Gas-water-rock interactions in Frio Formation following CO 2 injection: Implications for the storage of greenhouse gases in sedimentary basins

Abstract

To investigate the potential for the geologic storage of CO 2 in saline sedimentary aquifers, 1600 t of CO 2 were injected at 1500 m depth into a 24-m-thick sandstone section of the Frio Formation, a regional brine and oil reservoir in the U.S. Gulf Coast. Fluid samples obtained from the injection and observation wells before CO 2 injection showed a Na-Ca-Cl–type brine with 93,000 mg/L total dissolved solids (TDS) at near saturation with CH 4 at reservoir conditions. Following CO 2 breakthrough, samples showed sharp drops in pH (6.5–5.7), pronounced increases in alkalinity (100–3000 mg/L as HCO 3 ) and Fe (30–1100 mg/L), and significant shifts in the isotopic compositions of H 2 O, dissolved inorganic carbon (DIC), and CH 4 . Geochemical modeling indicates that brine pH would have dropped lower but for the buffering by dissolution of carbonate and iron oxyhydroxides. This rapid dissolution of carbonate and other minerals could ultimately create pathways in the rock seals or well cements for CO 2 and brine leakage. Dissolution of minerals, especially iron oxyhydroxides, could mobilize toxic trace metals and, where residual oil or suitable organics are present, the injected CO 2 could also mobilize toxic organic compounds. Environmental impacts could be major if large brine volumes with mobilized toxic metals and organics migrated into potable groundwater. The δ 18 O values for brine and CO 2 samples indicate that supercritical CO 2 comprises ∼50% of pore-fluid volume ∼6 mo after the end of injection. Postinjection sampling, coupled with geochemical modeling, indicates that the brine gradually will return to its preinjection composition.