Geo-Frontiers 2011 ASCE 2011 836

Modeling of Heavy Metals Transport in High Acid Buffering Soil During

Electrokinetic Remediation

Ashraf Z. Al-Hamdan1 A.M. ASCE and Krishna R. Reddy2, M. ASCE

1
Lecturer, Department of Civil and Environmental Engineering, University of
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Alabama in Huntsville, 301 Sparkman Drive, Huntsville, AL 35899; email:

alhamdan@eng.uah.edu
2
Professor, Department of Civil and Materials Engineering, University of Illinois at
Chicago, 842 West Taylor Street, Chicago, IL 60607; email: kreddy@uic.edu

ABSTRACT

This paper addresses the soil-contaminant-water interactions in a high acid

buffering soil during electrokinetic remediation. A one-dimensional transport model
was developed to predict the transport and speciation of heavy metals (chromium,
nickel, and cadmium) in high acid buffering glacial till soil during electrokinetics.
The developed model assimilates geochemical reactions into electrokinetic transport
modeling. The transport model incorporates: (1) presence of carbonates in soil; (2)
adsorption of contaminants to soil surface; and (3) synergistic effects of multiple
chemical species on contaminant transport during electrokinetic remediation. The
model was validated with bench-scale electrokinetic experiments. The predicted pH
profiles, electroosmotic flow, and contaminant distribution of chromium, nickel, and
cadmium in glacial till soil during electrokinetic remediation were found to agree with
the experimental results. The model also predicted the contaminant speciation and
form (aqueous, adsorbed, and precipitated) in soil during electrokinetics. The model
showed that chemical precipitation and adsorption are, respectively, the main fixation
mechanisms for the cationic (nickel cadmium) and anioinic (hexavalent chromium)
metals in glacial till during electrokinteic remediation. Overall, the model predictions
allowed for an understanding of the transport and physico-chemical processes that
control electrokinetic remediation of high acid buffering contaminated soil.

INTRODUCTION

Electrokinetic remediation is one of the developing techniques that have

significant potential for in-situ remediation of heavy metal fine-grained contaminated
soils. The implementation of eletrokinetic remediation involves inserting electrodes
into the soil to encompass the contaminated/plume area and applying low electric
potential across the electrodes. The electric potential induces the migration of
contaminants towards the electrodes by two primary transport processes, namely,
electromigration and electroosmosis. The transported contaminants to the cathodes
can then be extracted by different methods such as electroplating, precipitation,

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complexing with ion-exchange resins, or pumping the water near the electrode
with proper disposal (Acar and Alshawabkeh 1993; Lindgren et al. 1992).

Although electrokinetic remediation technology is simple and easy to

implement, the chemistry of heavy metals in soils under the application of electric
potential is complex. The application of a direct electric current to a soil system
results in several changes within the soil medium such as pH, redox potential and
electrolyte concentration. Such changes may impact the nature of the pore water and
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clay surface chemistry and the success of the electrochemical remediation. In

addition, the driving mechanisms for flux occur at interface between the soil particles
and solution, and the nature of this interface affect the elecktrokinetic response of the
system. Moreover, the total system response depends on the interaction of a complex
set of interrelated system variables and parameters. Electrokinetic modeling is a key
element in understanding the various changes within the soil-water system during
electrokinetics. In literature, many models have been developed to predict
contaminant transport during electrokinetic remediation (Kim, 1998; Haran et al.
1997; Yu and Neretnieks 1996; Menon 1996; Choi and Lui 1995; Yeung and Dalta
1995; Jacobs et al. 1994; Eykholt and Daniel 1994; Shapiro and Prbshtein 1993;
Alshawabkeh and Acar 1992). However, many of these models are limited to a single
contaminant and do not account for the geochemistry of heavy metals accurately.
Furthermore, the major drawbacks of these models are that they (1) do not account for
the synergistic effects of multiple chemical species on electrokinetics (2) do not
account for the presence of carbonates or reducing agents in soil (3) do not account
for the sorption reactions or the pH-dependent of contaminant adsorption to the soil,
and/or (4) neglect the effect of pH changes and ionic strength of pore water on the
surface potential of the solid surfaces. In addition, these models are validated for one
simulation time that is the treatment duration. However, most of these studies were
concerned with the residual contaminant distribution in the soil and the overall
removal efficiency after the elctrokinetic treatment. Unfortunately, these studies do
not investigate a detailed chemical speciation of the contaminants or how the
contaminants are held (retained and bounded) to the soil constituents. A detailed
assessment of speciation and distribution of contaminants will provide possible
reasons for low contaminant removal under elecktrokinetics. Furthermore,
understanding the contaminant retaining mechanisms in soil-water system during
electrokinetics will provide a rational approach to engineer the chemistry for
enhanced contaminant remediation. Al-Hamdan and Reddy (2008) developed a 1-D
transport model that predicts reactive multi-species in a soil during electrokinetic
remediation. The model addressed some of the contaminant-soil interactions such as
adsorption of contaminants to the soil surface, sensitivity of soil surface potential to
the pore water properties, and synergistic effects of multiple chemical species on
electrokinetics. However, the model was developed for a specific soil system.
Moreover, the model did not consider the presence of carbonates or iron in the
system, making the model inapplicable for high buffering soils containing reducing
agents.

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This paper presents a one-dimensional transport model that predicts reactive

multi-species in glacial till soil during electrokinetic remediation. The model
calculates the concentration of the chemical species during electrokinetics as a
function of time and space. The model is capable of predicting the chemical
speciation of the contaminants as well as the form that they would exist within the
soils (i.e., aqueous, adsorbed or precipitated). The model addresses the following
contaminant-soil interactions that occur during electrokinetics: (1) presence of
carbonates in the soil, (2) adsorption of contaminants to the soil surface, and (3)
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synergistic effects of multiple chemical species on electrokinetics.

MODELING APPROACH

The modeling approach in this study involves modeling the transport processes
that induce the contaminant transport as well as the geochemical processes that occur
within the electrokinetic system. The general framework of the model consists of a
two-step approach that separates the transport and chemical processes in the system
during electrokinetics into two sub-models, namely, contaminant transport sub-model
and chemical speciation sub-model. The transport sub-model takes into consideration
the transport processes in soils under electric fields, namely, diffusion,
electromigration, hydraulic advection, and electroosmotic (i.e., electric advection).
The chemical speciation sub-model takes into consideration the acid-base,
precipitation-dissolution, oxidation-reduction, and adsorption-desorption reactions. A
solution to the transport governing equation in the transport sub-model provides an
initial estimate of concentrations. A second step corrects these concentrations using
the chemical sub-model to account for the partitioning of mass due to a suite of
chemical reactions. However, the chemical sub-model is initially used to calculate the
initial speciation of each contaminant (aqueous, precipitated or/and adsorbed) before
applying electrokinetics. Once the direct current is applied across the soil, the
contaminant transport sub-model employs the chemical sub-model results (i.e.,
aqueous mobile portions of the contaminants) as initial conditions to calculate the
new aqueous concentrations of each contaminant at each space increment. The
transported portion of the contaminant at each space increment is added to the
previously (i.e., previous time increment) retained portion at the same space
increment in order to get the total contaminant concentration profile. Then, the
chemical sub-model uses the new total concentration to find the speciation and the
mobile and fixed portions for each space increment at time-step (tm). The new mobile
concentrations for the time step tm are the initial conditions for the next time step
(tm+t) in the transport sub-model.

Mathematical Modeling of Transport Processes

The multi-species transport model developed by Alshawabkeh et al. (1992) was

adopted as transport model for this study. In the presence of hydraulic, electrical and
chemical gradients, the one-dimensional total flux of species j per unit area of the soil
medium is given by Alshawabkeh and Acar (1992) as follows:

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C j
J j = D *j
x
( h
C j u *j + K e
x
) Ex C K
j (1)
h

where Cj is the concentration of species j, D *j is the effective diffusion coefficient of

species j, D *j = D j .n , Dj is the diffusion coefficient of species j in free solution at
infinite dilution, is the tortuousity factor, n is the soil porosity, u *j is the effective
D *j z j F
ionic mobility of species j, u *j = , F is Faraday constant, T is the absolute
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RT
temperature, R is the ideal gas constant, zj is the charge of species j, Ke is the
o
electroosmotic permeability, K e = n , is permittivity of the medium, o is

permittivity of the vacuum (8.854x10-12 C/V.m), is the zeta potential of the solid
surface, is viscosity of the pore water, E is the electrical potential, Kh is hydraulic
conductivity, and h is the hydraulic head

The one-dimensional time-dependent equation for the transport of solute

based on the conservation of mass as given by Alshawabkeh and Acar (1992) is:
nC j J j
= + nR j (2)
t x
where Rj is the production rate of the aqueous species j per fluid volume due to
chemical reactions. Without the chemical reaction part, the transport equation then is
given as:

nC j 2C j 2E C j E 2h C j h
=D *
j + (u *j + K e )C j + (u *
j + K e ) + K C
h j + Kh (3)
t x 2 x 2
x x x 2
x x

In this study, the following simplifying assumptions were made for the
transport model: (1) the flux due to hydraulic gradient is negligible since the water
levels difference of the electrode reservoirs maintained zero during the performed
electrokinetic experiments; (2) the electrical field (E/x) is assumed to be constant in
time across the specimen; (3) the soil porosity and hydraulic conductivity are constant
in time and space, and (5) no chemical reactions involved in the transport model since
all the chemical reactions of the contaminants including their adsorption processes to
the soil surface are implemented in the chemical submodel. These conditions will
simplify the governing transport model of the contaminant to the following equation:
nC j 2C j C j
= D *j Vj (4)
t x 2
x
where
E
(
V j = u *j + K e
x
) (5)
Crank-Nicholson implicit finite difference technique is used to solve the main
transport equations. This method is used because it is unconditionally stable and
provides a second order accuracy.

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Mathematical Modeling of Chemical Reactions

In this study, the chemical speciation sub-model is developed to calculate the

speciation of each contaminant as well as the mobile (i.e., aqueous) and fixed (i.e.,
precipitated or/and adsorbed) portions of each contaminant. The sub-model is
developed based on the mass balance of all species of interest that exist within the
system including the solid (soil) surface. The sub-model implements the important
chemical reactions that occur in soils during electrokinetic treatment, including, acid-
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base reactions (reaction of an acid or a base with water), adsorption-desorption (the

interaction of a substance between the liquid phase and the solid phase/soil surface),
precipitation-dissolution reactions (reactions in which a substance precipitates or
dissolute based on its solubility and concentration), and oxidation-reduction reactions
(reactions in which a substance loses/donates or gains/accepts electrons). The redox
reactions during electrokinetics were modeled in this study by defining the activity
ratio between the two members of a redox couple (such as Cr6+/Cr3+ couple) when the
system is at equilibrium with another redox couple in the presence of reducing or
oxidizing agents (i.e., Fe2+/Fe3+ couple). The resulting mass balance equations of the
species in the soil system form a set of algebraic equations for activity of each species
in terms of independent variables. Newton-Raphson iterative solution technique is
used to solve the resulting non-linear set of mass balance equations to get the
concentrations of all chemical species exist in the system. After the chemical sub-
model calculates the concentrations of species, it checks for the precipitations of the
contaminants. The sub-model implements the precipitation reactions by comparing
the solubility of the contaminant or the Ion Activity Product (IAP) with the total
aqueous form of the contaminant or its solubility constant, respectively. For each
contaminant, the amount of precipitation is subtracted from its concentration in the
aqueous state. The adjusted contaminant concentrations are returned to the mass
balance equations and solved for new activities.

In order to address the presence of carbonate and carbonate minerals in the

soil, the reactions of H2CO3, HCO3, and CaCO3 were implemented in the sub-model.
In modeling a carbonate system, one must first decide the nature of the carbonate
system whether it is open or closed one. This step is important because the carbonate
species can be involved in homogenous solution equilibria as well as heterogeneous
gas/liquid and liquid/solid equilibria. In the electrokinetic system of this study, the
system is closed to the atmosphere and tends to be in equilibrium with a carbonate-
containing solid (i.e., calcite). The model also addresses the synergistic effects of
multiple chemical species on electrokinetics through implementing the species
activities corrections. In ideal solution, it is valid to assume that the thermodynamic
activities of the ions are same as their concentrations since the ions behave
independently of one another. However, as the concentration of ions in solution
increases, electrostatic interactions between the ions increases, making the
thermodynamic activities of the ions less than their measured or analytical
concentrations (Snoeyink and Jekins 1980). The relation between the activity of an
ion and its concentration is given by ( a j = j C j ) where a j is the thermodynamic

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activity of the aqueous species j, j is the activity coefficient of the aqueous species
j, Cj is the concentration of the aqueous species j.

MODEL PREDICTIONS

Model Input Parameters

The electrokinetic model is used to simulate the contaminant concentration, pH,

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and electroosmotic flow profiles in space and time. The predictions of the developed
model were compared with electrokinetic experimental results conducted by Al-
Hamdan (2002). Al-Hamdan (2002) performed four electrokinetic experiments with
1, 2, 4, and 10 days of treatment time to assess the transient behavior of chromium,
nickel, and cadmium in glacial till during electrokinetic remediation. In all tests, the
contaminants were Cr(VI), Ni(II), and Cd(II) combined in the soil with concentrations
of 1000 mg/kg, 500 mg/kg, and 250 mg/kg, respectively. The model input parameters
in the current study are set to mimic the initial conditions of the electrokinetic system
in the experiments of Al-Hamdan (2002). The chemical components in the
electrokinetic system are Ni+2, Cd+2, Cr+3, CrO42-, K+, Cl-, CO32-, HCO3-, Fe2+, Fe3+,
Ca2+, H+, and OH-. The electrical potential is 1.0 VDC/cm with a total treatment time
of 240 hours. The length of the contaminated soil sample is 19.1 cm and the number
of space elements is 40 (i.e., space increment is 0.4475 cm and total number of nodes
is 41). The time increment for all simulations is 10 seconds and the resulting
concentrations profiles are printed every 8640 time steps (i.e., every 24 hours).

Soil properties input values (i.e., porosity and tortuosity factor) as well as
chemical properties input values (i.e., ion diffusion coefficient) are obtained from the
literature. Glacial till porosity value is 0.3 (Reddy et al., 2001). The tortousity factor
value used in this study for kaolin is 0.44 (Shapiro and Probstein, 1993). The model
input values of diffusion coefficient of charged ions at infinite dilution (Dj) are also
obtained from literature (Lide 1993). The input values for adsorption-desorption
models of contaminants on kaolin are the parameters are based on the potentiometric
(titration) and adsorption batch experiments of glacial till and the heavy metals:
Cr(VI), Cr(III), Ni(II), and Cd(II) performed by Al-Hamdan and Reddy (2006) (i.e.,
Freundlich Model: n = 0.68, 0.89, 0.72, 1.27, and log K = -0.14, 0.36, 0.69, -1.15,
respectively, for Cd, Ni, Cr(III) and Cr(VI)). Depending on the charge of the
component, two types of boundary conditions exist, namely, Dirichlet (i.e., the known
magnitude of variable at the boundary) and Neumann (i.e., the known flux at the
boundary). For a positively charged component, Dirichlet boundary condition is used
at the anode (i.e., 0), while Neumann condition is used at the cathode (i.e., the cation
is moving towards the cathode) ( C / t = 0 ). If the component is negatively charged,
then Dirichlet condition is used at cathode and Neumann at the anode. For H+ and
OH- ions concentrations, the boundary conditions are assumed to be exponentially
changing as a function of time. This assumption is based on the pH results at the
electrode reservoirs of the conducted electrokinetic experiments by Al-Hamdan
(2002) (i.e., at anode H+ = 10-(-0.4177ln(t)+3.997) mole/L, and at cathode OH- = 10-
(0.468ln(t)+11.095)
mole/L, where t is time in hours).

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pH Profiles and Metal Migration

Comparisons between the predicted and experimental pH profiles for glacial

till after 1, 2, 4, and 10 days are depicted in Figure 1. A reasonable agreement is
obtained with the experimental results for both soils. Figure 1 demonstrates clearly
that the rate of advancement of the base front (OH-) generated within the soil near the
cathode is superior to the acid front. Moreover, the acid front was hindered from
getting into the soil, which results in alkaline conditions throughout the soil sample
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during electrokinetic remediation. Therefore, the carbonate in glacial till plays the
most significant role in contaminant behavior during electrokinetics in glacial till.
14

12

10

8
pH

Initial
1day-Model
6
2 days-Model
4 days-Model
4 10 days-Model
1 day-Exp
2 2 days-Exp
4 days-Exp
10 days -Exp
0
0 0.2 0.4 0.6 0.8 1
Normalized Distance From Anode

Figure 1. pH profiles during electrokinetics

The model predicts the distribution of the total metal, form (i.e., aqueous,
adsorbed, or precipitated), and metal species in glacial till. Only nickel and chromium
results are presented in this paper in order to cut down the number of the pages of this
article. However, the modeling results showed that cadmium and nickel have similar
behavior in glacial till during electrokinetic remediation. Figure 2 shows a
comparison between predicted and experimental results of nickel concentration in
glacial till during electrokinteic remediation. This figure shows that model results and
experimental results of nickel migration in glacial till are in a good agreement.
However, any variation between the model predictions and experimental results could
be attributed to the simplifications and assumptions made in this model. Figure 2 also
shows that no nickel transport occurred with time in glacial till. The model results
showed that nickel totally precipitated in the soil after 10 days of treatment (i.e.,
Figure 3) because the acid front did not develop in this soil due to the consumption of
H+ ions by the carbonate.
Unlike the model predicted results of nickel, the predicted results of
hexavalent chromium in glacial till showed that hexavalent chromium transported
from the cathode towards the anode (Figure 4). Figure 5 shows that, after 10 days of
treatment, some hexavalent chromium was retarded in glacial till because of the
adsorption process. The model was also used to determine the species of the metals in
the soils after electrokinetics. Figure 6 shows the predicted species of nickel

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chromium across the soil in glacial till. Figure 6 suggests that the precipitated form of
nickel after 10 days of electrokinetic treatment is Ni(OH)2. The figure also showed
that among the aqueous species of chromium, HCrO4-, Cr2O72-, and CrO42- are the
predominant species in glacial till during electrokinetic remediation.
200 200
Glacial Till-Ni Glacial Till-Ni
(10 days) Aqueous
150 150 Adsorbed
Precipitated
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C/Co (%)

C/Co (%)
100 100
Initial
1 day-Model
2 day-Model
4 day-Model
50 10 day-Model 50
1 day-Exp
2 day-Exp
4 day-Exp
10 day-Exp
0 0
0 0.2 0.4 0.6 0.8 1 0.0 0.1 0.3 0.5 0.7 0.9 1.0
Normalized Distance From Anode Normalized Distance From Anode

Figure 2. Nickel distribution in glacial till Figure 3. Nickel form in glacial till

160 160
Glacial Till-Cr(VI)
Glacial Till-Cr(VI)
140 140 (10 day)
Initial
120 1 day - Model 120
2 day - Model
100 4 day - Model
100
C/Co (%)

C/Co (%)

10 day - Model
Aqueous
1 day -Exp
80 2 day-Exp 80 Adsorbed
4 day -Exp
Precipitated
60 10 day -Exp
60

40 40

20 20

0 0
0 0.2 0.4 0.6 0.8 1 0.0 0.2 0.4 0.6 0.8 1.0
Normalized Distance From Anode Normalized Distance From Anode

Figure 4. Chromium distribution Figure 5. Chromium form in glacial till

1.0E+00 1.0E+00
Glacial Till-Cr(VI)
1.0E-02 Ni++ 1.0E-02 (10 day)
NiOH+
1.0E-04 Glacial Till-Ni Ni(OH)2 aq 1.0E-04
(10 days) Ni(OH)3 -
C o ncentration (M )

Concentration (M)

1.0E-06 NiHCO3 + 1.0E-06 CrO4 2-

NiCO3 Cr2O7 2-
1.0E-08 Ni(CO3)2 2- 1.0E-08 HCrO4 -
NiCl + H2CrO4 aq
1.0E-10 NiCl2 1.0E-10 CrO3Cl -
SONi+
KCrO4 -
1.0E-12 Ni(OH)2 (solid) 1.0E-12 SOH2CrO4
1.0E-14 1.0E-14
1.0E-16 1.0E-16
1.0E-18 1.0E-18
1.0E-20 1.0E-20
0 0.2 0.4 0.6 0.8 1 0 0.2 0.4 0.6 0.8 1
Normalized Distance From Anode Normalized Distance From Anode
Figure 6. Contaminant speciation in soil after 10 days: (a) Nickel; (b) Chromium

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SUMMARY AND CONCLUSIONS

An electrokinetic model was developed in this study based on the convective

equation including ion transport by electroosmosis, electromigration, and diffusion, as
well as fixation mechanisms to account for chemical reactions including complex
formation, adsorption, and precipitation. The model results and their comparisons
with the experimental results demonstrate that the principles of multispecies transport
under an electric field are understood. The model results were in a good agreement
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with the experimental results for the removal of nickel, cadmium and chromium from
glacial till. However, any variations between the model predictions and experimental
results could be attributed to the aforementioned assumptions made in this model. The
model demonstrated that the carbonates in glacial till play the most significant role in
contaminant behavior during electrokinetics in glacial till as they hinder the acid front
from getting into the soil creating an alkaline conditions, facilitating the precipitation
and adsorption of heavy metals in soil. It is noted that transport occurs only when
metal exists in the aqueous form, while the adsorbed and precipitated form of metal
remain immobilized in the soil. Moreover, the model indicated that adsorption and
precipitation are the hindering and fixation mechanisms for the removal of cationic
(nickel cadmium) and anioinic (hexavalent chromium) metals from glacial till soil
during electrokinetics, respectively.

Overall, utilizing the model described herein could be a cost-effective way to

choose optimum conditions for further study to enhance the removal of heavy metals
from glacial till soil. However, the model should be improved to develop into a design
or analysis tool in electrokinetic remediation. In order to get a better representation
for the actual electrokinetic system, model should be modified to eliminate its
constraints. For example, the model assumes that the electrical field is constant in
time across the specimen which may not entirely be valid since that while the initial
electrical potential drop through the sample is linear, the potential drop becomes
increasingly nonlinear over time (Eykholt 1992). In addition, the model ignores the
adsorption of Na+ and K+ to the solid surface as well as their competition with the
metals for adsorption. Also, the metal adsorption in the model is considered as a free
metal (Mz+) adsorption. This assumption some how is not valid since the metal
hydroxo complexes (MOH+) are appreciably more adsorbable than free metal cation.
The developed model ignores the effect of the temperature on the position of the
equilibrium. The chemical part of the developed models assumes the temperature is
constant at 25oC. However, during electrokintics, the high ionic concentrations in the
pore water leads to a high current passing through the soil, causing an increase in the
temperature of the system. Moreover, temperature has a great affect on the
equilibrium constant values of the chemical reactions as well as on soil surface
potential.

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