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Engineering and technology
- Homogeneous catalysis
- Reacting systems
- Chemical kinetics and thermodynamics
- Modelling, simulation and optimisation
- Intensification
Nowadays, there is a strong drive to design new and optimize existing large-scale chemical processes in the pursuit of sustainability and increased profitability. Theoretical and computational advances have made predictive first principles based modelling of gas-phase processes feasible, e.g. oxidation. This is in sharp contrast with the limited fundamental understanding of homogeneous catalyzed reactions important for many liquid-phase processes. Systematically resolving this knowledge gap is the objective of this project. To realize this, experimental, theoretical and kinetic modelling work will be combined. The liquid-phase autoxidation of cyclohexane to cyclohexanone and cyclohexanol will be investigated as proof of concept, because it is an important industrial process for the synthesis of nylon-6(,6) which is only partially understood. For this, Genesys, an in-house developed code to automatically build detailed microkinetic models, will be extended to include the effect of homogeneous catalysis. The core of the kinetic model is its data for which high-level quantum chemical calculations will be carried out. The resulting kinetic model will be validated using a unique set of existing and newly acquired experimental data. Finally, the model will be used to study the effect of process conditions on the desired product yields and by-product formation. This approach will be applicable to numerous other homogeneous catalyzed processes such as cumene and p-xylene oxidation.