(600v) Thermodynamic and Kinetic Modeling of the SILP Reaction for the Hydrogenation of Propene, the Water Gas Shift Reaction and the Hydroformylation of 1-Butene

Supported Ionic Liquid Phase (SILP) catalyst systems have been successfully applied in continuous gas phase reactions using homogenous catalysts in fixed bed reactors. The homogenously dissolved transition metal complex is immobilized in the thin film of an ionic liquid (IL) dispersed on the high area surface of an inorganic carrier and therefore bridging the gap between homogenous and heterogeneous catalysis.

In this work we present a rigorous thermodynamic reaction modeling for a chemical reaction at a SILP catalyst. The conversion can only be measured in the bulk gas phase. In order to characterize the actual conditions in the reactive IL phase, the phase equilibria of all components are used. The kinetics of the reaction is described by a power law expression, but in contrast to the commonly used concentrations, for the modeling activities are taken. Therefore, a consequent thermodynamic description of the kinetics can be achieved. Furthermore, it is possible to predict the equilibrium conversion which can be used in the modeling process.

For the validation of the developed model, we used experimental data sets of a model system, the hydrogenation of propene, and two technical interesting reactions, the water gas shift reaction and the hydroformylation of 1-butene.

Using the derived model it is possible to describe the reaction properly in different ILs.

The activation energy, determined through the thermodynamic and the kinetic model, is different to the observable activation energy. This is explainable, due to the inclusion of the solvation step in the modelling.

The determined real kinetic parameters and the thermodynamic properties of the IL allow to predict the temperature dependency of the reaction, as well the reaction rate for other ILs.