Use this URL to cite or link to this record in EThOS: https://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.798593
Title: The development of microreactor technology for the study of multistep catalytic systems and rapid kinetic modelling
Author: Waldron, Conor John
ISNI:       0000 0004 8507 8869
Awarding Body: UCL (University College London)
Current Institution: University College London (University of London)
Date of Award: 2019
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Abstract:
Microreactor technology was applied to the study of catalytic systems because their high rates of heat and mass transport, improved safety and ease of automation makes them particularly effective research tools in this area. A multistep flow system for the synthesis of benzylacetone from benzyl alcohol via oxidation, aldol condensation and reduction reactions was developed by utilising three micropacked bed reactors and a gas liquid membrane separator. This reaction had previously been conducted in batch cascade, however, the multistep flow system enabled the achievement of higher yields with lower catalyst contact times because separating each reaction into its own reactor allowed greater freedom to tailor the operating conditions for each reaction. The multistep system also allowed the catalysts to be studied in a process wide environment, leading to the identification of significant catalyst inhibition due to by and co-products from upstream reactions. An automated closed loop microreactor platform was developed which utilised Model-Based Design of Experiments (MBDoE) algorithms for rapid kinetic modelling of catalytic reactions. The automated platform was first applied to the homogenous esterification of benzoic acid with ethanol using a sulfuric acid catalyst, where a campaign of steady-state experiments designed by online MBDoE led to the estimation of kinetic parameters with much higher precision than a factorial campaign of experiments. This reaction was then conducted with MBDoE designed transient experiments, which dramatically reduced the experimental time required. The same reaction was studied using a heterogeneous Amberlyst-15 catalyst, and by combining factorial designs, practical identifiability tests and MBDoE for model discrimination and parameter precision, a practical kinetic model was identified in just 3 days. The automated platform was applied to the oxidation of 5-hydroxymethylfurfural in a micropacked bed reactor with gas-liquid flow using AuPd/TiO2 catalysts, however due to poor experimental reproducibility, a kinetic model was not identified.
Supervisor: Gavriilidis, A. Sponsor: Not available
Qualification Name: Thesis (Ph.D.) Qualification Level: Doctoral
EThOS ID: uk.bl.ethos.798593  DOI: Not available
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