Abstract
Geochemical reactions can play important role in the long-term geological storage of CO2 in sites where the target formations have reactive minerals. Although the use of batch models (experimental or theoretical) is expedient, it leaves questions unanswered about how to interpret or predict field-scale injection over long time periods. In this study we present results of coupled multiphase, multicomponent reactive transport simulation using geochemistry data derived from Cranfield site, Mississippi, USA, a site that has long been used for carbon sequestration R&D activities. The simulation was performed using PFLOTRAN, an open-source parallel reactive transport code. The geochemical system consists of 22 primary or basis species, in situ CO2 and O2 gaseous components, and 5 minerals. In this model, there are 37 secondary elements with brine molality being 1.81. The fluid chemical compositions were measured from production fluids, and mineral composition of the formation was obtained from XRD analysis of core samples. Results show how brine chemistry changes in the reservoir and shed insights into the need to monitor the mobility of cations such as Mg, Ca, Al, Mn, Fe, Cu, Zn, Sr, Ba, and Cd. We delineate the reservoir volume that is affected in order to provide simultaneous potential mobile inventory of these metals in the storage formations and warn possible risks through leakage into overlying zone. It is found that during injection period considered in this study dissolved CO2 can spread about 3.5 km2 area around the injection well and, as a result, pH drops to as low as 3.3–5.5 at the farthest location affected. Among the metals considered, only concentrations of Ca and Al are increased by 1 and 2 orders, respectively. In longer periods, Al concentration can increase by orders of magnitude of EPA’s threshold limit. Compared to no reactions, the CO2 plume’s extent area is 50 % less in 20 years; however, more CO2 is trapped in solution.
















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References
Anne SM (2013) Modeling of CO2–water–rock interactions in Mississippian sandstone reservoir of Kentucky. Department of Earth and Environmental Sciences University of Kentucky, Lexington
Benson SM, Cole DR (2008) CO2 sequestration in deep sedimentary formations. Elements 4:325–331
Cardoso S, Andres J (2014) Geochemistry of silicate-rich rocks can curtail spreading of carbon dioxide in subsurface aquifers. Nat Commun 5:5743–5748
Druckenmiller ML, Maroto-Valer M, Hill M (2006) Investigation of carbon sequestration via induced calcite formation in natural gas well brine. Energy Fuels 20:172–179
Duan Z, Sun R (2003) An improved model calculating CO2 solubility in pure water and aqueous NaCl solutions from 273 to 533 K and from 0 to 2000 bar. Chem Geol 193:257–271
Dumkwu FA, Islam AW, Carlson ES (2012) Review of well models and assessment of their impacts on numerical reservoir simulation performance. J Pet Sci Eng 82–83:174–186
Ellis AJ, Godling RM (1963) The solubility of carbon dioxide above 100 C in water and in sodium chloride solutions. Am J Sci 261:47–60
Ennis-King J, Paterson L (2005) Role of convective mixing in the long-term storage of carbon dioxide in deep saline formations. SPE J 10:349–356
Fan Y, Durlofsky L, Tchelepi H (2012) A fully-coupled flow-reactive-transport formulation based on element conservation, with application to CO2 storage simulations. Adv Water Resour 42:47–61
Fu X, Luis Cueto-Felgueroso L, Juanes R (2013) Pattern formation and coarsening dynamics in three-dimensional convective mixing in porous media. Phylosophical Trans R Spciey A 371:20120355
Fu X, Cueto-Felgueroso L, Bolster D, Juanes R (2015) Rock dissolution patterns and geochemical shutdown of CO2-brine-carbonate reactions during convective mixing in porous media. J Fluid Mech 764:296–315
Ghesmat K, Hassanzadeh H, Abedi J (2011) The impact of geochemistry on convective mixing in a gravitationally unstable diffusive boundary layer in porous media: CO2 storage in saline aquifers. J Fluid Mech 673:480–512
Gunter WD, Perkins EH, McCann TJ (1993) Aquifer disposal of CO2 rich greenhouse gases: reaction design for added capacity. Energy Convers Manag 34:941–948
Gunter WD, Wiwchar B, Perkins EH (1997) Aquifer disposal of CO2-rich greenhouse gases: extension of the time sacle of experiment for CO2 sequestering-reactions by geochemical modeling. Mineral Petrol 59:121–140
Guo B, Bandilla KW, Doster F, Keilegavlen E, Celia MA (2013) A vertically integrated model with vertical dynamics for CO2 storage. Water Resour Res 50:6269–6284
Hassanzadeh H, Pooladi-Darvis M, Keith D (2007) Scaling behavior of convective mixing, with application to geological storage of CO2. AIChE J 53:1121–1131
Islam AW, Carlson ES (2012) Application of SAFT equation for CO2 + H2O phase equilibrium calculations over a wide temperature and pressure range. Fluid Ph Equilibria 321:17–24
Islam A, Sun A (2015) Quantification of CO2 masses trapped through free convection process in isothermal brine reservoir. Int J Heat Mass Transfer 87:128–137
Islam AW, Sharif MA, Carlson ES (2013) Numerical investigation of double diffusive natural convection of carbon dioxide in a brine saturated geothermal reservoir. Geothermics 38:101–111
Islam A, Korrani A, Sepehrnoori K, Patzek T (2014) Effects of geochemical reaction on double diffusive natural convection of CO2 in brine saturated geothermal reservoir. Int J Heat Mass Transfer 77:519–528
Islam A, Sun A, Yang C (2016) Reactive transport modeling of the enhancement of density-driven CO2 convective mixing in carbonate aquifers and its potential implication on geological carbon sequestration. Sci Rep 6:24768
Johnson JW, Nitao JJ (2002) Enhanced caprock integrity and self-sealing of the immiscible plume through mineral trapping during prograde and retrograde CO2 sequestration in saline aquifers. AAPG Bull 86:161–162
Jun Y-S, Giammar D, Werth C (2012) Impacts of geochemical reactions on geologic carbon sequestration. Environ Sci Technol 47:3–8
Knauss KG, Johnson JW, Steefel CI (2005) Evaluation of the impact of CO2, co-contaminant gas, aqueous fluid, and reservoir rock interactions on the geologic sequestration of CO2. Chemical Geol 217:339–350
Kneafsey TJ, Pruess K (2010) Laboratory flow experiments for visualizing carbon dioxide -induced, density-driven brine convection. Transp Porous Media 82:123–139
Lindeberg E, Wessel-Berg D (1997) Vertical convection in an aquifer column under a gas cap of CO2. Energy Convers Manag 38:S229–S234
Litchner PC (1996) Continuum formulation of multicomponent-multiphase reactive transport. Reactive transport in porous media. Rev Mineral 34:1–81
Lu C, Lichtner P (2007) High resolution numerical investigation on the effect of convective instability on long term CO2 storage in saline aquifers. J Phys Conf Ser 78:012042
Lu J, Kharaka Y, Thordsen J, Horita J, Karamalidis A, Griffith C, Hakala J, Ambats G, Cole DR, Phelps T, Manning M, Cook PJ, Hovorka SD (2012) Co2–rock-brine interactions in lower tuscaloosa formation at Cranfield CO2 sequestration site, Mississipi, USA. Chem Geol 291:269–277
Meckel T, Bryant S, Ganesh R (2015) Characterization and prediction of CO2 saturation resulting from modeling buoyant fluid migration in 2D heterogeneous geologic fabrics. Int J Greenh Gas Control 34:85–96
Metz B, Davidson O, de Conick H, Loos M, Meyer L (2005) Intergovernmental panel on climate change. IPCC special report on carbon dioxide capture and storage, New York, p 53
Noh M, Lake LW, Bryant SL, Araque-Martinez A (2004) Implication of coupling fractional flow and geochemistry for CO2 injection in aquifers. SPE/DOE Symposium on Improved Oil Recovery, Tulsa
Okamoto I, Mito S, Ohsumi T (2009) A sensitivity study of CO2 mineralization using GEM-GHG simulator. Energy Procedia 1:3323–3329
Palandri JL, Kharaka YK (2004) A compilation of rate parameters of water-mineral interaction kinetics for application to geochemical modeling. Open File Report, US Geological Survey 64, Menlo Park, CA
Ren B, Sun Y, Bryant S (2014) Maximizing local capillary trapping during CO2 injection. Energy Procedia 63:5562–5576
Saatlink MW, Vilarrasa V, de Gaspari F, Silva O, Carrera J, Rotting TS (2013) A method for incorporating equilibrium chemical reactions into multiphase flow models for CO2 storage. Adv Water Resour 62:431–444
Solomon S (2007) Climate change 2007: the physical science basis. Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change, New York
Spycher N, Pruess K (2010) A phase-partitioning model for CO2-brine mixtures at elevated temperatures and pressures: application to CO2-enhanced geothermal systems. Transport Porous Media 82:173–196
Stewart PB, Munjal PK (1970) The solubility of carbon dioxide in pure water, synthetic sea water and synthetic sea-water concentration at -5 to 25 C and 10 to 45 atm pressure. J Chemi Eng Data 1591:67–71
Ward T, Jensen O, Power H, Riley D (2014) High-Rayleigh-number convection of a reactive solute in a porous medium. J Fluid Mech 760:95–126
Weir GJ, White SP, Kissling WM (1996) Reservoir storage and containment of greenhouse gases. Transport Porous Media 23:37–60
Wellman TP, Grigg RB, McPherson BJ, Svec RK, Lichtner PC (2003) Evaluation of CO2–brine–reservoir rock interaction with laboratory flow tests and reactive transport modeling. International Symposium on Oilfield Chemistry, Houston
White SP, Allis RG, Moore J, Chidsey T, Morgan C, Gwynn W, Adams M (2005) Simulation of reactive transport of injected CO2 on the Colorado Plateau. Chem Geol 217:387–405
World Health Organization (1998) Guidelines for drinking water quality. Health criteria and other supporting information, Geneva
Xu T, Pruess K (2001) Modeling multiphase non-isothermal fluid flow and reactive geochemical transport in variably saturated fractured rocks. Am J Sci 301:16–33
Xu T, Apps JA, Pruess K (2003) Reactive geochemical transport simulation to study mineral trapping for CO2 disposal in deep arenaceous formations. J Geophys Res B Solid Earth 108:3–13
Xu T, Apps J, Pruess K (2004) Numerical simulation to study mineral trapping for CO2 disposal in deep aquifers. Appl Geochem 19:917–936
Xu T, Apps JA, Pruess K (2005) Mineral sequestration of carbon dioxide in a sandstone-shale system. Chem Geol 217:295–318
Xu T, Sonnethel EI, Spycher N, Pruess K (2006) TOUGHREACT: a simulation program for non-isothermal multiphase reactive geochemical transport in variably saturated geologic media. Computer Geosci 32:145–165
Xu T, Kharaka Y, Doughty C, Freifeld B, Daley T (2010) Reactive transport modeling to study changes in water chemistry by CO2 injection at the Frio-I Brine Pilot. Chem Geol 271:153–164
Zerai B, Saylor BZ, Matisoff G (2006) Computer simulation of CO2 trapped through mineral precipitation in the Rose Run Sandstone. Appl Geochem 21:223–240
Acknowledgments
This work was partly funded by the US Department of Energy under award no. DE-FE0012231. The first author acknowledges TACC (Texas Advanced Computing Center) for providing high performance computational support. He greatly thanks Dr. Peter Lichtner, director, OFM Research, for helpful discussions on PFLOTRAN.
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Islam, A., Sun, A. & Lu, J. Simulating in-zone chemistry changes from injection time to longer periods of CO2 storage. Environ Earth Sci 75, 1346 (2016). https://doi.org/10.1007/s12665-016-6153-9
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DOI: https://doi.org/10.1007/s12665-016-6153-9


