Development of aminopolycarboxylate chelants (APCs) having enhanced biodegradability is gaining increasing focus to replace the EDTA and its homologs with those used widely for the ex situ treatment of contaminated soils and are potential eco-threats. The paper reports the chelant-assisted extraction of the toxic metals (Cd, Cu, Pb, and Zn) from the metal-spiked European reference soils (Eurosoil 1 and Eurosoil 4) using biodegradable APCs, namely EDDS, GLDA, and HIDS. The effects of chelant-to-metal molar ratio, solution pH, and metal/chelant stability constants were evaluated, and compared with that of EDTA. The selectivity aptitude of the biodegradable chelants towards the toxic metals was assumed from the speciation calculations, and a proportionate correlation was observed at neutral pH. Pre- and post-extractive solid phase distributions of the target metals were defined using the sequential extraction procedure and dissolution of metals from the theoretically immobilized fraction was witnessed. The effect of competing species (Al, Ca, Fe, Mg, and Mn) concentrations was proven to be minimized with an excess of chelant in solution. The highlight of the outcomes is the superior decontamination ability of GLDA, a biodegradable APC, at minimum chelant concentration in solution and applicability at a wide range of pH environments.
This is a preview of subscription content, log in to check access.
Buy single article
Instant access to the full article PDF.
Price includes VAT for USA
Subscribe to journal
Immediate online access to all issues from 2019. Subscription will auto renew annually.
This is the net price. Taxes to be calculated in checkout.
Abollino, O., Giacomino, A., Malandrino, M., Mentasti, E., Aceto, M., & Barberis, R. (2006). Assessment of metal availability in a contaminated soil by sequential extraction. Water, Air, and Soil Pollution, 173, 315–338.
Abumaizar, R., & Khan, L. I. (1996). Laboratory investigation of heavy metal removal by soil washing. Journal of the Air & Waste Management Association, 46, 765–768.
Abumaizar, R. J., & Smith, E. H. (1999). Heavy metal contaminants removal by soil washing. Journal of Hazardous Materials, 70, 71–86.
Alderighi, L., Gans, P., Ienco, A., Peters, D., Sabatini, A., & Vacca, A. (1999). Hyperquad simulation and speciation (HySS): a utility program for the investigation of equilibria involving soluble and partially soluble species. Coordination Chemistry Reviews, 184, 311–318.
Arwidsson, Z., Elgh-Dalgren, K., von Kronhelm, T., Sjöberg, R., Allard, B., & van Hees, P. (2010a). Remediation of heavy metal contaminated soil washing residues with amino polycarboxylic acids. Journal of Hazardous Materials, 173, 697–704.
Arwidsson, Z., Johansson, E., von Kronhelm, T., Allard, B., & van Hees, P. (2010b). Remediation of metal contaminated soil by organic metabolites from fungi. I—Production of organic acids. Water, Air, and Soil Pollution, 205, 215–226.
Barona, A., Aranguiz, I., & Elías, A. (2001). Metal associations in soils before and after EDTA extractive decontamination: implications for the effectiveness of further clean-up procedures. Environmental Pollution, 113, 79–85.
Begum, Z. A., Rahman, I. M. M., Sawai, H., Tate, Y., Maki, T., Hasegawa, H. (2012a). Stability constants of Fe(III) and Cr(III) complexes with dl-2-(2-carboxymethyl)nitrilotriacetic acid (GLDA) and 3-hydroxy-2,2′-iminodisuccinic acid (HIDS) in aqueous solution. Journal of Chemical & Engineering Data, 57, 2723–2732.
Begum, Z. A., Rahman, I. M. M., Tate, Y., Egawa, Y., Maki, T., Hasegawa, H. (2012b). Formation and stability of binary complexes of divalent ecotoxic ions (Ni, Cu, Zn, Cd, Pb) with biodegradable aminopolycarboxylate chelants (DL-2-(2-carboxymethyl)nitrilotriacetic acid, GLDA, and 3-hydroxy-2,2′-iminodisuccinic acid, HIDS) in aqueous solutions. Journal of Solution Chemistry, doi:10.1007/s10953-012-9901-9.
Begum, Z. A., Rahman, I. M. M., Tate, Y., Sawai, H., Maki, T., & Hasegawa, H. (2012). Remediation of toxic metal contaminated soil by washing with biodegradable aminopolycarboxylate chelants. Chemosphere, 87, 1161–1170.
Bricka, R. M., Williford, C. W., & Jones, L. W. (1993). Technology assessment of currently available and developmental technique for heavy metals-contaminated soils treatment (technical report IRRP-93-4). Vicksburg: U.S. Army Corps of Engineers, Waterways Experiment Station.
Dahlin, C. L., Williamson, C. A., Keith Collins, W., & Dahlin, D. C. (2002). Sequential extraction versus comprehensive characterization of heavy metal species in Brownfield soils. Environmental Forensics, 3, 191–201.
Davidge, J., Thomas, C. P., & Williams, D. R. (2001). Conditional formation constants or chemical speciation data? Chemical Speciation and Bioavailability, 13, 129–134.
Davis, A. P., & Singh, I. (1995). Washing of zinc(II) from contaminated soil column. Journal of Environmental Engineering-ASCE, 121, 174–185.
Dermont, G., Bergeron, M., Mercier, G., & Richer-Laflèche, M. (2008a). Metal-contaminated soils: remediation practices and treatment technologies. Practice Periodical of Hazardous, Toxic, and Radioactive Waste Management, 12, 188–209.
Dermont, G., Bergeron, M., Mercier, G., & Richer-Laflèche, M. (2008b). Soil washing for metal removal: a review of physical/chemical technologies and field applications. Journal of Hazardous Materials, 152, 1–31.
Dermont, G., Bergeron, M., Richer-Laflèche, M., & Mercier, G. (2010). Remediation of metal-contaminated urban soil using flotation technique. Science of the Total Environment, 408, 1199–1211.
Ebina, Y., Okada, S., Hamazaki, S., Ogino, F., Li, J. L., & Midorikawa, O. (1986). Nephrotoxicity and renal cell carcinoma after use of iron- and aluminum-nitrilotriacetate complexes in rats. Journal of the National Cancer Institute, 76, 107–113.
Elliott, H. A., & Brown, G. A. (1989). Comparative evaluation of NTA and EDTA for extractive decontamination of Pb-polluted soils. Water, Air, and Soil Pollution, 45, 361–369.
Evanko, C. R., & Dzombak, D. A. (1997). Remediation of metals-contaminated soils and groundwater (TE-97-01). Pittsburgh: Ground-Water Remediation Technologies Analysis Center (GWRTAC).
Fischer, K., & Bipp, H. P. (2002). Removal of heavy metals from soil components and soils by natural chelating agents. Part II. Soil extraction by sugar acids. Water, Air, and Soil Pollution, 138, 271–288.
Gawlik, B. M., Lamberty, A., Muntau, H., & Pauwels, J. (2001a). EUROSOILS—a set of CRMs for comparability of soil-measurements. Fresenius’ Journal of Analytical Chemistry, 370, 220–223.
Gawlik, B. M., Lamberty, A., Pauwels, J., & Muntau, H. (2001b). Certification of soil-pH (suspensions of water and CaCl 2 ) and adsorption coefficients for atrazine, 2,4-D and lindane in six different reference soils (EUROSOILS): IRMM-443. Luxembourg: Directorate-General for Research, European Commission.
Griffiths, R. A. (1995). Soil-washing technology and practice. Journal of Hazardous Materials, 40, 175–189.
Hasegawa, H., Rahman, I. M. M., Kinoshita, S., Maki, T., & Furusho, Y. (2010). Non-destructive separation of metal ions from wastewater containing excess aminopolycarboxylate chelant in solution with an ion-selective immobilized macrocyclic material. Chemosphere, 79, 193–198.
Hasegawa, H., Rahman, I. M. M., Nakano, M., Begum, Z. A., Egawa, Y., Maki, T., Furusho, Y., & Mizutani, S. (2011). Recovery of toxic metal ions from washing effluent containing excess aminopolycarboxylate chelant in solution. Water Research, 45, 4844–4854.
Hauser, L., Tandy, S., Schulin, R., & Nowack, B. (2005). Column extraction of heavy metals from soils using the biodegradable chelating agent EDDS. Environmental Science & Technology, 39, 6819–6824.
Hong, J., & Pintauro, P. N. (1996). Desorption–complexation–dissolution characteristics of adsorbed cadmium from kaolin by chelators. Water, Air, and Soil Pollution, 86, 35–50.
Horn, R., Taubner, H., Wuttke, M., & Baumgartl, T. (1994). Soil physical properties related to soil structure. Soil and Tillage Research, 30, 187–216.
IUSS Working Group WRB. (2007). World reference base for soil resources 2006, first update 2007. World soil resources reports no. 103. Rome: The Food and Agriculture Organization (FAO).
Jiang, W., Tao, T., & Liao, Z. (2011). Removal of heavy metal from contaminated soil with chelating agents. Open Journal of Soil Science, 1, 70–76.
Kim, C., & Ong, S.-K. (1999). Recycling of lead-contaminated EDTA wastewater. Journal of Hazardous Materials, 69, 273–286.
Kumpiene, J., Lagerkvist, A., & Maurice, C. (2008). Stabilization of As, Cr, Cu, Pb and Zn in soil using amendments—a review. Waste Management, 28, 215–225.
Leštan, D., Luo, C. L., & Li, X. D. (2008). The use of chelating agents in the remediation of metal-contaminated soils: a review. Environmental Pollution, 153, 3–13.
Li, X., Coles, B. J., Ramsey, M. H., & Thornton, I. (1995). Chemical partitioning of the new National Institute of Standards and Technology standard reference materials (SRM 2709-2711) by sequential extraction using inductively coupled plasma atomic emission spectrometry. Analyst, 120, 1415–1419.
Lim, T. T., Tay, J. H., & Wang, J. Y. (2004). Chelating-agent-enhanced heavy metal extraction from a contaminated acidic soil. Journal of Environmental Engineering-ASCE, 130, 59–66.
Löser, C., Zehnsdorf, A., Hoffmann, P., & Seidel, H. (2007). Remediation of heavy metal polluted sediment by suspension and solid-bed leaching: estimate of metal removal efficiency. Chemosphere, 66, 1699–1705.
Maiz, I., Arambarri, I., Garcia, R., & Millán, E. (2000). Evaluation of heavy metal availability in polluted soils by two sequential extraction procedures using factor analysis. Environmental Pollution, 110, 3–9.
Martell, A. E., & Hancock, R. D. (1996). Metal complexes in aqueous solutions. New York: Plenum Press.
Martell, A. E., Smith, R. M., & Motekaitis, R. J. (2004). NIST standard reference database 46: NIST critically selected stability constants of metal complexes database (version 8.0 for windows). College Station: Texas A&M University.
Mulligan, C. N., & Wang, S. (2006). Remediation of a heavy metal-contaminated soil by a rhamnolipid foam. Engineering Geology, 85, 75–81.
Mulligan, C. N., Yong, R. N., & Gibbs, B. F. (2001). Remediation technologies for metal-contaminated soils and groundwater: an evaluation. Engineering Geology, 60, 193–207.
Nowack, B. (2002). Environmental chemistry of aminopolycarboxylate chelating agents. Environmental Science & Technology, 36, 4009–4016.
Nowack, B. (2008). Chelating agents and the environment. Environmental Pollution, 153, 1–2.
Orama, M., Hyvonen, H., Saarinen, H., Aksela, R. (2002). Complexation of [S,S] and mixed stereoisomers of N,N′-ethylenediaminedisuccinic acid (EDDS) with Fe(III), Cu(II), Zn(II) and Mn(II) ions in aqueous solution. Journal of the Chemical Society, Dalton Transactions, 1, 4644–4648.
Papassiopi, N., Tambouris, S., & Kontopoulos, A. (1999). Removal of heavy metals from calcareous contaminated soils by EDTA leaching. Water, Air, and Soil Pollution, 109, 1–15.
Peters, R. W. (1999). Chelant extraction of heavy metals from contaminated soils. Journal of Hazardous Materials, 66, 151–210.
Ph, Q. (2002). Operationally-defined extraction procedures for soil and sediment analysis. Part 3: new CRMs for trace-element extractable contents. TrAC-Trends in Analytical Chemistry, 21, 774–785.
Pichtel, J., & Pichtel, T. M. (1997). Comparison of solvents for ex situ removal of chromium and lead from contaminated soil. Environmental Engineering Science, 14, 97–104.
Pickering, W. F. (1986). Metal ion speciation—soils and sediments (a review). Ore Geology Reviews, 1, 83–146.
Polettini, A., Pomi, R., & Rolle, E. (2007). The effect of operating variables on chelant-assisted remediation of contaminated dredged sediment. Chemosphere, 66, 866–877.
Pueyo, M., Rauret, G., Bacon, J. R., Gomez, A., Muntau, H., Quevauviller, P. F., & Lopez-Sanchez, J. (2001). A new organic-rich soil reference material certified for its EDTA- and acetic acid-extractable contents of Cd, Cr, Cu, Ni, Pb and Zn, following collaboratively tested and harmonised procedures. Journal of Environmental Monitoring, 3, 238–242.
Rampley, C. G., & Ogden, K. L. (1998). Preliminary studies for removal of lead from surrogate and real soils using a water soluble chelator: adsorption and batch extraction. Environmental Science & Technology, 32, 987–993.
Rauret, G., Lopez-Sanchez, J. F., Bacon, J., Gomez, A., Muntau, H., & Quevauviller, P. (2001). Certification of the contents (mass fractions) of Cd, Cr, Cu, Ni, Pb and Zn in an organic-rich soil following harmonised EDTA and acetic acid extraction procedures: BCR-700. Luxembourg: Directorate-General for Research, European Commission.
Steele, M. C., & Pichtel, J. (1998). Ex-situ remediation of a metal-contaminated superfund soil using selective extractants. Journal of Environmental Engineering-ASCE, 124, 639–645.
Stumm, W. (1992). Chemistry of the solid water interface: processes at the mineral–water and particle–water interface in natural systems. New York: Wiley.
Sun, B., Zhao, F. J., Lombi, E., & McGrath, S. P. (2001). Leaching of heavy metals from contaminated soils using EDTA. Environmental Pollution, 113, 111–120.
Tandy, S., Bossart, K., Mueller, R., Ritschel, J., Hauser, L., Schulin, R., & Nowack, B. (2004). Extraction of heavy metals from soils using biodegradable chelating agents. Environmental Science & Technology, 38, 937–944.
Tessier, A., Campbell, P. G. C., & Bisson, M. (1979). Sequential extraction procedure for the speciation of particulate trace metals. Analytical Chemistry, 51, 844–851.
Vandevivere, P., Hammes, F., Verstraete, W., Feijtel, T., & Schowanek, D. (2001). Metal decontamination of soil, sediment, and sewage sludge by means of transition metal chelant [S, S]-EDDS. Journal of Environmental Engineering-ASCE, 127, 802–811.
Vangronsveld, J., Herzig, R., Weyens, N., Boulet, J., Adriaensen, K., Ruttens, A., Thewys, T., Vassilev, A., Meers, E., Nehnevajova, E., van der Lelie, D., & Mench, M. (2009). Phytoremediation of contaminated soils and groundwater: lessons from the field. Environmental Science and Pollution Research, 16, 765–794.
Virkutyte, J., Sillanpää, M., & Latostenmaa, P. (2002). Electrokinetic soil remediation—critical overview. Science of the Total Environment, 289, 97–121.
Wolf, C. A. D., Lepage, J. N., & Bemelaar, J. H. (2010). Acidic aqueous solution containing a chelating agent and the use thereof. USA: United States Patent Application Publication. Akzo Nobel N.V.
Zhang, T., Shan, X., & Li, F. (1998). Comparison of two sequential extraction procedures for speciation analysis of metals in soils and plant availability. Communications in Soil Science and Plant Analysis, 29, 1023–1034.
Zhang, L., Zhu, Z., Zhang, R., Zheng, C., Zhang, H., Qiu, Y., & Zhao, J. (2008). Extraction of copper from sewage sludge using biodegradable chelant EDDS. Journal of Environmental Sciences, 20, 970–974.
Zou, Z., Qiu, R., Zhang, W., Dong, H., Zhao, Z., Zhang, T., Wei, X., & Cai, X. (2009). The study of operating variables in soil washing with EDTA. Environmental Pollution, 157, 229–236.
This research was partially supported by the Grants-in-Aid for Scientific Research (24310056 and 24·02029) from the Japan Society for the Promotion of Science. Additionally, the authors (ZAB and IMMR) wish to thank Mr. Rauful Alam (Department of Organic Chemistry, Stockholm University, Sweden) for his generous support in collecting the literatures.
About this article
Cite this article
Begum, Z.A., Rahman, I.M.M., Sawai, H. et al. Effect of Extraction Variables on the Biodegradable Chelant-Assisted Removal of Toxic Metals from Artificially Contaminated European Reference Soils. Water Air Soil Pollut 224, 1381 (2013). https://doi.org/10.1007/s11270-012-1381-4
- Soil remediation
- Ex situ
- Aminopolycarboxylate chelants
- Chelant-to-metal molar ratio
- Metal/chelant stability constant
- Sequential extraction