Chemo-hydro-mechanical effects of CO2 injection into a permeable limestone

CO2 storage in carbonate aquifers is a way to mitigate atmospheric CO2 emissions, but it leads to acid-producing reactions that may induce alterations in the rock pore structure and hydromechanical properties. To gain a better understanding of these changes in rock properties, percolation experiments under constant flow-rate conditions with (i) CO2-saturated water (PCO2 = 100 bar and T = 60 °C) and (ii) HCl solutions (P = 1 bar and T = 60 °C) were performed on centimetric cores of the grain-supported Pont du Gard Limestone (permeability about 10−14–10−13 m2). Effluent chemistry analyses, X-ray imaging, and measurements of the hydromechanical properties of intact and altered specimens were used to quantify acid-induced changes in the two acid-rock systems. Experimental results show that the rock dissolution patterns highly depend on the acid type and pore space heterogeneity. Under the flow conditions of these experiments, complete HCl dissociation (strong acid) and rapid HCl-rock reaction result in a compact dissolution pattern that only affects the hydromechanical properties of the core inlet. Conversely, partial dissociation of H2CO3 (weak acid) produces chemical reactions all along the core. Initial structural heterogeneities localize chemical reactions along preferential flow pathways, causing instabilities in the reaction front and wormhole formation, which markedly enhances permeability. A powerlaw relationship with a very large exponent (as high as 24) accounts for the variation in permeability as a function of porosity. Altered cores render both a significant attenuation in mechanical rock properties and ultrasonic velocities, which is reproduced using a Differential Effective Medium (DEM) homogenization approach. The high-pressure percolation experiments of this study using CO2-saturated water represent an extreme scenario of CO2-brine-rock interactions in carbonate reservoirs, which needs to be considered to improve the prediction and monitoring of the storage performance.