Development of two simplified geochemical models for permeability evolution due to calcite dissolution in preferential pathways in caprock

Abstract:

Leakage through faults and fractures in caprocks is a major concern for geologic carbon sequestration in deep saline aquifers. Current leakage models assume constant permeabilities of pathways, but CO₂-acidified brine may cause minerals to dissolve, leading to permeability alteration. Calcite could cause significant permeability alteration, because it is abundant, thermodynamically unstable at low pH, and kinetically fast-reacting. We developed two simplified geochemical models to describe Permeability Evolution due to Calcite dissolution (PEC) in 1D flow paths through caprocks. The first is a numerical reactive transport model that couples solute advection and diffusion with carbonate reactions. The PEC model was used to examine geochemical and mineralogical conditions that lead to extensive permeability alterations. It was found that formations with larger amounts of calcite ultimately have larger final permeabilities, but the change is slower because extensive calcite dissolution buffers the reaction and retards the advance of the dissolution front. The second model, PEC Reaction Progress (PECRP), is a semi-analytical model developed to replicate the predictions of the PEC model but with much shorter run times. The PECRP model is based on assumptions of spatial homogeneity, sharp reacting front, and no reactions above the front. We simulated a synthetic system, the Eau Claire formation, and a sandstone in the Paris Basin to assess PECRP model performance. We found 1) for most cases the PECRP model causes a slightly shorter breakthrough time than the PEC model without affecting the final permeability; 2) when initial porosity is low, we observe temporary permeability decrease in the PEC model, while permeability never decreases in the PECRP model; 3) the PECRP model tends to fail to reproduce results from the PEC model with low Péclet numbers; 4) the PECRP model is not suitable for for pathways with certain types and degrees of mineral spatial heterogeneity. In summary, there are many conditions for which the fast PECRP model could be used to predict reaction-induced permeability evolution in a leakage estimation simulator, but it should be used with caution in flow paths with low initial porosity, low Péclet number, and substantial mineral spatial heterogeneity.