sci.
ISSN: 0009-2509
eISSN: 1873-4405


Abstract

Rapid methods are very valuable in the determination of the kinetic and mass transfer effects for heterogeneously catalyzed reactions. The total pressure method is a classical tool in the measurement of the kinetics of gas-phase reactions, but it can be successfully applied to the kinetic measurements of gas-phase processes enhanced by solid catalysts. A general theory for the analysis of heterogeneously catalyzed gas-phase kinetics in gradientless batch reactors was presented for the case of intrinsic kinetic control and combined kinetic-diffusion control in porous catalysts. The concept was applied to gas-phase synthesis of methanol from carbon monoxide and hydrogen on a commercial copper-based catalyst (CuO/ZnO/Al2O3 R3-12 BASF). The reaction temperature was 180–210 °C and the initial total pressure was varied between 11 and 21 bar in a laboratory-scale autoclave reactor equipped with a rotating basket for the catalyst particles. The initial molar ratios CO-to-H2 were approximately 1:2, 1:3 and 1:4. The experimental data from methanol synthesis were compared with numerical simulations and a good agreement between the experiments and model simulations was achieved. The predicted equilibrium agrees with previously reported values.


Keywords

Gradientless reactor, Methanol synthesis, Solid catalyst, Total pressure method

Last updated on 2020-07-06 at 03:35