Correlation of the Growth Rate of the Hydrate Layer at a Guest/Liquid-Water Interface to Mass Transfer Resistance

Abstract: Growth rate of a hydrate layer at the guest/liquid-water interface is analyzed considering the conjugate process of the mass-transfer and hydrate crystal growth. Hydrate-layer growth rate data in the literature are often compiled according to the system subcooling (∆T ≡ T_eq − T_ex, where T_eq is the equilibrium dissociation temperature of the hydrate and T_ex is the system temperature), suggesting predominant heat transfer limitations. In this paper, we investigate how the existing data on hydrate-layer growth is better correlated to mass transfer of the guest species in liquid water in three-phase equilibrium with bulk guest fluid and hydrate. We have analyzed the conjugate processes of mass-transfer/hydrate-layer-growth following our previous study on the hydrate crystal growth into liquid water saturated with a guest substance. A dimensionless parameter representing the hydrate-layer growth rate is derived from the analysis. This analysis is based on the idea that the growth rate is controlled by the mass transfer of the hydrate-guest substance, dissolved in the bulk of liquid water, to the front of the growing hydrate-layer along the guest/water interface. The variations in the hydrate-layer growth rate observed in the previous studies are related to the dimensionless parameter.