Vanessa Loodts

Impact of pressure, salt concentration, and temperature on the convective dissolution of carbon dioxide in aqueous solutions

The convective dissolution of carbon dioxide (CO2) in salted water is theoretically studied to determine how parameters such as CO2 pressure, salt concentration, and temperature impact the short-time characteristics of the buoyancy-driven instability. On the basis of a parameter-free dimensionless model, we perform a linear stability analysis of the time-dependent concentration profiles of CO2 diffusing into the aqueous solution. We explicit the procedure to transform the predicted dimensionless growth rate and wavelength of the convective pattern into dimensional ones for typical laboratory-scale experiments in conditions close to room temperature and atmospheric pressure. This allows to investigate the implicit influence of the experimental parameters on the characteristic length and time scales of the instability. We predict that increasing CO2 pressure, or decreasing salt concentration or temperature destabilizes the system with regard to convection, leading to a faster dissolution of CO2 into salted water.

Enhanced steady-state dissolution flux in reactive convective dissolution

Chemical reactions can accelerate, slow down or even be at the very origin of the development of dissolution-driven convection in partially miscible stratifications when they impact the density profile in the host fluid phase. We numerically analyze the dynamics of this reactive convective dissolution in the fully developed non-linear regime for a phase A dissolving into a host layer containing a dissolved reactant B. We show for a general A + B → C reaction in solution, that the dynamics vary with the Rayleigh numbers of the chemical species, i.e. with the nature of the chemicals in the host phase. Depending on whether the reaction slows down, accelerates or is at the origin of the development of convection, the spatial distributions of species A, B or C, the dissolution flux and the reaction rate are different. We show that chemical reactions can enhance the steady-state flux as they consume A and can induce more intense convection than in the non-reactive case. This result is important in the context of CO2 geological sequestration where quantifying the storage rate of CO2 dissolving into the host oil or aqueous phase is crucial to assess the efficiency and the safety of the project.