Removal of Multiple Metallic Species

from Sludge by Electromigration

Claudio Cameselle 1 and Susana Gouveia 2

Abstract: The treatment of runoff waters from a lignite mine and a power plant generated a sludge heavily polluted with metals.
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Electromigration laboratory experiments were conducted to evaluate the feasibility of this technology for the removal of metals from
the sludge. The experimental results proved that the mobilization of heavy metals could be achieved by the acidification of the sludge.
The electro-oxidation of water in the anode can be used as a source of Hþ to mobilize the metals transported toward the cathode. The
suppression of OH− generation at the cathode by the controlled addition of nitric or sulfuric acid increased the electric conductivity of
the sludge specimen and the electric current intensity. The increase in the current intensity in the electrokinetic cell resulted in more
Hþ ions electrogenerated at the anode, favoring mobilization of the metals by the direct attack of the Hþ ions. The electrokinetic tests
proved that acid pH in the cathode resulted in higher electric current intensity and faster metal mobilization and removal, but the energy
consumption sharply increased. A trade-off occurred among metal removal, energy consumption, and the pH in the catholyte. The best results
were achieved by using sulfuric acid to control the pH in the catholyte at 4. The average metal removal was: Fe 27%, Ca 68%, Mg 24%,
Na 25%, Mn 68%, Sr 33%, Zn 60%, and Cu 60%. Other elements such as Al, K, Ti, and Zr associated with the crystalline structure of
minerals were not affected by the electrokinetic treatment. DOI: 10.1061/(ASCE)HZ.2153-5515.0000470. © 2019 American Society of Civil
Engineers.
Author keywords: Electrokinetic remediation; Heavy metal; Sludge; Manganese.

Introduction
Electrokinetic remediation has by now demonstrated several
successes in the treatment of heavy metal contaminated soils,
sediments, and sludges (Reddy and Cameselle 2009). The term
electrokinetics is used to refer to the movement of water, ions, and
charged particles relative to a solid matrix under the action of an
applied DC electric field (Ricart et al. 1999). In a porous compacted
matrix of surface-charged particles, such as soil, the ion-containing
pore fluid may be forced to flow to collection sites under the
applied field (Cameselle 2015). Both ionic and nonionic chemical
species are transported through the soil toward the main electrodes.
These compounds may subsequently be removed from the elec-
trode site via collection systems engineered for each specific appli-
cation (Reddy and Cameselle 2009).
Two mechanisms were proposed for the movement of the
contaminants in electrokinetics. For components with an ionic
nature, the transport takes place mainly by electromigration. For
nonionic species, the transport is by electroosmotic flow (Reddy
and Cameselle 2009). The extraction of contaminants by electro-
kinetic methods is based on the assumption that the contaminant is
1
Associate Professor, BiotecnIA, Dept. of Chemical Engineering,
Univ. of Vigo, Rua Maxwell s/n, Building Fundicion, Vigo 36310, Spain
(corresponding author). ORCID: https://orcid.org/0000-0003-4785-1585.
Email: claudio@uvigo.es
2
Postdoctoral Researcher, BiotecnIA, Dept. of Chemical Engineering,
Univ. of Vigo, Rua Maxwell s/n, Building Fundicion, Vigo 36310,
Spain. ORCID: https://orcid.org/0000-0003-4591-3228. Email: gouveia@
uvigo.es
Note. This manuscript was submitted on February 6, 2019; approved on
June 18, 2019; published online on August 28, 2019. Discussion period
open until January 28, 2020; separate discussions must be submitted for
individual papers. This paper is part of the Journal of Hazardous, Toxic,
and Radioactive Waste, © ASCE, ISSN 2153-5493.
in the liquid phase in the soil pores (Cameselle and Pena 2016). The
benefits of increased proton concentration at the anode from
the electrolysis of water are evident in the extraction of metals.
The pH contributes to metal removal through the following two
mechanisms (Cameselle et al. 2003): (1) affect the surface charge
characteristics of clay soils (the cation retention capacity of the clay
decreases in a low pH environment); and (2) create suitable envi-
ronments for the metal ions to remain in solution in the bulk pore
liquid. Thus, they can be extracted in a feasible manner (Kim et al.
2011; Yang et al. 2014). However, the generation of OH– in the
cathode may cause the precipitation of ionic species, reducing sep-
aration efficiency (Ricart et al. 1999). Electroosmosis has been re-
ported as not the dominant mechanism in the electrokinetic removal
of heavy metals, especially when present at a high concentration
(Ricart et al. 2004; Ottosen et al. 2009). Thus, the operating con-
dition in the electrokinetic tests must be adjusted for the mobiliza-
tion of metals and transportation by electromigration (Cameselle
and Pena 2016).
Ricart et al. (1999, 2004) used in kaolinite and sediment samples
to prove that the mobilization and transportation of Mn2þ toward
the cathode are possible through electrokinetics. However, the col-
lection of Mn in the cathode chamber is limited by the premature
precipitation of Mn in the soil sample with the OH– electrogener-
ated at the cathode. Several solutions have been proposed in the
literature to avoid precipitation and enhance the transportation
of heavy metals to the electrode chambers. Ottosen et al. (2009)
analyzed the possibilities of electrokinetics for the removal of
heavy metals from soils, sediments, and sludge. These authors dis-
cussed several solutions to enhance the removal of heavy metals.
The depolarization of the reduction of water in the cathode with
the controlled addition of an acid is the simplest solution to the
premature precipitation of heavy metals in the soil (Colacicco
et al. 2010). As an alternative, complexing agents can be used
to favor the extraction of heavy metals from the solid matrix

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 and keep the metals in solution, forming soluble complexes or
chelates (Zhang et al. 2014). In general, because these complexes
or chelates are stable in a wide range of pH, they are not affected
by the pH gradient generated in the soil during electrokinetics
(Figueroa et al. 2016; Cameselle and Pena 2016). The main limi-
tation of the complexing agents is the cost associated with their
use. Merdoud et al. (2016) reported that using complexing agents
must be associated with a recovery system that permits the re-
utilization of the complexing agents to reduce treatment costs.
Pedersen et al. (2019) proposed the use of ionic exchange mem-
branes between the soil and the electrode chambers. Thus, a
cationic exchange membrane on the cathode side prevents the pen-
etration of OH– into the soil. These authors also use an anionic
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Materials and Methods
Electrokinetic Cell
The experiments were conducted in an electrokinetic cell depicted
in Fig. 1 (Ricart et al. 1999; Figueroa et al. 2016). The electroki-
netic cell was made of glass and was composed of two electrode
chambers (volume: 300 mL) connected to a central cylindrical tube
(diameter: 3.2 cm; length: 10 cm) that held the sludge specimen.
The sludge was characterized (Table 1) for hydraulic permeability
[ASTM D2434 (ASTM 2006)]; grain size distribution [ASTM
D422 (ASTM 2007)]; organic matter content [ASTM D2974
(ASTM 2014a)]; specific gravity [ASTM D854 (ASTM 2014b)];

exchange membrane on the anode side. The simultaneous use of water content [ASTM D2216 (ASTM 2019a)]; and pH, oxidation-
those two membranes permits the transportation of ions out of reduction potential (ORP) and electric conductivity (EC) [ASTM
the soil but avoids the penetration of ions from the electrode D4972 (ASTM 2019b)]. The electrode chambers and the sludge
solutions into the soil. Ricart et al. (2004) tested several mem- specimen were separated by a glass microfiber filter (Whatman,
brane configurations in the electrodialytic treatment of heavy grade GF/A, Buckinghamshire, UK) and a porous stone. The
metal-contaminated sludge and compared the results with the elec- processing fluid in the electrode chambers was homogenized
trokinetic treatment. These authors concluded that strong acidifi- with a magnetic stirrer. The electrodes—an anode and a cathode—
cation favored the mobilization and removal of heavy metals from were made of graphite and connected to a direct current (DC)
the solid matrix. Such acidification can only be achieved using
electrokinetic treatment without membranes. The ionic exchange
membranes limited the total intensity of the electric current
through the specimen, the electrogeneration of Hþ in the anode,
and the electromigration of protons into the soil. Overall, the most
appropriate solution for the electrokinetic treatment of a sludge
contaminated with multiple heavy metals seems to be the electro-
kinetic treatment favoring the advance of the acid front from the
anode and depolarizing the reduction of water in the cathode with
the controlled addition of acid.
The sludge used in the current study came from a treatment
plant used to treat the runoff water at a mining site (Galicia in
northwest Spain). The runoff waters from the mine were charac-
terized by low pH and significant heavy metal concentration. In
the mine, the actual pH and metal concentrations largely vary
from one site to another and are also strongly affected by rain
(intensity and pace). The presence of pyrites in the subsoil is
responsible for the low pH and heavy metals in the mine effluent.
The most abundant heavy metal in the mine effluent is Mn. In
the past, the release of Mn from the mine created deposits in the
riverbed and basin that received the effluent from the mine. Fig. 1. Experimental setup for electrokinetic tests. (1) sludge speci-
The treatment plant was designed and constructed to ameliorate men; (2) cathode; (3) anode; (4) valves for processing fluid: anolyte
the effect of the mine in the surrounding ecosystem. The acid and catholyte; (5) anode chamber; (6) cathode chamber; (7) power sup-
mine effluent is neutralized in the plant with lime, and the heavy ply; (8) multimeter; (9) magnetic stirrer; (10) measurement cylinders
for electroosmotic flow; (11) store bottles for processing fluid: anolyte
metals are precipitated in the same treatment. Thus, the ecosys-
and catholyte; (12) electric connection in electrode; (13) Pasteur pipet
tem is protected from the contaminants that originated in the
for sampling; and (14) expansion vessel.
mine. The sludge from the treatment plant contains the precipi-
tated metals and other solid particles (clay, silt, and sand parti-
cles) carried by the water from the mine. This sludge is deposited
in a secure deposit given the risk of mobilization of the metals if
conditions change at the mid or long term. The treatment of the Table 1. Characterization of sludge
sludge to remove the toxic metals reduces future risks and sim- Parameter Sludge Test method
plifies its management.
Water content (%, wet basis) 45  1 ASTM D2216
The objective of this work is the assessment of electrokinetic
Grain size ASTM D422
remediation as a possible technology for the removal of heavy met- Gravel (%) 2  0.5
als from contaminated sludge. Based on the results in the literature, Sand (%) 35  0.5
nitric and sulfuric acids are proposed to depolarize the reduction of Silt and clay (%) 63  0.5
water in the cathode. Despite the capability of organic acids to neu- Permeability (cm/s) 3.08 · 10−5 ASTM D2434
tralize the alkaline front in the cathode, this group of compounds is Specific gravity 2.36  0.05 ASTM D854
not considered given the high Ca content in the sludge. Ca reacts pH 7.60  0.30 ASTM D4972
with the organic acids forming complexes or precipitates, thereby ORP (mV) 250  7.50
reducing the complexing capacity of organic acids with other harm- EC (mS=cm) 6670  125
Organic matter (%) 2  0.06 ASTM D2974
ful heavy metal ions.

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 Table 2. Metal content in sludge specimen used in three tests determined was selected based on previous tests (Ricart et al. 2004) using a
as per USEPA Method 3050B (USEPA 1996) sludge of similar characteristics. The voltage gradient was in-
Element Concentration in sludge (mg=kg) creased in tests EK2 and EK3 to favor the mobilization and removal
of metals. The operation time of the tests was adjusted for a similar
Al 87,323  3,602
Fe 39,891  595 total charge passing through the sludge specimen. Test EK1 has a
K 15,440  294 total electric charge much smaller than the other two tests but was
Ca 10,863  181 terminated after 23.4 days when the current intensity was 0.2 mA
Ti 5,661  63 and achieving the same total electric charge in a practical period
Mg 4,597  239 was not possible. Periodically, the electric current intensity and
Na 6,967  622 fluid pH in the electrode compartment were measured and regis-
Mn 878  24 tered. At the completion of all experiments, samples were taken
Zr 468  32 from cathode and anode solutions and the sludge for heavy metal
Sr 216  15
analysis. The sludge sample was divided into five sections of equal
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Zn 192  13
Cu 100  9
power supply at a constant voltage of 15–30 V. A multimeter was
installed in the electric circuit to continuously read the intensity
of the electric current. Pasteur pipets were used for periodical
sampling of the processing fluid in the anode and cathode for
pH measurement. The electrode chambers were open to atmos-
phere, and a constant liquid level was maintained to avoid hydraulic
flow through the sludge specimen by the pressure gradient.
Analytical Methods
The test protocols for chemical extraction and analysis procedures
were performed in accordance with EPA Method 3010A: Acid
Digestion of Aqueous Samples and Extracts for Total Metals for
Analysis by FAA and ICP Spectroscopy (USEPA 1992) and
Method 3050B: Acid Digestion of Sediments, Sludges, and Soils
(USEPA 1996). Flame atomic absorption (FAA) Spectroscopy was
used to determine the heavy metal concentration in the sludge and
electrode solutions before and after the experiments (Pamukcu and
Wittle 1992). Sludge pH was measured by mixing 1 g of a sludge
sample with 2.5 mL of KCl 1 M. After 1 h of contact, the pH was
measured in the supernatant liquid (Hansen et al. 1997). Table 2
indicates the elemental composition of the sludge. The initial
sludge pH was 7.6.
Methodology
The heavy metal contaminated sludge was introduced into the
central tube of the electrokinetic cell, and then the electrode com-
partments were installed and filled with deionized water. Three
experiments were performed in different conditions (Table 3). In
experiment EK1, the pH in the electrode chambers was not con-
trolled and evolved according to the electrolysis of the water in the
anode and cathode. In experiments EK2 and EK3, the pH in the
catholyte was controlled at pH 2 with nitric acid (EK2 test) and
pH 4 with sulfuric acid (EK3 test). The electrodes were connected
to a DC power supply, and a constant voltage drop was applied for a
period ranging from 8 to 23 days. The EK1 test was operated at a
constant voltage of 15 V [1.5 DC voltage (DCV)/cm]. Tests EK2
and EK3 were operated at 30 V (3 DCV/cm). The voltage gradient
size, namely, from 1 to 5 from anode to cathode. Liquid samples
were collected from the anode and cathode compartments. All sam-
ples were stored at 4°C before analysis for pH and heavy metal
concentration.
Results
Experiments Performed under No pH Control
In this work, the sludge from an industrial wastewater treatment
plant was used to determine the feasibility of the electrokinetic
technology in the removal of heavy metals with the aim of valor-
izing the sludge and reducing the environmental risk. This sludge
contains a wide variety of metals (Table 2) and, among them, Mn
was of special concern given its high concentration and mobility,
as well as the former impact of Mn in the river basin where the
treatment plant was located. Thus, special attention has been paid
in this work to Mn removal.
Experiment EK1 was carried out in the electrokinetic cell with a
voltage drop of 15 DCV (1.5 DCV=cm). During the experiment,
the current intensity profile increased continuously and reached
a maximum value of 0.6 mA on the sixth day. Then, the current
intensity decreased slowly until it was 0.2 mA at the end of the
experiment. This behavior is common for the current intensity evo-
lution in electrokinetic tests. The increase in the current intensity
was the result of the increasing amount of mobile ions in the
interstitial fluid of the sludge. Then, those ions were transported
toward the anode and cathode, decreasing the ion concentration in
the interstitial fluid, resulting in a decrease in the current intensity
(Reddy and Ala 2005).
The evolution of pH in electrode chambers was the result of
water electrolysis (Cameselle 2015). The pH in the anode de-
creased from the initial pH 5.5 to pH 2 in six days, remaining al-
most constant until the end of the experiment. In the cathode, the
pH value increased up to pH 11 during the same period. The elec-
tromigration of Hþ and OH− ions toward the cathode and anode,
respectively, resulted in modification of the pH in the sludge speci-
men (Fig. 2). The pH decreased on the anode side and increased
on the cathode side. The initial pH value of the sludge was approx-
imately 7.6. After the experiment, the pH of the first section of
sludge (the one close to the anode) was 5.5. In the second section,

Table 3. Experimental conditions of electrokinetic tests and results of Mn removal and power consumption
Voltage Treatment Mn in cathode Residual Mn Power consumption Acid consumed
Test (V) time (d) solution (%) in sludge (%) (Wh/kg sludge) (mol Hþ =kg sludge)
EK1 15 23.4 0.85 98.87 0.016 0
EK2 30 8.2 68.1 24.62 2.85 3.32
EK3 30 23.0 66.3 26.95 2.94 3.46

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 12
only occurred in the first section of the sludge specimen, in which
10
the pH decreased by the Hþ ions from the anode. In this section, a
decrease was found in Ca, Mg, Sr, Zn, and Mn concentrations
8 (Figs. 3 and 4). The dissolved metals electromigrated toward the
pH (KCl)

Initial pH cathode but precipitated when reaching a higher pH zone. There-

6 fore, an increase was found in the concentration of these elements
in Sections 2–5. The actual sludge section in which those metals
4 precipitated depended on the sludge pH and the chemical nature of
each element (Cameselle and Pena 2016). All Mn removed from
2
Section 1 was accumulated in Section 2 (Fig. 3), as well as Zn
(Fig. 4). However, Ca concentration decreased in Sections 1 and
0
1 2 3 4 5 2 and accumulated in Sections 4 and 5 (Fig. 4). Ca was easily dis-
Soil section (anode-cathode) solved from carbonates and hydroxides in the sludge by the attack
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of Hþ ions.
Fig. 2. pH profile in sludge after experiments EK1, EK2, and EK3.

Experiments Performed under pH Controlled

the pH remained in the initial value, and in Sections 3, 4, and 5, the
pH ranged from 8.3 to 9.3. The Hþ ions electrogenerated in the
anode were transported by electromigration into the sludge speci-
men. Protons that reacted with sludge components (e.g., carbonates,
hydroxides) dissolved heavy metals that were then free to be trans-
ported by electromigration. Heavy metals can also be dissolved by
direct attack of Hþ ions from the mineral matrix. This phenomenon
Conditions
Given the strong influence of pH in the mobilization and transpor-
tation of heavy metals from the sludge, experiments EK2 and EK3
were carried out under pH control conditions in the cathode solu-
tion. In experiment EK2, the pH in the cathode was adjusted
to pH 2 with nitric acid. The acid environment in the cathode
avoided the alkalization of the sludge specimen and increased
its electric conductivity; therefore, the electric current intensity

Fig. 3. Normalized concentration of Al, Na, Fe, Mn, K, and Zr elements in sludge specimen at end of experiments EK1, EK2, and EK3.

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Fig. 4. Normalized concentration of Ca, Sr, Ti, Zn, Mg, and Cu elements in sludge specimen at end of experiments EK1, EK2, and EK3.

in the electrokinetic cell increased. In these conditions, the acid
front that electrogenerated in the anode was able to acidify the
sludge specimen from pH 7.6 to ph 4 in just eight days (Fig. 2).
The anode pH dropped to 1 in this test (EK2). Given the acidifi-
cation of the sludge specimen, the electrical resistance of the entire
system decreased; therefore, the current intensity continuously in-
creased up to 268 mA (in 8 d). This increase was the result of the
large amount of ions available to transport the electric current in the
sludge. The main ions responsible for the transport of the charge
include protons, and the other metal ions dissolved from the sludge
by the acid attack. The power consumption was 2.85 Wh=kg of
sludge (331 Wh), much higher than the consumption in the EK1
test (Table 3). The nitric acid consumed in the neutralization of the
catholyte was a relatively high 3.32 mol Hþ =kg of sludge. In this
experiment, a significant reduction in metal content in the sludge
was observed, especially for the elements Fe, Ca, Mg, Na, Mn, Sr,
Zn, and Cu (Figs. 3 and 4, Table 4). The final concentration profile
remained nearly constant for most of the metals removed, sug-
gesting that the maximum removal was achieved for those species,
and the residual element in the sludge was associated with the crys-
talline structure of the minerals and cannot be removed by electro-
kinetics. This nonremoval is not a problem because the metals in
the crystalline structure are not bioavailable (Cameselle et al.
2003). A sample of 2 g of dried sludge was placed in a flask with
100 mL of HCl 1 M to confirm the maximum metal extraction with
acid leaching. The mixture was shaken for 24 h at room temper-
ature. Then, the metal concentration was measured in the superna-
tant fluid. The results in Table 4 proved that the acid leaching was
able to remove Fe, Ca, Mg, Na, Mn, Sr, Zn, and Cu, whereas minor
amounts of Al, K, Ti, and Zr could be solubilized. The assumption

Table 4. Heavy metal removal in electrokinetics tests and heavy metal solubilization in acid leaching with HCl 1 M
Heavy metal removal/solubilization (%)
Test Al Fe K Ca Ti Mg Na Mn Zr Sr Zn Cu
EK1 2 1 — 4 3 — 3 — 7 3 4 —
EK2 — 27 — 68 — 24 25 68 2 33 60 60
EK3 8 21 3 61 1 30 — 66 — 21 56 30
Acid leaching (HCl 1 M) 12 60 5 95 1 45 47 92 5 40 80 81

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 was that these metals were components of the mineral matrix of
silicates and micas, among others, and are not affected by acid
extraction.
Experiment EK3 was carried out to neutralize the catholyte with
the controlled addition of sulfuric acid. The pH in the cathode was
controlled to pH 4. Similar to the EK2 test, the pH in anolyte
dropped to pH 1, but the acidification of the sludge specimen in
this test (EK3) was slower. The electric current intensity continu-
ously increased along the treatment time but not as fast as observed
in experiment EK2. After 23 days, the current intensity was only
62 mA. The power consumption was almost the same as observed
in experiment EK2 at 2.94 kWh=kg of sludge (359 Wh), as well as
acid consumption of 3.46 mol Hþ =kg of sludge. At the end of the
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test, the pH in sludge reached a very low value (pH 2), the result of
slow acidification by the acid front for 23 d. The metal removal was
similar in these two experiments EK2 and EK3 (Figs. 3 and 4,
Table 4), although some metals indicated better removal in test
EK3. The acid leaching of the sludge is responsible for maximum
heavy metal removal that can be achieved by electrokinetics with
pH control in the cathode. As is indicated in Table 4, higher re-
moval could be achieved for several metals, such as Mn, Sr, Zr,
and Cu. Therefore, the electrokinetic treatment should be extended
to reach the maximum removal of heavy metals, and the most
favorable conditions are those used in experiment EK3 (pH control
of 4 in the cathode) to avoid higher energy and acid consumption.
Overall, these results suggest that the electrokinetic remediation
can be used for the removal of heavy metals from the sludge as the
first step in its valorization. The relatively high energy and acid
consumption are the main limitations for scaling up the electro-
chemical treatment of the sludge.
Conclusions
Electrokinetic remediation was proven to be a useful technology
for the removal of metals from the sludge. The removal of metals
requires the acidification of the sludge and the mobilization of the
metals. Thus, the metals can be transported by electromigration
toward the cathode. The pH is the key variable to achieve metal
extraction and dissolution from the sludge. Metals are dissolved by
the acid attack of carbonates, hydroxides, and other solid compo-
nents in the sludge. The pH value in the sludge and in the anolyte
and catholyte has a critical influence on the current intensity, elec-
trical resistance, electric field distribution, and power consumption.
The results presented in this study confirmed that the cathode
pH should be acidic to obtain large metal removal during short
treatment time, but very low pH in the cathode tends to increase
the consumption of acid and energy. Therefore, an intermediate
pH value should be selected at the cathode (e.g., pH 4) to favor
metal removal without significantly increasing energy and chemi-
cals costs.
Data Availability Statement
Some or all of the data, models, or code generated or used during
the study are available from the corresponding author by request
(sludge characteristics, metal concentrations in sludge before and
after the treatments, test conditions, and experimental setup).
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