Journal of Electroanalytical Chemistry 880 (2021) 114890

Contents lists available at ScienceDirect

Journal of Electroanalytical Chemistry

journal homepage: www.elsevier.com/locate/jelechem

Effects of electro-osmosis on the properties of high plasticity clay soil:

Chemical and geotechnical investigations
Hossein Azizi Mir Mahalleh, Mehdi Siavoshnia , Maryam Yazdi
⁎
Islamic Azad University, Central Branch, Tehran, Iran

A R T I C L E I N F O A B S T R A C T

Article history: Electro-osmosis is a phenomenon describing the motion of liquid adjacent to a charged surface under the influence of
Received 23 July 2020 an electric field. Electro-osmosis is considered as an efficient soft soil improvement technique.
Received in revised form 21 November 2020 In this study, series of laboratory tests were performed utilizing graphite and stainless steel electrodes under three
Accepted 25 November 2020
levels of voltage gradients for 28 days using the soil from north of Iran to investigate the effect of various parameters
Available online 28 November 2020
on electro-osmotic and geotechnical properties. Moreover, the microstructure and chemical analyses of the soil before
Keywords:
and after treatment gave an in-depth perspective to underlying mechanism of this process.
Electro-osmosis processing Water drainage which has the most important effect on consolidation of soils, terminated after a few days. The termi-
Ion migration nation time for stainless steel is smaller than graphite and the whole drained water volume is larger in case of stainless
Dewatering steel compared to graphite.
Plastic soil The strength around the anode is larger than that of the cathode zone and the stainless steel electrode induced larger
Microstructure strength than the graphite electrode.
The SEM images exhibited the agglomeration of the soil after electro-osmosis treatment, and some precipitation was
also identified, which was attributed to iron based compounds. Chemical analysis illustrated that the concentration
of calcium ions decreased around the anode and increased near the cathode while Fe and Al amount did not change
significantly, implying the ion exchange and ion migration due to the electro-osmosis process. Additionally, the stain-
less steel electrode introduced iron and chrome ions to the soil, which affected structure and chemical distribution of
the ions.

1. Introduction disturbing the local activities [11]. The application of electro-osmosis on

Electro-osmosis is the process of water transport from the anode to the
cathode through a porous media under the influence of an electric field.
This was first described by Reuss [1] by placing a powdered quartz at the
bottom of a U-tube and applying an electric current to it. He observed
the rise of the water in the arm containing the cathode. It was concluded
that water can overcome to the gravity under electric field without any
mechanical power.
From a geotechnical viewpoint, soil acts as the porous media. This phe-
nomenon has promising applications in various fields, such as petroleum
[2] as well as heavy metals removal from the soil [3–5], soil improvement
[6], and dewatering of sludge [7], mine tailing [8], and clays [9]. Among
these applications, electro-osmosis displays great advantage in remediation
of low permeable soils. The first research on this field was performed by
Casagrande at 1952 [10]. Since then, electro-osmosis has attracted increas-
ing attention to enhance the physical and mechanical properties of the low
permeable soils, owing to its advantage of cost-effectiveness, rapid installa-
tion, easy operation, relatively short duration of the treatment, and not
engineering properties of soil was investigated by various research groups
[12–16].
The clay particles are negatively charged and the cations are adsorbed
on their surface due to the attractive forces. Water generates a double dif-
fuse layer (DDL) in aqueous conditions. The inner layer is a zone where cat-
ions are held tightly, and this immobile layer is called the Stern layer. The
outer layer, which is called the diffusion layer, attaches loosely to the parti-
cles and is mobile [17]. When an electric field is applied to the wet soil, the
cations and water molecules that clump around the particles in the diffu-
sion layer migrate toward the cathode, whereas anions flow in the opposite
direction, creating chemical, electrical, and hydraulic gradients [18]. When
electro-osmotic flow occurs, water is effectively pumped through the capil-
lary pore network of the soil that separates the cathode and anode [19].
This flow carries out via four main mechanisms including electrolysis,
electro-osmosis, electrophoresis, and electro-migration. The intricacies
of this process in microscopic level is due to numerous geochemical as
well as electrochemical reactions, such as cation exchange, hydrolysis,
electrophoresis, and diffusion which take place during the treatment [11].

⁎ Corresponding author.
E-mail address: meh.siavoshnia@iauctb.ac.ir (M. Siavoshnia).

http://dx.doi.org/10.1016/j.jelechem.2020.114890
1572-6657/© 2020 Elsevier B.V. All rights reserved.
H.A.M. Mahalleh et al. Journal of Electroanalytical Chemistry 880 (2021) 114890

The combined effects of these incidents cause significant changes in physi- Table 1
cal and engineering properties of the soil. The clay soil microstructure con- Properties of the test soil.
taining silicate plates have edge to face or face to face contacts with Values
significant voids separating them. Electro-osmosis treatment also makes Unified soil classification CH
changes in this structure. Abraham et al. investigated the effect of electro- Specific gravity 2.43
osmosis process using an AC power source on oil sands tailings. They re- Maximum dry density(g/cm3) 1.76
ported the collapse of the stable structure of the soil during the dewatering In-situ water content% 32.27
Optimum moisture content 19.9
process [20]. Change of the morphology of the soil after the electro-osmosis
LL% 54
treatment was also reported by other researchers. Peng et al. reported that PL% 23
the pore size distribution in clay was impacted due to the electro-osmosis PI% 31
flow [21]. Compressive strength (kPa) 72
Multiple parameters affect the performance of the process, such as volt-
age level, electrode spacing and initial water content. It is well-established
that electrode material is a critical factor for this process. Several electrode 2.2. Experimental setup and sample preparation
materials including metallic and nonmetallic ones have been tested on var-
ious kinds of soil. For instance, Liu compared Aluminum and copper elec- The electro-osmotic tests were performed in a Plexiglass box 50 cm in
trodes by testing them on sludge and found that Al yielded a faster length 30 cm in width and 20 cm in height. Schematic diagram of the appa-
drainage and lower energy consumption than copper [22]. Tao [23] inves- ratus used in the experiments is shown in Fig. 1. Two series of Experiments
tigated the effect of ferrum, graphite, copper, and aluminum on typical were conducted using tubular stainless steel pipes and the graphite pipes
Hangzhou soft soil consolidation and concluded that the performance of with 15 mm diameter and 12 cm length as electrodes. In order to enable
the electrode depends on the voltage level. Ferrum and graphite electrodes the liquid to move freely, holes were pierced on the electrodes. The test
were reported to have quite similar performance under a higher voltage was carried out with two anodes and two cathodes placed in a rectangular
gradient, and both are better than copper electrode. Conversely, in a configuration. The space between identical electrodes was 15 cm while the
lower voltage gradient, a copper electrode is better than a ferrum electrode distance between non-identical electrodes was 30 cm.
and both are better than graphite. In contrast, Zhou [24] found that the per- As other researchers suggested, continuous flow of water from anode
formance of graphite was better in high voltages than metal electrodes. improves the electro-osmosis flow through the soil [18]. Thus, excess
Overall, considering the different ions which were added to soil due to elec- water was supplied to the soil from the external reservoir and via the
trode corrosion, they suggested the iron electrode as the efficient one [24]. holes on anode. The untreated soil was oven dried, pulverized, and then
Hu [25] and co-authors tested three types of electrode on sodium bentonite
soil and reported the same energy consumption per milliliter water for Al,
stainless steel, and graphite, although copper showed better water drain-
age. Peng et al. used a titanium mesh coated with iridium oxide as the cor-
rosion resistant electrode [21]. Recently, use of new materials, such as
geotextiles, were also reported. Fourie et al. reported the successful use of
geotextile electrode materials in mine tailing dewatering. They observed
no sign of electrode deterioration even after 2 months of usage. However,
the applied voltage gradient in their work was 0.11 V/cm which is too
low compared to other researchers [8]. Estabragh et al. used the electrical
vertical drains (EVD) in the form of a sheet made of copper foil in the mid-
dle, surrounded by conductive polymer [26]. Kaniraj et al. also used EVD
for strengthening of the peat of North Sarawak. They used commercially
available EVD consisting of polyethylene core which encapsulated a
90 mm wide copper foil [27]. Overall, the results obtained from various
studies do not support each other.
According to inconsistent results, the value of the electrode depends
largely on the type of the soil as well as test conditions, which prevents ap-
plying the results to other soils and conditions. Therefore, studies on the ef-
fect of electrode materials on electro-osmosis treatment are still required. In
this paper the soil from north of Iran, where the soft soils are fairly wide-
spread, is used for treatment. Two kinds of electrode containing stainless
steel and graphite are investigated in detail. For further examination, mi-
grated ions and microscopic structure of the soil were also studied by scan-
ning electron microscopy and Energy Dispersive X-ray Spectroscopy (EDS).

2. Materials and methods

2.1. Soil properties

The soil sample was obtained from 1 to 1.5 m depth of Hassan-Roud re-
gion, Ruodsar, Guilan province, Iran. The original physical and mechanical
properties of crude soil are determined by conducting various analyses in-
cluding specific gravity, water content, density, and liquid limit (LL), plastic Fig. 1. a-Schematic configuration of electro-osmotic apparatus. b- Plan view of the
limit (PL), and plasticity index (PI). The results are presented in Table 1. laboratory setup. 1: Penetration test locations and 2: The cathode, the middle, and
This soil is categorized in high plasticity clays (CH) group based on the the anode zone.
Unified Soil Classification System.

2
H.A.M. Mahalleh et al.
mixed with enough water to reach the moisture content of the local soil.
Then, it was placed in a cell in layers and compacted to a final height of
16 cm. The cell was left stationary for 24 h in order to stabilize the water
content of the soil. Then, the locations of the electrodes were evacuated
from the soil before electrodes were placed in the soil. Electrodes were con-
nected to a direct current (DC) power supply. Experiments were repeated
for each electrode with varying levels of voltage gradients of 0.5, 1, and 2
(V/cm). Discharged water was drained via a vacuum pump which was
placed adjacent to the cathode and leading to a reservoir. The experiments
were carried out at room temperature and surface of the soil was in contact
with air.
2.3. Analysis and measurements
Compressive strength of the soil was evaluated by an Elijkelkamp
pocket penetrometer during the test. Penetration readings were recorded
at four points for each region on the surface of the soil that is marked in
Fig. 1 at time intervals of 7, 14, and 28 days. Atterberg limits and water con-
tent were detected as important physical characteristic of the soil from
three regions around the cathode, the anode, and the middle part. The mea-
surements of Atterberg limits and water content were performed according
to the ASTM D4318 and ASTM D2216, respectively. Volume of the
discharged water was also monitored daily during the process.
The microstructure and elemental content of the soil which were
treated under 2 (V/cm) was investigated before and after process. The mi-
croscopic morphology was investigated by SEM (FEI ESEM QUANTA 200)
and the elemental contents of soil measured by EDS (Silicon Drift 2017)
analysis.
3. Result and discussion
3.1. Physical and engineering properties
Fig. 2 represents accumulative water drainage as a function of time up
to 28 days for graphite and stainless steel electrodes under different voltage
gradients—0.5, 1, and 2 (V/cm). As noted in Fig. 2, the volume of drained
water showed rapid growth at first and then reached a steady state. For in-
stance, the 80% of total drainage was extracted at less than 5 days for stain-
less steel and voltage gradient 2(V/cm).
Increasing the voltage gradient increased the water drainage volume of
the system and decreased the termination time for both electrodes. High
water drainage translates to more electro-osmosis flow. This is due to en-
hancement of the field strength between the cathode and the anode by in-
creasing the voltage gradient. This caused more water drainage and also
accelerated the transport of the water. This is evident by the overall
Fig. 2. Accumulative water drainage for graphite (G) and stainless steel (S.S.)
electrodes.
3
Journal of Electroanalytical Chemistry 880 (2021) 114890
decrease in the cessation time shown in Fig. 2. Other researchers also
have reported the enhancement of drained water volume by increasing
the voltage gradient [24,28,29].
In the case of stainless steel electrode, termination time of dewatering
are 27, 20, and 13 days for 0.5, 1, and 2 (V/cm), respectively. Termination
time of water flow shifted to longer values, and water drainage is also
lowered by exploiting the graphite electrode compared to stainless steel.
The differences increased further by increasing the voltage gradient
which was associated with a more efficient performance for the stainless
steel electrodes over the graphite in all voltages, owing to more conductiv-
ity of stainless steel.
Drained water volume after 28 days and under voltage gradient of
2(V/cm) was 2802 (ml) for stainless steel electrode which is 10% larger
compared to the graphite electrode with 2528 (ml) drained water in similar
conditions. Iron electrode was reported to have better performance com-
pared to graphite electrode especially at low voltage, since increasing the
potential gradient enhances the performance of the latter more than former
[24]. It is worth to mention that Xu have carried out the experiments for
30 h and subsequently their results [24] are not expandable to 28 days.
Water drainage of each day for both electrodes is illustrated in Fig. 3,
which shows that the water flow is more homogenous in graphite than
stainless steel. This could be attributed to corrosion of stainless steel elec-
trodes, which cause the decrement in conductivity and the drainage. In ad-
dition, corrosion changes soil composition due to entrance of Fe ions. Note
that drainage is slower and more homogenous in graphite electrode due to
inert nature of it.
The parameter governing the electro-osmotic flow in a soil mass is
the coefficient of electro-osmotic permeability, Ke, defined by an empirical
relation:
Qe ¼ Ke E ð1Þ
Where Qe is the flow rate per cross section area normal to flow direction
(m/s), Ke is the coefficient of electro-osmotic permeability (or electro-
osmotic permeability) (m2/(s × V)), and E is the electrical field intensity
(V/m) [30]. The values of Ke were calculated considering the Eq. 1 and
using the drained water volume of both electrodes under voltage gradient
1 (V/cm). The results were illustrated in Fig. 4. The initial values of Ke de-
creased rapidly with time in all experiments and reached equilibrium after
some days. Decrement of Ke with time during electro-osmosis treatment
also have been reported by other [29,31].The results show that the
coefficient of electro-osmotic permeability for stainless steel electrode
was higher compared to graphite electrode. However, the differences
Fig. 3. Water drainage per day for two electrodes.
H.A.M. Mahalleh et al.
Fig. 4. Variation of electro-osmotic permeability coefficient versus treatment time
for stainless steel and graphite electrodes under voltage gradient 1 (V/cm).
were considerable in first five days, and they reach to almost same quantity
after a few days.
Water content of the soil in different samples in the anode, the cathode
and the middle are reported in Figs. 5 to 7, respectively. Unlike water drain-
age, the water content decreased continuously for 28 days. Water content
might have decreased due to electro-osmosis flow as well as evaporation.
Considering the high slope of drained water volume during the first days
in Fig. 2, one can conclude that electro-osmosis is more significant during
this interval. The electrical resistance of soil, which causes the generation
of heat due to the applied electric field, as well as exothermic reactions
which take place in soil generate tremendous amounts of heat in the soil.
Therefore, the evaporation could also play a role in decreasing the water
content. Zhang et al. reported the temperature of 260 °C in some part of
the soils which can induce high evaporation of water [6].
Under voltage gradient 2(V/cm), water content for stainless steel and
graphite electrodes around the anode were respectively 21.21 and 22.7%
after 14 days. Around the cathode, the same value increased to 25.76 and
27.45%, respectively. Cations migrate from the anode to the cathode
under the potential gradient while carrying the drained water. Thus,
Fig. 5. Water content of the soil at anode vicinity.
4
Journal of Electroanalytical Chemistry 880 (2021) 114890
Fig. 6. Water content of the soil at middle zone.
orientation of the electro-osmosis flow is from the anode toward the cath-
ode, leading to less water content in the anode zone compared to that of
the cathode.
Increasing the voltage made the water content diminish due to more
electro-osmosis flow and more heat generation. Voltage gradient of 0.5
(V/cm) results in 14% decrement in water content in the anode zone after
14 days. However, increasing the voltage gradient to 2 (V/cm) for same du-
ration of time decreases the water content by 31.8%. This behavior was also
reported by Bergado et al. [32].
Figs. 8 to 10 illustrate the compressive strength of the soil in the anode,
middle, and cathode zones after 7, 14, and 28 days of treatment under volt-
age gradients of 0.5, 1, and 2 (V/cm) for the graphite and stainless steel
electrodes. The strength increases during the time and the slope is greater
for the first 14 days, and then, it decreases for further days. Additionally,
the strength is also larger in the anode than the middle and the cathode.
Considering the voltage effect, it appears that soil strength increased with
increasing voltage gradients and the best improved result belongs to the
voltage gradient of 2(V/cm). In case of stainless steel electrode, the strength
of the anode part increased for 24% after 7 days and 70% after 28 days,
Fig. 7. Water content of the soil at cathode vicinity.
H.A.M. Mahalleh et al.
Fig. 8. Compressive strength of anode zone under various voltage gradient for two
electrodes.
both under 0.5(V/cm) compared to untreated soil. Increasing the voltage
gradient to 1 (V/cm) changed the former to 39% and the latter to 107%.
Maximum increase in strength is 126% which was recorded after 28 days
under voltage gradient of 2(V/cm) in stainless steel electrode.
Although appreciable improvements of strength were observed around
the cathode and middle, the larger increase in strength are noted around
the anode for both electrodes. This trend also was reported by other re-
searchers [27,32]. For instance, the strength increased to 59% in the vicin-
ity of the anode for the graphite electrode after 14 days and under voltage
gradient of 1(V/cm). The strength increased by about 52% and 25%,
respectively, for the middle and the cathode area.
Although both graphite and stainless steel electrodes showed the same
trend under different voltage and time, the stainless steel electrode had su-
perior effects than the graphite electrode. For instance, the soil in the anode
zone of stainless steel electrode showed 92% increase in strength, after
14 days under voltage gradient of 2(V/cm), while for graphite electrode
Fig. 9. Compressive strength of middle part under various voltage gradient for two
electrodes.
5
Journal of Electroanalytical Chemistry 880 (2021) 114890
Fig. 10. Compressive strength of cathode zone under various voltage gradient for
two electrodes.
in the same conditions it represented 69% improvement. This trend was ex-
pectable due the direction of electro-osmosis flow and was also observed by
Kaniraj et al. [27].
Consolidation of soil can be achieved through various mechanisms. The
pore water was dragged from the anode to the cathode due to cation migra-
tion in response to the electric field. The flow leads to negative pore pres-
sure, which destroys the pores, consolidates the soil, and increases the
soil's strength. This phenomenon can be inferred from SEM images which
will be discussed further in the next sections. The second mechanism in-
volves the diffuse layer flow under electric field from the anode to the cath-
ode, which drags more water toward the cathode and also imposes viscous
attraction to the pore free water. Moreover, replacement of the cations with
smaller hydrated ions in DDL decreased the layer thickness. This made the
soil particles to be densely packed and the soil to be strengthened. This
mechanism is also confirmed by chemical analysis of the soil in next
section.
Fig. 11. Water content and compressive strength of anode zone under various
voltage gradient for stainless steel electrode.
H.A.M. Mahalleh et al. Journal of Electroanalytical Chemistry 880 (2021) 114890

Fig. 12. Water content and compressive strength of cathode zone under various Fig. 14. Water content and compressive strength of cathode zone under various
voltage gradient for stainless steel electrode. voltage gradient for graphite electrode.

Considering the above mentioned mechanisms, one can notice that
these mechanisms are related to water content of the soil, which is observed
in the results. As shown in Figs. 11 to 14 water content decreased from the
cathode to the anode, while the strength of soil increased for both elec-
trodes. Increasing the voltage also increased the water drainage and de-
creased the water content, thereby improving the strength. The direct
relationship between strength of soil and water content has been confirmed
almost by all researchers [32,33].
On the other hand, transportation of cations through the soil accompa-
nied by pH gradient enhanced the probability of the different reactions be-
tween various cations and the soil, which in turn changed the chemical
content of the soil. Cementation is one of these reactions which could
help improve the soil strength. In our case, the calcium ions of the soil as
well as the Fe ions released from stainless steel electrode participated in
the cementation process which will be discuss in the elemental analysis
section. This could be a reason for improved strength of the soil in the
case of stainless steel electrode rather than graphite.
Although the water drainage due to electro-osmosis process reduce sig-
nificantly after 14 days, the strength of the soil continues to increase with
low rate. Drying of soil could also have role in strengthening the soil after
14 days. The electrical resistance of soil, which causes the generation of
heat due to the electric current in the soil, as well as exothermic reactions,
which take place in soil, generate tremendous amounts of heat in the soil.
This heat could cause evaporation of water and decreasing the water con-
tent. Thus, one might consider its role in strengthening the soil [18].
In summary, the most strengthening of the soil relies on the contribu-
tions from electro-osmosis phenomenon, including the main mentioned
mechanisms. Alongside with electro-osmosis flow, drying and cementation
also could be considered as other mechanisms. Ion diffusion was also men-
tioned as another mechanism by other researchers after termination of
electro-osmosis flow [18].
Table 2 summarizes LL, PL, and PI of untreated and treated soil after
28 days under the voltage gradient of 2(V/cm) in the anode and the cathode
zone. LL decreased about 9 and 7% in the anode zone, whereas it increased
about 1.9 and 3% in the cathode zone of stainless steel and graphite elec-
trodes, respectively, after 28 days. The same trend was observed in plastic
limit around the anode and the cathode. PL showed 7.8 and 6.5% decrease
around the stainless steel and graphite anodes, respectively. Additionally,
remarkable decrease (about 15%) in the cathode region of both electrodes
were observed as well. PI decreased due to the combined effect of LL and PL
in all parts of the soil, which indicated the reduction of water adsorption

Table 2
Liquid limit(LL), Plastic limit(PL) and plasticity index(PI) of untreated and treated
soil after 28 days under the voltage gradient of 2(V/cm) in anode and cathode zone.
Electrode Location Atterberg limits

LL PL PI

Untreated 54.69 23.34 31.35

Fe Anode 49.8 21.5 28.3
Middle 50.45 25.1 25.35
Cathode 55.75 26.8 28.95

Gr Anode 50.8 21.8 29

Middle 50.9 24.8 26.1
Fig. 13. Water content and compressive strength of anode zone under various
Cathode 56.4 26.9 29.5
voltage gradient for graphite electrode.

6
H.A.M. Mahalleh et al.
capacity of the soil. The change of the PI, which stabilized with stainless
steel electrode, was larger than that of the graphite electrode. These re-
sponses could be attributed to charge on soil's surface due to the change
in pH as well as the change in the thickness of double diffuse layers.
Electric current causes electrolysis of water around the electrodes [34].
Oxidation occurs at the anode, while reduction takes place at the cathode.
These reactions can be expressed as:
Anode : 2H2 O þ 4e− ! O2 þ 4Hþ
Cathode : 2H2 O þ 2e− ! H2 þ 2OH−
Reactions generate H+ at the anode, resulting in an acidic front, and
OH− at the cathode, inducing an alkaline front. The pH affects the surface
charge of the soil particles. By increasing the pH from the anode to the cath-
ode, negative surface charge of the soil particles is increased and causes the
PL to increase as well.
On the other hand, ion exchange during the electro-osmosis caused the
replacement of high valence ions such as Al3+ and Fe3+ in immobile water
layer around the soil particles and decreased the double layer thickness. In
addition, the attraction force of the soils particles reduced PL. Ion exchange
also resulted in the agglomeration and flocculation of the soil and changed
the microstructure of the soil as will be discussed in the next section.
3.2. Elemental investigation of the soil
EDS analysis was performed to determine the distribution of the ele-
ments before and after the electro-osmosis process. The obtained results
in the case of graphite electrode are illustrated in Fig. 15.
Al exhibited uniform presence throughout the soil, and their variation
was insignificant after electro-osmosis treatment, indicating the immobility
of these ions. This might result of exchange of these ions with low valence
ions in the soil [6] which could impede their migration and lead to uniform
distribution of the ions. Clay minerals adsorb different cations in their dou-
ble diffuse layers. Adsorbed cations can be replaced by other cations and
the replacing power depends on valence, concentration, and the hydrated
radius of the cations. In equal conditions the lower valence ions are re-
placed by higher valence ones. In this case, the Fe3+ and Al3+ would
Fig. 15. Ion distrbution in anode, cathode and middle part of graphite electrode.
7
Journal of Electroanalytical Chemistry 880 (2021) 114890
replace the calcium ions, and the exchanged calcium, then, enters the free
pore water, migrates toward the cathode, and the Fe3+ and Al3+ remain
in double layer. This process will decrease the thickness of double layers
and cause the shrinkage of the soil. Fe increased steadily in the concentra-
tion across the soil, but the insignificant variation implies the migration
of smaller amounts of Fe ions and their immobilization in major parts.
No notable variance in calcium content of middle and cathode parts was
observed, while both are much higher compared to the anode, implying the
migration of calcium ions through the soil from the anode to the cathode.
Thus, a decrease in the stability of the ions by increasing the pH and conse-
quent precipitation in the middle area is observed.
Mg also has uniform distribution in various areas, but the amount of
total Mg after treatment is less than that of the initial soil, indicating partic-
ipation of Mg in electro-osmosis flow and its depletion by the drainage
water. The change in distribution of elements confirmed the electro-
osmosis effects on chemical structure of soils which also induced changes
in geotechnical properties [24,35]. There have been also reports of change
in the concentration of elements by other researchers [36].
Distribution of elements before and after electro-osmotic stabilization in
different parts of the soil is demonstrated in Fig. 16 in the case of stainless
steel electrodes. EDS analysis revealed the significant increase of chromium
and iron ions, which are generated due to oxidation reactions of stainless
steel anode electrodes during the treatment.
The Chromium distribution after the electro-osmosis process demon-
strated the accumulation of ions around the anode. A fairly small content
could also be traced in other parts, indicating low migration of the chro-
mium under the influence of electric field, which is probably due to high va-
lence and weight of this ion. Fig. 15 shows that the Fe content around the
anode is much lower than the cathode and the middle part, with the latter
having the highest Fe concentration. This feature is completely different in
the case of the graphite electrode experiments. The amount of Fe ions near
the anode is almost equal to the initial concentration, indicating an almost
complete replacement of initial iron in the double layer and making these
ions immobile. However, increase in Fe concentration due to corrosion of
the anode caused these ions to be mobile.
Iron exists as soluble ions in acidic atmosphere and tends to precipitate
as iron oxide or iron hydroxide in higher pH. In the stainless steel elec-
trodes, oxidation of anode introduces the iron ion in the form of Fe2+ or
Fe3+ as active species directly into the soil. Then, they move toward the
Fig. 16. Ion distrbution in anode, cathode and middle part of stainless steel
electrode.
H.A.M. Mahalleh et al.
Fig. 17. a-. SEM images of the precipitated part in middle b- EDS analysis of the mentioned part.
cathode due to their mean mobility under the influence of electric field. As
mentioned above, the oxidation reactions near the anode and reduction re-
action near the cathode make a pH gradient in the soil that increases from
the anode to the cathode. Thus, as the ions moved further, pH and the con-
centration of the ions increased. Iron ions were precipitated as iron oxide or
Iron hydroxide at suitable pH. Consequently, the migration was stopped. To
further examine this process, SEM analysis was carried out and the images
confirm the existence of precipitate in the middle part— see Fig. 17-a. EDS
analysis of the precipitations showed high concentration of Fe in these pre-
cipitates which is consistent with more concentration of Fe in the middle
part (Fig. 17-b) and is in good agreement with the above mentioned expla-
nation. Different cementation products were introduced, including CaCl2,
calcium silicate hydrate (CSH) [37], 3CaO - 2SiO2-4H2O [38], iron oxides,
and calcium-aluminate [37]. These are believed to have roles in strengthen-
ing the soil.
It is noteworthy to mention that the pH of different parts was changed
during the process. Thus, the precipitation could be formed in different
parts at different times. Cementation of iron affects the strength and perme-
ability of the soil region.
Although there is some correspondence between these results and other
reports regarding various ion migrations and depletion, they are mainly dif-
ferent. For example, Hu et al. reported the poor migration of Fe in the soil
[6] which is consistent with our results in the case of graphite electrode.
However, they reported an increase in Ca content around the anode and
less migration of Ca ions which is not in agreement with our results.
Fig. 18. Microstructure of untreated soil.
8
Journal of Electroanalytical Chemistry 880 (2021) 114890
These inconsistencies could be attributed to higher Na concentration of
their soils.
As mentioned by Mitchell and Soga, the replacement of the ions, which
depends on some factors including relative abundance, translates to compo-
sition of untreated soils. In fact, the behavior of ions depend on the soil
composition and the condition of the tests including voltage gradient, dura-
tion of the process, and electrode materials [39].
Stainless steel electrode provides more ions to the soil, and therefore,
the substitution of exchangeable ions, such as Ca and Mg, was more com-
plete in the case of this electrode. This caused more transportation of ions
by pore free water and lead to greater decrease in the number of these
ions near the stainless steel anode compared to the graphite anode.
Trivial amount of calcium remained around the stainless steel anode,
and high concentration of it remained around the cathode. The former re-
sulted in high mobility of this ion through the soil, and the latter induced
the precipitation of calcium containing compounds around the cathode
which is observed macroscopically by white precipitation around the cath-
ode. It should be noted that the calcium solution is appropriate for improv-
ing the electro-osmosis performance due to its high ionic movement in the
soil. This process increases the electro-osmosis flow as well as the cementa-
tion process, which improves the soil's strength. This idea has been con-
firmed by various researches [28], but most of them presented no
chemical analysis after the injection. Thus, the reason for it was interpreted
by theory [40]. The calcium concentration in the middle part in the case of
graphite electrode is much higher than the stainless steel electrode in which
H.A.M. Mahalleh et al.
Fig. 19. Morphology of the soil at a- anode zone b- middle part c- anode zone after electro-osmosis with stainless steel electrode.
the calcium content of the middle zone is almost zero. This different feature
could be attributed to various pH gradients in the case of graphite and stain-
less steel electrodes. One reason for this is due to less conductivity of graph-
ite with respect to stainless steel and the unequal generation of H+ and
OH− ions at the two electrodes. Moreover, competing anodic dissolution
reaction of stainless steel electrodes leads to a smaller rate of H+ produc-
tion compared to OH−.
Although Al behaved similar in presence of both electrodes, the content
of Al in the stainless steel anode zone was slightly smaller than the graphite
anode. This result implied that the replacement of some of the Al3+ ions
with Fe ions that are provided by corrosion of the electrode.
3.3. Changing the microstructure
In order to obtain detailed structural information of the soil, SEM imag-
ing was performed, and the morphology of the untreated and treated soil,
which was due to the use of stainless steel and graphite electrode at differ-
ent part of the soil, was investigated. Fig. 18 illustrates the microstructure of
the air-dried soil prior to the electro-osmosis process wherein a two-
dimensional view of the porosities can be observed. Untreated soil exhib-
ited typical structure of soils consisting clumps of soil, which was the result
of the interaction between water and the soil. Silicate plates have edge to
face or face to face contacts with significant voids separating them and
causing high porosity. The structure of the soil in presence of water was
well exhibited by Abraham et al. [20] and Peng et al. [21], both of whom
9
Journal of Electroanalytical Chemistry 880 (2021) 114890
used Freeze Drying Scanning Electron Microscopy (FDSEM) technique to
demonstrate the clay structure.
Fig. 19 shows the effect of electro-osmosis in stainless steel electrode on
the morphology of the soil at different locations. Significant change in mi-
crostructure is detected. The soil near the anode part as well as in the mid-
dle part showed agglomeration of the clay plates, which due to their close
packing decreased the porosity. It is evident from the SEM images that
the aggregates oriented more face to face than face to edge. This highly
packed particles make the dense and impermeable structure of the soil. De-
creasing the porosity and agglomeration of the plates were less observed in
the cathode part—see Fig. 19-c.
As mentioned in previous sections, microstructure changes could be at-
tributed to two main mechanisms. First, the ion exchange process during
the electro-osmosis decreased DDL and packed the plate close to each
other. Consequently, the silicate layers moved closer to one another. Sec-
ond, depleting of the water from capillary pores induced a negative pres-
sure in the pores and either cause a decrease in the pore volume or
resulted in their disappearance. These two phenomena are most obvious
in the anode and decrease from that to the cathode as it is observable in
the images. The results of elemental analysis further support this
observation.
The SEM images of the soil after electro-osmosis treatment with graph-
ite electrode is shown in Fig. 20. Decrement of porosity also observed in the
case of graphite electrode, but its value was less than that of the stainless
steel electrode.
H.A.M. Mahalleh et al.
Fig. 20. Morphology of the soil at a- anode zone b- middle part c- anode zone after electro-osmosis with graphite electrode.
4. Conclusion
Series of electro-osmosis tests were conducted using graphite and stain-
less steel electrodes under three levels of voltage gradients for 28 days. The
influence of electro-osmosis treatment on the chemical and geotechnical
properties of the high plasticity clay soil was then discussed.
Water drainage was fast during the first days, but then, reached a steady
state. Water depletion was larger and faster in the stainless steel electrode,
while it was more homogeneous in the graphite electrode.
Strength of the soil decreased from anode to cathode for both electrodes
which was consistent with the water content as well as the direction of the
electro-osmotic flow. The best results were obtained for voltage gradient of
2(V/cm) for the stainless steel electrode which showed superior effects
compared to the graphite electrode.
Investigation of the concentration of the various ions in different parts
of the soil using EDS data confirmed the high mobility of some ions, includ-
ing Ca and Mg ions as well as the low mobility of others such as Cr, Fe, and
Al. Moreover, the corrosion of the stainless steel also influenced the electro-
osmosis process, because Fe and Cr ions are released in soil due to corro-
sion, which promote the conductivity of the soil as well as changing the
composition of it. Thus, it results in a different behavior from the soil in
presence of the electric field. The SEM images illustrated the agglomeration
of the soil particles and the decrease in void volume of the soil. The agglom-
eration decreased from the anode to the cathode, which is in agreement
with the change in strength.
Intellectual property
We confirm that we have given due consideration to the protection of
intellectual property associated with this work and that there are no
10
Journal of Electroanalytical Chemistry 880 (2021) 114890
impediments to publication, including the timing of publication, with re-
spect to intellectual property. In so doing we confirm that we have followed
the regulations of our institutions concerning intellectual property.
Research ethics
We further confirm that any aspect of the work covered in this manu-
script that has involved human patients has been conducted with the ethi-
cal approval of all relevant bodies and that such approvals are
acknowledged within the manuscript.
IRB approval was obtained (required for studies and series of 3 or more
cases).
Written consent to publish potentially identifying information, such as
details or the case and photographs, was obtained from the patient(s) or
their legal guardian(s).
Authorship
The International Committee of Medical Journal Editors (ICMJE) rec-
ommends that authorship be based on the following four criteria:
1. Substantial contributions to the conception or design of the work; or
the acquisition, analysis, or interpretation of data for the work; AND
2. Drafting the work or revising it critically for important intellectual
content; AND
3. Final approval of the version to be published; AND
4. Agreement to be accountable for all aspects of the work in ensuring
that questions related to the accuracy or integrity of any part of the
work are appropriately investigated and resolved.
All those designated as authors should meet all four criteria for author-
ship, and all who meet the four criteria should be identified as authors. For
H.A.M. Mahalleh et al.
more information on authorship, please see http://www.icmje.org/
recommendations/browse/roles-and-responsibilities/defining-the-role-of-
authors-and-contributors.html#two.
All listed authors meet the ICMJE criteria. We attest that all authors con-
tributed significantly to the creation of this manuscript, each having ful-
filled criteria as established by the ICMJE.
One or more listed authors do(es) not meet the ICMJE criteria.
We believe these individuals should be listed as authors because:
[Please elaborate below]
We confirm that the manuscript has been read and approved by all
named authors.
We confirm that the order of authors listed in the manuscript has been
approved by all named authors.
Funding
No funding was received for this work.
CRediT author statement
Hossein Azizi Mir Mahalleh: Methodology, Investigation, Visualiza-
tion, Resources, Funding acquisition. Mehdi Siavoshnia: Conceptualiza-
tion, Validation, Writing - Review & Editing, Supervision Maryam Yazdi:
Writing - Original Draft, Project administration
Declaration of Competing Interest
None.
References
[1] F.F. Reuss, Notice sur un nouvel effet de l'électricité galvanique, Mémoires de la Société
Impériale des Naturalistes de Moscou 2 (1809) 327–337.
[2] C.-S. Jeon, J.-S. Yang, K.-J. Kim, K. Baek, Electrokinetic removal of petroleum hydrocar-
bon from residual clayey soil following a washing process, CLEAN – Soil Air Water 38
(2) (2010) 189–193.
[3] S.-O. Kim, S.-H. Moon, K.-W. Kim, Removal of heavy metals from soils using enhanced
electrokinetic soil processing, Water Air Soil Pollut. 125 (1) (2001) 259–272.
[4] P.V. Sivapullaiah, B.S.N. Prakash, B.N. Suma, Electrokinetic removal of heavy metals
from soil, J. Electrochem. Sci. Eng. 5 (1) (2015) 47–65.
[5] K.N.O. Silva, S.S.M. Paiva, F.L. Souza, D.R. Silva, C.A. Martínez-Huitle, E.V. Santos, Ap-
plicability of electrochemical technologies for removing and monitoring Pb2+ from
soil and water, J. Electroanal. Chem. 816 (2018) 171–178.
[6] L. Zhang, L.-p. Jing, N.-w. Wang, C. Fang, Y.-q. Li, Z.-d. Shan, Electro-osmosis chemical
treatment of high-salinity soft marine soils: laboratory tests, Open Civil Eng. J. 11
(2017) 109–120.
[7] M. Iwata, T. Tanaka, M.S. Jami, Application of electroosmosis for sludge dewatering—A
review, Dry. Technol. 31 (2) (2013) 170–184.
[8] A.B. Fourie, D.G. Johns, C.F. Jones, Dewatering of mine tailings using electrokinetic
geosynthetics, Can. Geotech. J. 44 (2) (2007) 160–172.
[9] A. Dizon, M.E. Orazem, Advances and challenges of electrokinetic dewatering of clays
and soils, Curr. Opinion Electrochem. 22 (2020) 17–24.
[10] I.L. Casagrande, Electro-osmosis in soils, Géotechnique 1 (3) (1949) 159–177.
[11] N. Mosavat, E. Oh, G. Chai, A review of electrokinetic treatment technique for improv-
ing the engineering characteristics of low permeable problematic soils, Int. J. Geomate 2
(2012) 266–272.
11
Journal of Electroanalytical Chemistry 880 (2021) 114890
[12] L. Bjerrum, J. Moum, O. Eide, Application of electro-osmosis to a foundation problem in
a norwegian quick clay, Géotechnique 17 (3) (1967) 214–235.
[13] L. Casagrande, Stabilization of soils by means of electroosmotic, J. Boston Soc. Civil
Eng. ASCE 69 (1983) 255–302.
[14] M.I. Esrig, Pore pressures, consolidation and electro-kinetics, J. Soil Mech. Found. Div.
ASCE 94 (1968) 899–921.
[15] A.S. Burton, J.B. Clifford, Electroosmotic contaminant removal processes, J. Environ.
Eng. 118 (1) (1992) 84–100.
[16] J.Q. Shang, K.Y. Lo, Electrokinetic dewatering of a phosphate clay, J. Hazard. Mater. 55
(1) (1997) 117–133.
[17] B.K. Pandey, S. Rajesh, Enhanced engineering characteristics of soils by electro-osmotic
treatment: an overview, Geotech. Geol. Eng. 37 (6) (2019) 4649–4673.
[18] S. Jayasekera, Electrokinetics to modify strength characteristics of soft clayey soils: a
laboratory based investigation, Electrochim. Acta 181 (2015) 39–47.
[19] J.G. Sunderland, Electrokinetic dewatering and thickening. I. Introduction and histori-
cal review of electrokinetic applications, J. Appl. Electrochem. 17 (5) (1987) 889–898.
[20] T. Abraham, N. Lam, J. Xu, D. Zhang, H. Wadhawan, H.J. Kim, M. Lee, T. Thundat, Col-
lapse of house-of-cards clay structures and corresponding tailings dewatering induced
by alternating electric fields, Dry. Technol. 37 (9) (2019) 1053–1067.
[21] C. Peng, H. Lai, M.E. Orazem, S. Moghaddam, Microstructure of clay fabric in electroki-
netic dewatering of phosphatic clay dispersions, Appl. Clay Sci. 158 (2018) 94–101.
[22] Y.-m. Liu, H.-f. Xu, Experimental study of the electrode material for electro-osmosis in
mudflat sludge, IOP Conference Series: Earth and Environmental Science 2017,
p. 012093.
[23] Y. Tao, J. Zhou, X. Gong, Comparative experiment of electroosmosis of ferrum, graphite,
copper and aluminum electrode, Yanshilixue Yu Gongcheng Xuebao/Chin. J. Rock
Mech. Eng. 32 (2013) 3355–3362.
[24] J. Zhou, Y.L. Tao, C.J. Xu, X.N. Gong, P.C. Hu, Electro-osmotic strengthening of silts
based on selected electrode materials, Soils Found. 55 (5) (2015) 1171–1180.
[25] L. Hu, H. Wu, J.N. Meegoda, Effect of electrode material on electro-osmotic consolida-
tion of bentonite, Jpn. Geotech. Soc. Specl. Publ. 2 (59) (2016) 2027–2032.
[26] A.R. Estabragh, M. Naseh, A.A. Javadi, Improvement of clay soil by electro-osmosis
technique, Appl. Clay Sci. 95 (2014) 32–36.
[27] S.R. Kaniraj, H.L. Huong, J.H.S. Yee, Electro-osmotic consolidation studies on peat and
clayey silt using electric vertical drain, Geotech. Geol. Eng. 29 (3) (2011) 277–295.
[28] C.-Y. Ou, S.-C. Chien, Y.-G. Wang, On the enhancement of electroosmotic soil improve-
ment by the injection of saline solutions, Appl. Clay Sci. 44 (1) (2009) 130–136.
[29] L. Zhang, B.-H. Wang, L.-Y. Wang, L.-P. Jing, C. Fang, Z.-D. Shan, Performance improve-
ment in pile anchor system for deep foundation excavation using electroosmotic chem-
ical treatment, Adv. Civil Eng. 2019 (2019) 3168912.
[30] J.Q. Shang, Zeta potential and electroosmotic permeability of clay soils, Can. Geotech.
J. 34 (4) (1997) 627–631.
[31] J. Hamed, Y.B. Acar, R.J. Gale, Pb(II) removal from kaolinite by Electrokinetics, J.
Geotech. Eng. 117 (2) (1991) 241–271.
[32] D.T. Bergado, A.S. Balasubramaniam, M.A.B. Patawaran, W. Kwunpreuk, Electro-
osmotic consolidation of soft Bangkok clay with prefabricated vertical drains, Proc.
Inst. Civil Eng. - Ground Improv. 4 (4) (2000) 153–163.
[33] S. Jayasekera, S. Hall, Modification of the properties of salt affected soils using electro-
chemical treatments, Geotech. Geol. Eng. 25 (1) (2006) 1–10.
[34] A. Asadi, B.B.K. Huat, H. Nahazanan, H.A. Keykhah, Theory of electroosmosis in soil,
Int. J. Electrochem. Sci. 8 (1) (2013) 1016–1025.
[35] S. Yang, F. Jianting, S. Wen, Q. Chenchen, Effects of voltage gradients on electro-
osmotic characteristics of Taizhou soft clay, Int. J. Electrochem. Sci. 14 (3) (2019)
2136–2159.
[36] H. Wu, L. Hu, Microfabric change of electro-osmotic stabilized bentonite, Appl. Clay Sci.
101 (2014) 503–509.
[37] M. Kitazume, State of practice report– field and laboratory investigations, properties of
binders and stabilized soil, International Conference on Deep Mixing Best Practice and
Recent Advances 2005, pp. 660–684.
[38] S.-C. Chien, C.-Y. Ou, Y.-H. Wang, Soil improvement using electroosmosis with the in-
jection of chemical solutions: laboratory tests, J. Chin. Inst. Eng. 34 (7) (2011) 863–875.
[39] J.K. Mitchell, K. Soga, Fundamentals of Soil Behavior, Wiley, 2005.
[40] S.-C. Chien, C.-Y. Ou, M.-K. Wang, Injection of saline solutions to improve the electro-
osmotic pressure and consolidation of foundation soil, Appl. Clay Sci. 44 (3) (2009)
218–224.