In geologic carbon sequestration, reliable predictions of CO2 storage require understanding the capillary behavior of supercritical (sc) CO2. Given the limited availability of measurements of the capillary pressure (Pc) dependence on water saturation (Sw) with scCO2 as the displacing fluid, simulations of CO2 sequestration commonly rely on modifying more familiar air/H2O and oil/H2O Pc(Sw) relations, adjusted to account for differences in interfacial tensions. In order to test such capillary scaling-based predictions, we developed a high-pressure Pc(Sw) controller/meter, allowing accurate Pc and Sw measurements. Drainage and imbibition processes were measured on quartz sand with scCO2-brine at pressures of 8.5 and 12.0 MPa (45°C), and air-brine at 21°C and 0.1 MPa. Drainage and rewetting at intermediate Sw levels shifted to Pc values that were from 30% to 90% lower than predicted based on interfacial tension changes. Augmenting interfacial tension-based predictions with differences in independently measured contact angles from different sources led to more similar scaled Pc(Sw) relations but still did not converge onto universal drainage and imbibition curves. Equilibrium capillary trapping of the nonwetting phases was determined for Pc = 0 during rewetting. The capillary-trapped volumes for scCO2 were significantly greater than for air. Given that the experiments were all conducted on a system with well-defined pore geometry (homogeneous sand), and that scCO2-brine interfacial tensions are fairly well constrained, we conclude that the observed deviations from scaling predictions resulted from scCO2-induced decreased wettability. Wettability alteration by scCO2 makes predicting hydraulic behavior more challenging than for less reactive fluids.
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