Hydrogen wettability in carbonate reservoirs: Implication for underground hydrogen storage from geochemical perspective

Hydrogen has been considered as a promising renewable source to replace fossil fuels to meet energy demand and achieve net-zero carbon emission target. Underground hydrogen storage attracts more interest as it shows potential to store hydrogen at large-scale safely and economically. Meanwhile, wettability is one of the most important formation parameters which can affect hydrogen injection rate, reproduction efficiency and storage capacity. However, current knowledge is still very limited on how fluid-rock interactions affect formation wettability at in-situ conditions. In this study, we thus performed geochemical modelling to interpret our previous brine contact angle measurements of H₂-brine-calcite system. The calcite surface potential at various temperatures, pressures and salinities was calculated to predict disjoining pressure. Moreover, the surface species concentrations of calcite and organic stearic acid were estimated to characterize calcite-organic acid electrostatic attractions and thus hydrogen wettability. The results of the study showed that increasing temperature increases the disjoining pressure on calcite surface, which intensifies the repulsion force of H₂ against calcite and increases the hydrophilicity. Increasing salinity decreases the disjoining pressure, leading to more H₂-wet and contact angle increment. Besides, increasing stearic acid concentration remarkably strengthens the adhesion force between calcite and organic acid, which leads to more hydrophobic and H₂-wet. In general, the results from geochemical modelling are consistent with experimental observations that decreasing temperature and increasing salinity and organic acid concentration increase water contact angle. This work also demonstrates the importance of involving geochemical modelling on H₂ wettability assessment during underground hydrogen storage.