Use this URL to cite or link to this record in EThOS: http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.607254
Title: Reaction kinetics in formulated industrial catalysts
Author: Wilkinson, Sam K.
ISNI:       0000 0004 5362 9902
Awarding Body: University of Birmingham
Current Institution: University of Birmingham
Date of Award: 2014
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Abstract:
In heterogeneous catalysis, a fundamental understanding of the necessary physico-chemical requirements for a catalyst formulation is essential to its success. Understanding of reaction kinetics via modelling can demonstrate how catalysts work, providing functional information around surface active sites and reaction mechanism. This tool, combined with well-designed laboratory experiments to test a catalyst under steady and/or non-steady state conditions, can provide insight into the links between catalyst formulation and reaction performance. The aim of this project is to develop novel strategies and methods in these areas utilising a range of Johnson Matthey catalysts and reaction systems. This thesis places significant focus on obtaining mechanistically and statistically sound kinetic models with reliable model parameter estimates. Methods for this are developed using a batch liquid phase hydrogenation system using a Pt/TiO2 catalyst. Subsequently, non-steady state analysis of catalyst formulations has been explored. This includes the initial transient behaviour of a fresh vanadium phosphorus oxide selective oxidation catalyst under reaction conditions which allowed understanding of the evolution of distinct active site populations on the catalyst surface. A subsequent study of copper-based methanol synthesis catalysts explored the impact of gas phase conditions on the catalyst state. A mixture of steady-state testing and transient response experiments (i.e. via an imposed change in gas phase conditions over the catalyst) provided new insights into the evolution of active site populations and populations of surface species on the catalyst surface. Overall, the reaction kinetics studies demonstrated across this thesis demonstrate not only a series of methods to understand catalyst behaviour in depth but also to understand the key functional requirements for an effective industrial catalyst.
Supervisor: Not available Sponsor: Not available
Qualification Name: Thesis (D.Eng.) Qualification Level: Doctoral
EThOS ID: uk.bl.ethos.607254  DOI: Not available
Keywords: TP Chemical technology
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