Kinetics of CO₂ dissolution in brine : experimental measurement and application to geologic storage

A novel approach to geologic CO₂ sequestration is the surface dissolution method. This method involves lifting native brine from an aquifer, dissolution of CO₂ into the brine using pressurized mixing and injection of the CO₂ saturated brine back into the aquifer. This approach has several advantages over the conventional approach, including minimization of the risk of buoyancy driven leakage and dramatic reduction in the extent of pressure elevation in the storage structure. The mass transfer coefficient for the CO₂/brine two-phase system and associated transport calculations allow efficient design of the surface equipment required to dissolve CO₂ under pressure. This data was not previously available in the literature. Original experimental data on the rate of dissolution of CO₂ into Na-Ca-Cl brines across a range of temperatures and wet CO₂ densities are presented. From this data, the intrinsic mass transfer coefficient between CO₂-rich and aqueous phases has been calculated. The statistically significant variation in the mass transfer coefficient was evaluated and compared with the variation caused by the experimental method. An empirical correlation was developed that demonstrates that the mass transfer coefficient is a function of the NaCl salinity, temperature and wet CO₂ density. For the conditions tested, the value of the coefficient is in the range of 0.015 to 0.056 cm/s. Greater temperature and smaller NaCl salinity increases the mass transfer coefficient. There is an interaction effect between temperature and wet CO₂ density, which increases or decreases the mass transfer coefficient depending on the value of each. CaCl₂ salinity does not have a statistically significant effect on the mass transfer coefficient. The transport calculations demonstrate that wellhead co-injection of CO₂ and brine is feasible, providing the same technical outcome at lower cost. For example, assuming a 2000 ft deep well and typical aquifer injection conditions, complete dissolution of the bulk COv phase can be achieved at 670 ft for bubbles of 0.16 cm initial radius. Using a horizontal pipe or mixing tank was also shown to be feasible. Gas entrainment was shown to provide a marked reduction in size of mixing apparatus required.