Interfacial phenomena in gas hydrate systems.

Gas hydrates are crystalline inclusion compounds, where molecular cages of water trap lighter species under specific thermodynamic conditions. Hydrates play an essential role in global energy systems, as both a hinderance when formed in traditional fuel production and a substantial resource when formed by nature. In both traditional and unconventional fuel production, hydrates share interfaces with a tremendous diversity of materials, including hydrocarbons, aqueous solutions, and inorganic solids. This article presents a state-of-the-art understanding of hydrate interfacial thermodynamics and growth kinetics, and the physiochemical controls that may be exerted on both. Specific attention is paid to the molecular structure and interactions of water, guest molecules, and hetero-molecules (e.g., surfactants) near the interface. Gas hydrate nucleation and growth mechanics are also presented, based on studies using a combination of molecular modeling, vibrational spectroscopy, and X-ray and neutron diffraction. The fundamental physical and chemical knowledge and methods presented in this review may be of value in probing parallel systems of crystal growth in solid inclusion compounds, crystal growth modifiers, emulsion stabilization, and reactive particle flow in solid slurries.