No abstract
During the last few decades integrated reaction and separation processes have proven to be quite a promising alternative to current methods in terms of process intensification and cost reduction. The goals are an increased conversion of reactants and an efficient suppression of side reactions. In particular, reactive extraction processes are further used to enable the recycling of expensive catalysts like transition metal based catalysts. These catalysts enable high selectivities under mild reaction conditions in homogeneously catalyzed reaction systems.In this work the telomerization of butadiene with ethylene glycol has been carried out in a reactive extraction process. Ethylene glycol and water compose the stationary catalyst phase, butadiene and the product compose the organic transport phase.First a detailed thermodynamic analysis had to be accomplished, determining side reactions, reaction kinetics and physical properties of the component system. Utilizing this information in the generic process synthesis strategy, an advantageous process design has been developed. For reactive and separative functionalities a spatial arrangement could be found which on one hand allows increased conversion and selectivity towards the desired product and on the other hand improves the separation and recyclation of the catalyst.The process design developed has been experimentally investigated and compared to conventional co-current and counter-current processes in a miniplant. In addition to the experiments simulations of all process alternatives were made using the simulation tool ASPEN PLUS. P 4.10Einige der gegenwärtig anspruchsvollsten ingenieurtechnischen Herausforderungen der chemischen Industrie ergeben sich aus Gleichge-wichtslimitierungen chemischer Umsetzungen sowie aus den häufig begrenzten Selektivitäten moderner Katalysatoren bezüglich des gewünschten Wertproduktes. Ziel der hier vorgestellten Arbeit ist es, diese Limitierungen durch innovative Prozessstrukturen integrierter Reaktions-und Trennverfahren zu durchbrechen, gleichzeitig aber die Freiheitsgrade für das Prozessdesign nicht übermäûig einzuschränken. Dabei kommt der Verteilung reaktiver und trennender Funktionalitäten innerhalb des Prozesses besondere Bedeutung zu (s. Abb.).Es wurde eine vom genutzten Trennverfahren unabhängige, systematische Prozesssynthesestrategie entwickelt, die den integrierten Apparat als mehrphasige Einheit mit mindestens einer reaktiven Phase und einer Trans-Abbildung. Abnahme der prozesstechnischen Freiheitsgrade bei zunehmendem Integrationsgrad.
During the last few decades integrated reaction and separation processes have proven to be quite a promising alternative to current methods in terms of process intensification and cost reduction. The goals are an increased conversion of reactants and an efficient suppression of side reactions. In particular, reactive extraction processes are further used to enable the recycling of expensive catalysts like transition metal based catalysts. These catalysts enable high selectivities under mild reaction conditions in homogeneously catalyzed reaction systems.In this work the telomerization of butadiene with ethylene glycol has been carried out in a reactive extraction process. Ethylene glycol and water compose the stationary catalyst phase, butadiene and the product compose the organic transport phase.First a detailed thermodynamic analysis had to be accomplished, determining side reactions, reaction kinetics and physical properties of the component system. Utilizing this information in the generic process synthesis strategy, an advantageous process design has been developed. For reactive and separative functionalities a spatial arrangement could be found which on one hand allows increased conversion and selectivity towards the desired product and on the other hand improves the separation and recyclation of the catalyst.The process design developed has been experimentally investigated and compared to conventional co-current and counter-current processes in a miniplant. In addition to the experiments simulations of all process alternatives were made using the simulation tool ASPEN PLUS. P 4.10Einige der gegenwärtig anspruchsvollsten ingenieurtechnischen Herausforderungen der chemischen Industrie ergeben sich aus Gleichge-wichtslimitierungen chemischer Umsetzungen sowie aus den häufig begrenzten Selektivitäten moderner Katalysatoren bezüglich des gewünschten Wertproduktes. Ziel der hier vorgestellten Arbeit ist es, diese Limitierungen durch innovative Prozessstrukturen integrierter Reaktions-und Trennverfahren zu durchbrechen, gleichzeitig aber die Freiheitsgrade für das Prozessdesign nicht übermäûig einzuschränken. Dabei kommt der Verteilung reaktiver und trennender Funktionalitäten innerhalb des Prozesses besondere Bedeutung zu (s. Abb.).Es wurde eine vom genutzten Trennverfahren unabhängige, systematische Prozesssynthesestrategie entwickelt, die den integrierten Apparat als mehrphasige Einheit mit mindestens einer reaktiven Phase und einer Trans-Abbildung. Abnahme der prozesstechnischen Freiheitsgrade bei zunehmendem Integrationsgrad.
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