Experimental Study of Porosity Changes in Shale Caprocks Exposed to Carbon Dioxide-Saturated Brine Ⅱ: Insights from Aqueous Geochemistry

摘要

Laboratory experiments evaluated two shale caprock formations, the Gothic Shale and Marine Tuscaloosa Formation, at conditions relevant to carbon dioxide (CO2) sequestration. Both rocks were exposed to CO2-saturated brines at 160 degrees C and 15MPa for approximate to 45 days. Baseline experiments for both rocks were pressurized with argon to 15MPa for approximate to 35 days. Varying concentrations of iron, aqueous silica, sulfate, and initial pH decreases coincide with enhanced carbonate and silicate dissolution due to reaction between CO2-saturated brine and shale. Saturation indices were calculated and activity diagrams were constructed to gain insights into sulfate, silicate, and carbonate mineral stabilities. Upon exposure to CO2-saturated brines, the Marine Tuscaloosa Formation appeared to be more reactive than the Gothic Shale. Evolution of aqueous geochemistry in the experiments is consistent with mineral precipitation and dissolution reactions that affect porosity. This study highlights the importance of tracking fluid chemistry to clarify downhole physicochemical responses to CO2 injection and subsequent changes in sealing capacity in CO2 storage and utilization projects.