Effect of variable solubility on reactive dissolution in partially miscible systems

When two partially miscible systems are put in contact, one phase, A, can dissolve into the other one with a given solubility. Chemical reactions in the host phase can impact this dissolution by consuming A and by generating products that impact the solubility of A. Here, we study theoretically the optimal conditions for transfer of a reactant A in a host phase containing a species B when a bimolecular A + B -* C reaction generates a product C that linearly decreases the solubility of A. We have quantified numerically the influence of this variable solubility on the reaction-diffusion (RD) concentration profiles of all species in the host phase, on the temporal evolution of the position of the reaction front, and on the flux of A through the interface. We have also computed the analytical asymptotic concentration profiles, solutions at long times of the RD governing equations. For a fixed negative effect of C on the solubility of A, an increase in the initial concentration of reactant B or an increase in the diffusion rate of species B and C results in a larger flux of A and hence a larger amount of A dissolved in the host solution at a given time. However, when the influence of C on the solubility increases, the mass transfer decreases. Our results help understand to what extent a chemical reaction can optimize the reactive transfer of a solute to a host phase with application to, among other things, the geological sequestration of carbon dioxide in an aquifer.

Automated summary

When two partially miscible systems are in contact, the solubility of phase A in the other phase can be affected by chemical reactions that consume A and generate products impacting the solubility of A. This study examines the optimal conditions for the transfer of reactant A in a host phase containing species B, considering a reaction that produces a product C decreasing the solubility of A linearly. The results show that an increase in the initial concentration of reactant B or the diffusion rate of species B and C leads to a larger flux of A dissolved in the host solution, but as the influence of C on the solubility increases, the mass transfer decreases. The findings contribute to the understanding of how chemical reactions can optimize the transfer of solutes into a host phase, with potential applications in carbon dioxide sequestration in aquifers.