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As in any other phase transition, hydrate phase transition kinetics involves an implicit coupling of phase transition thermodynamic control and the associated dynamics of mass and heat transport. This work provides a brief overview of certain selected hydrate film growth models with an emphasis on analyzing the hydrate phase transition dynamics. Our analysis is based on the fundamental properties of hydrate and hydrate/liquid water interfaces derived from molecular modeling. We demonstrate that hydrate phase transitions involving water-dominated phases are characterized by heat transport several orders of magnitude faster than mass transport, strongly suggesting that any hydrate phase transition kinetic models based on heat transport will be entirely incorrect as far as thermodynamics is concerned. We therefore propose that theoretical studies focusing on hydrate nucleation and growth should be based on concepts that incorporate all the relevant transport properties. We also illustrate this point using the example of a fairly simplistic kinetic model, that of classical nucleation theory (CNT), modified to incorporate new models for mass transport across water/hydrate interfaces. A novel and consistent model suitable for the calculation of enthalpies is also discussed and appropriate calculations for pure components and relevant mixtures of carbon dioxide, methane, and nitrogen are demonstrated. This residual thermodynamic model for hydrate is consistent with the free energy model for hydrate and ensures that our revised CNT model is thermodynamically harmonious.

Modeling Heat Transport in Systems of Hydrate-Filled Sediments Using Residual Thermodynamics and Classical Nucleation Theory