Environmental Earth Sciences

, Volume 68, Issue 7, pp 1835–1848 | Cite as

The effect of heterogeneity of diffusion parameters on chloride transport in low-permeability argillites

Original Article

Abstract

Understanding flow and transport in low-permeability media is very important in the context of nuclear waste disposal, oil and gas reservoirs and long term evolution of groundwater systems. In low-permeability media, transport by diffusion is often the most important mass transport process. This study investigates the effect of the heterogeneity of diffusion parameters on mass transport in low-permeability media. A geostatistical approach for integrating heterogeneity of diffusion parameters in groundwater flow and transport models is proposed and applied to the Toarcian argillites in France which are studied in the framework of feasibility of storing radioactive waste in deep clayey massifs. Stochastic fields of the diffusion parameters of the Toarcian argillites (France) are generated based on 64 measured values of diffusion coefficient and diffusion accessible porosity and used as input for a 3D local-scale groundwater flow and transport model. The chloride concentrations computed by these heterogeneous models are compared to the measured chloride concentrations and to concentrations calculated with a model in which the Toarcian argillites are subdivided into several homogeneous zones. The heterogeneous simulations result in a slightly better correspondence between measured and calculated values and have the additional advantage that the measured diffusion coefficient values in the Toarcian are perfectly honored in the model. This study shows that small-scale variability of diffusion parameters has a significant effect on solute concentrations and omitting this heterogeneity may be a problem in transport calculations in low-permeability media, depending on the specific setting and objectives of the study.

Keywords

Diffusion Geostatistics Nuclear waste disposal Chloride transport Heterogeneity Porosity 

Notes

Acknowledgments

The authors wish to acknowledge the Fund for Scientific Research—Flanders for providing a Postdoctoral Fellowship to the first author. The authors thank IRSN for providing the necessary data for this study.

References

  1. Acero P, Auque LF, Gimeno MJ, Gomez JB (2010) Evaluation of mineral precipitation potential in a spent nuclear fuel repository. Environ Earth Sci 59(8):1613–1628CrossRefGoogle Scholar
  2. Ball WP, Liu C, Xia G, Young DF (1997) A diffusion-based interpretation of tetrachloroethene and trichloroethene concentration profiles in a groundwater aquitard. Water Resour Res 33:2741–2757CrossRefGoogle Scholar
  3. Barnwart S, Wikberg P, Olsson O (1997) A testbed for underground nuclear repository design. Environ Sci Technol 31:510–514CrossRefGoogle Scholar
  4. Barone FS, Rowe RK, Quigley RM (1992) A laboratory estimation of diffusion and adsorption coefficients for several volatile organics in a natural clayey soil. J Contam Hydrolol 10:225–250CrossRefGoogle Scholar
  5. Boisson J-Y, Cabrera J, De Windt L (1998) Fluid flow through faults and fractures in argillaceous formations. In: OECD proceedings. Joint NEA/EC workshop on fluid flow through faults and fractures in argillaceous formations, Bern, Switzerland, 10–12 June 1996, pp 207–222Google Scholar
  6. Boisson J-Y, Bertrand L, Heitz J-F, Moureau-Le Golvan Y (2001) In situ and laboratory investigations of fluid flow through an argillaceous formation at different scales of space and time, Tournemire tunnel, southern France. Hydrogeol J 9:108–123CrossRefGoogle Scholar
  7. Bonin B (1998) Deep geological disposal in argillaceous formations: studies at the Tournemire test site. J Contam Hydrolol 35:315–330CrossRefGoogle Scholar
  8. Bradbury KR, Eaton TT, Gotkowitz MB, Hart DJ, Cherry JA, Parker BL, Borchardt MA (2006) Contaminant transport through aquitards: technical guidance for aquitard assessment. AWWA Research Foundation, DenverGoogle Scholar
  9. Bredehoeft JD, England AW, Stewart DV, Trask NJ, Winograd IJ (1978) Geologic disposal of high-level radioactive wastes - Earth science perspectives. US Geol Surv Circ 779:1–15Google Scholar
  10. Bredehoeft JD, Neuzil CE, Milly PCD (1983) Regional flow in the Dakota Aquifer: a study of the role of confining layers. US Geol Surv Water Supply Pap 2237:1–45Google Scholar
  11. Cherry JA, Parker BL, Bradbury KR, Eaton TT, Gotkowitz MB, Hart DJ, Borchardt MA (2006) Contaminant transport through aquitards: a state of the science review. AWWA Research Foundation, DenverGoogle Scholar
  12. Crooks VE, Quigley RM (1984) Saline leachate migration through clay: a comparative laboratory and field investigation. Can Geotech J 21:349–362CrossRefGoogle Scholar
  13. Desaulniers DE, Cherry JA, Fritz P (1981) Origin, age and movement of pore water in argillaceous quaternary deposits at four sites in southwestern Ontario. J Hydrol 50:231–257CrossRefGoogle Scholar
  14. Desaulniers DE, Kaufman RS, Cherry JA, Bentley HW (1986) 37Cl–35Cl variations in a diffusion-controlled groundwater system. Geochimica Cosmochimica Acta 50:1757–1764CrossRefGoogle Scholar
  15. Deutsch CV, Journel AG (1998) GSLIB geostatistical software library and user’s guide. Oxford University Press, New YorkGoogle Scholar
  16. Goodall DC, Quigley RM (1977) Pollutant migration from two sanitary landfill sites near Sarnia, Ontario. Can Geotech J 14:223–236CrossRefGoogle Scholar
  17. Horseman ST, Higgo JJW, Alexander J, Harrington JF (1996) Water, gas and solute movement through argillaceous media. Nuclear Energy Agency, Organisation for Economic Co-operation and Development, ParisGoogle Scholar
  18. Hummel W, Schneider JW (2005) Safety of nuclear waste repositories. Chimia 59(12):909–915CrossRefGoogle Scholar
  19. Huysmans M, Dassargues A (2005) Review of the use of Péclet numbers to determine the relative importance of advection and diffusion in low permeability environments. Hydrogeol J 13(5–6):895–904CrossRefGoogle Scholar
  20. Huysmans M, Dassargues A (2006) Stochastic analysis of the effect of spatial variability of diffusion parameters on radionuclide transport in a low permeability clay layer. Hydrogeol J 14(7):1094–1106CrossRefGoogle Scholar
  21. Huysmans M, Dassargues A (2007) Equivalent diffusion coefficient and equivalent diffusion accessible porosity of a stratified porous medium. Transp Porous Media 66(3):421–438CrossRefGoogle Scholar
  22. Isaaks EH, Srivastava RM (1989) An introduction to applied geostatistics. Oxford University Press, New YorkGoogle Scholar
  23. Johnson RL, Cherry JA, Pankow JF (1989) Diffusive contaminant transport in natural clay: a field example and implications for clay-lined waste disposal sites. Environ Sci Technol 23:340–349CrossRefGoogle Scholar
  24. Larrondo P, Deutsch CV (2004) Accounting for geological boundary uncertainty for simulation of multiple rock types. In: Proceedings of Geostats2004, the seventh international geostatistics congress, September 26–October 1, 2004, Banff, CanadaGoogle Scholar
  25. Mallants D, Marivoet J, Sillen X (2001) Performance assessment of the disposal of vitrified high-level waste in a clay layer. J Nucl Mater 298(1–2):125–135CrossRefGoogle Scholar
  26. Mazurek M, Alt-Epping P, Bath A, Gimmi T, Waber HN, Buschaert S, De Cannière P, De Craen M, Gautschi A, Savoye S, Vinsot A, Wemaere I, Wouters L (2011) Natural tracer profiles across argillaceous formations. Appl Geochem 26:1035–1064CrossRefGoogle Scholar
  27. Neuman SP, Witherspoon PA (1972) Field determination of hydraulic properties of leaky multiple aquifer systems. Water Resour Res 8(5):1284–1298CrossRefGoogle Scholar
  28. Neuzil CE (1986) Groundwater flow in low-permeability environments. Water Resour Res 22:1163–1195CrossRefGoogle Scholar
  29. Oz B, Deutsch CV, Tran TT, Xie Y (2003) DSSIM-HR: a FORTRAN 90 program for direct sequential simulation with histogram reproduction. Comput Geosci 29(1):39–51CrossRefGoogle Scholar
  30. Patriarche D, Michelet J-L, Ledoux E, Savoye S (2004a) Diffusion as the main process for mass transport in very low water content argillites: 1. Chloride as a natural tracer for mass transport—diffusion coefficient and concentration measurements in interstitial water. Water Resour Res 40(1):W01517. doi:10.1029/2003WR002700 Google Scholar
  31. Patriarche D, Ledoux E, Michelet J-L, Simon-Coinçon R, Savoye S (2004b) Diffusion as the main process for mass transport in very low water content argillites: 2. Fluid flow and mass transport modelling. Water Resour Res 40(1):W01516. doi:10.1029/2003WR002600 Google Scholar
  32. Remenda VH, van der Kamp G, Cherry JA (1996) Use of vertical profiles of d18O to constrain estimates of hydraulic conductivity in a thick, unfractured aquitard. Water Resour Res 32:2979–2987CrossRefGoogle Scholar
  33. Ringwood AE (1985) Disposal of high-level nuclear wastes—a geological perspective. Miner Mag 49(351):159–176CrossRefGoogle Scholar
  34. Schwartz M (2009) Modelling groundwater contamination above the Asse 2 medium-level nuclear waste repository, Germany. Environ Earth Sci 59(2):277–286CrossRefGoogle Scholar
  35. Shackelford CD, Daniel DE (1991) Diffusion in saturated soil. I: background. J Geotech Eng 117:467–484CrossRefGoogle Scholar
  36. Therrien R, Sudicky EA (1996) Three-dimensional analysis of variably-saturated flow and solute transport in discretely-fractured porous media. J Contam Hydrol 23(1–2):1–44CrossRefGoogle Scholar
  37. Therrien R, Sudicky EA, McLaren RG (2003) FRAC3DVS: an efficient simulator for three-dimensional, saturated-unsaturated groundwater flow and density dependent, chain-decay solute transport in porous, discretely-fractured porous or dual-porosity formations. User’s guideGoogle Scholar

Copyright information

© Springer-Verlag 2012

Authors and Affiliations

  1. 1.Applied Geology and Mineralogy, Department of Earth and Environmental SciencesKatholieke Universiteit LeuvenHeverleeBelgium
  2. 2.Hydrogeology and Environmental Geology, Department of Architecture, Geology, Environment, and Civil Engineering (ArGEnCo)Université de LiègeLiègeBelgium

Personalised recommendations