Britton, Phyllida Margaret Mary; (2025) A crystal engineering approach to the development of Covalent Organic Frameworks sustained by carbon-carbon bonds. Doctoral thesis (Ph.D), UCL (University College London).

Text BRITTON THESIS.pdf - Accepted Version Access restricted to UCL open access staff until 1 June 2027. Download (13MB)

Abstract

The overarching aim of this research project addresses the challenges in the development of COFs for practical applications. This is achieved via a pioneering approach involving the use of a design-led crystal engineering strategy. Specifically, we aim to prepare unprecedentedly crystalline, chemically stable and structurally diverse COFs through a unique two-step synthetic method. In the first step we will design and prepare porous, crystalline hydrogen bonded frameworks, which are chemically unstable, yet highly crystalline and solution processable. In the second step, we will transform the unstable hydrogen-bond linkages into highly stable C-C covalent bonds through a UV-light induced photoreaction, while preserving the porosity and functionality of the original framework structure. We expect that this synthetic strategy will deliver previously inaccessible, two- and three-dimensional COFs based solely on carbon-carbon bonds (CC-COFs). We anticipate that CC-COFs will meet current requirements for the capture of CO2, as well as those for the sequestration, storage and separation of other environmentally and industrially relevant gases and fuels (e.g. H2), thus offering concrete and executable solutions for some of the most pressing materials engineering challenges of the 21st century.

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