Wettability Phenomena at the CO₂–Brine–Mineral Interface: Implications for Geologic Carbon Sequestration

Geologic carbon sequestration (GCS) in deep saline aquifers results in chemical and transport processes that are impacted by the wettability characteristics of formation solid phases in contact with connate brines and injected CO₂. Here, the contact angle (θ) at the CO₂–brine–mineral interface is studied for several representative solids including quartz, microcline, calcite, kaolinite, phlogopite, and illite under a range of GCS conditions. All were found to be water wetting (θ < 30°) with subtle but important differences in contact angles observed between the surfaces. Temperature and pressure conditions affected the results but did not produce discernible trends common to all surfaces. Brine composition, in terms of pH and ionic strength, was a better predictor of interfacial behavior. For the nonclays, the wettability is impacted by the pH at the point of zero charge of the solid. For the clays, the response was more complex. Under nonequilibrium conditions, hysteretic effects were observed when CO₂ was dissolving into the bulk fluid and this effect varied between minerals. Contact angle was found to decrease during the CO₂ phase transition from supercritical or liquid phase to gas phase. These results are useful for developing a more complete understanding of leakage through caprocks and capillary trapping in GCS.