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Laboratory Experiment on Electrokinetic Remediation of Soil
Abstract
Electrokinetic remediation is a method of decontaminating soil containing heavy metals and polar organic contaminants by passing a direct current through the soil. An undergraduate chemistry laboratory is described to demonstrate electrokinetic remediation of soil contaminated with copper. A 30 cm electrokinetic cell with an applied voltage of 30 V is used to demonstrate the redistribution of copper in sand initially contaminated with 0.24 M copper chloride solution. The copper content in sand is measured by acid extraction followed by complexometric titration. The measurement of the pH across the cell is used to demonstrate the difference in mobility between the H+ and OH– ions during the electrokinetic process.
... Bessaim et al. 2020 [19] have successfully reduced the soil salinity with a rate of 100% from three sections from soil samples, by using a voltage gradient of 1.5 and 2.0 V cm −1 . Similar results have been demonstrated in other laboratory studies [19][20][21][22][23][24][25][26][27][28][29]. ...
Chemical spills are common at oil and gas facilities and traditionally remediation occurs by excavating and removing the contaminated soil, which is environmentally destructive and financially expensive. Electrokinetic (EK) remediation is an alternative method that can reduce the amount of soil that is removed and relies on the electromigration of ions towards the electrodes after a current is applied. We investigated whether EK remediation would affect soil electrical conductivity (EC), Na⁺, K⁺, Mg²⁺, Ca²⁺, Cl–, and SO42– concentrations at various soil depths. The study occurred at a decommissioned oil wellsite in northern Alberta, where processed water spills had occurred. The treatments included (1) one EK run + 100 kW power [Zones E and G], (2) one EK run + 300 kW power [Zones B and H], (3) two EK runs + 100 kW power [Zones C and F]. The treatments reduced EC within the top 2 m of the soil, which was associated with reductions in Na⁺ and Cl– in Zones BH and EG, and reductions in Mg²⁺ in Zones CF. Sulfates were elevated in the top 2 m in all treatments relative to the control. Higher EC values were observed in Zones BH (300 kW) relative to Zones EG (100 kW) at all depths. In addition, Zones CF (2 EK cycles) had higher EC than Zones EG (1 EK cycle). When initial concentrations are considered, increased power and duration may improve efficacy. EK technology can be a tool to remediate sites and potentially reduce the impacts on the environment.
Graphical abstract
... These reports included new instrumental techniques that allow the determination of levels of metals in soils and living organisms, 2−4 remediation strategies 5 that have been addressed using different complexing agents and surfactants, 6 adsorption processes using bioadsorbents to immobilize metals in soil, 7 phytoremediation, 8 and electro-kinetic techniques and separation methods, including flotation and other methods. 9,10 Copper is an essential nutrient for plants, and its concentration in natural soils is highly dependent on the parent material. The copper concentration is high in basic rocks (90−100 mg kg −1 ) and low in acidic rocks such as granite (10− 13 mg kg −1 ). ...
National legislation concerning soil pollution by heavy metals in different countries is mostly based on the total heavy metal concentration levels allowed in different soils. As soil pollution is an issue of worldwide concern, here we develop a laboratory exercise for students in which they must check the suitability of a total metal concentration for soil pollution assessment. Undertaking two different Cu extractions promotes student discussion about soil pollution by heavy metals: Cu extracted with EDTA and Cu extracted with DTPA. These two extractions are commonly used by the soil science community to estimate the potentially available Cu for plants, which is compared with information about total Cu that is provided to the students. The results of this laboratory exercise demonstrate that the total concentration of Cu in the soil is not suitable for decision-making about whether a soil is polluted. However, establishing reference values from EDTA and DTPA extractions or EDTA/Total and DTPA/Total ratios may result in better indicators to establish the possible environmental risks from the presence of Cu in soils with which to make critical decisions about soil remediation strategies.
The classroom exercise outlined here is a self-directed assignment that connects students to the environmental contamination problem surrounding the DePue Superfund site. By connecting chemistry knowledge gained in the classroom with a real-world problem, students are encouraged to personally connect with the problem while simultaneously developing skills in data management and interpretation. Designed for first-year undergraduate, general chemistry students, each of the four primary exercises builds upon the skills developed in those before it. This approach makes it easy to tailor this assignment to the needs of individual classrooms. This assignment was given as the first laboratory course assignment to a pilot group of 178 general chemistry undergraduate students at Northwestern University. Students enrolled in this course had already completed the first of two accelerated general chemistry courses. Over 75% of students scored in the 85% to 100% grade range, illustrating that the majority of students who completed this assignment demonstrated a high level of comprehension.Keywords: Interdisciplinary/Multidisciplinary; Environmental Chemistry; First-Year Undergraduate/General; Inquiry-Based/Discovery Learning; Internet/Web-Based Learning; Communication/Writing; Public Understanding/Outreach; Applications of Chemistry; Laboratory Instruction; Geochemistry
The feasibility of using electrokinetics to extract contaminants from soils has been established by bench-scale laboratory experiments and small-scale field tests. However, the physics and chemistry associated with the innovative remediation technology are not yet fully understood. Many physicochemical reactions occur simultaneously during the process. These reactions may enhance or reduce the cleanup efficiency of the process. They are particularly important in fine-grained soils because the large specific surface area of the soil provides numerous active sites for these reactions. In this paper, several prominent physicochemical soil-contaminant interactions during electrokinetic extraction and their influences on the cleanup efficiency of the technology are discussed. These interactions include: (1) change of zeta potential at the soil particle/pore fluid interface; (2) resistance of the soil-fluid-contaminant system to pH change; and (3) sorption/desorption of reactive contaminants onto or from the soil particle surface and precipitation/dissolution of metallic contaminants in the pore fluid. The effects on these interactions of injecting an enhancement fluid into the contaminated soil are also discussed. In addition, a brief review on the state-of-development of the technology is presented.
Work on electrokinetic technology started in the Netherlands around 1985 with Geokinetics. In 1994 the company teamed up with Hak Milieutechniek (HMT), which became full owner of the company in 1999.This paper briefly compares and contrasts Geokinetics' and HMT's commercially driven approach with that of the more traditional and academic approach adopted by many other workers in the field. It outlines our primary attention and focus on electrokinetic technology to solubilize and recover ionic contamination from ground and groundwater. The simple fact that most of the contaminated sites all over the world contain more often than not a mixture of both inorganic and organic components forced us to extend the use of electricity to cope with all sorts of pollution. The knowledge we gained and the challenges of this opportunity lead us to the development of electro-remediation, a combination of techniques having electricity as the common denominator:–electrokinetic recovery of inorganic contamination and electroheated recovery of organic contamination in combination with soil vapour extraction and low flow groundwater extraction;–electroheated and electrokinetically enhanced biodegradation in combination with addition of nutrients and electron donors or acceptors;–electrokinetic containment and remediation of polluted sites and groundwater plumes.The paper gives an overview and description of a number of benchmark projects in the aforementioned areas.
Lead alloy bullets used at the 2600 military small arm ranges and 9000 nonmilitary outdoor shooting ranges in the United States are a source of mobilized lead ions under conditions of low pH, significant changes in ionic strength, changes in the reduction oxidation potential (redox), and through binding metal ions to soil organic matter. Once mobile, these lead ions can contaminate adjacent soil and water. Batch adsorption kinetic and isotherm studies were conducted to compare and evaluate different types of adsorbents for lead ion removal from aqueous media. The effects on lead ion absorption from pH changes, competing ions, and temperature increases were also investigated. Adsorbent materials such as activated carbon and naturally occurring zeolites (clinoptilolite and chabazite) were selected because of their relative low cost and because the zeolites are potential point-of-use materials for mitigating wastewater runoff. Molecular sieves, Faujasite (13X) and Linde type A (5A) were selected because they provide a basis for comparison with previous studies and represent well-characterized materials. The relative rate for lead ion adsorption was: 13X > chabazite > clinoptilolite > 5A > activated carbon. Modeling lead ion adsorption by these adsorbents using the Langmuir and Freundlich isotherm expressions determined the adsorbents' capacity for lead ion removal from aqueous media. 13X, 5A, and activated carbon best fit the Langmuir isotherm expression; chabazite and clinoptilolite best fit the Freundlich isotherm. Applications of chabazite would require pH values between 4 and 11, clinoptilolite between 3 and 11, while activated carbon would operate at a pH above 7. Ionic competition reduced lead ion removal by the zeolites, but enhanced activated carbon performance. Increasing temperature improved adsorption performance for the zeolites; activated carbon lead ion adsorption was temperature independent.
The fifth International Symposium on electrokinetic remedi-ation of soils (EREM 2005) was held in Ferrara, from 22 May to 25 May 2005. Some communications dealt with the scientific and commercial aspects of permeable reactive barriers (PRBs), more suitable for the treatment of polluted ground waters. The impetuous industrial development during the second half of the XIX and the whole XX century has undoubtedly allowed the obtainment of important technological results and clear improvements in different aspects of the human life. Nevertheless , while most of the attention has been addressed to the quantity and quality of industrial production, much less effort has been devoted to the minimization of the environmental impact of industrial activities. The dramatic consequence of this component of technological progress has been the uncontrolled injection of a huge variety of xenobiotic substances into the environment, and their accumulation in soils and groundwater. More recently, the increasing attention of media and updated legislations have properly activated the development of cleaner production processes and of remediation technologies. The latter issue is of extreme importance, in view of the urgency of pollution abatement in the vicinity of densely populated sites, where the presence of highly toxic, biorefractory species deteriorates water for civil uses and prevents the further expansion of urbanization. Ordinary depollution techniques are quite often either inapplicable or scarcely effective, and anyway expensive. The need of alternative innovative approaches, which should move from the bench scale to the commercial application, is more and more strongly felt, the main obstacle being the multicultural character of the approach involving competences from quite different areas, like hydrogeology, geophysics, electrochemistry and microbiology.
Pilot-scale electrokinetic remediation equipment suitable to the geological characteristics of South Korean nuclear facility sites was developed for the remediation of radioactive soil. The optimal experiment conditions were chosen through pilot-scale electrokinetic remediation experiments, and the experimental results are presented. The removal efficiencies of Co2+ and Cs+ from artificially contaminated soil after 15 days were 98.4 and 94.9, respectively, and the generated effluent volume was 3.4ml/g. The removal efficiencies of 60Co and 137Cs by nitric acid were increased by 3.1% and 2.0% more than those by acetic acid. Moreover, when nitric acid instead of acetic acid was used, it had an advantage of a reducing electricity consumption due to its higher electrolytic conductivity. The higher the radioactivity concentration of the soil was, the more the removal efficiencies of 60Co and 137Cs were increased. Namely, the removal efficiencies of 60Co and 137Cs from the soil of high concentrations were increased by 14.4% and 3.8% more than those from the soil of low concentrations. The larger the particle size of the soil was, the more the removal efficiency of 137Cs increased. Namely, the removal efficiency of 137Cs from the soil of an average 1.4mm particle size was increased by about 2.3% more than that from the soil of an average 0.7mm particle size. Also, the removal efficiencies of 60Co and 137Cs by the application of an electric current of 15mA/cm2 were increased by 1.4% and 4.4% more than those by the application of 10mA/cm2. Therefore, the total removal efficiency of 60Co and 137Cs from the radioactive soil of about 2000Bq/kg was 95.8% by an electrokinetic remediation by the application of an electric current of 15mA/cm2 for 55 days.
Electrochemical remediation of the environment is gaining widespread acceptance due to the mild conditions used, the cleanliness of the electron as a reagent, the easiness for automation, its versatility, etc. In this paper three phenomena are presented at the microscale level, originating from the application of an electric field to a simulated soil sample: a) Demonstration of metal ion migration, b) Demonstration of the creation and movement of an acidic and a basic front, and c) Demonstration of water movement through soil. Keywords (Domain): Laboratory Instruction
The objective of this experiment is to destroy, at the microscale level, a sample of surrogate organic waste by generating a powerful oxidizer at the anode of an electrochemical cell. This generated species oxidizes the waste to harmless products. The oxidizer can then be regenerated and recycled. Specifically, this experiment utilizes a redox mediator with a high standard potential (i.e., the Co (III/II) couple, E° = 1.82 V) to destroy a surrogate organic waste (e.g., glycerin or acetic acid) by converting it into CO2 and water. Students can observe the end of the reaction signaled by a color change of the electrolytic medium (from pink to gray-light purple) as well as the evolution of CO2 which precipitates CaCO3 from a Ca(OH)2 solution. The Co(II) solution and the electrodes can then be reused. Keywords (Audience): Second-Year Undergraduate
Electrokinetic remediation, variably named as electrochemical soil processing, electromigration, electrokinetic decontamination or electroreclamation uses electric currents to extract radionuclides, heavy metals, certain organic compounds, or mixed inorganic species and some organic wastes from soils and slurries. An overview of the principals of the electrokinetic remediation technique in soils is presented. The types of waste and media in which the technology could potentially be applicable are outlined and some envisioned environmental uses of conduction phenomena in soils under electric fields are presented. The current status of the electrokinetic remediation technique and its limitations are discussed through a review of the bench-scale and pilot-scale tests. The recent findings of research on different techniques that may improve the technology's effectiveness are mentioned and the status of ongoing efforts in wide-scale implementation and commercialization of the technique in the USA are described.
In recent years, there has been increasing interest in finding new and innovative solutions for the efficient removal of contaminants from soils to solve groundwater, as well as soil, pollution. The objective of this review is to examine several alternative soil-remediating technologies, with respect to heavy metal remediation, pointing out their strengths and drawbacks and placing an emphasis on electrokinetic soil remediation technology. In addition, the review presents detailed theoretical aspects, design and operational considerations of electrokinetic soil-remediation variables, which are most important in efficient process application, as well as the advantages over other technologies and obstacles to overcome. The review discusses possibilities of removing selected heavy metal contaminants from clay and sandy soils, both saturated and unsaturated. It also gives selected efficiency rates for heavy metal removal, the dependence of these rates on soil variables, and operational conditions, as well as a cost–benefit analysis. Finally, several emerging in situ electrokinetic soil remediation technologies, such as Lasagna™, Elektro-Klean™, electrobioremediation, etc., are reviewed, and their advantages, disadvantages and possibilities in full-scale commercial applications are examined.
When the electrokinetic method is used to remove metals from soils, metals may precipitate as hydroxides in the region of the soil where pH is raised, which limits the remediation efficiency. The pH rise is caused by the generation of hydroxide ions as a result of electrolysis of water during the remediation. This paper proposes a new technique in which a conductive solution is inserted between the cathode and the soil to be treated. By this approach, the pH in the soil can be kept low so that no metal precipitation will occur. Thus metal ions may migrate out of the soil and precipitate in the inserted solution. Laboratory experiments have been carried out to remove copper and zinc from sand by the proposed technique. The experimental results show that metal removal efficiencies depend on the duration of the treatment and the content of electrolytes in the solution. Metal removal efficiencies of > 96% can be reached for both copper and zinc.
Analysis of polarization processes at electrokinetic remediation of clay soils and evaluation of the contribution of various components into the transport of charged contaminants are performed. The peculiarities of soil decontamination at constant and pulse voltages are investigated using kaolinite and mixture of montmorillonite and sand contaminated with radionuclides (137Cs, 90Sr, U) and heavy metals (Co) as model systems. It is shown that the use of unipolar pulse voltage changes the distribution of contaminations in soil and allows to decrease power inputs. It is also demonstrated that the introduction of cation-exchangers CU-2-8 into electrode chambers considerably improves the degree of soil decontamination. The most effective method to intensify the decontamination of clay soils from radionuclides and heavy metals is the wetting of soil with enhancement reagents (acetic, nitrilotriacetic and ethylenediaminetetraacetic acid).
Zeolites are used in environmental remediation of soil or water to immobilize or remove toxic materials by cation exchange. An experiment was conducted to test the use a low electric field to direct the toxic cations towards the zeolite. An electrokinetic cell was constructed using carbon electrodes. Synthetic Linde Type A (LTA) zeolite was placed in the cell. Copper(II) chloride dissolved in water was used as a contaminant. The Cu(2+) concentration was measured for ten hours with and without an applied electric field. The removal of the Cu(2+) ions was accelerated by the applied field in the first two hours. For longer time, the electric field did not improve the removal rate of the Cu(2+) ions. The presence of zeolite and applied electric field complicates the chemistry near the cathode and causes precipitation of Cu(2+) ions as copper oxide on the surface of the zeolite. With increased electric field the zeolite farther away from the cathode had little cation exchange due to the higher drift velocity of the Cu(2+) ions. The results also show that, in the LTA Zeolite A pellets, the cation exchange of Cu is limited to a shell of several tens of micrometers.
To simultaneously avoid a decrease of electro-osmotic flow by hydrogen ions and to increase heavy metal precipitation due to hydroxide ions, simulated electrokinetic remediation was conducted in saturated kaolinite specimens loaded with lead(II) using an electrolyte circulation method to control electrolyte pH. At an electrolyte circulation rate of 1.1 ml/min, it was possible to increase the anolyte pH from 2 to 4 and decrease the catholyte pH from 12 to 8. Using electrolyte circulation, it was observed that the rate of decrease of clay pH due to the change of electrolyte pH was reduced. As a result, the operable period was extended and the removal efficiency for lead(II) was also increased. It was observed that most of the effluent lead(II) from the cathode compartment was electroplated onto the cathode and that residual effluent lead(II) did not precipitate onto, or adsorb to, the clay at the anode compartment during circulation. Therefore, there was no need to treat the electrolyte because there was virtually no effluent from the cathode compartment in the circulation system. It was also found that the electrolyte volume required to sustain the electrolytic reaction was sufficient for the whole electrokinetic remediation process.
Polycyclic aromatic hydrocarbon (PAH)-contaminated soils exist at numerous sites, and these sites may threaten public health and the environment because many PAH compounds are toxic, mutagenic, and/or carcinogenic. PAHs are also hydrophobic and persistent, so conventional remediation methods are often costly or inefficient, especially when the contaminants are present in low permeability and/or organic soils. An innovative technique, electrokinetically enhanced in situ flushing, has the potential to increase soil-solution-contaminant interaction and PAH removal efficiency for low permeability soils; however, the electrolysis reaction at the anode may adversely affect the remediation of low acid buffering capacity soils, such as kaolin. Therefore, the objective of this study was to improve the remediation of low acid buffering soils by controlling the pH at the anode to counteract the electrolysis reaction. Six bench-scale electrokinetic experiments were conducted, where each test employed one of three different flushing solutions, deionized water, a surfactant, or a cosolvent. For each of these solutions, tests were performed with and without a 0.01 M NaOH solution at the anode to control the pH. The test using deionized water with pH control generated a higher electroosmotic flow than the equivalent test performed without pH control, but the electroosmotic flow difference between the surfactant and cosolvent tests with and without pH control was minor compared to that observed with the deionized water tests. Controlling the pH was beneficial for increasing contaminant solubilization and migration from the soil region adjacent to the anode, but the high contaminant concentrations that resulted in the middle or cathode soil regions indicates that subsequent changes in the soil and/or solution chemistry caused contaminant deposition and low overall contaminant removal efficiency.
The effect of enhancement reagents on the efficiency of electrokinetic remediation of Cu contaminated red soil is evaluated. The enhancement agents were a mix of organic acids, including lactic acid+NaOH, HAc-NaAc and HAc-NaAc+EDTA. The soil was prepared to an initial Cu concentration of 438 mgkg(-1) by incubating the soil with CuSO4 solution in a flooded condition for 1 month. Sequential extraction showed that Cu was partitioned in the soil as follows: 195 mgkg(-1) as water soluble and exchangeable, 71 mgkg(-1) as carbonate bound and 105 mgkg(-1) as Fe and Mn oxides. The results indicate that neutralizing the catholyte pH maintains a lower soil pH compared to that without electrokinetic treatment. The electric currents varied depending upon the conditioning solutions and increased with an increasing applied voltage potential. The electroosmotic flow rate changed significantly when different conditioning enhancing reagents were used. It was observed that lactic acid+NaOH treatments resulted in higher soil electric conductivities than HAc-NaAc and HAc-NaAc+EDTA treatments. Ultimately, enhancement by lactic acid+NaOH resulted in highest removal efficiency (81% Cu removal) from the red soil. The presence of EDTA did not enhance Cu removal efficiencies from the red soil, because EDTA complexed with Cu to form negatively charge complexes, which slowly migrated toward the anode chamber retarding Cu2+ transport towards the cathode.
An innovative remediation system of electrokinetic process coupled with permeable reaction barrier (PRB) was proposed for arsenic removal in soil matrix. Batch tests with PRB media of Fe(0) and FeOOH under potential gradient of 2 V cm(-1) for 5d duration were conducted to evaluate the removal mechanisms of arsenic. Arsenic enhancement of 1.6-2.2 times was achieved when a PRB system was installed in an electrokinetic system. A best performance was found in system with FeOOH layer located in the middle of elctrokinetic cell. This was largely because of higher surface area of FeOOH and the moving of HAsO(4)(2-) to the anode side by electromigration effect was inhibited by the electroosmosis flow. The surface characteristics of PRB media, which were qualified by SEM coupled with energy dispersive spectroscopy (EDS), were clearly confirmed that arsenic was found on the passive layer surface. Results indicated that the removal of As in EK/PRB systems was much more contributed by surface adsorption/precipitation on PRB media than by EK process. Furthermore among the electrical removal mechanisms, electromigration was predominant than electrosmotic flow. Surface adsorption and precipitation were respectively the principal removal mechanism under acid environment, e.g. near anode side, and under basic environment, e.g. near cathode side. The results reported in the present work will be beneficial to optimizing design of batch EK/PRB system and enlarging to the field scale system.
The formation and stability of a pH junction was investigated, and the precipitation and accumulation of a metal hydroxide at the pH junction was confirmed. Moreover, the possibility that metal ions could be accumulated as a Me-EDTA complex at the pH junction was demonstrated. As a result, the pH junction where the acidic and alkali fronts of soil meet and the pH of soil changes rapidly, appeared at the 0.6 position in the EK process for 6-12 h. Copper ions accumulated in the form of copper hydroxide. EDTA was also concentrated in the position, in general agreement with the position of the pH junction. In addition to copper hydroxide, a copper-EDTA complex was concentrated at the 0.6 position from the anode after EK treatment for 12 h. The copper-EDTA complex was retained in 0.7 position from the anode after 12 h and, after 24 h, the position shifted to 0.8-0.9 from the anode. The possibility of accumulating metal ions within a narrow area, such as a pH junction was demonstrated.
This paper presents a systematic bench-scale laboratory study performed to assess the transient behavior of chromium, nickel, and cadmium in different soils during electrokinetic remediation. A series of laboratory electrokinetic experiments was conducted using two different clayey soils, kaolin and glacial till. For each type of soil, four electrokinetic experiments with 1, 2, 4, and 10 d of treatment time were performed. In all tests, the contaminants were Cr(VI), Ni(II), and Cd(II) combined in the soil. A geochemical assessment was performed using the geochemical model MINEQL(+) to determine the partitioning of the heavy metals in soils as precipitated, adsorbed, and aqueous forms. Results showed that in kaolin, the extent of Ni(II) and Cd(II) migration towards the cathode increased as the treatment time increased. Unlike kaolin, in glacial till treatment time had no effect on nickel and cadmium migration because of its high buffering capacity. In both kaolin and glacial till, the extent of Cr(VI) migration towards the anode increased as the treatment time increased. However, Cr(VI) migration was higher in glacial till as compared to kaolin because of the high pH conditions that existed in glacial till. In all tests, some Cr(VI) was reduced to Cr(III), and the Cr(VI) reduction rate to Cr(III) as well as the Cr(III) migration were significantly affected by the treatment time. Overall, this study showed that the electroosmotic flow as well as the direction and extent of contaminant migration and removal depend on the polarity of the contaminant, the type of soil, and the treatment duration.
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- R J Gale
- A N Alshawabkeh
- R E Marks
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