Thesis
Synthetic approaches to tune gas sorption properties in new lantern-type metal-organic polyhedral
- Creator
- Rights statement
- Awarding institution
- University of Strathclyde
- Date of award
- 2024
- Thesis identifier
- T17022
- Person Identifier (Local)
- 202087376
- Qualification Level
- Qualification Name
- Department, School or Faculty
- Abstract
- Metal-organic porous materials are studied for different applications such as catalysis, gas sorption or gas separation. These materials present high synthetic tunability, which affects their properties. This thesis aims to give a better insight on how these synthetic methods affect the crystal structure and gas sorption properties in Metal-Organic Polyhedra (MOPs). In this thesis, synthetic approaches such as ligand design, ligand scrambling and post-synthetic modification are employed to tune the gas sorption properties in new MOPs. To achieve this, the new ligands, L1H2 (based on terphenyl units) and L2H2 and its derivatives (based on bicyclo[2.2.2]-oct-7-ene units) were designed and used to synthesise novel MOPs. The intrinsic and extrinsic porosity for these cages was studied using crystallographic methods, showing differences induced by ligand design. Subsequent gas sorption measurement prove that all of these cages exhibited permanent porosity with high uptakes for N2, CO2 and CH4 compared to other lantern-type cages, with one of the cages displaying the highest reported surface area in lantern-type cages. L2H2 and its derivatives were used to synthesise scrambled cages. One family of scrambled cages show better uptake than their homoleptic parent cages, induced by the creation of mesopores due to inefficient packing, validating this approach to modify the gas sorption properties of MOPs. Post-synthetic modification of MOPs using single-crystal-to-single-crystal approach to form linear polymers showed that these polymeric structures exhibited worse gas sorption properties, due to a reduction of the available open-metal sites. Overall, this thesis shows the balance of multiple factors that are involved in determining the gas uptake, selectivity and surface area in MOPs. Relationship between these factors makes prediction of these properties a challenge, but this thesis provides a foundation for further studies.
- Advisor / supervisor
- Craig, Gavin, 1979-
- Fletcher, Ashleigh
- Resource Type
- DOI
- Embargo Note
Relations
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File | 2024-07-30 | Embargo |