Sodium diffusion in heterogeneous porous media: Connecting laboratory experiments and simulations
Abstract
Sodium has been suggested as a tracer for brine in reservoir formations where a significant amount of sodium ion is found mainly in the aqueous phase. Fortunately, the most abundant sodium isotope, 23Na, is Nuclear Magnetic Resonance (NMR) active, making it possible to study the structure and dynamical properties of both bulk and pore confined fluid systems. We investigated the diffusion of key dissolved sodium species in bulk solution and porous media as a function of composition, ionic strength, and permeability of the carbonate samples using NMR relaxometry and pulsed-field gradient (PFG) NMR techniques. We use Indiana limestone as an example of natural porous media and water as a freely diffusible tracer and carrier. We demonstrate apparent diffusion measurement of sodium based on changes in spin–spin relaxation time (T2) signal in pore confinement. The diffusion rate of sodium decreases with increasing counter-ion size. This effect is greater at higher ionic strengths and lower chemical potentials in porous media. The reactive transport code, CrunchFlow, was used to complement the NMR experiments to simulate diffusion behavior in porous media. Combining these two methods provides a powerful approach to estimating effective diffusion coefficients in heterogeneous matrices. The modeling considers the influence of physicalmore »
- Authors:
-
- The Ohio State Univ., Columbus, OH (United States)
- Peking Univ., Beijing (China)
- Publication Date:
- Research Org.:
- The Ohio State Univ., Columbus, OH (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1903218
- Alternate Identifier(s):
- OSTI ID: 1960663
- Grant/Contract Number:
- SC0006878
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Geochimica et Cosmochimica Acta
- Additional Journal Information:
- Journal Volume: 338; Journal ID: ISSN 0016-7037
- Publisher:
- Elsevier; The Geochemical Society; The Meteoritical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 58 GEOSCIENCES; diffusion; solute transport; sodium; Indiana limestone; porous media; NMR; Crunchflow
Citation Formats
Hwang, Bohyun, Srivastava, Deepansh J., Deng, Hang, Grandinetti, Philip J., and Cole, David R. Sodium diffusion in heterogeneous porous media: Connecting laboratory experiments and simulations. United States: N. p., 2022.
Web. doi:10.1016/j.gca.2022.09.028.
Hwang, Bohyun, Srivastava, Deepansh J., Deng, Hang, Grandinetti, Philip J., & Cole, David R. Sodium diffusion in heterogeneous porous media: Connecting laboratory experiments and simulations. United States. https://doi.org/10.1016/j.gca.2022.09.028
Hwang, Bohyun, Srivastava, Deepansh J., Deng, Hang, Grandinetti, Philip J., and Cole, David R. Wed .
"Sodium diffusion in heterogeneous porous media: Connecting laboratory experiments and simulations". United States. https://doi.org/10.1016/j.gca.2022.09.028. https://www.osti.gov/servlets/purl/1903218.
@article{osti_1903218,
title = {Sodium diffusion in heterogeneous porous media: Connecting laboratory experiments and simulations},
author = {Hwang, Bohyun and Srivastava, Deepansh J. and Deng, Hang and Grandinetti, Philip J. and Cole, David R.},
abstractNote = {Sodium has been suggested as a tracer for brine in reservoir formations where a significant amount of sodium ion is found mainly in the aqueous phase. Fortunately, the most abundant sodium isotope, 23Na, is Nuclear Magnetic Resonance (NMR) active, making it possible to study the structure and dynamical properties of both bulk and pore confined fluid systems. We investigated the diffusion of key dissolved sodium species in bulk solution and porous media as a function of composition, ionic strength, and permeability of the carbonate samples using NMR relaxometry and pulsed-field gradient (PFG) NMR techniques. We use Indiana limestone as an example of natural porous media and water as a freely diffusible tracer and carrier. We demonstrate apparent diffusion measurement of sodium based on changes in spin–spin relaxation time (T2) signal in pore confinement. The diffusion rate of sodium decreases with increasing counter-ion size. This effect is greater at higher ionic strengths and lower chemical potentials in porous media. The reactive transport code, CrunchFlow, was used to complement the NMR experiments to simulate diffusion behavior in porous media. Combining these two methods provides a powerful approach to estimating effective diffusion coefficients in heterogeneous matrices. The modeling considers the influence of physical properties (porosity and tortuosity) and chemical properties (geochemical composition and chemical gradients). The results presented in this work highlight the advantage of measuring apparent diffusivity using NMR T2 relaxometry in conjunction with numerical simulation to derive effective diffusivity and the corresponding matrix properties (i.e., tortuosity) of the system.},
doi = {10.1016/j.gca.2022.09.028},
journal = {Geochimica et Cosmochimica Acta},
number = ,
volume = 338,
place = {United States},
year = {Wed Sep 28 00:00:00 EDT 2022},
month = {Wed Sep 28 00:00:00 EDT 2022}
}
Works referenced in this record:
Estimating geological CO2 storage security to deliver on climate mitigation
journal, June 2018
- Alcalde, Juan; Flude, Stephanie; Wilkinson, Mark
- Nature Communications, Vol. 9, Issue 1
Determination of the leachability of solids
journal, April 1978
- Anders, O. U.; Bartel, J. F.; Altschuler, S. J.
- Analytical Chemistry, Vol. 50, Issue 4
Characterization and Analysis of Porosity and Pore Structures
journal, January 2015
- Anovitz, Lawrence M.; Cole, David R.
- Reviews in Mineralogy and Geochemistry, Vol. 80, Issue 1
The Electrical Resistivity Log as an Aid in Determining Some Reservoir Characteristics
journal, December 1942
- Archie, G. E.
- Transactions of the AIME, Vol. 146, Issue 01
CO2 Sequestration in Deep Sedimentary Formations
journal, October 2008
- Benson, S. M.; Cole, D. R.
- Elements, Vol. 4, Issue 5
Diffusion of sea water ions—I. Diffusion of sea water into a dilute solution
journal, December 1972
- Ben-Yaakov, S.
- Geochimica et Cosmochimica Acta, Vol. 36, Issue 12
Thermoddem: A geochemical database focused on low temperature water/rock interactions and waste materials
journal, October 2012
- Blanc, Ph.; Lassin, A.; Piantone, P.
- Applied Geochemistry, Vol. 27, Issue 10
Tracer diffusion coefficients in sedimentary rocks: correlation to porosity and hydraulic conductivity
journal, December 2001
- Boving, Thomas B.; Grathwohl, Peter
- Journal of Contaminant Hydrology, Vol. 53, Issue 1-2
Importance of classical diffusion in NMR studies of water in biological cells
journal, June 1979
- Brownstein, K. R.; Tarr, C. E.
- Physical Review A, Vol. 19, Issue 6
Comparative study of the kinetics and mechanisms of dissolution of carbonate minerals
journal, December 1989
- Chou, Lei; Garrels, Robert M.; Wollast, Roland
- Chemical Geology, Vol. 78, Issue 3-4
Diffusion of dissolved CO2 in caprock
journal, February 2009
- Fleury, Marc; Berne, Philippe; Bachaud, Pierre
- Energy Procedia, Vol. 1, Issue 1
Simulating Donnan equilibria based on the Nernst-Planck equation
journal, July 2018
- Gimmi, Thomas; Alt-Epping, Peter
- Geochimica et Cosmochimica Acta, Vol. 232
Effective Gradients in Porous Media Due to Susceptibility Differences
journal, April 1998
- Hürlimann, Martin D.
- Journal of Magnetic Resonance, Vol. 131, Issue 2
Effects of sorption competition on caesium diffusion through compacted argillaceous rock
journal, May 2009
- Jakob, Andreas; Pfingsten, Wilfried; Van Loon, Luc
- Geochimica et Cosmochimica Acta, Vol. 73, Issue 9
Diffusion in Nanoporous Materials: Novel Insights by Combining MAS and PFG NMR
journal, September 2018
- Kärger, Jörg; Freude, Dieter; Haase, Jürgen
- Processes, Vol. 6, Issue 9
Tables of the dynamic and kinematic viscosity of aqueous NaCl solutions in the temperature range 20–150 °C and the pressure range 0.1–35 MPa
journal, January 1981
- Kestin, Joseph; Khalifa, H. Ezzat; Correia, Robert J.
- Journal of Physical and Chemical Reference Data, Vol. 10, Issue 1
Self-Diffusion and Viscosity in Electrolyte Solutions
journal, September 2012
- Kim, Jun Soo; Wu, Zhe; Morrow, Andrew R.
- The Journal of Physical Chemistry B, Vol. 116, Issue 39
NMR and computational molecular modeling studies of mineral surfaces and interlayer galleries: A review
journal, July 2015
- Kirkpatrick, R. James; Kalinichev, Andrey G.; Bowers, Geoffrey M.
- American Mineralogist, Vol. 100, Issue 7
Carbonate and Bicarbonate Ion Transport in Alkaline Anion Exchange Membranes
journal, January 2013
- Kiss, Andrew M.; Myles, Timothy D.; Grew, Kyle N.
- Journal of The Electrochemical Society, Vol. 160, Issue 9
The impact of reactive surface area on brine-rock-carbon dioxide reactions in CO2 sequestration
journal, January 2017
- Kweon, Hyukmin; Deo, Milind
- Fuel, Vol. 188
Can sodium NMR provide more than a tracer for brine in petrophysics?
journal, October 2016
- Mitchell, Jonathan
- Journal of Petroleum Science and Engineering, Vol. 146
Sodium-23 NMR in porous media
journal, October 2018
- Mitchell, Jonathan; Fordham, Edmund J.
- Microporous and Mesoporous Materials, Vol. 269
Multicomponent Ionic Transport Modeling in Physically and Electrostatically Heterogeneous Porous Media With PhreeqcRM Coupling for Geochemical Reactions
journal, December 2019
- Muniruzzaman, Muhammad; Rolle, Massimo
- Water Resources Research, Vol. 55, Issue 12
New experimental observations of the behavior of sodium ions in saturated rock samples
journal, May 2019
- Nimerovsky, Evgeny
- Journal of Magnetic Resonance, Vol. 302
Fluid Behavior in Nanoporous Silica
journal, August 2020
- Ok, Salim; Hwang, Bohyun; Liu, Tingting
- Frontiers in Chemistry, Vol. 8
Benchmarks for multicomponent diffusion and electrochemical migration
journal, May 2015
- Rasouli, Pejman; Steefel, Carl I.; Mayer, K. Ulrich
- Computational Geosciences, Vol. 19, Issue 3
Sodium NMR relaxation in porous materials
journal, March 2004
- Rijniers, L. A.; Magusin, P. C. M. M.; Huinink, H. P.
- Journal of Magnetic Resonance, Vol. 167, Issue 1
Statistical learning of NMR tensors from 2D isotropic/anisotropic correlation nuclear magnetic resonance spectra
journal, October 2020
- Srivastava, Deepansh J.; Grandinetti, Philip J.
- The Journal of Chemical Physics, Vol. 153, Issue 13
Reactive transport codes for subsurface environmental simulation
journal, September 2014
- Steefel, C. I.; Appelo, C. A. J.; Arora, B.
- Computational Geosciences, Vol. 19, Issue 3
Spin Diffusion Measurements: Spin Echoes in the Presence of a Time‐Dependent Field Gradient
journal, January 1965
- Stejskal, E. O.; Tanner, J. E.
- The Journal of Chemical Physics, Vol. 42, Issue 1
Relationship between mineralogy and porosity in seals relevant to geologic CO2 sequestration
journal, June 2014
- Swift, Alexander M.; Anovitz, Lawrence M.; Sheets, Julia M.
- Environmental Geosciences, Vol. 21, Issue 2
Compaction, dilatancy, and failure in porous carbonate rocks: COMPACTION POROUS CARBONATE ROCKS
journal, May 2004
- Vajdova, Veronika; Baud, Patrick; Wong, Teng-fong
- Journal of Geophysical Research: Solid Earth, Vol. 109, Issue B5
A modified version of Archie’s law to estimate effective diffusion coefficients of radionuclides in argillaceous rocks and its application in safety analysis studies
journal, August 2015
- Van Loon, Luc R.; Mibus, Jens
- Applied Geochemistry, Vol. 59
Effect of confining pressure on the diffusion of HTO, 36Cl− and 125I− in a layered argillaceous rock (Opalinus Clay): diffusion perpendicular to the fabric
journal, October 2003
- Van Loon, L. R.; Soler, J. M.; Jakob, A.
- Applied Geochemistry, Vol. 18, Issue 10
Origins of concentration gradients for diffusiophoresis
journal, January 2016
- Velegol, Darrell; Garg, Astha; Guha, Rajarshi
- Soft Matter, Vol. 12, Issue 21
Effect of Ions on the Self-diffusion and Structure of Water in Aqueous Electrolytic Solutions
journal, September 1954
- Wang, Jui H.
- The Journal of Physical Chemistry, Vol. 58, Issue 9
Characterizing porous media with NMR methods
journal, November 1997
- Watson, A. Ted; Chang, C. T. Philip
- Progress in Nuclear Magnetic Resonance Spectroscopy, Vol. 31, Issue 4
NMR relaxation of spin-3/2 nuclei: Effects of structure, order, and dynamics in aqueous heterogeneous systems
journal, January 2001
- Woessner, Donald E.
- Concepts in Magnetic Resonance, Vol. 13, Issue 5
23 Na and 1 H NMR Relaxometry of Shale at High Magnetic Field
journal, May 2016
- Yang, Donghan; Kausik, Ravinath
- Energy & Fuels, Vol. 30, Issue 6
Internal Domains of Natural Porous Media Revealed: Critical Locations for Transport, Storage, and Chemical Reaction
journal, February 2016
- Zachara, John; Brantley, Sue; Chorover, Jon
- Environmental Science & Technology, Vol. 50, Issue 6
Salinity and crop yield
journal, September 2018
- Zörb, C.; Geilfus, C. ‐M.; Dietz, K. ‐J.
- Plant Biology, Vol. 21, Issue S1