Multi-scale characterization of shell thickness and effective volume fraction during gas hydrates formation: a kinetic study

Abstract Gas hydrates have gained increasing attention in energy and environmental fields and have potential applications in gas storage and transport, carbon dioxide sequestration, and flow assurance. Nevertheless, the kinetics of hydrate formation are still not well understood. In situ high-resolution X-ray computed tomography measurements were performed to monitor xenon hydrate formation on water droplets and ice spheres. For the first time, three-dimensional thickness meshes were used to quantify and visualize the kinetics of hydrate formation. The evolution of the hydrate morphology was investigated, and the time-dependent kinetic parameters were obtained, including the hydrate shell thickness and inner and outer diameters and the effective volume fraction of hydrate particles. The results indicate that the formation of gas hydrates undergoes an initial reaction-controlled stage followed by a mass-transfer-limited growth stage. For hydrate formation from a water droplet with an initial diameter of 1.66 mm, the hydrate shell thickness was approximately 30 μm and the effective volume fraction of hydrate particles was approximately 11% at 12 h after hydrate formation began. The standard deviation of the shell thickness, which indicates the surface roughness of the hydrate shell, increased with time for hydrate formation from water droplets. The results presented in this study renew our knowledge on the kinetics of hydrate formation, which is essential for their use in flow assurance and other hydrate-related technologies.