The impact of geochemistry on convective mixing in a gravitationally unstable diffusive boundary layer in porous media: CO2 storage in saline aquifers

The storage of carbon dioxide and acid gases in deep geological formations is considered a promising option for mitigation of greenhouse gas emissions. An understanding of the primary mechanisms such as convective mixing and geochemistry that affect the long-term geostorage process in deep saline aquifers is of prime importance. First, a linear stability analysis of an unstable diffusive boundary layer in porous media is presented, where the instability occurs due to a density difference between the carbon dioxide saturated brine and the resident brine. The impact of geochemical reactions on the stability of the boundary layer is examined. The equations are linearised, and the obtained system of eigenvalue problems is solved numerically. The linear stability results have revealed that geochemistry stabilises the boundary layer as reaction consumes the dissolved carbon dioxide and makes the density profile, as the source of instability, more uniform. A detailed physical discussion is also presented with an examination of vorticity and concentration eigenfunctions and streamlines' contours to reveal how the geochemical reaction may affect the hydrodynamics of the process. We also investigate the effects of the Rayleigh number and the diffusion time on the stability of a boundary layer coupled with geochemical reactions. Nonlinear direct numerical simulations are also presented, in which the evolution of density-driven instabilities for different reaction rates is discussed. The development of instability is precisely studied for various scenarios. The results indicate that the boundary layer will be more stable for systems with a higher rate of reaction. However, our quantitative analyses show that more carbon dioxide may be removed from the supercritical free phase as the measured flux at the boundary is always higher for flow systems coupled with stronger geochemical reactions.