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Electrochimica Acta
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Application of solar-cells in the electrokinetic remediation of

As-contaminated soil
Eun-Ki Jeon a , So-Ri Ryu a , Kitae Baek a,b, *
Department of Environmental Engineering, Chonbuk National University, 567 Baekje-daero, Deokjin-gu, Jeonju 561-756, Republic of Korea
Department of Bioactive Material Sciences, Chonbuk National University, 567 Baekje-daero, Deokjin-gu, Jeonju 561-756, Republic of Korea


Article history: In this study, we evaluated the effectiveness of the solar-powered electrokinetic process for the
Received 14 January 2015 remediation of As-contaminated soil in order to reduce the electrical energy consumption on a pilot scale,
Received in revised form 9 March 2015 and this study also investigated the influence of oxalic acid for the treatment of As bound to amorphous
Accepted 9 March 2015
iron-oxide. The soil was collected from a former refinery plant located in Janghang, Chungnam, Republic
Available online xxx
of Korea. The experiments were designed two different power supply systems: a normal power supply
and a solar-powered system, and operated the experiments for five weeks. The normal direct current
(DC)-powered system removed 32% of the As, but the solar-powered system removed 27% of the As from
green remediation
solar cell
the soil over the five weeks of electrokinetic operation. The energy expenditure of the solar-based system
pulse was just 50% of that of the DC-powered system. The results show that the solar-powered electrokinetic
oxalic acid process can remove slightly smaller amounts of contaminants with much less electrical energy. Based on
these results, the solar-based electrokinetic process could be applied in order to remediate As-
contaminated soil. However, enhanced As removal should be achieved for actual application.
ã 2015 Elsevier Ltd. All rights reserved.

1. Introduction factors, such as soil characteristics, cost of electricity, installation of

equipment, and depth of contamination, influence the overall cost
Many remediation processes have been developed and applied of the EKR process [1,2,12]. Among these economic factors of the
in order to remediate various types of contaminated soil and EKR process, electric energy accounts for 10–15% of the total cost
ground-water [1]. In order to select the remediation process, [2]. Alshawabkeh et al. [1] reported that the electric cost was 16.1%
several factors including soil characteristics, contaminant type, of the total cost of the EKR process. The total energy expenditure
economic feasibility, and field applicability should be duly was influenced by soil characteristics, contamination conditions,
considered [1–3]. Among these factors, soil with a portion of fine and electrode configuration or spacing [1,12]. However, several
grained particles makes most remediation processes unfeasible factors that influenced the energy expenditure of the EKR process
due to its low hydraulic conductivity and strong affinity to were discussed with the conventional DC power supply under
contaminants [1,4]. Soil washing, including physical separation constant voltage or current. In addition, the EKR process using
and chemical extraction, is the most common technique used to constant voltage caused a risk for electrode corrosion by the
remediate metal-contaminated soil in Korea. However, the polarization effect [13,14]. The solar-based EKR process that
removal of metals in fine-grained soil is not achievable by soil generates electric power by itself has attracted attention recently
washing [5–8]. Electrokinetic remediation (EKR) is one remedia- [11]. The electric energy generated by a solar-cell depended on the
tion technology be applicable for the treatment of fine-particle and daylight, in other words, the electrical potential was influenced by
clay-like soil [1,2,4,6,9,10]. In order to enhance the performance of the weather conditions and was an attractive energy source
the EKR process, many studies have investigated the feasibility of because it is a renewable energy source and is environmentally
certain additives to enhance the mobility of the pollutants. friendly [15–18]. Furthermore, the solar-cell generated DC power
However, the use of the EKR process to reduce the operation cost and was beneficial for the EKR process because it did not need to
or electric energy expenditure was relatively limited [11]. Several use an AC to DC power converter for application to the EKR process
[11,18]. Yuan et al. [11] reported that the solar-based EKR process
was more economical than the traditional EKR process, and Kim
* Corresponding author. Tel.: +82 63 270 2437; fax: +82 63 270 2449. et al. [19] reported that the solar-based EKR process consumed less
E-mail address: (K. Baek). energy for the removal of similar amounts of salts from soil.
0013-4686/ ã 2015 Elsevier Ltd. All rights reserved.

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texture, and the initial pH and electrical conductivity (EC) were

measured with a pH & EC meter (IsTek Korea), respectively. The soil
was calcined at 550  C in order to measure the organic matter.
The soil composed of 26.8% sand, 9.9% silt, and 63.3% clay was
classified as clay. The initial concentrations of As (219.3 mg/kg), Cd
(4.6 mg/kg), Cu (304.5 mg/kg), and Pb (608.8 mg/kg) exceeded the
Korean regulatory standards (As: 25 mg/kg, Cd: 4 mg/kg, Cu:
150 mg/kg, and Pb: 200 mg/kg) (Table 1). The soil sample was
contaminated by many metals, but this study focused on reducing
the As concentration. The details of the soil properties are
summarized in Table 1.

2.2. Experimental set-up

A schematic of the electrokinetic remediation system used in

this study is shown in Fig. 1. It was provided direct current to
operating the pilot system in two different ways: the electrical
potential from a solar cell and that from a DC power supply. The DC
power supply generated an electrical potential of 40 V continu-
ously and the solar-cell can generate an electrical potential during
day time (with sunlight) up to 40 V. The EK testing apparatus was a
square type (H: 1 m, L: 1 m, W: 1 m) and divided the reactor into
two equal sections. Each section was provided electrical potential
by the DC supply and solar-based power. The electrode was
installed in a parallel configuration, and the electrode spacing
between the anode and cathode was 0.3 m. The spacing for the
same polarity electrode was 0.23 m (Fig. 1). The electrode system
Fig. 1. Schematic diagram of electrode configuration and Osmosis flow circulation

However, the studies on solar-based EKR were limited based on the

small laboratory scale and there have not been any pilot or field-
scale studies even though they are required to evaluate the
feasibility of the solar-based EKR process.
The objective of this study was to evaluate the effectiveness of a
solar-cell in order to reduce the electrical energy consumption for
the remediation of As-contaminated paddy soil on a pilot scale.

2. Experimental

2.1. Soil characteristics

The heavy metals-contaminated soil used in this study was

collected near a former metal refinery. The soil sample was air-
dried and sieved using a No. 10 mesh sieve. This experiment used
soil with a particle size smaller than 2 mm. The American standard
test method (ASTM D422-62) was used in order to measure the soil

Table 1
Preperties and Initial concentration of heavy-metals of soil used in this study.

Category Result
Soil texture Clay
Sand (%) 26.8
Silt (%) 9.9
Clay (%) 63.3
Soil pH 7.04
Conductivity (uS/cm) 267.1
Soil organic matter (%) 4.6

Concentration of heavy metals (mg/kg) Regulation level (mg/kg)

As 219.3 25
Cd 4.6 4
Cu 304.5 150
Pb 608.8 200
Ni 9.9 100
Zn 207.1 300

Fig. 2. Schematic diagram of electrode system.

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Table 2
Experimental conditions for EKR process.

Power supply Potential gradient (V/cm) Pretreatment agent Electrolyte Duration (day)

Anolyte Catholyte
D.C supply Constant at 1.33 Oxalic acid Tap water Oxalic acid 35
Solar-cell Ranged at 0 to 1.33

was composed of two parts a polyvinyl chloride (PVC) casing and amorphous hydrous oxide-bound (F3), crystalline hydrous oxide-
an iron electrode (Fig. 2). Before installing the electrode in the soil, bound (F4), and residual (F5).
the PVC casing was wrapped with filter cloth in order to prevent
electrolyte spillage, and each electrode casing was directly 3. Results and discussion
connected to the electrode tank. The level of each electrolyte
was controlled to maintain equal amounts. The overflow of the 3.1. Change in electrolyte pH
electrolyte was collected to measure the direction and amounts of
electro-osmotic flow (EOF). The electrolyte was circulated by a The change in electrolyte pH during the experimental period is
peristaltic pump at a flow rate of 2 ml/min. A concentration of 0.1 M shown in Fig. 4a and b. In the early phase, the pH of the anolyte
oxalic acid was applied as a catholyte pursing solution in order to decreased rapidly in both of the experiments. There was no
supply oxalate to both of the EK systems. The experimental difference in anolyte pH between the solar-cell and the DC supply
conditions are summarized in Table 2. The contaminated soil was despite differences in the current values observed in the two
pre-treated with a pursing solution at 30% water-content for experiments. The EK system used an iron electrode in order to
24 hours and packed the pre-treated soil into the pilot reactor prevent acidification of the anodic region, because iron oxidation
(H: 0.2 m, L: 0.45 m, W: 1 m). The experiments were carried out for instead of water oxidation did not generate hydrogen ions.
five weeks (35 days). The soil samples were collected at three However, in the actual experiment, the soil was acidified by the
points between the anode and cathode by hand auger, and the pretreatment and the circulation of the catholyte by oxalic acid.
soil samples were divided into two 10-cm-deep layers (top layer Therefore, the effects of the iron anode were not clearly observed.
(0.0–0.1 m), bottom layer (0.1–0.2 m)). During the experimental On the other hand, the pH of the catholyte remained at the initial
period, soil samples were collected four times every week (first, value from the beginning to the end of the experimental period
second, third, and fifth samplings for weeks 1, 2, 3, and 5) (Fig. 3). because the oxalic acid was circulated. However, the pH of the DC
supply was slightly higher than the pH value of the solar-cell. An
2.3. Analytical methods experiment using a solar-cell showed that it only generated OH
intermittently during the “on” time, therefore causing the differ-
The electrical conductivity (EC) of the soil and the water content ences in pH value.
and pH of the soil were determined using the Korean standard test
method (KSTM). The heavy-metals were extracted from the 3.2. Distribution of soil pH and accumulated electro-osmotic flow
contaminated soil with an aqua-regia extraction solution (HCl:
HNO3 = 3:1), then the mixture was heated at 70  C for 1 hour, and The soil pH for each of the soil samples and the electro-osmotic
the extractant was filtered using 5B filter paper. The filtrate was flow volume accumulation are shown in Fig. 4c and d. The soil pH
analyzed using induced coupled plasma optical emission spec- was initially 7.0 and was lowered to 4 after pre-treatment with
trometry (ICP-OES, Agilent 720, USA). The fractionation of As in the oxalic acid. The average pH value of each of the soil samples was 4.4
soil was analyzed according to the sequential extraction method (1 weeks), 4.3 (2 weeks), 3.7 (3 weeks), and the pH value for the
suggested by Wenzel et al. [20] and was sorted into the following solar-powered system were 3.9 (5 weeks) in the DC supply,
categories: non-specifically-bound (F1), specifically-bound (F2), respectively, and 4.5 (1 weeks), 4.4 (2 weeks), 4.1 (3 weeks), and 4.2

Fig. 3. Sampling point of this experiments during the experimental period.

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7 2.5
Change of electrolyte pH (a) : Anolyte Anolyte of Solar-cell (b) : Catholyte
6 Anolyte of DC supply



2 Catholyte of Solar-cell
0.5 Catholyte of DC supply

0 0.0
0 200 400 600 800 1000 0 200 400 600 800 1000

Time/ h Time /h
8 8
(c) : DC supply 1st sampling (d) : Solar-cell
2nd sampling
3rd sampling
Soil pH distribution

6 5th sampling 6

4 4

2 2

0 0
Anode Middle Cathode Anode Middle Cathode

(e) Solar-cell
Electro-osmotic flow /L

DC supply
Accumulated Reverse





0 200 400 600 800 1000

Time /h
Fig. 4. Electrolyte pH distribution ((a): Anolyte, (b): Catholyte) and change of the soil pH((c): DC supply, (d): Solar-cell) and accumulated electro-osmotic flow volume (L) (e).

(5 weeks) during the same time period (Fig. 4c and d). The decrease positive by soil acidification, which influenced the velocity
in soil pH was strongly related to the electrolysis reaction, which distribution between the electrical force and the mobile cations
was directly proportional to the amount of electrical energy [21]. These experiments pre-treated the soil using 0.1 M oxalic acid
supplied. Therefore, the solar-powered system used less electrical in order to enhance the removal efficiency of the metals, and the
energy because the system could not generate electrical energy direction of flow was highly dependent on the chemical agent used
during the night time. for enhancing the efficiency. In general, the direction of the electro-
The electro-osmotic flow was influenced by several conditions, osmotic flow is from anode to cathode. However, the direction in
such as the zeta potential, the relative permittivity, and the this study was the opposite, that is, from cathode to anode.
viscosity [21]. The surface charge of the soil was changed to The acidification due to pretreatment with oxalic acid and the

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circulation of the acid in the catholyte changed the surface charge 50

of the soil to positive, which led to reverse electro-osmotic flow. (a) Solar-cell
DC supply
The overall volume of osmotic flow was 46.2 L and 23.2 L for the DC
supply and the solar-cell experiments, respectively (Fig. 4e). In the

Potential drop /V
experiment with the DC power supply, the voltage was continu-
ously supplied because the electric field, a driving force for electro- 30
osmotic flow, was generated continuously [22]. It is possible to
explain the correlation between the driving force of the EOF and 20
the electrical current using the electroosmotic permeability
coefficient, Ke (m2 V 1 s 1) in the following equation: 10
Qe=KeieA (1),
where Qe(mL/day) is the flow rate of the electroosmotic flow, ie
(V cm 1) is the voltage gradient, and A (m2) is the cross-sectional
area of the EKR system [21,23]. The average electroosmotic 0.5
permeability of the solar-cell was 6.05 * 10 10 m2 V 1 s 1 for only (b)

Current density /A cm-2

the “on” time, and that of the DC power was 1.21 * 10 9 m2 V 1 s 1.
These results indicate that the electroosmotic flow rate is
considerably correlated with the electrical current.

3.3. Current change and accumulated energy consumption

The normal DC power supply provided a constant voltage of
40 V to the system during the entire experimental period (Fig. 5a). 0.1
However, the solar-powered system supplied an electrical poten-
tial to the system ranging from 0 V to a maximum of 40 V. During
the day, the voltage was similar to the normal DC power. However,
the voltage decreased sharply to almost 0 V after sunset. The
voltage could also change during the day depending on the 80
Energy consumption /kWh m

presence of direct sunshine. (c)

Initially, the current value in the normal DC power system was
maintained at 40 mA until 75 hours, after which time the current 60
increased rapidly to 200 mA. The average current during the entire
experiment was approximately 140 mA (Fig. 5b). The continuous
supply of conducting ions, including oxalate and H+, greatly
increased the current, and the neutralization reaction between the
H+ and OH decreased the current value. However, the current in
the solar-power system was highly dependent on the voltage
generated by the solar cell, with an average current of approxi-
mately 80 mA, just 57% of that of the normal DC-powered system.
Although the average current produced by the solar power was 0 200 400 600 800 1000
lower than that of the DC-powered system, the maximum current
value of the solar power was approximately 2 times higher than
Time /h
that of the DC power. The transport of ions was enhanced by the Fig. 5. Change of Potential value (a), current density (b), and accumulated electric
higher current value during the day time in the solar-power energy consumption (c) during the experimental period.
system. This probably occurred due to the depolarization effect,
which reduced the diffusion phenomenon during the “off” period After five weeks, the As removal rate in the anode region, middle
[2,4,24–28]. section, and cathode region was 23.2, 31.7 and 41.1%, respectively,
In general, H+ and OH are continuously generated in the EKR which indicated that the As was transported from the cathode
process because of the constant voltage, and this phenomenon toward the anode (Fig. 6a and b). These results indicate that the
leads to decreases in the electrical gradient. It also causes a primary removal mechanism of As is electromigration of oxy-
diffusion effect on the direction of the EOF because the H+ and OH anionic As toward the anode. In addition, the direction of the
are moved into the soil section [28]. However, an intermittent electro-osmotic flow enhanced the transport or removal of the As
cathode reaction led to the depolarization effect and prevented a toward the anode.
decrease in the electric current and a change in the soil pH because It is well known that oxalic acid is a strong chelating agent with
the discontinuous cathode reaction reduced the quantity of OH Fe(II) and Fe(III) [30,31], and it can extract Fe from soil by chelating,
[2,23,29]. The abovementioned results of the catholyte pH, which is enhanced by acidic conditions. The chelation of oxalic acid
maintenance of the soil pH value, and continuous current value with Fe can release As to soil water. In addition, oxalic acid can
indicate that the EKR process with a solar-cell can effectively reduce Fe(III) to Fe(II) and/or As(V) to As(III); the reduction of Fe
prevent the polarization effect. (III) can enhance the release of As(V); and the reduction of As(V) to
As(III) can decrease the re-adsorption of As onto the positively-
3.4. Removal efficiency of As, Cu, and Pb charged soil surface due to acidification [30,32]. As(III) is a neutral
compound below pH 9. Therefore, the transport direction of As(III)
The removal of As increased to 17.7, 23.0, 30.4, and 32.0% after was highly dependent on the direction of electro-osmotic flow,
one, two, three, and five weeks in the normal DC power system. which accelerated the accumulation of As near the anode. Various

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Fig. 6. Concentration change of As during the experimental period ((a): DC supply, (b): Solar-cell) and Fractionation change of As ((c): DC supply, (d): Solar-cell) during the
experimental period. Fractionation of As analyzed by Wenzel method.

chemical solutions including acids or chelating agents have been time”), such as activation, resistance, and concentration polariza-
used to enhance the desorption of metals from soil [9,33]. In tion [2,29,39,40]. Additional advantages of the solar-powered EK
addition, arsenic (As) can be extracted or released into solution system are its environmental friendliness and the lower operating
from soil by the application of ethylenediaminetetraacetic acid cost.
(EDTA) due to its ability to extract Fe from the soil, where most of
the As exists with Fe oxyhydroxides. However, EDTA has an adverse 3.5. Fractionation changes
effect on the environment because of its low biodegradability
[34,35]. Oxalic acid has the advantage of causing less damage to the Initially 64.2% of As in the soil existed as a form bound to
soil environment than that caused by chelating agents, however, it amorphous iron oxide (F3); the electrokinetic treatment lowered
is apprehended that the soil pH will be acidified continuously the fraction of As to 22.8% in the DC-powered system and 20.6% in
circulated oxalic acid rather than circulation of EDTA. [36]. Oxalic the solar-powered system (Fig. 6c and d). In addition, the fraction
acid can form stable complexes with Fe. Therefore, they precipitate of As bound to crystalline iron oxide changed from 14.0% to 3.6% for
in the form of ferrous oxalate, with indicates that iron can return to the normal DC-powered system and to 3.4% for the solar-powered
the soil after washing [37,38]. system. The fractions of other compounds were not changed
In the solar-powered system, the removal of As increased to significantly. Oxalic acid can extract Fe from the soil though
15.1, 15.4, 24.8, and 27.0% after one, two, three, and five weeks chelating-enhanced extraction, and amorphous Fe can be easily
(Fig. 5b). Even though the removal was enhanced with operation extracted by the oxalic acid in comparison to the crystalline Fe. The
time, the removal efficiency of As was lower than that of the extraction of Fe by oxalic acid released the As bound to the fraction,
DC-powered system due to a small supply of current or energy. The which was transported by electromigration and/or electro-osmotic
DC-powered system consumed 67.5 KWh/m3, while the solar- flow.
powered system used 33.7 KWh/m3 (Fig. 5c). The solar-powered
system removed 27.0% of the As from the system with approxi- 4. Conclusions
mately 50% less energy than the DC-powered system (32% removal
of As after five weeks). In general, the removal of contaminants in This study investigated the electrokinetic process powered by
electrokinetic remediation is proportional to the energy supplied. solar energy in order to reduce the energy cost, a major portion
Therefore, similar removal with expenditure of much less energy is of the operating cost of the process, for the remediation of
abnormal. The enhanced removal of As by solar power can As-contaminated soil on a pilot scale. The pretreatment and
probably be explained by the influence of pulsed power. The circulation of the catholyte using oxalic acid acidified the soil and
variation in the voltage gradient from the solar-cell according to changed the surface charge of the soil to positively, which led to
daylight was similar to the pattern of pulsed current that reverse electro-osmotic flow. The As was transported toward the
periodically repeated during the “on/off time” using the DC power anode by electromigration and reverse electro-osmotic flow.
supply. The application of pulsed current “off time” can diminish Oxalic acid extracted the As bound to the amorphous iron oxide
the negative effects of the polarization effect (during the “on to the pore solution via chelation with Fe. The solar-powered

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Please cite this article in press as: E.-K. Jeon, et al., Application of solar-cells in the electrokinetic remediation of As-contaminated soil,
Electrochim. Acta (2015),