Novel EDTA-Based Method of Washing Pb Contaminated Soils: Hazard Mitigation and Sustainable Soil Use (original) (raw)
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EDTA-Enhanced Washing for Remediation of Pb and/or Zn-Contaminated Soils
Journal of Environmental Engineering-asce, 2006
The effects of the operating conditions, the initial concentrations of heavy metals in soils, and the competition among heavy metals during ethylenediaminetetraacetic acid ͑EDTA͒-enhanced soil washing were extensively investigated using batch experiments with Pb-and/or Zn-contaminated soils aiming to determine the heavy-metal removal for different types of contaminations and to optimize the process parameters. Pb or Zn removal efficiency was found to be dependent on contact time, pH, concentrations of EDTA, and their initial concentrations in contaminated soils. The experimental results showed that the heavy-metal removal efficiency increased with a higher initial concentration of heavy metals in soils, and the concentrations of heavy metals in the solutions after washing were linearly correlated with their initial concentrations in soils. The study of the competition among heavy metals indicated that when EDTA was present in solution with the concentration less than the stoichiometric requirements, Pb removal efficiency was higher than that of Zn; on the other hand, when EDTA concentration was greater, Pb and Zn removal efficiencies were almost the same.
Sustainability, 2018
This paper presents the results of an experimental study aimed at investigating the applicability of ethylenediamine-N,N-disuccinic acid (EDDS) as a washing solution for the remediation of Pb-contaminated soil. All aspects of the treatment are analyzed and optimized, including the reuse and the final disposal of the EDDS spent solution. Different molar concentrations of the washing solutions and the efficiencies of varying solid/liquid ratio are tested at different pH values. More than 90% of the mobile Pb fraction is removed in about 24 h at pH 6. Accordingly, soil toxicity strongly decreases as a consequence of the treatment. The regenerated solution exhibits a reduced, but not negligible, extractive capacity. The total extraction of Pb is approximately 50% of the initial value after one regeneration cycle, and almost 20% after a second regeneration cycle. Respirometric tests, conducted using an activated sludge sampled in a municipal wastewater treatment plant, indicate that the spent solutions are not biodegradable, but they do not exert any toxic effect on the biomass. On the contrary, tests on regenerated solutions displayed the same biodegradability as the fresh ones.
Multi-step leaching of Pb and Zn contaminated soils with EDTA
Chemosphere, 2007
The efficiency of multi-step leaching of heavy metal contaminated soils was evaluated in a laboratory scale study. Four different soils contaminated with Pb (1136 ± 16-4424 ± 313 mg kg À1 ) and Zn (288 ± 5-5489 ± 471 mg kg À1 ) were obtained from industrial sites in the Mežica Valley, Slovenia and Príbram district, Czech Republic. Different dosages (2.5-40 mmol kg À1 ) of ethylenediamine tetraacetate (EDTA) were used to treat soils in 1-10 leaching steps. Higher EDTA dosages did not result in a proportional gain in Pb and Zn removal. EDTA extracted Pb more efficiently than Zn from three of four tested soils. The percentage of removed Zn did not exceed 75% regardless of the soil, EDTA dosage and leaching steps. Significantly more Pb (in three of four soils) and Zn were removed from soils when the same amount of EDTA was applied in several leaching steps. The interference of major soil cations Fe and Ca with EDTA complexation as a possible factor affecting Pb and Zn removal efficiency with multi-step heap leaching was examined and is discussed. The results of our study indicate that, for some soils, using multi-step leaching instead of the more traditionally used single dose EDTA treatment could improve heavy metal removal efficiency and thus the economics of soil remediation.
Remediation by means of EDTA of an agricultural calcareous soil polluted with Pb
Environmental Geochemistry and Health, 2020
The dispersion of mine tailings affects ecosystems due to their high content of potentially toxic elements. Environmental risk increases when the soil impacted by tailings is used for agriculture; this use may result in health impacts. This study analyzes the feasibility of remediating a calcareous soil (used for maize cultivation) polluted with lead in the semiarid zone of Zimapán, México, by using EDTA as an extractant. Total geoavailable and bioaccessible concentrations in the gastric and intestinal phases were determined to evaluate lead availability and health risk. The soil was then washed with EDTA, and the geochemical fractionation (interchangeable, carbonates, Fe/Mn oxy-hydroxides, organic matter-sulfides, and residual) and impact on the mesophile bacteria and fungi/yeast populations were analyzed. The results showed total Pb concentrations up to 647 ± 3.50 mg/ kg, a 46% bioaccessible fraction (297 ± 9.90 mg/kg) in the gastric phase and a 12.2% (80 ± 5 mg/kg) bioaccessible fraction in the intestinal phase, indicating a health and environmental risk. Meanwhile, the geochemical fractionation before washing showed a Pb fraction mainly consisting of Fe/Mn oxy-hydroxides (69.6%); this reducible fraction may progressively increase its bioaccessibility. Geochemical fractionation performed in the washed soil showed differences from that determined before the treatment; however, the iron and manganese fraction, at 42.4%, accounted for most of the Pb. The soil microbiology was also modified by EDTA, with an increase in aerobic bacteria and a decrease in fungi/yeast populations. Although 44% total lead removal was achieved, corresponding to a final concentration of 363.50 ± 43.50 mg/kg (below national and USEPA standards), washing with EDTA increased the soluble and interchangeable lead concentrations. Statistical analysis indicated a significant effect (p \ 0.05) of EDTA on the soil's geochemical fractionation of lead.
Chemosphere, 2019
The use of EDTA-based soil washing is prevented by chelant environmental persistence and the hazard of toxic post-remedial emissions. Calcareous and acidic soils with 828 and 673 mg Pb kg-1 , respectively, and co-contaminated with Zn and Cd, were washed with 90 and 60 mM EDTA, respectively, to remove 67 and 80% of Pb. Washed soils were rinsed until 6.5 and 5.1 mM EDTA, respectively, was measured in the final rinsing solutions. Emissions of residual EDTA and chelated metals from remediated soils were mitigated by adsorption on zero-valent Fe (ZVI), which was added (0.5-1.5%, w/w) to the slurry of washed soil immediately before rinsing. ZVI addition prevented the initial post-remedial surge of toxic metals leachability and minimised toxic emissions from calcareous and acidic soil as soon as 6 and 7 days after remediation, respectively. The extractability/leachability of EDTA and toxic metals from remediated and ZVI amended soils diminished to close to emissions from the original soils, frequently below the limit of quantification by flame-AAS, and was not affected by the pH of the leaching solutions. Efficient curbing of toxic post-remediation emissions as demonstrated herein is of paramount importance for recognition of EDTA-based remediation as environmentally safe.
Comparative evaluation of NTA and EDTA for extractive decontamination of Pb-polluted soils
Water, Air, and Soil Pollution, 1989
Nitrilotriacetic acid (NTA) and ethylenediaminetetraacetic acid (EDTA) were compared for their ability to solubilize Pb from a highly-contaminated (PbT=21%) soil collected from a battery recycling facility. For chelant concentrations below 0.04 M (representing a 1:1 chelant-to-Pb T molar ratio), EDTA released 10 to 30% more Pb than NTA. NTA-to-Pb. r ratios greater than 1:1 reduced Pb recovery because of readsorption of Pb(NTA)24-onto positively-charged oxide soil components at pH < 8.5. For the EDTA system, however, complexation completely bound all coordination sites of Pb and EDTA, leaving no functional groups available for surface adsorption. Thus, Pb recovery progressively increased with higher EDTA concentrations, although the additional Pb release with each EDTA increment became smaller. For pH < 5 and EDTA/Pb of 2:1, Pb recovery exceeded 90%. The addition of 0.5 M NaC104 enhanced Pb recovery by EDTA for pH 5 to 12, but substantially suppressed recovery by NTA for pH < 11. Because Pb release by NTA was diminished by high ionic strength and chelant-to-metal ratios, NTA may be limited as a soil washing reagent. Stronger complexation and consistent Pb desorption behavior by EDTA favors its use.
Electrochemical EDTA recycling after soil washing of Pb, Zn and Cd contaminated soil
Journal of Hazardous Materials, 2011
Recycling of chelant decreases the cost of EDTA-based soil washing. Current methods, however, are not effective when the spent soil washing solution contains more than one contaminating metal. In this study, we applied electrochemical treatment of the washing solution obtained after EDTA extraction of Pb, Zn and Cd contaminated soil. A sacrificial Al anode and stainless steel cathode in a conventional electrolytic cell at pH 10 efficiently removed Pb from the solution. The method efficiency, specific electricity and Al consumption were significantly higher for solutions with a higher initial metal concentration. Partial replacement of NaCl with KNO 3 as an electrolyte (aggressive Cl − are required to prevent passivisation of the Al anode) prevented EDTA degradation during the electrolysis. The addition of FeCl 3 to the acidified washing solution prior to electrolysis improved Zn removal. Using the novel method 98, 73 and 66% of Pb, Zn and Cd, respectively, were removed, while 88% of EDTA was preserved in the treated washing solution. The recycled EDTA retained 86, 84 and 85% of Pb, Zn and Cd extraction potential from contaminated soil, respectively.
Removal of Pb and MDF from contaminated soils by EDTA and SDS-enhanced washing
Chemosphere, 2007
Heavy metal- and organic-contaminated sites are ubiquitous, but few studies have been conducted to address such an issue. EDTA- and SDS-enhanced washing was studied for remediation of Pb- and/or marine diesel fuel (MDF)-contaminated soils. The feasibility of recovery and reuse of EDTA and SDS, as well as the physicochemical interactions among the chemical agents, contaminants and soils were extensively investigated using batch experiments. The optimal washing sequence was then determined. The experimental results showed that EDTA could be recovered and reused for four cycles without significant loss of its chelating capacity, while the extraction capability of SDS was noticeably reduced after each reuse cycle. The free phase of marine diesel fuel (MDF) in soils physically isolated the sorbed Pb on soils and thus reducing its extraction by EDTA. The presence of SDS alone or together with low concentration of EDTA was found to enhance Pb removal probably via electrostatic interaction and dissolution of soil organic matter. However, it hindered Pb extraction by high concentration of EDTA, because of the potential formation of complexes between some strongly-bound Pb and SDS, that are more resistant to desorption. Therefore, EDTA washing followed by SDS achieved the highest Pb removal efficiency. On the other hand, MDF removal by SDS was significantly hindered by coexisting Pb in soils, probably because the formation of Pb-dodecyl sulfate (DS) complex would decrease the effective amount of SDS available for forming micelles in solution and enhance MDF sorption. EDTA alone or together with SDS could enhance MDF removal, but the residual MDF after EDTA-washing became more resistant to SDS removal. Consequently, SDS washing followed by EDTA is considered as the optimal washing sequence for MDF removal.
Remediation of contaminated soil using soil washing-a review
Pb, Zn, Ni, Cu, Mn and Cd are heavy metals occur naturally as trace elements in many soils. The present paper reviews the remediation of heavy metals of contaminated soil by soil washing using different agents. It was noted that the contact time, pH, concentration of extract ant and agitation speed were affected the process while remediation, so accordingly select the conditions to obtain efficiency which is mainly depend upon the type of soil, contaminationtype, contamination period and metals present in it.EDTA is effective when compared with other chelating agents for heavy metals especially for lead but it has low biodegradation. Because of the nature of low biodegradability, EDTA can be reusedfurther by membrane separation and electrochemical treatment, or degraded by advanced oxidation processes.
Chemosphere, 2008
The feasibility of a novel two-phase method for remediation of Pb (1374 mg kg À1 ), Zn (1007 mg kg À1 ), and Cd (9.1 mg kg À1 ) contaminated soil was evaluated. In the first phase we used EDTA for leaching heavy metals from the soil. In the second phase we used an electrochemical advanced oxidation process (EAOP) for the treatment and reuse of washing solution for soil rinsing (removal of the soilretained, chelant-mobilized metallic species). In EAOP, a boron-doped diamond anode was used for the generation of hydroxyl radicals and oxidative decomposition of EDTA-metal complexes at a constant current density (15 mA cm À2 ). The released metals were removed from the solution by filtration as insoluble participate and by electro-deposition on the cathode. Four consecutive additions of 5.0 mmol kg À1 EDTA (total 20 mmol kg À1 ) removed 44% Pb, 14% Zn and 35% Cd from the soil. The mobility of the Pb, Zn and Cd (Toxicity Characteristic Leaching Procedure) left in the soil after remediation was reduced by 1.6, 3.4 and 1.5 times, respectively. The Pb oral availability (Physiologically Based Extraction Test) in the simulated stomach phase was reduced by 2.4 and in the intestinal phase by 1.7 times. The discharge solution was clear, almost colorless, with pH 7.73 and 0.47 mg L À1 Pb, 1.03 mg L À1 Zn, bellow the limits of quantification of Cd and 0.023 mM EDTA. The novel method enables soil leaching with small water requirements and no wastewater generation or other emissions into the environment.