In partially miscible two-layer systems within a gravity field, buoyancy-driven convective motions can appear when one phase dissolves with a finite solubility into the other one. We investigate the influence of chemical reactions on such convective dissolution by a linear stability analysis of a reaction-diffusion-convection model. We show theoretically that a chemical reaction can either enhance or decrease the onset time of the convection, depending on the type of density profile building up in time in the reactive solution. We classify the stabilizing and destabilizing scenarios in a parameter space spanned by the solutal Rayleigh numbers. As an example, we experimentally demonstrate the possibility to enhance the convective dissolution of gaseous CO_{2} in aqueous solutions by a classical acid-base reaction.
Dissolution-driven convection occurs in the host phase of a partially miscible system when a buoyantly unstable density stratification develops upon dissolution. Reactions can impact such convection by changing the composition and thus the density of the host phase. Here we study the influence of A+B→ C reactions on such convective dissolution when A is the dissolving species and B a reactant initially present in the host phase. We perform a linear stability analysis of related reaction-diffusion density profiles to compare the growth rate of the instability in the reactive case to its non reactive counterpart when all species diffuse at the same rate. We classify the stabilizing or destabilizing influence of reactions on the buoyancy-driven convection in a parameter space spanned by the solutal Rayleigh numbers R A,B,C of chemical species A, B, C and by the ratio β of initial concentrations of the reactants. For R A > 0, the non reactive dissolution of A in the host phase is buoyantly unstable. In that case, we show that reaction is enhancing convection provided C is sufficiently denser than B. Increasing the ratio β of initial reactant concentrations increases the effect of chemistry but does not significantly impact the stabilizing/destabilizing classification. When the non reactive case is buoyantly stable (R A < 0), reactions can create in time an unstable density stratification and trigger convection if R C > R B . Our theoretical approach allows classifying previous results in a unifying picture and developing strategies for chemical control of 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 CO geological sequestration where quantifying the storage rate of CO dissolving into the host oil or aqueous phase is crucial to assess the efficiency and the safety of the project.
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