Experimental determination of porosity and permeability changes induced by injection of CO2 into carbonate rocks

A set of four reactive flow-through experiments at temperature T = 100 °C and total pressure P = 12 MPa was performed in limestone reservoir samples. By using various ranging from 0.7 to 10 MPa, these experiments mimic mass transfers occurring (1) near the injection well, where the brine is almost saturated with CO2 (i.e. PCO2 ≈ P), and (2) at increasing distances from the injection well, where the fluid displays lower values and higher divalent cation concentrations due rock dissolution along the fluid pathway. Results for PCO2 = 10 MPa show non-uniform dissolution features associated with transport-controlled mass transfer, while reaction-controlled uniform dissolution is observed for PCO2 = 2.5 MPa. The experiment with PCO2 = 6 MPa allows investigating in detail the transition from transport- to reaction-controlled dissolution. Conversely, the experiment reproducing conditions far from the injection well (PCO2 = 0.7 MPa), shows a decrease of porosity triggered by the precipitation of Mg-rich calcite. For all the dissolution experiments, the time-resolved porosity ϕ(t) can be modeled by a simple non-linear equation including parameters that characterise the dissolution regime triggered by the reactivity of the inlet fluid (measured by the Damköhler number, Da). Furthermore, all dissolution experiments display power scaling between permeability (k) and porosity (ϕ) with distinctly different scaling exponents characterising the reactivity of the fluid percolating the sample, independently from the decrease with time of the reactive surface area. It is shown also that dissolution at moderate positive values of Da seems the most efficient to increase permeability and promote a rapid spreading of the reaction front, while inducing minimal modification of the porosity in the vicinity of the CO2 injection well. These results can be used to parameterize the k–ϕ function for modeling the earliest dissolution processes occurring in the vicinity of the reaction front.