Thermodynamics and kinetics studies of formation and decomposition of clathrates hydrates of methane, carbon dioxide and their mixtures using a differential heat flux calorimeter

[摘要] A high pressure heat flux calorimeter in isobaric, temperature-ramping mode has been used to measure the solubility of pure methane, pure carbon dioxide and methane-carbon dioxide mixtures. The solubility measurements emphasize a crystallization-like process taking place during hydrate formation and show a striking divergence from Henry's Law, the frequently used calculation procedure, prior to and during hydrate formation. These measurements were further used to determine the enthalpies of solution/dissociation, and entropies change. Moreover, the hydration numbers of these compounds provide some explanations and criteria of stability of the cages of gas hydrates in the host lattice.Finally, a kinetic study confirms the crystallization process of hydrate formation and exhibits a high level of supersaturation prior to hydrate formation and also a high consumption rate during hydrate formation.

[发布机构] Rice University

[效力级别] engineering