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Solvothermal stability studies of porous inorganic and metal-organic materials

Minkiewicz, Justyna 2021. Solvothermal stability studies of porous inorganic and metal-organic materials. PhD Thesis, Cardiff University.
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The increasing interest of green chemistry in the use of greener solvents, has led to a surge in the need of solid materials stable in liquid phase processes. In particular, the use of porous materials such as zeolites and their related Metal Organic Framework (MOF) counterparts as catalysts or membranes has drawn great attention. Yet even though zeolites are already widely used in petrochemical applications, their commercialisation in liquid phase operations has not yet been achieved. A major reason for this is that the stability of zeolites and MOFs in water has not yet been fully evaluated and understood. In order to tackle the (in)stability challenge, various points call for attention. This mainly includes identification of porous materials that possess sufficient stability in solvent media. As such, the aim of this thesis is to present a detailed investigation of the stability of various porous materials in water and organic solvents. Detailed understanding of material degradation upon direct contact with solvents at elevated temperatures is provided, by focusing on different analytical techniques and spectroscopic studies. This work begins in Chapter 3, by exploring how different zeolite structures of various framework densities, pore volumes and aluminium contents are modified upon water treatment in continuous flow reactors (CFR) at elevated temperature and pressure. Chapter 4 focuses on the investigation of the MFI framework and the role of aluminium content in hydrothermal stability in CFR. Subsequently, in Chapter 5, the stability of MOF structures as analogues to zeolites is investigated in CFR. Preliminary investigations led to the selection of UiO-66(Zr)-H structure as the most robust in water. Subsequently, the choice of metal, linker and operational conditions are determined regarding MOF (in)stability. In closing, Chapter 6 evaluates the findings of this study and describes the potential further questions that raise.

Item Type: Thesis (PhD)
Date Type: Completion
Status: Unpublished
Schools: Chemistry
Date of First Compliant Deposit: 10 January 2022
Last Modified: 05 Aug 2022 01:37

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