| Summary: | Society is now dependent on the continued development and access to modern technology. Materials science therefore stands at the forefront of resolving and tuning functional materials properties, and designing technologies to improve our health, economy and environment. The content of this thesis covers a wide range of methods and approaches for understanding the chemical complexities, and tuneable properties of a unique subset of materials named metal-organic frameworks. The number of available precursor components for synthesising MOFs has led to a plethora of possible final crystal structures, with vast differences in observed material properties. The use of computational approaches in the prediction of potential functional frameworks, and also for resolving the origin behind observed phenomena, is essential for directing further work in the field. Work in this thesis includes the parameterisation of an approach that would allow a large-scale and cheap screening procedure of the thermodynamic properties of MOFs. Other work in this thesis includes the calculation of defective framework structures and the thermodynamics associated with their formation. Defects that occur in MOFs, when compared to inorganic binary materials such as oxides, can be considered as severe and non-dilute. The concentration and distribution of potential defects and the stability of the framework as a function of these factors, is a poorly understood area in the research field of MOFs. Finally, interfacing MOFs with surfaces is a relatively new approach for designing functional devices for applications such as gas absorption and photovoltaics. In this thesis we calculate interface binding sites and energetics of adhesion of an archetypal example of a MOF interfacing a metal oxide. Each approach and direction taken in the work forming this thesis were taken to resolve the theory behind observed phenomena in experiments, and to provide a platform for investigating the potential material properties of yet unsynthesised MOFs.
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