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We report results from grand-canonical Monte Carlo simulations of methane andcarbon dioxide adsorption in structure sI gas hydrates. Simulations of purecomponent systems show that all methane sites are equivalent, while carbondioxide distinguishes between two types of sites, large or small. The adsorbedmixture can be regarded as ideal, as long as only large sites are occupied. Astrong preference is demonstrated for methane, when the smaller sites becomefilled.  The molar heat of adsorption of methane decreases with composition, while themolar heat of adsorption for carbon dioxide passes an extremum, essentially inaccordance with the observation on the site sizes. The Helmholtz energies ofthe hydrate with CO$_2$-CH$_4$ gas mixture for temperatures between 278 and 328K and pressures between 10$^4$ and 10$^9$ Pa indicate that certain mixtures aremore stable than others. The results indicate that a thermodynamic path existsfor conversion of a pure methane hydrate into a pure carbon dioxide hydratewithout destroying the hydrate structure.

Adsorption of CO$_2$ and CH$_4$ and their mixtures in gas hydrates