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Navajo Sandstone–brine–CO2 interaction: implications for geological carbon sequestration

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Abstract

The injection of CO2 into deep saline aquifers is being considered as an option for greenhouse gas mitigation. However, the response of an aquifer to the injected CO2 is largely unknown. Experiments involving the reaction of Navajo Sandstone with acidic brine were conducted at 200°C and 25 or 30 MPa to evaluate the extent of fluid–rock interactions. The first experiment examined sandstone interaction with CO2-impregnated brine; the second experiment examined sandstone dissolution in CO2-free acidic brine; the third one is carried out in a mixed-flow reactor and designed to measure sandstone dissolution rates based on time-series Si concentrations. The solution chemistry data indicate that the SiO2(aq) increases gradually and pH increases slowly with reaction progress. Silicate minerals in the sandstone display textures (dissolution features, secondary mineralization), indicating that these phases are reacting strongly with the fluid. Dissolution of feldspars and conversion of smectite to illite are likely to be the two reactions that contribute to the release of SiO2(aq). The product minerals present at the end of the experiments are illite, illite/smectite, allophane, and carbonate minerals (for the CO2-charged system). Dissolved CO2 is likely to acidify the brine and to provide a source of carbon for the precipitation of carbonate minerals. Mineral trapping through the precipitation of carbonate minerals is favored thermodynamically and was observed in the experiments. The chemical reactions likely increase the bulk porosity of the sandstone due to dissolution of silicate minerals. However, allophane and illite/smectite fill voids in sandstone grains. There is no evidence for the removal of clay coatings due to chemical reactions. It is uncertain whether the mechanical forces near an injection well would mobilize the smectite and allophane and clog pore throats. Trace amounts of metals, including Cu, Zn, and Ba, were mobilized.

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Acknowledgments

Material in this paper is based upon work supported by the US Department of Energy under Award No. DE-FG26-04NT42125 to C.Z. and W.E.S. Any opinions, findings, and conclusions or recommendations expressed in this material, however, are those of the authors and do not necessarily reflect the views of the United States Government or any agency thereof. We thank Rick Knurr at University of Minnesota for chemical analyses of fluid samples.

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Authors and Affiliations

  1. Department of Geological Sciences, Indiana University, Bloomington, IN, 47405, USA

    Peng Lu, Anne Hereford & Chen Zhu

  2. Department of Geology and Geophysics, University of Minnesota, Minneapolis, MN, 55455, USA

    Qi Fu & William E. Seyfried Jr

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  1. Peng Lu
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  2. Qi Fu
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  3. William E. Seyfried Jr
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Correspondence to Peng Lu.

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Lu, P., Fu, Q., Seyfried, W.E. et al. Navajo Sandstone–brine–CO2 interaction: implications for geological carbon sequestration. Environ Earth Sci 62, 101–118 (2011). https://doi.org/10.1007/s12665-010-0501-y

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