Environmentally benign alternatives for solvents and catalysts are essential for the development of sustainable chemical processes. Toward this end, we focused our research on the design of novel solvents and catalysts that reduce the environmental impact of these important materials. In this research, we develop switchable and tunable systems that couple reaction and separation to ease the processing requirements for product isolation and catalyst recovery. The switchable solvents use a ¡°switch¡± to transition from non-volatile, polar, aprotic solvents to volatile gases that can be easily separated. This allows us to facilitate reactions within the solvent and then enable easy separation through activation of the switch. We have used these materials for numerous reaction applications, including difficult reactions involving highly immiscible compounds. We also extended the work to acid-catalyzed reactions, in which we can avoid wasteful neutralization processes that are often associated with homogeneous acid catalysis. The tunable solvents use carbon dioxide pressure to ¡°tune¡± into desired solvent properties. We enable this through the dissolution of carbon dioxide into organic solvents, which generates gas-expanded liquids with solvent properties highly dependent on the carbon dioxide pressure. We can use this effect to couple homogeneous reaction with heterogeneous separation, allowing for recovery of expensive catalysts and ligands. In this work, we assess the possibilities of using liquid polyethylene glycol in the tunable systems, studying the phase behavior and industrial applications.
| Identifer | oai:union.ndltd.org:GATECH/oai:smartech.gatech.edu:1853/24749 |
| Date | 30 June 2008 |
| Creators | Donaldson, Megan Elizabeth |
| Publisher | Georgia Institute of Technology |
| Source Sets | Georgia Tech Electronic Thesis and Dissertation Archive |
| Detected Language | English |
| Type | Dissertation |
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