Skip to main content
Log in

Measurement of CO2 diffusivity in synthetic and saline aquifer solutions at reservoir conditions: the role of ion interactions

  • Original
  • Published:
Heat and Mass Transfer Aims and scope Submit manuscript

Abstract

Storage and disposal of CO2 as the main component of greenhouse gases in saline aquifers require careful measurement of diffusivity for predicting rate of transfer and cumulative amount of trapped gas. Little information is available on diffusion of CO2 in highly concentrated saline aquifers at reservoir conditions. In this study, diffusivity of CO2 was measured into different solutions, including saline aquifer taken from oil field, distilled water and synthetic solutions prepared from four most common ions, Mg2+, Ca2+, K+, Na+. The roles of salvation effect and hydration phenomenon were studied on diffusivity of dissolved CO2. Synthetic solutions were prepared at concentration ranges of 83–200 g/l. Experimental measurements were reported at temperature and pressure ranges of 30–40 °C and 5,880–6,265 kPa, respectively. Results show that both type and concentration of ion affect CO2 diffusivity. Diffusion coefficient was found dependent on effective radius of hydrated ions. Also, CO2 diffusivity increase by increasing strength of bonds between ion and neighbor water molecules. Also, presence of ions in water solution creates hydration competition between solution metal ions and aqua ions from diffusive gas. The Mg2+ cation, which has strongest hydration competition among other ions, has an increasing effect on gas diffusivity into saline aquifer. However, increasing ion concentration in solution decreases diffusivity of CO2 due to growth in fraction of contact ion pairs. Results of this study provide unique measures of CO2 diffusion coefficient in saline aquifer at high pressure and temperature conditions and conceptual information about effect of each common saline formation ion on gas diffusivity.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Fig. 1
Fig. 2
Fig. 3
Fig. 4

Similar content being viewed by others

Abbreviations

C* :

Equilibrium concentration of CO2 in brine (kmol/m3)

D :

Diffusion coefficient (m2/s)

K h :

Henry’s law constant (kPa.m3/kg)

L :

Height of gas in diffusion cell (m)

m d :

Diffused gas into the saline aquifer (kg)

M :

Molecular mass of gas (kg/kmol)

N :

Normality

P :

Pressure (kPa)

R :

Universal gas constant

S :

Weight fraction of sodium chloride

t :

Time (s)

T :

Temperature (K or °C)

Z :

Compressibility factor

E :

Equilibrium value

I :

Initial value

References

  1. IPCC (2005) Special report on carbon dioxide capture and storage. In: Metz B, Davidson O, de Coninck HC, Loos M, Meyer LA (eds) Prepared by working group III of the intergovernmental panel on climate change. Cambridge University Press

  2. Huang T (2012) Molecular Dynamics Simulation of Carbon Dioxide in Aqueous Electrolyte Solution. Dissertation submitted in fulfillment of the Requirements for the Degree of Doctor of Philosophy, Swinburn University of Technology

  3. Mortimer RG (2008) Physical chemistry, 3rd edn. Academic Press, Waltham

    Google Scholar 

  4. Du H, Rasaiah JC, Miller JD (2007) Structural and dynamic properties of concentrated alkali halide solutions: a molecular dynamics simulation study. J Phys Chem B 111:209–217

    Article  Google Scholar 

  5. Nakajima H (2011) Dissolution trapping of carbon dioxide in reservoir formation brine—a carbon storage mechanism. Mass Transfer: Advanced Aspects. InTech

  6. Wang JH (1954) Effects of ions on the self-diffusion and structure of water in aqueous electrolytic solutions. Paper presented at the symposium on the solutions of electrolytes, New Haven, June 16

  7. Zeebe RE (2011) On the molecular diffusion coefficients of dissolved CO2, HCO3 , and CO3 and their dependence on isotopic mass. Geochem Cosmochim Acta 75:2483–2498

    Article  Google Scholar 

  8. Garcia-Ratés M, de Hemptinne JC, Avalos JB, Nieto-Draghi C (2012) Molecular modeling of diffusion coefficient and ionic conductivity of CO2 in aqueous ionic solutions. J Phys Chem B 116:2787–2800

    Article  Google Scholar 

  9. Tae Kwak H, Zhang G, Chen S (2005) The effects of salt type and salinity on formation water viscosity and NMR responses. Paper presented at the international symposium of the society of core analysts, Toronto, Canada, 21–25 August

  10. Unver AA, Himmelblau DM (1964) Diffusion coefficients of CO2, C2H4, C3H6, and C4H8 in water from 6 to 65 °C. J Chem Eng Data 9:428

    Article  Google Scholar 

  11. Thomas WJ, Adams MJ (1965) Measurement of the diffusion coefficient of carbon dioxide and nitrous oxide in water and aqueous solution of glycerol. Trans Faraday Soc 61:668

    Article  Google Scholar 

  12. Tamimi A, Rinker EB, Sandall OC (1994) Diffusion coefficients for hydrogen sulfide, carbon dioxide and nitrous oxide in water over the temperature range 293–368 K. J Chem Eng Data 39:330

    Article  Google Scholar 

  13. Frank MJW, Kuipers AMJ, van Swaaij WPM (1996) Diffusion coefficients and viscosities of CO2+H2O, CO2+CH3OH, NH3+H2O and NH3+CH3OH liquid mixtures. J Chem Eng Data 41:297

    Article  Google Scholar 

  14. Jähne B, Heinz G, Dietrich W (1987) Measurement of the diffusion coefficients of sparingly soluble gases in water. J Geophys Res 92:767

    Google Scholar 

  15. Hirai S, Okazaki K, Yazawa H, Ito H, Tabe Y, Hijikata K (1997) Measurement of CO2 diffusion coefficient and application of LIF in pressurized water. Energy 22:363–367

    Article  Google Scholar 

  16. Tewes F, Boury F (2005) Formation and rheological properties of the supercritical CO2–water pure interface. J Phys Chem B 109:3990

    Article  Google Scholar 

  17. Renner TA (1988) Measurement and correlation of diffusion coefficient for CO2 and rich-gas applications. J Chem Eng Data 3:517–523

    Google Scholar 

  18. Wang LS, Lang ZX, Guo TM (1996) Measurement and correlation of the diffusion coefficients of carbon dioxide in liquid hydrocarbons under elevated pressures. Fluid Phase Equilib 117:364–372

    Article  Google Scholar 

  19. Bahar M, Liu K (2008) Measurement of the Diffusion coefficient of CO2 in formation water under reservoir conditions: implications for CO2 storage. Paper presented at the SPE 116513, SPE Asia pacific oil and gas conference and exhibition, Perth, Australia, 20–22 October

  20. Yang C, Gu Y (2006) Accelerated mass transfer of CO2 in reservoir brine due to density-driven natural convection at high pressures and elevated temperatures. Ind Eng Chem Res 45(8):2430–2436

    Article  Google Scholar 

  21. Moghaddam RN, Rostami B, Pourafshary P, Fallahzadeh Y (2012) Quantification of density-driven natural convection for dissolution mechanism in CO2 sequestration. Transp Porous Media 92:439

    Article  Google Scholar 

  22. Azin R, Mahmoudy M, Jafari Raad SM, Osfouri S (2013) Measurement and modeling of CO2 diffusion coefficient in saline aquifer at reservoir conditions. Cent Eur J Eng 3:585–594

    Google Scholar 

  23. Sheikha H, Pooladi-Darvish M, Mehrotra AK (2005) Development of graphical methods for estimating the diffusivity coefficient of gases in bitumen from pressure-decay data. Energy Fuels 19:2041

    Article  Google Scholar 

  24. Duan Z, Sun R, Zhu C, Chou I (2006) An improved model for the calculation of CO2 solubility in aqueous solutions containing Na+, K+, Ca2+, Mg2+, Cl, and SO4 2−. Mar Chem 98:131–139

    Article  Google Scholar 

  25. Persson I (2010) Hydrated metal ions in aqueous solution: how regular are their structures? Pure Appl Chem 82(10):1901–1917

    Article  Google Scholar 

  26. Ohtaki H, Tamas R (1993) Structure and dynamics of hydrated ions. Chem Rev 93(3):1157–1204

    Article  Google Scholar 

  27. Richens DT (1997) The chemistry of aqua ions. Wiley, London

    Google Scholar 

  28. Burgess J (1978) Metal ions in solution. Ellis Horwood, Chichester

    Google Scholar 

  29. Köddermann T, Ludwig R, Paschek D (2008) On the validity of Stokes–Einstein and Stokes–Einstein–Debye relations in ionic liquids and Ionic–liquid mixtures. Chem Phys Chem 9(13):1851–1858. doi:10.1002/cphc.200800102

    Google Scholar 

Download references

Acknowledgments

The assistance of Messrs Mohammad Mahmoodi and Yasin Gholami in running part of experiments are acknowledged. Also, the authors acknowledge the National Elite Foundation and Persian Gulf University for financial support of this study under contract number 1389-19/1302.

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to Reza Azin.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Jafari Raad, S.M., Azin, R. & Osfouri, S. Measurement of CO2 diffusivity in synthetic and saline aquifer solutions at reservoir conditions: the role of ion interactions. Heat Mass Transfer 51, 1587–1595 (2015). https://doi.org/10.1007/s00231-015-1508-4

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s00231-015-1508-4

Keywords

Navigation