Intermolecular interactions in supercritical fluid solutions from fluorescence spectroscopy
Brennecke, Joan F.
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https://hdl.handle.net/2142/23786
Description
Title
Intermolecular interactions in supercritical fluid solutions from fluorescence spectroscopy
Author(s)
Brennecke, Joan F.
Issue Date
1989
Doctoral Committee Chair(s)
Eckert, Charles A.
Department of Study
Engineering, Chemical
Discipline
Engineering, Chemical
Degree Granting Institution
University of Illinois at Urbana-Champaign
Degree Name
Ph.D.
Degree Level
Dissertation
Keyword(s)
Engineering, Chemical
Language
eng
Abstract
Much of the unusual behavior in supercritical fluids (SCF's), including enhanced solubilities, synergistic effects of mixed solutes, and entrainer effects, may be explained by a region around the solute that has a higher density than the bulk. We present a new technique to investigae SCF's using fluorescence spectroscopy to probe the local interactions. In contrast to thermodynamic measurements, this technique determines the strength of interactions on a molecular scale, which is important in the development of more accurate thermodynamic models. For pyrene, naphthalene, dibenzofuran and carbazole in SCF CO$\sb2$, C$\sb2$H$\sb4$ and CF$\sb3$H, the results indicate stronger solute/solvent interactions near the critical point and local densities that are liquid-like, even when the bulk density is quite low. We also present excimer fluorescence data that emphasize the importance of solute/solute interactions in dilute supercritical fluid solutions. Finally, results from exciplex fluorescence studies of a solute/SCF/entrainer system indicate a dramatic solvent effect on the photophysical kinetics.
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