The synthesis and characterisation of photoresponsive metal organic frameworks and the implementation of cavity perturbation theory in the study of liquid chromatography

Kidwell, Luke 2020. The synthesis and characterisation of photoresponsive metal organic frameworks and the implementation of cavity perturbation theory in the study of liquid chromatography. PhD Thesis, Cardiff University. Item availability restricted.

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Abstract

This thesis describes the process of designing a MOF that incorporates a spiropyran molecule as a linker, as well as the use of a dielectric measurement technique to measure separation in MOFs. Chapter 1 covers the basics of MOF synthesis and techniques that facilitate the incorporation of functionalities into MOFs, as well a small review of existing photoresponsive MOFs. This is followed by a brief summary of the challenges faced in xylene and styrene separation in industrial settings as well as some examples of MOFs used in these separations. Followed by some oversight into microwave studies on MOFs. Chapter 2 describes the synthesis and characterisation of 10 novel organic compounds that have the spiropyran functionality that have potential as an organic linker in a MOF. First describing the minutiae of optimising the parameters sufficiently to progress to the synthesis of the MOFs, followed by a study that compares the NMR and UV-Vis spectra of the ligands and how slight variations in regiochemistry can affect the photoisomerization of the ligands synthesised. Chapter 3 describes the combinatorial synthesis undergone which resulted in the synthesis of three novel materials that use some of the ligands, synthesised in chapter 2. This is then followed by a description of the characterisation of each of the frameworks, and in the case of LK-1 and LK-2 further reaction optimisation to obtain a phase-pure product. Chapter 4 describes the work involved in designing an experimental set up that can analyse, in-situ, the chromatographic separation of analytes in MOFs. The chapter begins with a summary of the fundamentals of microwave cavity perturbation theory, sufficiently for the understanding of this work. The chapter then goes onto describe the details of the method development, eventually attempting chromatography with compounds typically found in industrial feedstocks for styrene and xylene production.

Item Type:	Thesis (PhD)
Date Type:	Completion
Status:	Unpublished
Schools:	Chemistry
Date of First Compliant Deposit:	14 May 2021
Last Modified:	14 May 2022 01:30
URI:	https://orca.cardiff.ac.uk/id/eprint/141371

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