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• Capillary pressures in different directions are presented in this study. • Hydrate formation makes the skewness of capillary pressure finer slanting degrees. • The heterogeneity in hydrate formation determines capillarity in anisotropy. • The stronger capillary heterogeneity occurs in the vertical direction. The random nucleation and growth of hydrates in the pore space contribute to the heterogeneity of hydrate sediments, which results in anisotropic fluid flow. An exact forecast for capillary pressure in different directions, which governs the gas/water distribution and the volume of residual water saturation in porous sediments, is of significant importance for hydrate exploitation. In this study, the index properties of the artificial hydrate sediment were characterized through X-ray computed tomography (CT) visualization scanning. The spatial structure feature of hydrate sediment was captured via a topological pore network, which was established from CT imaging. Then, the evolution of capillary pressure in anisotropy with the formation of hydrates was simulated and discussed. The results indicated that with hydrate formation, the capillary pressure curves became steeper, representing skewness with finer slanting degrees and poor sorting. Moreover, the differences in capillary pressure with the same hydrate saturation between different directions was enlarged. Stronger capillary heterogeneity in the vertical direction represents greater heterogeneity, according to the Leverett J-Function. [ABSTRACT FROM AUTHOR]

Natural gas hydrate is recognized as an ideal substitute for traditional energy resources. Gas production from hydrate reservoirs is accompanied by the phase transition of solid hydrate, which inevitably results in changes to the microstructure of hydrate sediments. Therefore, the interaction mechanism between the microstructure and permeation characteristics of hydrate sediments must be investigated, especially permeability anisotropy. In this study, we assess the variations in permeability anisotropy during krypton hydrate formation using a pore network model and X-ray computed tomography. The results showed that absolute permeability in the vertical (k v) and horizontal (k h) directions both decreased throughout the formation process, but that the decline in k v was steeper, thus resulting in a sharp increase in the degree of permeability anisotropy (k h /k v). The relative permeability to gas was always higher in the horizontal direction than of that in the vertical direction, whereas the relative permeability to water was the opposite. Moreover, the difference in the relative permeability to water and gas between the two directions increased with the increasing hydrate saturation (S h). When extrapolating to the field-scale for hydrate field trials, we consider that horizontal wells provide a better option for gas production, especially for hydrate reservoirs with a higher hydrate saturation. • Prediction of permeability anisotropy during hydrate formation is presented. • Hydrate formation increases the degree of permeability anisotropy (k h /k v). • Difference in gas/water flow between two directions increases with high S h. • Horizontal wells are found to be a better option for gas hydrate production. [ABSTRACT FROM AUTHOR]

Hydrate‐saturation‐dependent permeability in sediments is largely affected by the pore morphology of hydrate. Hydrate pore morphology evolves from a single pore habit, which depends on its formation conditions, toward a sophisticated hybrid habit with increased hydrate saturation. Resulted permeability reduction curves in hydrate‐bearing sediments are diverse and lack universal models. By using a two‐parameter logistic function to link microscale hydrate pore habit evolution with macroscale permeability variations, this study establishes a pore‐morphology‐weighted permeability model that well captures the permeability evolution in hydrate‐bearing sediments at various conditions. The universality of this model is validated and the values of the two parameters in the model are calibrated using published laboratory and pressure core data. This newly proposed model offers a mechanistic understanding of the permeability in hydrate‐bearing sediments and an elegant expression that can be implemented in reservoir simulators for field‐scale gas production estimation. Plain Language Summary: Permeability of hydrate‐bearing sediments governs the gas and water flow, and thus plays important roles in many energy, environment, and climate related processes including the formation and evolution of hydrate deposits, the recovery of hydrate resources, and the release of methane from hydrates into the ocean and the atmosphere. Existing models of permeability in hydrate‐bearing sediments assume single and simplified hydrate pore morphology, and thus, fail to capture the dynamic evolution of permeability in sediments with changing hydrate saturation. With recent advances of direct observations of hydrate crystallization in sediments using microfocus X‐ray computed tomography, much has been learned about the dynamic evolution of hydrate morphology in sediment pores, based on which we established a physical model to quantitatively correlate the dynamic evolution of hybrid hydrate pore morphology to the permeability variation in sediments in this study. The robustness and universality of this new model are validated using published data from both laboratory synthesized and naturally occurred hydrate‐bearing samples. The results of this study enhance the physical understandings of flow in hydrate‐bearing sediments and shed light to hydrate reservoir evolution. Key Points: The evolution of hydrate pore morphology depends on hydrate formation conditions, exerting diverse controls over permeabilityThe relation between permeability and the saturation and pore morphology of hydrate is quantitatively described and analyzedThe new permeability model is universal and can capture measurements under excess‐gas, excess‐water, and dissolved‐gas conditions [ABSTRACT FROM AUTHOR]

[Display omitted] Gas hydrates have gained great interest in the energy and environmental field as a medium for gas storage and transport, gas separation, and carbon dioxide sequestration. The presence of small doses of surfactants in the aqueous phase has been reported to enhance hydrate formation; however, the underlying mechanisms remain poorly understood. Thus, in situ high-resolution X-ray computed tomography measurements were performed to monitor the upward water migration and the resulting hydrate nucleation and growth. It was found that the presence of hydrate crystals at the gas–liquid–solid contact line triggered the enhanced growth of hydrates on the reactor wall. A time delay was observed between the disappearance of the bulk water reservoir and its transformation into hydrate. The lower interfacial tension between the hydrate surface and the solution facilitated its adsorption onto the reactor wall once a thin film of hydrate nucleated on the solid wall surface. These hydrate layers present on the reactor wall were found to be porous, wherein the porosity decreased with increased subcooling. These fundamental results will be of value in understanding the mechanism of hydrate growth in the presence of surfactants and its potential application in hydrate-based technologies. [ABSTRACT FROM AUTHOR]

• 3D morphologies and time-dependent parameters of the hydrate shell are obtained. • Water is more mobile than gas in hydrates in the diffusion-controlled growth stage. • Protrusions growth on the outer surface of a hydrate shell is due to water permeation. • Effective diffusion coefficients of gas and water in hydrate are determined. Understanding the transport properties of water and guest molecules in dense hydrate structures is pivotal in controlling their formation and stability; this is nevertheless hindered by challenges in characterizing the time-varying diffusion and permeation process. This paper reports experimental results on the mass-transfer characteristics of water and guest molecules across hydrate shells during their formation from water droplets. The time-dependent 3D morphologies and parameters of hydrate shells were in-situ obtained via X-ray computed tomography to reveal the transport mechanism in hydrates. It was found that in the mass-transfer-limited stage, hydrate growth occurred primarily at the hydrate-gas interface, indicating a more mobile characteristic of water molecules in those hydrate shells than gas. The resulting outward permeation of water led to the growth of hydrate protrusions on the outer surface of the hydrate shell, suggesting a transition of the water transport schema through the hydrate shell from diffusion to permeation. Consequently, a diffusion-based shell growth model was developed to quantify the diffusivity of gas and water molecules in hydrates. Combining the measurements in the temperature range of 275.15–283.15 K, the effective diffusion coefficient of gas through the hydrates was estimated to be in the range of 1.34 × 10−14 − 1.90 × 10−13 m2/s, with that of interstitial water in the range of 2.87 × 10−12 − 3.83 × 10−11 m2/s. These results are of fundamental value in developing an improved understanding of the kinetics of hydrate formation from gas-water interfaces, which is essential in the optimization of hydrate-based techniques. [ABSTRACT FROM AUTHOR]