Interfacial tensions in the (CH4 + CO2 + H2O) system under two- and three-phase conditions

Abstract

Interfacial properties of the (CH4 + CO2 + H2O) system are of great importance in many geotechnical engineering applications. In this study, we report the first experimental measurements of the interfacial tensions in the (CH4 + CO2 + H2O) system under both three-phase (VLLE) and biphasic conditions. The measurements were made by the pendant drop method. The compositions of the coexisting phases were obtained from a previous study of the phase behavior and the phase densities were then calculated from an equation of state. IFTs along five isotherms in the VLLE region and along six isotherms in biphasic region are reported. In the VLLE region, the IFT between the water-rich liquid and the gas phase varied between (33 and 39) mN·m−1, with a sharp increase as the pressure increased along an isotherm towards the upper critical end point. In the same region, the IFT between the water-rich and CO2-rich liquids varied between (30 and 33) mN·m−1. The IFT between the gas phase and the CO2-rich liquid phase was too small to measure accurately but an approximate value was obtained which is consistent with Antonov's equality. In the biphasic region, measurements were made at temperatures up to 423 K and at pressures up to 30 MPa. As observed in other water-gas systems, the IFT declines monotonically along isotherms with increasing pressure and decreases with increasing temperature at constant pressure.