High-throughput synthesis and application development of water-stable MOFs
Schoenecker, Paul M.
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Metal-organic frameworks (MOFs) are porous networks of metal-centers connect by organic ligands, which have potential for an array of applications including gas separations and storage, drug delivery, and molecular sensing. A multitude of structures are reported with specific pore geometries and functionalities, but MOFs are not currently implemented in consumer or industrial applications. Two major setbacks have hindered their transition to the applied level. 1) Many MOFs are not stable in the presence of ambient moisture. 2) Most syntheses are costly and take place under batch-style solvothermal conditions. This thesis addresses both of these setbacks and examines the performance potential of water-stable MOFs for selective gas adsorption. A representative set of MOFs are exposed to water, and structural effects are monitored from a before and after comparison to identify properties of water-stable MOFs. A novel continuous-flow MOF synthesis process is reported along with preliminary optimization experiments, which yield direct suggestions for future process improvements. Batch-style scale-up experiments are also conducted for three other MOFs, which provide insight into synthesis phenomena. Application specific results are reported for toxic chemical filtration and carbon dioxide removal from flue gas using MOFs. The thesis concludes by summarizing the experimental findings, discussing the application potential of specific MOFs, and recommending topics for future research projects. Pitfalls observed during this research are also directly discussed along with potential solutions.