Reactivity of micas and cap-rock in wet supercritical CO2 with SO2 and O2 at CO2 storage conditions |
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| Institution: | 1. School of Earth Sciences, University of Queensland, QLD 4072, Australia;2. CO2CRC Ltd, Earth Sciences Building, The University of Melbourne, VIC 3010, Australia;3. School of Chemical Engineering, University of Queensland, QLD 4072, Australia;1. Institute of Environmental Assessment and Water Research (IDAEA), CSIC, c/ Jordi Girona 18, 08034 Barcelona, Spain;2. Associated Unit, Hydrogeology Group (UPC-CSIC), Spain;3. Géosciences Montpellier, UMR5243, CNRS-Université Montpellier, Place Eugène Bataillon, 34095 Montpellier, France;4. Department of Earth Sciences, Program for Air, Water and Landscape Sciences, Hydrology, Villav. 16, 752 36 Uppsala, Sweden;5. Environmental and Water Resources Engineering Ltd., 97a Yefe-Nof St., P.O. Box 6770 Haifa 34641, Israel;1. Department of Geosciences, University of Oslo, PO Box 1047 Blindern, 0316 Oslo, Norway;2. Norwegian Geotechnical Institute (NGI), PO Box 3930 Ullevaal Stadion, 0806 Oslo, Norway;1. Shell Global Solutions, Kesslerpark 1, 2288 GS Rijswijk, The Netherlands;2. Department of Earth Sciences, Utrecht University, Budapestlaan 4, 3584 CD Utrecht, The Netherlands;3. Clay and Interface Mineralogy, RWTH Aachen University, Intzestrasse 1, 52056 Aachen, Germany;4. Steinmann Institute, Bonn University, Poppelsdorfer Schloss, 53115 Bonn, Germany;1. Department of Geotechnology, Delft University of Technology, P.O. Box 5048, 2628 CN Delft, The Netherlands;2. Shell Global Solutions International BV, Kesslerpark 1, 228 8GS Rijswijk, The Netherlands;1. School of Environmental Studies, China University of Geosciences, Wuhan 430074, China;2. College of Resources and Environmental Engineering, Wuhan University of Science and Technology, Wuhan 430081, China;3. Hubei Key Laboratory of Marine Geological Resources, China University of Geosciences, Wuhan 430074, China |
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| Abstract: | Seal or cap-rock integrity is a safety issue during geological carbon dioxide capture and storage (CCS). Industrial impurities such as SO2, O2, and NOx, may be present in CO2 streams from coal combustion sources. SO2 and O2 have been shown recently to influence rock reactivity when dissolved in formation water. Buoyant water-saturated supercritical CO2 fluid may also come into contact with the base of cap-rock after CO2 injection. Supercritical fluid-rock reactions have the potential to result in corrosion of reactive minerals in rock, with impurity gases additionally present there is the potential for enhanced reactivity but also favourable mineral precipitation.The first observation of mineral dissolution and precipitation on phyllosilicates and CO2 storage cap-rock (siliciclastic reservoir) core during water-saturated supercritical CO2 reactions with industrial impurities SO2 and O2 at simulated reservoir conditions is presented. Phyllosilicates (biotite, phlogopite and muscovite) were reacted in contact with a water-saturated supercritical CO2 containing SO2, or SO2 and O2, and were also immersed in the gas-saturated bulk water. Secondary precipitated sulfate minerals were formed on mineral surfaces concentrated at sheet edges. SO2 dissolution and oxidation resulted in solution pH decreasing to 0.74 through sulfuric acid formation. Phyllosilicate dissolution released elements to solution with ～50% Fe mobilized. Geochemical modelling was in good agreement with experimental water chemistry. New minerals nontronite (smectite), hematite, jarosite and goethite were saturated in models. A cap-rock core siltstone sample from the Surat Basin, Australia, was also reacted in water-saturated supercritical CO2 containing SO2 or in pure supercritical CO2. In the presence of SO2, siderite and ankerite were corroded, and Fe-chlorite altered by the leaching of mainly Fe and Al. Corrosion of micas in the cap-rock was however not observed as the pH was buffered by carbonate dissolution. Ca-sulfate, and Fe-bearing precipitates were observed post SO2-CO2 reaction, mainly centered on surface cracks and an illite rich illite-smectite precipitate quantified. Water saturated impure supercritical CO2 was observed to have reactivity to rock-forming biotite, muscovite and phlogopite mineral separates. In the cap-rock core however carbonates and chlorite were the main reacting minerals showing the importance of assessing actual whole core. |
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| Keywords: | Cap-rock Gas-water-rock reaction |
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