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Modelling CO2-brine-rock interactions in the Upper Paleozoic formations of Ordos Basin used for CO2 sequestration

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Abstract

Subsurface immobilization and conversion of CO2 into solid mineral phases in deep siliciclastic saline formations containing silicate minerals, commonly known as “mineral trapping”, is gaining research attention as a significant option to reduce CO2 emissions in the atmosphere. Although mineral trapping of CO2 is a long-term process, a combination of short-term results from both laboratory experiments and numerical simulations can lead to some general understanding of the required long-term CO2 sequestration mechanisms. This is a 100 year preliminary batch simulation study of four sandstone samples, under CO2 saturated water at 75 °C from the Upper Permian formations in the Ordos Basin, using the TOUGHREACT/ECO2N module to simulate the CO2-brine-rock interaction processes in deep siliciclastic multilayered saline aquifers. The samples approximately correspond to the four target saline formations selected by the Shenhua Group for a CO2 sequestration field demonstration project in the Ordos Basin, PR China. Preliminary simulation results show that the initial salinity of formation brine plays a significant role in determining the amount of CO2 that will be sequestered by solubility or mineral trapping in a deep saline aquifer. Minimal differences between experimental results and numerical calculation occur in low salinity waters, and significantly larger differences in high salinity waters, which is still under the maximum acceptable difference between experimental and computed data (10 %). The upper Liujiagou formation, with the highest level of salinity (ca. 88.7 g/L TDS) and lowest level of CO2 solubility, offers the highest mineral trapping capacity, with a maximum carbonate mineral storage of ca. 0.7 kg/m3 of bulk rock over a 100 year period. Regardless of the initial acidity or alkalinity of the aquifer brine, injection of CO2 will inflict a sudden drop in pH of the brine to acidity levels in a range of 3.0–4.6. The subsequent amount of dissolved and precipitated minerals, arising from the CO2-brine-rock interaction, is site specific and mainly dependent on initial aquifer mineralogy and brine composition.

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Abbreviations

A n :

Specific reactive surface area per kg H2O of mineral n (m2/kg H2O)

C :

Component concentration (mol/L)

E a :

Activation energy (J)

K :

Equilibrium constant (–)

K 0 :

Thermodynamic equilibrium constant for each component (CO2 and H2O) at the conditions of reference pressure P 0 (equals to 1 bar) and temperature T (–)

k :

Permeability (m2)

k n :

Rate constant of mineral n (–)

\(\mathop k\limits^{ = }\) :

Rate constant when reaction mechanisms are considered (–)

\(\bar{k}_{25}\) :

Rate constant at 25 °C (–)

N p :

Number of minerals (–)

N c :

Number of components (–)

P :

Pressure (Pa)

R :

Gas constant (–)

\(\gamma_{x}^{\prime }\) :

Activity coefficient for aqueous CO2 (–)

T :

Temperature (°C)

\(\bar{V}\) :

Average partial molar volume of each phase (CO2 or water) (m3/mol)

X :

Mass fraction (–)

\(x_{{{\text{CO}}_{ 2} }}\) :

CO2 mole fraction in the aqueous phase (–)

\(y_{{{\text{H}}_{ 2} {\text{O}}}}\) :

Water mole fraction in the CO2-rich phase (–)

α :

Ionic activity (mol/m3)

γ :

Activity coefficient (–)

η :

Fitting parameter in kinetic rate equation (–)

θ :

Fitting parameter in kinetic rate equation (–)

\(\varPhi\) :

Fugacity coefficient of each component in the CO2-rich phase (–)

Ω :

Mineral saturation ratio (–)

c :

CO2

j :

Primary chemical component

n :

Power term in rate constant equation under consideration of reaction mechanisms

m :

Minerals under equilibrium state

n :

Minerals under kinetic rate control state

nu, H, OH:

Reaction is under neutral, acid and base mechanism, respectively

H2O, CO2 :

Components of H2O and CO2, respectively

CO2 (g):

CO2 component in gaseous phase

tot:

Total amount

References

  • Bachu S (2002) Sequestration of CO2 in geological media in response to climate change: roadmap for site selection using the transform of the geological space into the CO2-phase space. Energy Convers Manage 43:87–102

    Article  Google Scholar 

  • Bauer S, Class H, Ebert M, Feeser V, Götze H, Holzheid A, Kolditz O, Rosenbaum S, Rabben W, Schäfer D, Dahmke A (2012) Modeling, parameterization and evaluation of monitoring methods for CO2 storage in deep saline formations: the CO2-MoPa project. Environ Earth Sci 67:351–367

    Article  Google Scholar 

  • Benson SM, Cole DR (2008) CO2 sequestration in deep sedimentary formations. Elements 4:325–331

    Article  Google Scholar 

  • Bertier P, Swennen R, Laenen B, Lagrou D, Dreesen R (2006) Experimental identification of CO2–water–rock interactions caused by sequestration of CO2 in Westphalian and Buntsandstein sandstones of the Campine Basin (NE-Belgium). J Geochem Explor 89:10–14

    Article  Google Scholar 

  • Bjgfrlykke K, Chuhan F, Kjeldstad A, Gundersen E, Lauvrak O, Hgfeg K (2004) Modelling of sediment compaction during burial in sedimentary basins. In: Stephansson O, Hudson JA, Jing L (eds) Coupled thermo-hydro-mechanical-chemical processes in geo-systems-fundamentals, modelling, experiments and applications, Elsevier Geo-Engineering Book Series, vol 2, pp 699–708

  • Bowers TS, Helgeson HC (1983) Calculation of the thermodynamic and geochemical consequences of non-ideal mixing in the system H2O–CO2–NaCl on phase relations in geologic systems: equation of state for H2O–CO2–NaCl fluids at high pressures and temperatures. Geochim Cosmochim Acta 47:1247–1275

    Article  Google Scholar 

  • Dawson GKW, Sidiq H, Pearce J, Gao J-F, Golding SD, Rudolph V, Li Q, Xing H (2013) ANLEC Project 3-1110-0101: Review of laboratory-scale geochemical and geomechanical experiments simulating geosequestration of CO2 sandstone, and associated modeling studies. Australian National Low Emissions Coal Research and Development, Manuka, ACT

  • De Lucia M, Bauer S, Beyer C, Kühn M, Nowak T, Pudlo D, Reitenbach V, Stadler S (2012) Modelling CO2-induced fluid-rock interactions in the Altensalzwedel gas reservoir. Part I: from experimental data to a reference geochemical model. Environ Earth Sci 67:563–572

    Article  Google Scholar 

  • Dethlefsen F, Ebert M, Dahmke A (2014) A geological database for parameterization in numerical modeling of subsurface storage in northern Germany. Environ Earth Sci 71:2227–2244

    Article  Google Scholar 

  • Duan ZH, 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

    Article  Google Scholar 

  • Eide KE (2012) CO2 sequestration: the effect of carbonate dissolution on reservoir rock integrity. Master thesis in Norwegian University of Science and Technology, Norway

  • Eissa MA, Thomas JM, Hershey RL, Dawoud MI, Pohll G, Dahab KA, Gomaa MA, Shabana AR (2014) Geochemical and isotopic evolution of groundwater in the Wadi Watir watershed, Sinai Peninsula, Egypt. Environ Earth Sci 71:1855–1869

    Article  Google Scholar 

  • Fan M, Jiang XQ, Liu WX, Zhang JY, Chen HY (2007) Dissolution of carbonate rocks in CO2 solution under different temperatures. Acta Sedimentol Sin 25(6):825–830

    Google Scholar 

  • Fischer S, Zemke K, Liebscher A, Wandrey M, the CO2SINK Group (2011) Petrophysical and petrochemical effects of long-term CO2-exposure experiments on brine-saturated reservoir sandstones. Procedia Eng 4487–4494

  • Fischer S, Liebscher A, De Lucia M, Hecht L (2013) Reactivity of sandstone and siltstone samples from the Ketzin pilot CO2 storage site-laboratory experiments and reactive geochemical modeling. Environ Earth Sci 70(8):3687–3708

    Article  Google Scholar 

  • Gaupp R, Pudlo D, Kohlhepp B (2009) Investigation of reservoir facies and fluid-rock interaction in the Rotliegend sandstones of the Altensalzwedel Block. Altmark, Middle Clean report

    Google Scholar 

  • Gou Y, Hou ZM, Liu HJ, Zhou L, Were P (2014) Numerical simulation of carbon dioxide injection for enhanced gas recovery (CO2-EGR) in Altmark natural gas field. Acta Geotech 9:49–58

    Article  Google Scholar 

  • Gunter WD, Wiwchar B, Perkins EH (1997) Aquifer disposal of CO2-rich greenhouse gases: extension of the time scale of experiment for CO2-sequestering reactions by geochemical modelling. Miner Petrol 59:121–140

    Article  Google Scholar 

  • Heeschen K, Risse A, Ostertag-Henning C, Stadler S (2011) Importance of co-captured gases in the underground storage of CO2: quantification of mineral alterations in chemical experiments. Procedia Eng 4:4480–4486

    Article  Google Scholar 

  • Hellevang H (2006) Interactions between CO2, saline water and minerals during geological storage of CO2. PhD thesis in University of Bergen, Norway

  • Hitchon B (1996) Aquifer disposal of carbon dioxide: hydrodynamic and mineral trapping-proof of concept. Geoscience Publishing Ltd., Alberta

    Google Scholar 

  • Hou GC, Liang YP, Su XS, Zhao ZH, Tao ZP, Yin LH, Yang YC, Wang XY (2008) Groundwater systems and resources in the Ordos Basin, China. Acta Geol Sin-Engl 82(5):1061–1069

    Google Scholar 

  • Johnson JW, Nitao JJ, Steefel CI, Knauss KG (2001) Reactive transport modeling of geologic CO2 sequestration in saline aquifers: the influence of intra-aquifer shales and the relative effectiveness of structural, solubility, and mineral trapping during prograde and retrograde sequestration. In: UCRL-JC-146932, Proceedings of the First National Conference on Carbon Sequestration, Washington, DC

  • Kaszuba JP, Janecky DR, Snow MG (2003) Carbon dioxide reaction processes in a model brine aquifer at 200°C and 200 bars: implications for geologic sequestration of carbon. Appl Geochem 18:1065–1080

    Article  Google Scholar 

  • Kaszuba JP, Janecky DR, Snow MG (2005) Experimental evaluation of mixed fluid reactions between supercritical carbon dioxide and NaCl brine: relevance to the integrity of a geologic carbon repository. Chem Geol 217:277–293

    Article  Google Scholar 

  • Ketzer JM, Iglesias R, Einloft S, Dullius J, Ligabue R, de Lima V (2005) Water–rock–CO2 interactions in saline aquifers aimed for carbon dioxide storage: experimental and numerical modeling studies of the Rio Bonito Formation (Permian), southern Brazil. Appl Geochem 24:760–767

    Article  Google Scholar 

  • Kolditz O, Bauer S (2004) A process-oriented approach to computing multi-field problems in porous media. J Hydroinf 6:225–244

    Google Scholar 

  • Kühn M, Tesmer M, Pilz P, Meyer R, Reinicke K, Förster A, Kolditz O, Schäfer D, CLEAN Parterners (2012) CLEAN: project overview on CO2 large-scale enhanced gas recovery in the Altmark natural gas field (Germany). Environ Earth Sci 67:311–321

    Article  Google Scholar 

  • Labus K, Bujok P (2011) CO2 mineral sequestration mechanisms and capacity of saline aquifers of the Upper Silesian Coal Basin (Central Europe)—modeling and experimental verification. Energy 36:4974–4982

    Article  Google Scholar 

  • Lasaga AC, Soler JM, Ganor J, Burch TE, Nagy KL (1994) Chemical weathering rate laws and global geochemical cycles. Geochim Cosmochim Acta 58:2361–2386

    Article  Google Scholar 

  • Lee KY (1986) Geology of the coal and petroleum deposits in the Ordos basin, China. In: United States Department of the Interior Geological Survey Report, pp 86–278

  • Li Q, Liu GZ, Liu XH, Li XC (2013) Application of a health, safety, and environmental screening and ranking framework to the Shenhua CCS project. Int J Greenh Gas Con 17:504–514

    Article  Google Scholar 

  • Liu F, Lu P, Griffith C, Hedges SW, Soong Y, Hellevang H, Zhu C (2012) CO2-brine-caprock interaction: reactivity experiments on Eau Claire shale and a review of relevant literature. Int J Greenh Gas Con 7:153–167

    Article  Google Scholar 

  • Liu HJ, Hou ZM, Gou Y, Were P (2013) Simulation of CO2-water-rock interaction processes: mineral scaling problems in saline formations. In: Hou MZ, Xie HP, Were P (eds) Clean energy systems in the subsurface: production, storage and conversion, pp 233–248

  • Liu HJ, Hou ZM, Gou Y, Were P, Sun XL (2014) Simulation of CO2 plume movement in multilayered saline formations through multilayer injection technology in the Ordos Basin, China. Environ Earth Sci 71:4447–4462

    Article  Google Scholar 

  • Luquot L, Andreani M, Gouze P, Camps P (2012) CO2 percolation experiment through chlorite/zeolite-rich sandstone (Pretty Hill Formation-Otway Basin-Australia). Chem Geol 294–295:75–88

    Article  Google Scholar 

  • Ma RY, Zhu HP, Zhang DF, Pan AF (2009) Basement faults and their recent activity in Ordos Basin. Chin J Ear Sci Environ 31(4):400–408 (in Chinese)

    Google Scholar 

  • Palandri JL, Kharaka YK (2004) A compilation of rate parameters of water-mineral interaction kinetics for application to geochemical modeling. In: US Geological Survey Report 2004–1068

  • Pearce JM, Holloway S, Wacker H, Nelis MK, Rochelle C, Bateman K (1996) Natural occurrences as analogues for the geological disposal of carbon dioxide. Energy Convers Manage 37(6–8):1123–1128

    Article  Google Scholar 

  • Portier S, Rochelle C (2005) Modelling CO2 solubility in pure water and NaCl-type waters from 0 to 300 °C and from 1 to 300 bar application to the Utsira Formation at Sleipner. Chem Geol 217:187–199

    Article  Google Scholar 

  • Pruess K (2005) ECO2N: a TOUGH2 fluid property module for mixtures of water, NaCl, and CO2. In: Lawrence Berkeley Laboratory Report LBNL–57952, Berkeley

  • Pudlo D, Reitenbach V, Albrecht D, Ganzer L, Gernert U, Wienand J, Kohlhepp B, Gaupp R (2012) The impact of diagenetic fluid-rock reactions on Rotliegend sandstone composition and petrophysical properties (Altmark area, central Germany). Environ Earth Sci 67:369–384

    Article  Google Scholar 

  • Qin YY, Li KZ, Cheng QJ, Qin ZL, Chen FH, Xu BX (2006) Hydraulic fracturing technology in low permeability gas reservoir of Daniudi gas field. In: Proceedings of Sinopec oil and gas technology BBS, Haikou

  • Remoroza A, Doroodchi E, Moghtaderi B (2012) CO2-EGS in hot dry rock: preliminary results from CO2-rock interaction experiments. In: Proceedings of 37th Workshop on Geothermal Reservoir Engineering, 30 January-1 February, 2012, Stanford University, Stanford, California, SGP-TR-194

  • Rimmelé G, Barlet-Gouédard V, Renard F (2010) Evolution of the petrophysical and mineralogical properties of two reservoir rocks under thermodynamic conditions relevant for CO2 geological storage at 3 km depth. Oil Gas Sci Technol Rev IFP 65:565–580

    Article  Google Scholar 

  • Rochelle CA, Bateman K, Pearce JM (2002) Geochemical interactions between supercritical CO2 and the Utsira formation: an experimental study. In: British Geological Survey Commissioned Report, CR/02/060, p 62

  • Romanelli A, Londono OMQ, Martinez DE, Massone HE, Escalante AH (2014) Hydrogeochemistry and isotope techniques to determine water interactions in groundwater-dependent shallow lakes, Wet Pampa Plain, Argentina. Environ Earth Sci 71:1953–1966

    Article  Google Scholar 

  • Rosenbauer R, Koksalan T, Palandri JL (2005) Experimental investigation of CO2–brine–rock interactions at elevated temperature and pressure: implications for CO2 sequestration in deep-saline aquifers. Fuel Process Technol 86:1571–1597

    Google Scholar 

  • Schöner R (2006) Comparison of Rotliegend sandstone diagenesis from the northern and southern margin of the North German Basin, and implications for the importance of organic maturation and migration. PhD thesis in University of Jena, Germany

  • Scislewski A, Zuddas P (2010) Estimation of reactive mineral surface area during water–rock interaction using fluid chemical data. Geochim Cosmochim Acta 74:6996–7007

    Article  Google Scholar 

  • Shenhua Group (2012) Inner data of CO2 sequestration project launched in Ordos Basin (in Chinese)

  • Shiraki R, Dunn TL (2000) Experimental study on water-rock interactions during CO2 flooding in the Tensleep Formation, Wyoming, USA. Appl Geochem 15:265–279

    Article  Google Scholar 

  • Sorensena JA, Holubnyaka YI, Hawthornea SB, Millera DJ, Eylandsa K, Steadmana EN, Harju JA (2009) Laboratory and numerical modeling of geochemical reactions in a reservoir used for CO2 storage. Procedia Eng 3391–3398

  • Spycher N, Pruess K (2005) CO2-H2O mixtures in the geological sequestration of CO2. II. Partitioning in chloride brines at 12–100 °C and up to 600 bar. Geochim Cosmochim Acta 69(13):3309–3320

    Article  Google Scholar 

  • Ueda A, Kato K, Ohsumi T, Yajima T, Ito H, Kaieda H, Metcalfe R, Takase H (2005) Experimental studies of CO2-rock interaction at elevated temperatures under hydrothermal conditions. Geochem J 39:417–425

    Article  Google Scholar 

  • Wan YY (2012) Migration and transformation of CO2 in CO2 geological sequestration process of Shiqianfeng saline aquifers in Ordos Basin. PhD thesis in Jilin University, China (in Chinese)

  • Wang DQ, Liu ZZ, Yin LH (2005) Hydrogeological characteristics and groundwater systems of the Ordos Basin. Chin Quater Sci 25(1):6–14 (in Chinese)

    Google Scholar 

  • Wang YX, Mao XM, DePaolo D (2011) Nanoscale fluid-rock interaction in CO2 geological storage. Earth Sci J China U Geosci 36(1):171–263 (in Chinese)

    Google Scholar 

  • White S, Weir G, Kissling W (2001) Numerical simulation of CO2 sequestration in natural CO2 reservoirs on the Colorado Plateau. In: Proceedings of the first national conference on carbon sequestration, May 2001, Washington DC, USA  

  • Wigand M, Carey JW, Schütt H, Spangenberg E, Erzinger J (2008) Geochemical effects of CO2 sequestration in sandstones under simulated in situ conditions of deep saline aquifers. Appl Geochem 23:2735–2745

    Article  Google Scholar 

  • Xiao XM, Zhao BQ, Thu ZL, Song ZG, Wilkins RWT (2005) Upper Palaeozoic petroleum system, Ordos Basin, China. Mar Pet Geol 22:945–963

    Article  Google Scholar 

  • Xu TF, Apps JA, Pruess K (2001) Analysis of mineral trapping for CO2 disposal in deep aquifers. In: Lawrence Berkeley National Laboratory Report LBNL–49023, Berkeley, CA, USA

  • Xu TF, Apps JA, Pruess K (2005) Mineral sequestration of carbon dioxide in a sandstone-shale system. Chem Geol 217:295–318

  • Xu TF, Sonnenthal E, Spycher N, Pruess K (2006) TOUGHREACT—a simulation program for non-isothermal multiphase reactive geochemical transport in variably saturated geologic media: applications to geothermal injectivity and CO2 geological sequestration. Comput Geosci 32:145–165

    Article  Google Scholar 

  • Xue CJ, Xue W, Kang M, Tu QJ, Yang YY (2008) The fluid dynamic processes and its uranium mineralization of sandstone-type in Ordos basin, China. Earth Sci J China U Geosci 22(1):1–8 (in Chinese)

    Google Scholar 

  • Xue CJ, Chi GX, Xue W (2011) Effects of hydrocarbon generation on fluid flow in the Ordos Basin and its relationship to uranium mineralization. Front Earth Sci 2(3):439–447 (in Chinese)

    Google Scholar 

  • Yang YH, Nan JX, He J, Wang XF (2001) The microscopic characteristic of the sandstone reservoir of upper Paleozoic of Ordos basin and the affected factors of reservoir property. Chin Petro Explo 6(4):37–43 (in Chinese)

    Google Scholar 

  • Yang H, Fu ST, Wie XS (2004) Geology and exploration of oil and gas in the Ordos Basin. J Appl Geophys 1(2):103–109

    Article  Google Scholar 

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Acknowledgments

The work presented in this paper was funded by the Chinese Ministry of Science and Technology (Grant 2012DFA60760) in joint co-operation with the German Research Foundation (DFG) and the National Natural Science Foundation of China (NSFC) (Grant GZ573). We also want to show our special appreciation to the China Scholarship Council (CSC) for the financial support. We would like to express our gratitude to the Institute of Rock and Soil Mechanics in Wuhan, the Chinese Academy of Sciences and the China Shenhua Group Co. LTD for their basic data support. We would also like to show our gratitude to Professor Tianfu Xu from Jilin University for his invaluable time to guide the use of TOUGHREACT simulator.

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Authors and Affiliations

  1. Energie-Forschungszentrum Niedersachsen, Clausthal University of Technology (TUC), Am Stollen 19A, 38640, Goslar, Germany

    Hejuan Liu, Zhengmeng Hou, Patrick Were & Yang Gou

  2. Institute of Petroleum Engineering, Clausthal University of Technology, Agricola str. 10, 38678, Clausthal-Zellerfeld, Germany

    Zhengmeng Hou

  3. Sino-German Energy Research Center, Sichuan University, Chengdu, 610065, China

    Zhengmeng Hou, Yang Gou & Lun Xiong

  4. College of Mining Technology, Taiyuan University of Technology, Taiyuan, 030000, China

    Xiaoling Sun

  5. Ordos Vocational College, Ordos, 017000, China

    Xiaoling Sun

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  1. Hejuan Liu
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  2. Zhengmeng Hou
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  4. Yang Gou
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Correspondence to Hejuan Liu.

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Liu, H., Hou, Z., Were, P. et al. Modelling CO2-brine-rock interactions in the Upper Paleozoic formations of Ordos Basin used for CO2 sequestration. Environ Earth Sci 73, 2205–2222 (2015). https://doi.org/10.1007/s12665-014-3571-4

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