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The growth behavior of CH4 and SF6 mixture gas hydrate has been investigated by a combined approach of Raman spectroscopy and molecular modeling. Raman spectroscopy results presented that when CH4 is used only, CH4 guest molecule is inserted first into the large cavity of the host structure built by H2O molecules and then into the small cavity to stabilize the whole gas hydrate structure. In the other hand, when SF6 is mixed together, SF6 is favored over (or competing with) CH4 in being inserted into the large cavity and the small cavity still prefers CH4 insertion. The calculations of binding energies clearly supported this. While SF6 has a binding energy of -26.9 kcal/mol a little lower than -24.2 kcal/mol of CH4 in the large cavity, SF6 and CH4 has 1.2 kcal/mol and -22.0 kcal/mol, respectively, in the small cavity. It indicates that the sizable SF6 is not preferred in the small cavity but has a relative energetic advantage over CH4 in the large cavity.

Raman Spectroscopy and Molecular Modeling Study on the CH4and SF6Mixture Gas Hydrate Growth Behavior