Experimental investigation and modeling on the dissociation kinetics of methane hydrate in clayey silt cores in depressurization

Abstract

Natural gas hydrate (NGH) in clayey silts might be the majority of its global reserve. A thorough understanding on the dissociation kinetics of NGH in clayey silts is crucial for its safe and efficient exploitation. In this study, the dissociation characteristics of methane hydrate in quartz silts, montmorillonites and South China Sea (SCS) sediments made cores in multi-step depressurization was experimentally studied and modeled. In quartz silt core, methane hydrate thoroughly dissociated once the pressured is lowered to the equilibrium pressure in bulk. In montmorillonite and SCS sediment cores, methane hydrate dissociation initiated at higher pressure than quartz silt. Capillary and clay induced water activity depressions are suggested to be the major causes. Stepwise methane hydrate dissociation was discovered in the montmorillonite and SCS sediment cores in multi-stage depressurization. In one step depressurization, hydrate in the fine grain cores with larger surface area dissociated faster. In montmorillonite and SCS sediment cores, lower water content leads to faster dissociation at the same pressure, which may be attributed to the higher driven force for dissociation (fugacity difference fe-f). A kinetic model for NGH dissociation in clayey silts was established by introducing fitted equivalent diameter and surface area correction factor of hydrate particles to the Kim-Bishnoi model. In the model, the hydrate equilibrium conditions in clayey silts were predicted by the water activity measurement (WAM) technique. With a maximum deviation of 9.81% in gas production, the model prediction and experimental results are in good agreement. The experimental findings and model reported in this work may be helpful to understand the NGH phase transition mechanism in clayey silt sediments.