Environmental Modeling & Assessment

, Volume 13, Issue 1, pp 121–134 | Cite as

Soil heterogeneity effects on acid flushing of lead-contaminated soil

  • Kei Nakagawa
  • Shin-Ichiro Wada
  • Kazuro Momii
  • Ronny Berndtsson


A compact model for evaluation of acid flushing of heavy-metal-contaminated soil in a small-scale on-site treatment plant is proposed. The model assumes that the soil was re-packed in a container after excavation resulting in a soil structure with heterogeneous and random physical and chemical properties. To evaluate the effects of heterogeneity on the efficiency of contaminant removal by acid flushing, a numerical analysis of lead transport in the heterogeneous soil medium was performed. The model examines cation exchange and surface complexation reactions involving three cations (Ca, Pb, and H) and one anion (Cl) in both dissolved and exchangeable forms, two Pb surface complexes (SOPbCl and SOPbOH), and one Cl surface complex (SOH2Cl). The transport of these species during flushing with acid in a synthetically generated two-dimensional heterogeneous soil was simulated in the model. Results indicated that the flushing fluid preferentially followed pathways with large permeability. The heterogeneous cation exchange capacity (CEC) distribution and surface complexation sites had a significant effect on the transport of dissolved species. Because the CEC was set to a relatively low value, Pb was adsorbed mainly as surface complexes (SOPbCl and SOPbOH). Simulation results suggest that blocks of low hydraulic conductivity located in the upper part of the model domain greatly impede solute transport. Ponding conditions did not significantly affect the efficiency of decontamination. The model and its results are useful in the design of small-scale treatment plants for acid flushing.


lead-contaminated soil acid flushing numerical simulation cation exchange surface complexation 



This work was funded by Kyushu Industrial Technology Center. R. Berndtsson acknowledges support from the Swedish Research Council. We thank the editor and two anonymous reviewers for their helpful suggestions that improved clarity and quality of this paper.


  1. 1.
    Alshawabkeh, A. N., Bricka, R. M., & Gent, D. B. (2005). Pilot-scale electrokinetic clean of lead-contaminated soils. Journal of Geotechnical and Geoenvironmental Engineering, 131(3), 283–291.CrossRefGoogle Scholar
  2. 2.
    Appelo, C. A. J., & Postma, D. (1994). Geochemistry, groundwater and pollution. Rotterdam: A.A. Balkema.Google Scholar
  3. 3.
    Bain J. G., Mayer, K. U., Blowes, D. W., Frind, E. O., Molson, J. W. H., Kahnt, R., et al. (2001). Modelling the closure-related geochemical evolution of groundwater at a former uranium mine. Journal of Contaminant Hydrology, 52, 109–135.CrossRefGoogle Scholar
  4. 4.
    Bianchi, A., Petrangeli Papini, M., Corsi, A., Behra, P., & Beccari, M. (2003). Competitive transport of cadmium and lead through a natural porous medium: influence of the solid/liquid interface processes. Water Science and Technology, 48(3), 9–16.Google Scholar
  5. 5.
    Buruggenwert, M. G. M., & Kamphorst, A. (1979). Survey of experimental information on cation exchange in soil systems. In G. H. Boit (Eds.), Soil chemistry B. Physico-chemical models (pp. 141–203). Amsterdam: Elsevier.Google Scholar
  6. 6.
    Chiang, W. -H., & Kinzelbach, W. (2001). 3D-Groundwater modeling with PMWIN a simulation system for modeling groundwater flow and pollution. Berlin Heidelberg New York: Springer.Google Scholar
  7. 7.
    Christiansen J. S., Engesgaard, P., & Bjerg, P. L. (1998). A physically and chemically heterogeneous aquifer: field study and reactive transport modelling. In M. Herbert & K. Kovar (Eds.), Groundwater quality: Remediation and protection (pp. 329–336). IAHS Publ. 250.Google Scholar
  8. 8.
    Dagan, G. (1989). Flow and transport in porous formations. Berlin Heidelberg New York: Springer.Google Scholar
  9. 9.
    Dai, Z., Ritzi, R. W., Jr., Huang, C., Rubin, Y. N., & Dominic, D. F. (2004). Transport in heterogeneous sediments with multimodal conductivity and hierarchical organization across scales. Journal of Hydrology, 294, 68–86.CrossRefGoogle Scholar
  10. 10.
    Elfeki, A. M. M., Uffink, G. J. M., & Barends, F. B. J. (1997). Groundwater contaminant transport: Impact of heterogeneous characterisation: A new view on dispersion. Rotterdam: A. A. Balkema.Google Scholar
  11. 11.
    Engesgaard, P., & Traberg, R. (1996). Contaminant transport at a waste residue deposit: 2. Geochemical transport modeling. Water Resources Research, 32(4), 939–951.Google Scholar
  12. 12.
    Gelhar, L. W. (1993). Stochastic subsurface hydrology. New Jersey: Prentice-Hall.Google Scholar
  13. 13.
    Goldberg, S. (1992). Use of surface complexation models in soil chemical systems. Advances in Agronomy, 47, 233–329.Google Scholar
  14. 14.
    Harbaugh, A. W., Banta, E. R., Hill, M. C., & McDonald, M. G. (2000). MODFLOW-2000, The U.S. geological survey modular ground-water model-user guide to modularization concepts and ground-water flow process, U.S. Geological Survey Open-File Report 00-92.Google Scholar
  15. 15.
    Hill, M. C. (1990). Preconditioned conjugate-gradient 2 (PCG2), a computer program for solving ground-water flow equations, U.S. Geological Survey Water-Resources Investigations Report 90-4048.Google Scholar
  16. 16.
    Huyakorn, P. S., & Pinder, G. F. (1983). Computation method in subsurface flow. New York: Academic.Google Scholar
  17. 17.
    Lichtner, P. C. (1996). Continuum formulation of multicomponent–multiphase reactive transport. In P. C. Lichtner, C. I. Steefel, & E. H. Oelkers (Eds.), Reactive transport in porous media, (pp. 1–81), Reviews in Mineralogy, 34. Washington: Mineralogical Society of America.Google Scholar
  18. 18.
    Martin, T. A., & Rudy, M. V. (2004). Review of in situ remediation technology for lead, zinc, and cadmium in soil. Remediation Journal, 14(3), 35–53.CrossRefGoogle Scholar
  19. 19.
    Momii, K., Hiroshiro, Y., Jinno, K., & Berndtsson, R. (1997). Reactive solute transport with a variable selectivity coefficient in an undistributed soil column. Soil Science Society of America Journal, 61, 1539–1546.CrossRefGoogle Scholar
  20. 20.
    Mori Y., & Wada, S. -I. (2002). Acid extraction of cadmium from a smectitic paddy soil polluted with cadmium. Japanese Journal of Clay Science, 41, 196–201.Google Scholar
  21. 21.
    Nakagawa, K., Momii, K., & Berndtsson, R. (2005). Saltwater intrusion in coastal aquifer – comparison between the CIP and MOC simulation technique. Environmental Modeling and Assessment, 10(4), 323–329.CrossRefGoogle Scholar
  22. 22.
    Nakagawa, K., Wada, S.-I., & Momii, K. (2004). Multi-component reactive solute transport analysis in saturated soil based on CIP method and chemical equilibrium. Journal of Hydraulic, Coastal and Environmental Engineering, 761, 81–89.Google Scholar
  23. 23.
    Neuman, S. P. (1993). Eulerian–Lagrangian theory of transport in space–time nonstationary velocity fields: Exact nonlocal formalism by conditional moments and weak approximation. Water Resources Research, 29(3), 633–645.CrossRefGoogle Scholar
  24. 24.
    Parkhurst, D. L., Kipp, K. L., Engesgaard, P., & Charlton, S. R. (2004). PHAST – A program for simulating ground-water flow, solute transport, and multicomponent geochemical reactions, U.S. Geological Survey Techniques and Methods 6-A8.Google Scholar
  25. 25.
    Paschke, A., Wennrich, R., & Morgenstern, P. (1999). Comparison of 24 h and long-term pHstat leaching tests for heavy metal mobilization from solid matrices. Acta Hydrochimica et Hydrobiologica, 27(4), 223–229.CrossRefGoogle Scholar
  26. 26.
    Reddy, K. R., Chinthamreddy, S., & Al-Hamdan, A. (2001). Synergistic effect of multiple metal contaminants on electrokinetic remediation of soils. Remediation Journal, 11(3), 85–109.CrossRefGoogle Scholar
  27. 27.
    Rubin, Y., Cushey, M. A., & Wilson, A. (1997). The moments of the breakthrough curves of instantaneously and kinetically sorbing solutes in heterogeneous geologic media: Prediction and parameter inference from field measurements. Water Resources Research, 33(11), 2465–2481.CrossRefGoogle Scholar
  28. 28.
    Schäfer, W., & Kinzelbach, W. K. H. (1996). Transport of reactive species in heterogeneous porous media. Journal of Hydrology, 183, 151–168.CrossRefGoogle Scholar
  29. 29.
    Shaviv, A., & Mattigod, S. V. (1985). Cation exchange equilibria in soils expressed as cation–ligand complex formation. Soil Science Society of America Journal, 49, 569–573.CrossRefGoogle Scholar
  30. 30.
    Silliman, S. E. (1996). The importance of the third dimension on transport through saturated porous media: case study based on transport of particles. Journal of Hydrology, 179, 181–195.CrossRefGoogle Scholar
  31. 31.
    Steefel, C. I., & MacQuarrie, K. T. B. (1996). Approaches to modeling of reactive transport in porous media. In P. C. Lichtner, C. I. Steefel, & E. H. Oelkers (Eds.), Reactive transport in porous media, (pp. 83–129), Reviews in Mineralogy, 34. Washington: Mineralogical Society of America.Google Scholar
  32. 32.
    Steefel, C. I., & Yabusaki, S. B. (1996). OS3D/GIMRT, software for multicomponent–multidimensional reactive transport, user manual and programmer’s guide, PNL-11166, Pacific Northwest National Laboratory, Richland, Washington.Google Scholar
  33. 33.
    Takizawa, K., Yabe, T., Chino, M., Kawai, T., Wataji, K., Hoshino, H., et al. (2005). Simulation and experiment on swimming fish and skimmer by CIP method. Computers and Structures, 83, 397–408.CrossRefGoogle Scholar
  34. 34.
    U.S. Environmental Protection Agency (1997). Recent developments for in situ treatment of metal contaminated soils, EPA 542-R-97-004, Washington, DC.Google Scholar
  35. 35.
    Wada, S.-I., Nakagawa, K., Takagi, K., Okawa, K., & Arikawa, K. (2003). A numerical model for simulating acid-flushing of heavy metal polluted soils. Proceedings of the 38th Japan National Conference on Geotechnical Engineering, pp. 2313–2314.Google Scholar
  36. 36.
    Wildenschild, D., & Jensen, K. H. (1999). Laboratory investigations of effective flow behavior in unsaturated heterogeneous sands. Water Resources Research, 35(1), 17–27.CrossRefGoogle Scholar
  37. 37.
    Wildenschild, D., & Jensen, K. H. (1999). Numerical modeling of observed effective flow behavior in unsaturated heterogeneous sands. Water Resources Research, 35(1), 29–42.CrossRefGoogle Scholar
  38. 38.
    Wu, G., & Li, L. Y. (1998). Modeling of heavy metal migration in sand/ bentonite and the leachate pH effect. Journal of Contaminant Hydrology, 33, 313–336.CrossRefGoogle Scholar
  39. 39.
    Xu, T., Samper, J., Ayora, C., Manzano, M., & Custodio, E. (1999). Modeling of non-isothermal multi-component reactive transport in field scale porous media flow systems. Journal of Hydrology, 214, 144–164.CrossRefGoogle Scholar
  40. 40.
    Yabe, T., & Aoki, T. (1991). A universal solver for hyperbolic equations by cubic-polynomial interpolation I. One-dimensional solver. Computer Physics Communications, 66, 219–232.Google Scholar
  41. 41.
    Yabe, T., Ishikawa, T., Wang, P. Y., Aoki, T., Kadota, Y., & Ikeda, F. (1991). A universal solver for hyperbolic equations by cubic-polynomial interpolation II. Two- and three-dimensional solvers. Computer Physics Communications, 66, 233–242.Google Scholar
  42. 42.
    Yeh, G. T. & Tripathi, V. S. (1989). A critical evaluation of recent developments in hydrogeochemical transport models of reactive multichemical components. Water Resources Research, 25(1), 93–108.CrossRefGoogle Scholar
  43. 43.
    Yeh, G. T., & Tripathi, V. S. (1991). A model for simulating transport of reactive multispecies components: Model development and demonstration. Water Resources Research, 27(12), 3075–3094.CrossRefGoogle Scholar

Copyright information

© Springer Science+Business Media B.V. 2007

Authors and Affiliations

  • Kei Nakagawa
    • 1
  • Shin-Ichiro Wada
    • 2
  • Kazuro Momii
    • 1
  • Ronny Berndtsson
    • 3
  1. 1.Faculty of AgricultureKagoshima UniversityKagoshimaJapan
  2. 2.Faculty of AgricultureKyushu UniversityHigashikuJapan
  3. 3.Department of Water Resources EngineeringLund UniversityLundSweden

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