Multiphase Reactive Flow During CO<sub>2</sub> Storage in Sandstone

Rukuan Chai; Qianqian Ma; Sepideh Goodarzi; Foo Yoong Yow; Branko Bijeljic; Martin J. Blunt

doi:10.1016/j.eng.2025.01.016

PDF(5185 KB)

Engineering ›› 2025, Vol. 48 ›› Issue (5) : 81-91. DOI: 10.1016/j.eng.2025.01.016

Research

Article

Multiphase Reactive Flow During CO₂ Storage in Sandstone

Author information +

History +

Abstract

Geological CO₂ storage is a promising strategy for reducing greenhouse gas emissions; however, its underlying multiphase reactive flow mechanisms remain poorly understood. We conducted steady-state imbibition relative permeability experiments on sandstone from a proposed storage site, complemented by in situ X-ray imaging and ex situ analyses using scanning electron microscopy (SEM) and energy-dispersive X-ray spectroscopy (EDS). Despite our use of a brine that was pre-equilibrated with CO₂, there was a significant reduction in both CO₂ relative permeability and absolute permeability during multiphase flow due to chemical reactions. This reduction was driven by decreased pore and throat sizes, diminished connectivity, and increased irregularity of pore and throat shapes, as revealed by in situ pore-scale imaging. Mineral dissolution, primarily of feldspar, albite, and calcite, along with precipitation resulting from feldspar-to-kaolinite transformation and fines migration, were identified as contributing factors through SEM–EDS analysis. This work provides a benchmark for storage in mineralogically complex sandstones, for which the impact of chemical reactions on multiphase flow properties has been measured.

Keywords

Geological CO₂ storage / Multiphase reactive flow / Geochemical reactions / Reduced CO₂ relative permeability

Cite this article

EndNote

Ris (Procite)

Bibtex

Download citation ▾

Rukuan Chai, Qianqian Ma, Sepideh Goodarzi, Foo Yoong Yow, Branko Bijeljic, Martin J. Blunt. Multiphase Reactive Flow During CO₂ Storage in Sandstone. Engineering, 2025, 48(5): 81‒91 https://doi.org/10.1016/j.eng.2025.01.016

References

Publishing order | Descend order by publishing year | Descend order by cited within

[1]	Luderer G, Vrontisi Z, Bertram C, Edelenbosch OY, Pietzcker RC, Rogelj J, et al.Residual fossil CO₂ emissions in 1.5–2 °C pathways.Nat Clim Chang 2018; 8(7):626-633.

[2]	Climate change 2021: the physical science basis. Contribution of working group I to the Sixth Assessment Report of the IPCC. Report. Cambridge: Cambridge University Press; 2021.

[3]	Griscom BW, Adams J, Ellis PW, Houghton RA, Lomax G, Miteva DA, et al.Natural climate solutions.Proc Natl Acad Sci USA 2017; 114(44):11645-11650.

[4]	Liu Y, Hu T, Rui Z, Zhang Z, Du K, Yang T, et al.An integrated framework for geothermal energy storage with CO₂ sequestration and utilization.Engineering 2023; 30:121-130.

[5]	He Y, Liu Y, Li J, Fan P, Liu X, Chai R, et al.Experimental study on the effect of CO₂ dynamic sequestration on sandstone pore structure and physical properties.Fuel 2024; 375:132622.

[6]	Cui G, Ren S, Rui Z, Ezekiel J, Zhang L, Wang H.The influence of complicated fluid–rock interactions on the geothermal exploitation in the CO₂ plume geothermal system.Appl Energy 2018; 227:49-63.

[7]	Luhmann AJ, Kong XZ, Tutolo BM, Ding K, Saar MO, Seyfried WE Jr.Permeability reduction produced by grain reorganization and accumulation of exsolved CO₂ during geologic carbon sequestration: a new CO₂ trapping mechanism.Environ Sci Technol 2013; 47(1):242-251.

[8]	Ma J, Querci L, Hattendorf B, Saar MO, Kong XZ.Toward a spatiotemporal understanding of dolomite dissolution in sandstone by CO₂-enriched brine circulation.Environ Sci Technol 2019; 53(21):12458-12466.

[9]	Blunt MJ.Multiphase flow in permeable media: a pore-scale perspective.Report. Cambridge: CambridgeUniversity Press; 2017.

[10]	Shiraki R, Dunn TL.Experimental study on water–rock interactions during CO₂ flooding in the Tensleep Formation, Wyoming, USA.Appl Geochem 2000; 15(3):265-279.

[11]	Wang W, Yan Z, Chen D, He Y, Liang Z, Li Y, et al.The mechanism of mineral dissolution and its impact on pore evolution of CO₂ flooding in tight sandstone: a case study from the Chang 7 member of the Triassic Yanchang Formation in the Ordos Basin.China. Geoenergy Sci Eng 2024; 235:212715.

[12]	Tang Y, Lv C, Wang R, Cui M.Mineral dissolution and mobilization during CO₂ injection into the water-flooded layer of the Pucheng Oilfield.China. J Nat Gas Sci Eng 2016; 33:1364-1373.

[13]	Othman F, Yu M, Kamali F, Hussain F.Fines migration during supercritical CO₂ injection in sandstone.J Nat Gas Sci Eng 2018; 56:344-357.

[14]	De GD Silva, Ranjith P, Perera M, Dai Z, Yang S.An experimental evaluation of unique CO₂ flow behaviour in loosely held fine particles rich sandstone under deep reservoir conditions and influencing factors.Energy 2017; 119:121-137.

[15]	Ochi J, Vernoux JF.Permeability decrease in sandstone reservoirs by fluid injection: hydrodynamic and chemical effects.J Hydrol 1998; 208(3–4):237-248.

[16]	Dávila G, Dalton L, Crandall DM, Garing C, Werth CJ, Druhan JL.Reactive alteration of a Mt. Simon Sandstone due to CO₂–rich brine displacement.Geochim Cosmochim Acta 2020; 271:227-247.

[17]	Lamy-Chappuis B, Angus D, Fisher Q, Grattoni C, Yardley BWD.Rapid porosity and permeability changes of calcareous sandstone due to CO₂–enriched brine injection.Geophys Res Lett 2014; 41(2):399-406.

[18]	Zou Y, Li S, Ma X, Zhang S, Li N, Chen M.Effects of CO₂–brine–rock interaction on porosity/permeability and mechanical properties during supercritical-CO₂ fracturing in shale reservoirs.J Nat Gas Sci Eng 2018; 49:157-168.

[19]	Tang Y, Hu S, He Y, Wang Y, Wan X, Cui S, et al.Experiment on CO₂–brine–rock interaction during CO₂ injection and storage in gas reservoirs with aquifer.Chem Eng J 2021; 413:127567.

[20]	Sun Y, Dai C, Yu Z, Xin Y.The carbonic acid–rock reaction in feldspar/dolomite-rich tightsand and its impact on CO₂–water relative permeability during geological carbon storage.Chem Geol 2021; 584:120527.

[21]	Gholami R, Raza A.CO₂ sequestration in sandstone reservoirs: how does reactive flow alter trapping mechanisms?.Fuel 2022; 324:124781.

[22]	Sayegh SG, Krause FF, Girard M, DeBree C.Rock/fluid interactions of carbonated brines in a sandstone reservoir: Pembina Cardium, Alberta.Canada. SPE Form Eval 1990; 5(4):399-405.

[23]	Al-Yaseri A, Zhang Y, Ghasemiziarani M, Sarmadivaleh M, Lebedev M, Roshan H, et al.Permeability evolution in sandstone due to CO₂ injection.Energy Fuels 2017; 31(11):12390-12398.

[24]	Ge J, Zhang X, Othman F, Wang Y, Roshan H, Le-Hussain F.Effect of fines migration and mineral reactions on CO₂–water drainage relative permeability.Int J Greenh Gas Control 2020; 103:103184.

[25]	Kou Z, Wang H, Alvarado V, Nye C, Bagdonas DA, McLaughlin JF, et al.Effects of carbonic acid–rock interactions on CO₂/brine multiphase flow properties in the upper minnelusa sandstones.SPE J 2023; 28(02):754-767.

[26]	Liu L, Suto Y, Bignall G, Yamasaki N, Hashida T.CO₂ injection to granite and sandstone in experimental rock/hot water systems.Energy Convers Manage 2003; 44(9):1399-1410.

[27]	Kaszuba JP, Janecky DR, Snow MG.Carbon dioxide reaction processes in a model brine aquifer at 200 °C and 200 bars: implications for geologic sequestration of carbon.Appl Geochem 2003; 18(7):1065-1080.

[28]	Ilgen AG, Aman M, Espinoza DN, Rodriguez MA, Griego J, Dewers TA, et al.Shale–brine–CO₂ interactions and the long-term stability of carbonate-rich shale caprock.Int J Greenh Gas Control 2018; 78:244-253.

[29]	Fu Q, Lu P, Konishi H, Dilmore R, Xu H, Seyfried W Jr, et al.Coupled alkali-feldspar dissolution and secondary mineral precipitation in batch systems: 1. New experiments at 200 °C and 300 bars.Chem Geol 2009; 258(3–4):125-135.

[30]	Lu P, Fu Q, Seyfried WE Jr, Hedges SW, Soong Y, Jones K, et al.Coupled alkali feldspar dissolution and secondary mineral precipitation in batch systems 2: New experiments with supercritical CO₂ and implications for carbon sequestration.Appl Geochem 2013; 30:75-90.

[31]	Dawson G, Pearce J, Biddle D, Golding S.Experimental mineral dissolution in Berea Sandstone reacted with CO₂ or SO₂–CO₂ in NaCl brine under CO₂ sequestration conditions.Chem Geol 2015; 399:87-97.

[32]	Pearce JK, Dawson GKW, Blach TP, Bahadur J, Melnichenko YB, Golding SD.Impure CO₂ reaction of feldspar, clay, and organic matter rich caprocks: decreases in the fraction of accessible mesopores measured by SANS.Int J Coal Geol 2018; 185:79-90.

[33]	Pearce J, Dawson G, Golab A, Knuefing L, Sommacal S, Rudolph V, et al.A combined geochemical and μCT study on the CO₂ reactivity of Surat Basin reservoir and cap-rock cores: porosity changes, mineral dissolution and fines migration.Int J Greenh Gas Control 2019; 80:10-24.

[34]	Carroll SA, McNab WW, Dai Z, Torres SC.Reactivity of Mount Simon sandstone and the Eau Claire shale under CO₂ storage conditions.Environ Sci Technol 2013; 47(1):252-261.

[35]	Fuchs SJ, Espinoza DN, Lopano CL, Akono AT, Werth CJ.Geochemical and geomechanical alteration of siliciclastic reservoir rock by supercritical CO₂–saturated brine formed during geological carbon sequestration.Int J Greenh Gas Control 2019; 88:251-260.

[36]	Lin Q, Bijeljic B, Raeini AQ, Rieke H, Blunt MJ.Drainage capillary pressure distribution and fluid displacement in a heterogeneous laminated sandstone.Geophys Res Lett 2021; 48:e2021GL093604.

[37]	Fenghour A, Wakeham WA, Vesovic V.The viscosity of carbon dioxide.J Phys Chem Ref Data 1998; 27(1):31-44.

[38]	Abdulagatov IM, Zeinalova AB, Azizov ND.Viscosity of aqueous electrolyte solutions at high temperatures and high pressures. Viscosity B-coefficient. Sodium iodide.J Chem Eng Data 2006; 51(5):1645-1659.

[39]	Chalbaud C, Robin M, Lombard JM, Martin F, Egermann P, Bertin H.Interfacial tension measurements and wettability evaluation for geological CO₂ storage.Adv Water Resour 2009; 32(1):98-109.

[40]	Gao Y, Raeini AQ, Selem AM, Bondino I, Blunt MJ, Bijeljic B.Pore-scale imaging with measurement of relative permeability and capillary pressure on the same reservoir sandstone sample under water-wet and mixed-wet conditions.Adv Water Resour 2020; 146:103786.

[41]	Alhammadi AM, Gao Y, Akai T, Blunt MJ, Bijeljic B.Pore-scale X-ray imaging with measurement of relative permeability, capillary pressure and oil recovery in a mixed-wet micro-porous carbonate reservoir rock.Fuel 2020; 268:117018.

[42]	Krevor SCM, Pini R, Zuo L, Benson SM.Relative permeability and trapping of CO₂ and water in sandstone rocks at reservoir conditions.Water Resour Res 2012; 48(2):W02532.

[43]	Gao Y, Lin Q, Bijeljic B, Blunt MJ.Pore-scale dynamics and the multiphase Darcy law.Phys Rev Fluids 2020; 5(1):013801.

[44]	Raeini AQ, Bijeljic B, Blunt MJ.Generalized network modeling: network extraction as a coarse-scale discretization of the void space of porous media.Phys Rev E 2017; 96(1):013312.

[45]	AlRatrout A, Blunt MJ, Bijeljic B.Wettability in complex porous materials, the mixed-wet state, and its relationship to surface roughness.Proc Natl Acad Sci USA 2018; 115(36):8901-8906.

[46]	Foroughi S, Bijeljic B, Lin Q, Raeini AQ, Blunt MJ.Pore-by-pore modeling, analysis, and prediction of two-phase flow in mixed-wet rocks.Phys Rev E 2020; 102(2):023302.

[47]	Pettijohn FJ, Potter PE, Siever R.Sand and Sandstone.Springer Science &Business Media, Berlin (2012)

[48]	Chai R, Liu Y, Xue L, Rui Z, Zhao R, Wang J.Formation damage of sandstone geothermal reservoirs: during decreased salinity water injection.Appl Energy 2022; 322:119465.

[49]	Jeong GS, Lee J, Ki S, Huh DG, Park CH.Effects of viscosity ratio, interfacial tension and flow rate on hysteric relative permeability of CO₂/brine systems.Energy 2017; 133:62-69.

[50]	Akbarabadi M, Piri M.Relative permeability hysteresis and capillary trapping characteristics of supercritical CO₂/brine systems: an experimental study at reservoir conditions.Adv Water Resour 2013; 52:190-206.

[51]	Ruprecht C, Pini R, Falta R, Benson S, Murdoch L.Hysteretic trapping and relative permeability of CO₂ in sandstone at reservoir conditions.Int J Greenh Gas Control 2014; 27:15-27.

[52]	Abdoulghafour H, Sarmadivaleh M, Hauge LP, Fern Mø, Iglauer S.Capillary pressure characteristics of CO₂–brine–sandstone systems.Int J Greenh Gas Control 2020; 94:102876.

[53]	Meng S, Liu C, Liu Y, Rui Z, Liu H, Jin X, et al.CO₂ utilization and sequestration in organic-rich shale from the nanoscale perspective.Appl Energy 2024; 361:122907.

[54]	Alhosani A, Lin Q, Scanziani A, Andrews E, Zhang K, Bijeljic B, et al.Pore-scale characterization of carbon dioxide storage at immiscible and near-miscible conditions in altered-wettability reservoir rocks.Int J Greenh Gas Control 2021; 105:103232.

[55]	Blunt MJ, Lin Q, Akai T, Bijeljic B.A thermodynamically consistent characterization of wettability in porous media using high-resolution imaging.J Colloid Interface Sci 2019; 552:59-65.

[56]	Punase A, Prakoso A, Hascakir B.Effect of clay minerals on asphaltene deposition in reservoir rock: insights from experimental investigations.Fuel 2023; 351:128835.

[57]	Wang X, Yang H, Huang Y, Liang Q, Liu J, Ye D.Evolution of CO2 storage mechanisms in low-permeability tight sandstone reservoirs.Engineering. In press.