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

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.

Identiferoai:union.ndltd.org:RICE/oai:scholarship.rice.edu:1911/17065
Date January 1997
CreatorsBesnard, Guillaume
ContributorsKobayashi, Riki
Source SetsRice University
LanguageEnglish
Detected LanguageEnglish
TypeThesis, Text
Format187 p., application/pdf

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