High-pressure phase transition of methane hydrate in water–methane–ammonia system

Abstract

The phase transition of methane hydrate in water–methane–ammonia system was investigated under pressures up to 20 GPa using synchrotron X-ray powder diffraction (XRD) combined with diamond anvil cells. The XRD experiments revealed that the sI cage structure (MH-I) of methane hydrate transforms into an sH cage structure (MH-II) at approximately 1 GPa, further transforms into a filled-ice Ih structure (MH-III) at approximately 2 GPa, and remains in this structure under pressures up to at least 20 GPa. Ammonia was observed as ammonia hemihydrate phase-II above 3.8 GPa. It is therefore considered that methane hydrate can coexist with aqueous ammonia below 3.8 GPa and coexist with ammonia hemihydrate phase-II above 3.8 GPa. The transition pressures of methane hydrate in the investigated system were consistent with those in water–methane system. These results indicate that, although ammonia is thought to inhibit methane hydrate formation, methane hydrate can be stable in water–methane–ammonia system up to at least 20 GPa and at room temperature. The pressure range in this study covered the pressure conditions inside icy moons, indicating that methane hydrate has a potential to be the main constituent of them.