A generalized kinetic theory of Ostwald ripening in porous media

Abstract

Partially miscible bubbles (e.g., CO${}_2$) trapped inside a porous medium and surrounded by a wetting phase (e.g., water) occur in a number of applications including underground hydrogen storage, geologic carbon sequestration, and the operation of electrochemcial devices such as fuel cells and electrolyzers. Such bubbles evolve due to a process called Ostwald ripening that is driven by differences in their interfacial curvature. For spherical bubbles, small bubbles shrink and vanish while feeding into larger ones, resulting in one large bubble at equilibrium. Within the confinement of a porous medium, however, bubbles can attain a distribution of sizes at equilibrium that have identical curvature. This work concerns itself with the formulation of a kinetic theory that predicts the statistical evolution of bubble states, defined as the sizes of the pores within which bubbles are trapped and the extent to which those pores are saturated with bubbles. The theory consists of a population balance equation and appropriate closure approximations. Systematic comparisons against a previously published pore network model (PNM) are conducted to validate the theory. Our theory generalizes existing variants in the literature limited to spherical bubbles trapped in homogeneous media to non-spherical (deformed) bubbles inside microstructures with arbitrary heterogeneity and spatial correlation in pore/throat sizes. We discuss the applicability, limitations, and implications of the theory towards future extensions.