Potential environmental issues of CO2 storage in deep saline aquifers: Geochemical results from the Frio-I Brine Pilot test, Texas, USA

摘要

Sedimentary basins in general, and deep saline aquifers in particular, are being investigated as possible repositories for large volumes of anthropogenic CO2 that must be sequestered to mitigate global warming and related climate changes. To investigate the potential for the long-term storage of CO2 in such aquifers, 1600 t of CO2 were injected at 1500 m depth into a 24-m-thick "C" sandstone unit of the Frio Formation, a regional aquifer in the US Gulf Coast. Fluid samples obtained before CO2 injection from the injection well and an observation well 30 m updip showed a Na-Ca-Cl type brine with similar to 93,000 mg/L TDS at saturation with CH4 at reservoir conditions; gas analyses showed that CH4 comprised similar to 95% of dissolved gas, but CO2 was low at 0.3%. Following CO2 breakthrough. 51 h after injection, samples showed sharp drops in pH (6.5-5.7), pronounced increases in alkalinity (100-3000 mg/L as HCO3) and in Fe (30-1100 mg/L), a slug of very high DOC values, and significant shifts in the isotopic compositions of H2O. DIC, and CH4. These data, coupled with geochemical modeling, indicate corrosion of pipe and well casing as well as rapid dissolution of minerals, especially calcite and iron oxyhydroxides, both caused by lowered pH (initially similar to 3.0 at subsurface conditions) of the brine in contact with supercritical CO2. These geochemical parameters, together with perfluorocarbon tracer gases (PFTs), were used to monitor migration of the injected CO2 into the overlying Frio "B", composed of a 4-m-thick sandstone and separated from the "C" by similar to 15 m of shale and siltstone beds. Results obtained from the Frio "B" 6 months after injection gave chemical and isotopic markers that show significant CO2 (2.9% compared with 0.3% CO2 in dissolved gas) migration into the "B" sandstone. Results of samples collected 15 months after injection, however, are ambiguous, and can be interpreted to show no additional injected Cot in the "B" sandstone. The presence of injected CO2 may indicate migration from "C" to "B" through the intervening beds or, more likely, a short-term leakage through the remedial cement around the casing of a 50-year old well. Results obtained to date from four shallow monitoring groundwater wells show no brine or CO2 leakage through the Anahuac Formation, the regional cap rock. Published by Elsevier Ltd.