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Methane Hydrates (MHs) are a promising energy source abundantly available in nature. Understanding the complex processes of MH formation and dissociation is critical for the development of safe and efficient technologies for energy recovery. Many laboratory and numerical studies have investigated these processes using synthesized MH-bearing sediments. A near-universal issue encountered in these studies is the spatial heterogeneous hydrate distribution in the testing apparatus. In the absence of direct observations (e.g. using X-ray computed tomography) coupled with real time production data, the common assumption made in almost all numerical studies is a homogeneous distribution of the various phases. In an earlier study (Yin et al., 2018) that involved the numerical description of a set of experiments on MH-formation in sandy medium using the excess water method, we showed that spatially heterogeneous phase distribution is inevitable and significant. In the present study, we use as a starting point the results and observations at the end of the MH formation and seek to numerically reproduce the laboratory experiments of depressurization-induced dissociation of the spatially-heterogeneous MH distribution. This numerical study faithfully reproduces the geometry of the laboratory apparatus, the initial and boundary conditions of the system, and the parameters of the dissociation stimulus, capturing accurately all stages of the experimental process. Using inverse modelling (history-matching) that minimized deviations between the experimental observations and numerical predictions, we determined the values of all the important flow, thermal, and kinetic parameters that control the system behaviour, which yielded simulation results that were in excellent agreement with the measurements of key monitored variables, i.e. pressure, temperature, cumulative production of gas and water over time. We determined that at the onset of depressurization (when the pressure drop – the driving force of dissociation – is at its maximum), the rate of MH dissociation approaches that of an equilibrium reaction and is limited by the heat transfer from the system surroundings. As the effect of depressurization declines over time, the dissociation reaction becomes kinetically limited despite significant heat inflows from the boundaries, which lead to localized temperature increases in the reactor.

We analyse numerically an earlier experimental study that involved the formation of methane hydrates by the excess water method in a small reactor filled with a sandy porous medium, and seek to address questions about the type of the hydration reaction and the phase heterogeneity in the resulting hydrate-bearing sand. Using a fine discretization describing the reactor assembly, the experimental process is faithfully replicated numerically. The multi-stage process of hydrate formation is subdivided in 7 steps. The experimental data from the continuously-monitored pressure and temperature during each step are used for comparison against the numerical predictions, the identification of the dominant processes and the determination of the associated parameters through a history-matching process that minimizes deviations between observations and simulation results. The results of this first-ever study on this subject demonstrate unequivocally that the hydration reaction is a kinetic (as opposed to an equilibrium) process, and that the spatial distributions of the various phases (aqueous, gas and hydrate) at the end of the formation process are strongly heterogeneous. This has serious implications in simulation studies of hydrate dissociation that assume uniform initial phase saturation distributions. The history-matching process indicates that (a) the system behaviour is sensitive to some flow parameters (porosity and irreducible water saturation) only during the first water injection, (b) it is insensitive to the sand intrinsic permeability during all steps of the study, and (c) thermal processes dominate after the first water injection, yielding estimates of the thermal properties of the sand and of time-variable key parameters of the kinetic reaction.

Numerical simulation is essential for the prediction and evaluation of hydrocarbon reservoir performance. Numerical simulators developed for the description of the behavior of hydrates under production and the corresponding flow of fluids and heat accounting for all known processes are powerful, but they need validation through comparison to field or experimental data in order to instill confidence in their predictions. In this study, we analyze by means of numerical simulation the results of an experiment of methane hydrate dissociation by thermal stimulation in unconsolidated porous media heated through the vessel walls. The physics captured by the model include multicomponent heat and mass transfer, multiphase flow through porous media, and the phase behavior of the CH4 + H2O system involved in methane hydrate formation and dissociation. The set of governing equations consists of the mass and energy conservation equations coupled with constitutive relationships, i.e., the dissolution of gas in H2O, relative permeability and capillary pressure models, composite thermal conductivity models, and methane hydrate phase equilibria. The model geometry describes accurately the hydrate reactor used in a recent experimental study investigating methane hydrate dissociation behavior [Chong et. al. Appl. Energy 2016, 177, 409-421]. The cumulative gas production is estimated and validated against three tests of experimental data involving different boundary temperatures, showing a good agreement between observations and numerical predictions. The predicted evolution of the spatial distributions of different phases over time shows that hydrate dissociation progresses inward from the reactor boundary to the center, methane gas accumulates to the top of the reactor because of buoyancy, and water migrates down to the bottom of the reactor because of gravity. A sharp hydrate dissociation front is predicted, and the estimated location of hydrate dissociation front suggests a linear relationship with the square root of time. A sensitivity analysis on the thermal conductivity of sand under fully saturated conditions is conducted to elucidate its effect on the gas production behavior. In addition, the energy efficiency ratio computed from the simulation of this boundary-wall heating technique varies from 14.0 to 16.2. Deviations between observations and predictions of the evolution of the temperature profile are attributed to initial heterogeneous distribution of the hydrate phase in the hydrate reactor.