Permanent CO2 Trapping through Localized and Chemical Gradient-Driven Basalt Carbonation

Recent laboratory and field studies have demonstrated that basalt formations may present one of the most secure repositories for anthropogenic CO2 emissions through carbon mineralization. In this work, a series of high-temperature, high-pressure core flooding experiments was conducted to investigate how transport limitations, reservoir temperature, and brine chemistry impact carbonation reactions following injection of CO2-rich aqueous fluids into fractured basalts. At 100 °C and 6.3 mM [NaHCO3], representative of typical reservoir conditions, carbonate precipitates were highly localized on reactive mineral grains contributing key divalent cations. Geochemical gradients promoted localized reaction fronts of secondary precipitates that were consistent with 2D reactive transport model predictions. Increasing [NaHCO3] to 640 mM dramatically enhanced carbonation in diffusion-limited zones, but an associated increase in clays filling advection-controlled flow paths could ultimately obstruct flow and limit sequestration capacity under such conditions. Carbonate and clay precipitation were further enhanced at 150 °C, reducing the pre-reaction fracture volume by 48% compared to 35% at 100 °C. Higher temperature also produced more carbonate-driven fracture bridging, which generally increased with diffusion distance into dead-end fractures. In combination, the results are consistent with field tests indicating that mineralization will predominate in buffered diffusion-limited zones adjacent to bulk flow paths and that alkaline reservoirs with strong geothermal gradients will enhance the extent of carbon trapping.