Designing for sustainability with CO2-tunable solvents

Developing greener, more efficient, and less energy-intensive processes will lead the chemical industry into a more sustainable future. Gas-expanded liquids (GXLs) form a unique class of environmentally benign and tunable solvents that can be used in a variety of applications. Through the series of studies presented in this thesis, we have investigated both the properties and applications of GXLs. We have developed a more complete understanding of the interactions between the gas, the organic liquid, and solutes at the molecular level through kinetic and solvatochromic experiments. We have examined a Diels-Alder reaction and an SN2 reaction and have described the kinetic results in terms of intermolecular interactions and local composition enhancement. We have also demonstrated the use of Organic-Aqueous Tunable Solvents, a special case of GXLs, to recycle homogeneous hydroformylation catalysts. The results of this research can be used to guide future applications of GXLs as green reaction solvents.Ph.D.Committee Chair: Dr. Charles A. Eckert; Committee Co-Chair: Dr. Charles L. Liotta; Committee Member: Dr. Amyn Teja; Committee Member: Dr. Dennis W. Hess; Committee Member: Dr. Victor Breedvel