Light scattering studies of clathrate hydrate forming systems

The current importance of clathrate hydrates lies primarily in the problems they pose for the oil and gas industry; in the future they may represent an important source of energy. These studies were persued in an effort to determine the utility of light scattering for elucidating changes in the dynamical structure of aqueous solutions that occur prior to hydrate formation. Such an understanding has direct relevance to the kinetics of clathrate hydrate formation, and may contribute to our knowledge of the many other systems in which water plays an important role.; Aqueous solutions of tetrahydrofuran were at the center of this research which included experimental spectroscopic studies of such solutions as a function of temperature and system composition. Light scattering spectra were found to contain important information concerning the extent and nature of hydrogen bonding, and the structural changes that precede hydrate nucleation. Specifically, the OH stretching band due to water and the COC stretch band due to tetrahydrofuran were seen to vary in a predictable manner with changes in the composition, temperature, and thermal history of the system.; Computer simulation studies were performed and used to aid in the interpretation of experimental spectra. Low wavenumber polarizability fluctuations were calculated and found to give reorientation times in good agreement with those found using other methods.