Conclusions
The important role of multiple cage filling in kinetic mechanisms of hydrate formation is described. Possible mechanisms of the structure II hydrates formation by the most small molecules (Ar, Kr, N2, O2) and by mixtures of the structure-I formers are suggested on the base of new model of clathrate crystal nucleation. A generalization of the van der Waals-Platteeuw (vdW-P) statistical thermodynamic model of clathrate hydrates, applicable for arbitrary multiple filling, is formulated. The formulation in terms of grand canonical ensemble for the guest subsystem simplifies derivation of the results even in the ordinary case of single filling. Comparison with simple chemical kinetic model of multiple filling gives microscopic expressions for Langmuir’s constants.
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Pomeransky, A.A., Belosludov, V.R. (2004). Statistical Thermodynamic Model of Clathrate Hydrates with Multiple Filling of Cages. In: Taylor, C.E., Kwan, J.T. (eds) Advances in the Study of Gas Hydrates. Springer, Boston, MA. https://doi.org/10.1007/0-306-48645-8_2
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DOI: https://doi.org/10.1007/0-306-48645-8_2
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