Grammenou, Eleni; (2024) Development of Integrated Platforms for Automated Kinetic Profiling of Chemical Reactions. Doctoral thesis (Ph.D), UCL (University College London).

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Abstract

Continuous flow micro- and milli-scale reactors, as an alternative to conventional batch reactors, offer several advantages in the study of chemical reactions. Characterised by enhanced heat and mass transfer rates, ease of automation for precise control of reaction conditions, and seamless integration with inline and online analytical tools, miniaturised systems facilitate rapid acquisition of kinetic data, crucial for process scale-up. This thesis describes the development of automated platforms designed for the systematic acquisition of kinetic information for both heterogeneous and homogeneous systems. The core of this research involves the fabrication and utilisation of miniaturised reactors, readily integrated into experimental setups that are coupled with chromatographic and spectroscopic techniques. An automated open loop microreactor platform was developed for the kinetic model discrimination and parameter estimation of the heterogeneously catalysed levulinic acid esterification to ethyl levulinate. This reaction was conducted in a Single Pellet String Reactor and the associated hydrodynamics and liquid-to-solid external mass transfer process were numerically investigated at macroscopic and microscopic scales. Different aspect ratios were simulated that yielded empirical correlations for mass transfer in these systems, enhancing the understanding of the reaction dynamics. The potential of coupling non-invasive spectroscopy with continuous systems for real-time reaction monitoring and fast kinetic data acquisition were exemplified via the fabrication of a miniaturised CSTR unit integrated with a cooling/heating system, equipped with an inline Raman spectrometer probe. Its mixing characteristics were thoroughly investigated through both experimental and computational approaches and the efficacy to produce fast steady-state kinetic data, acting both as a reactor and a stirred flowcell, was shown for an imine synthesis reaction in an automated experimental platform. To further demonstrate the efficiency of the system, the same reaction was tested in intuitively designed transient experiments of single and multi-variable ramps, which dramatically reduced the experimental time required and led to higher precision in the parameter estimation.

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