A computational approach to solvent selection for biphasic reaction systems

Biphasic reaction systems with a reactive and a non-reactive phase are widespread in technical applications. The non-reactive phase serves as a reservoir of dissolved substrates at high concentrations and allows for the extraction of the product during the reaction. The proper choice of the phase combination will have manifold influence on catalytic parameters such as activity, selectivity, and stability, but also on maximum conversion or yield. To optimize such biphasic reactions, conversion and yield constitute concise targets of practical relevance for a rational solvent screening which requires thermodynamic information on coupled reactions and phase equilibria as input. Usually, the experimental determination of these data requires considerable laboratory effort. To minimize the experimental effort and to enlarge the dataspace for optimization, an in silico solvent screening for maximum conversion and yield in different biphasic catalyzed reactions is evaluated. The primary target of the investigations is in biocatalytic applications as these benefit greatly from the addition of organic non-reactive media to the reactive aqueous phase. The conductor-like screening model for realistic solvation (COSMO-RS) is used for the prediction of solute partitioning between organic solvents and a reaction medium. Although the calculated results show significant absolute deviations, COSMO-RS still predicts the correct trends for the partition coefficients of solutes in different solvents. Furthermore, a combination of statistical thermodynamics and classical quantum mechanics is used for the prediction of the reaction equilibria. The calculated overall reaction equilibrium using the calculated partition coefficients and the calculated equilibrium constants again results in the prediction of the best solvent combination regarding conversion and yield. Extending the approach with numerical simulations provides a more detailed insight into the reaction system.

Grantor dc:publisher

Publikationsserver der RWTH Aachen University

Year dc:date

2008

Author dc:creator

• Peters, Martina

Contributors dc:contributor

• Leitner, Walter

• info:eu-repo/classification/ddc/660
• Thermodynamik
• Phasengleichgewicht
• Computational chemistry
• Biokatalyse
• Technische Chemie
• COSMO-RS
• Vorhersage
• Zweiphasensysteme
• prediction
• biphasic systems

Statement dc:rights

• info:eu-repo/semantics/openAccess

Language dc:language

eng

Identifier

https://publications.rwth-aachen.de/search?p=id:%22RWTH-CONV-113337%22

OAI record oai:identifier

https://publications.rwth-aachen.de/oai2d?verb=GetRecord&metadataPrefix=oai_dc&identifier=oai%3Apublications.rwth-aachen.de%3A50811