Rock dissolution patterns and geochemical shutdown of CO₂–brine–carbonate reactions during convective mixing in porous media

Abstract

Motivated by the process of CO₂ convective mixing in porous media, here we study the formation of rock-dissolution patterns that arise from geochemical reactions during Rayleigh–Bénard–Darcy convection. Under the assumption of instantaneous chemical equilibrium, we adopt a formulation of the local reaction rate as a function of scalar dissipation rate, a measure that depends solely on flow and transport, and chemical speciation, which is a measure that depends only on the equilibrium thermodynamics of the chemical system. We use high-resolution simulations to examine the interplay between the density-driven hydrodynamic instability and the rock dissolution reactions, and analyse the impact of geochemical reactions on the macroscopic mass exchange rate. We find that dissolution of carbonate rock initiates in regions of locally high mixing, but that the geochemical reaction shuts down significantly earlier than shutdown of convective mixing. This early shutdown feature reflects the important role that chemical speciation plays in this hydrodynamics–reaction coupled process. Finally, we extend our analysis to three dimensions and explore the morphology of dissolution patterns in three dimensions.

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