Wettability shifts caused by CO2 aging on mineral surfaces

Abstract:

Interfacial forces at the CO₂/brine/mineral ternary interface have a well-established impact on multiphase flow properties through porous media. In the context of geologic carbon sequestration, this wettability will impact capillary pressure, residual trapping, and a variety of other key parameters of interest. While the wettability of CO₂ on pure mineral and real rock sample have been studied a great deal over the past few year, very little is known about how the wettability of these rocks could change over long time horizons as CO₂ interacts with species in the brine and on the mineral surface. In this work we sought to explore the role that dilute inorganic and organic species that are likely to exist in connate brines might have on a suite of mineral species. High-pressure contact angle experiments were carried out on a suite of polished mineral surfaces. Both static captive bubble and advancing/receding contact angle measurements were carried out. The effect of ionic strength, and in particular the valence of the dominant ions in the brine are found to have an important impact on the wettability which cannot be explained solely based on the shifts in the interfacial tension between the CO₂ and brine. More significantly, three organic species, formate, acetate, and oxalate, all three of which are representative species commonly encountered in the saline aquifers that are considered target repositories for carbon sequestration. All three organic species show impacts on wettability, with the organics generally increasing the CO₂ wetting of the mineral surface. Not all pure minerals respond the same to the presence of organics, with micas showing a more pronounced influence than quartz. Sandstone and limestone samples aged with different kinds of hydrocarbons, a surrogate for oil-bearing rocks, are generally more CO₂-wet, with larger contact angles in the CO₂/brine system. Over multiple days, the contact angle decreases, which could be attributed to partitioning of oil films off of the surface and into the CO₂ phase, which drives the wettability towards the original water-wet state. This effect could be particularly important for organic rich repositories like depleted oil and gas fields or fractured shale formations where organic species could be presented both on mineral surfaces and in the aqueous phase.

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