Navajo Sandstone-brine-CO₂ interaction: Implications for geological carbon sequestration

The injection of CO₂ into deep saline aquifers is being considered as an option for greenhouse gas mitigation. However, the response of an aquifer to the injected CO₂ is largely unknown. Experiments involving the reaction of Navajo Sandstone with acidic brine were conducted at 200°C and 25 or 30 MPa to evaluate the extent of fluid-rock interactions. The first experiment examined sandstone interaction with CO₂-impregnated brine; the second experiment examined sandstone dissolution in CO₂-free acidic brine; the third one is carried out in a mixed-flow reactor and designed to measure sandstone dissolution rates based on time-series Si concentrations. The solution chemistry data indicate that the SiO₂(aq) increases gradually and pH increases slowly with reaction progress. Silicate minerals in the sandstone display textures (dissolution features, secondary mineralization), indicating that these phases are reacting strongly with the fluid. Dissolution of feldspars and conversion of smectite to illite are likely to be the two reactions that contribute to the release of SiO₂(aq). The product minerals present at the end of the experiments are illite, illite/smectite, allophane, and carbonate minerals (for the CO₂-charged system). Dissolved CO₂ is likely to acidify the brine and to provide a source of carbon for the precipitation of carbonate minerals. Mineral trapping through the precipitation of carbonate minerals is favored thermodynamically and was observed in the experiments. The chemical reactions likely increase the bulk porosity of the sandstone due to dissolution of silicate minerals. However, allophane and illite/smectite fill voids in sandstone grains. There is no evidence for the removal of clay coatings due to chemical reactions. It is uncertain whether the mechanical forces near an injection well would mobilize the smectite and allophane and clog pore throats. Trace amounts of metals, including Cu, Zn, and Ba, were mobilized.