Carbon Capture and Storage (CCS) is one of the promising techniques to mitigate carbon dioxide emissions and move towards net zero targets. The efficiency of a geological storage process is, however, a complex function of CO2/rock/brine interactions. In particular, the effect of geochemical interactions among CO2/rock/brine systems in an aquifer and its associated impact on wetting behavior has not been rigorously investigated before.

In this work, we study the effect of the critical parameters affecting the CO2/rock/brine system wettability from a geochemical perspective. In particular, we study the effect of temperature, pressure, and salinity on the wettability of the CO2/calcite/brine system. The wettability was assessed based on the disjoining pressure, which was calculated from calcite surface potential. The geochemical simulator used is based on surface complexation modeling and takes dissolution and precipitations reactions of the minerals and aqueous species into account.

The results show that increasing pressure decreases the concentration of calcite surface species >CaOH2+ and >CO3, while it increases the calcite surface species >CaCO3. However, increasing temperature increases the concentration of calcite surface species >CaCO3 and >CO3, while it slightly decreases the calcite surface species >CaOH2+. The results also show higher calcite surface potential and disjoining pressure at higher temperatures and lower salinity, which reflects an increase in water wettability (or a decrease in CO2-wetness) and greater CO2 storage potential in calcite-rich aquifers at these conditions.

This paper provides insight into the effect of different influencing parameters on the CO2/rock/brine interactions and CO2/rock/brine wettability, which can help understand the geochemical processes involved in CCS projects under a wide range of operating conditions.

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