Environ. Sci. Technol.
2003, 37, 177-181
Speciation and Transport of Heavy
Metals and Macroelements during
Electroremediation
P A S C A L S U EÅ R , * , † , ‡
KATARINA GITYE,§ AND BERT ALLARD†
Man - Technology - Environment Research Centre, Örebro
University, 701 82 Örebro, Sweden, Swedish Geotechnical
Institute, 581 93 Linköping, Sweden, and Sydkraft Sakab AB,
692 85 Kumla, Sweden
Electroremediation makes treatment of contaminated clay
soils possible. The external electrical field causes several
transport processes and changes in soil chemistry. This
study concerns the leachability and transport of calcium,
magnesium, copper, zinc, lead, nickel manganese, chromium,
and iron during treatment with an electric field of soil
from a chlor-alkali factory. As expected, most elements
were removed from the acidic part of the soil and accumulated
in the zone where pH changed from acidic to alkaline.
However, acidic leaching of the soil in this zone did not
mobilize the elements. Lead formed both an anionic complex
which electromigration transported toward the anode as
well as a cationic lead fraction which moved toward the
cathode. The anionic complex could be lead sulfate. Lead
from both fractions was strongly attached to the soil
after treatment. The low availability of metals and
macroelements after electrokinetic remediation could
make electroremediation, excavation, and deposition of
the accumulation zone an alternative for the treatment of
contaminated soils.
Introduction
Many projects have shown the feasibility of removing
contaminants from soil by electroremediation. This might
prove very valuable for the remediation of contaminated
clay soils, which are difficult to treat with other technologies.
Successful lab-scale electroremediation has been reported
for both clayey and sandy soils (1-4). Successful field-scale
electroremediation has resulted in removal of copper,
cadmium, lead, zinc, and arsenic (5) and trichloroethylene
(6). Haus et al. transformed Cr(VI) to Cr(III), with some
transport of chromium to the anode (7).
The electric field that is applied to the soil causes
movement of charged elements in the soil (electromigration).
The electric field also causes movement of water (electroos-
mosis), usually toward the cathode. Uncharged contaminants
in the soil solution move with the water. Unlike hydraulic
transport, electrokinetic transport is not dependent on the
pore size distribution or the presence of macropores in the
soil. Electroremediation has mainly focused on metal con-
taminated soil, since electromigration in general has a higher
impact than electroosmosis (1, 2).
* Corresponding author phone: +46 13 201889; fax: +46 13
201909; e-mail: pascal.suer@swedgeo.se.
† Örebro University.
‡ Swedish Geotechnical Institute.
§ Sydkraft Sakab AB.
10.1021/es010226h CCC: $25.00  2003 American Chemical Society
Published on Web 12/03/2002
Electrochemical reactions at the electrodes are commonly
dominated by the dissociation of water. Hydrogen ions are
produced at the anode and electromigrate into the soil toward
the cathode. Hydroxide ions are produced at the cathode
and electromigrate into the soil from that direction. Thus,
pH is acidic near the anode, and alkaline near the cathode.
The transition from acidic pH to alkaline pH is usually within
a small region called the pH-shift. Metals are mobilized in
the acidic zone and transported toward the cathode. At the
pH-shift, metals accumulate. This is often attributed to
precipitation of metal hydroxides (1, 2, 8).
To evaluate electrokinetic treatment, it is desirable to know
the form of the pollutants that remain in the treated soil.
Knowledge of metal speciation also increases understanding
of the electroremediation process. The form of metals in the
soil can be assessed by selective leaching or sequential
extraction (9, 10). Although there exist some uncertainties
about the selectivity of the solutions and resorption during
the extractions, selective leaching provides a practical method
to assess the potential mobility of metals and gives an
indication as to which soil fraction the metal is associated
to. Ribeiro et al. report higher mobility for copper after
electroremediation, analyzed by sequential extraction. They
attribute this to accelerated weathering of soil material (11)
and to the transfer of copper from amorphous oxides and
organic matter to soluble and exchangeable forms (12). Kim
and Kim (13) report removal of lead, copper, cadmium, and
zinc from more accessible fractions of a tailing soil, while
sulfide and residual fractions were affected less by elec-
troremediation. Reddy et al. (14) report rapid migration of
soluble and exchangeable chromium, nickel, and cadmium.
The elements precipitated at high pH, possibly as hydroxides.
Reddy et al.’s study was performed on spiked soil, which
leads to a considerably more mobile contamination than is
found in industrially polluted soils.
In the present study electroremediation was applied to
contaminated soil from a chlor-alkali factory site. The main
contaminants in the soil are mercury, dioxins, and lead, while
other metals are present at elevated concentrations. The
transport of metals and macroelements during treatment
and the speciation of the elements after treatment are dis-
cussed. The behavior of mercury is discussed elsewhere (15).
Experimental Section
Soil. Several hundred kilograms of soil were taken at the site
of a chloralkali factory. The soil was mixed at the factory and
a subsample was used in this study. The soil was polluted
with mercury, polychlorinated dibensofurans, lead, and
several other heavy metals. Initial metal concentrations are
shown in Table 1. At the laboratory, the soil was sieved, and
the fraction smaller than 4 mm was used for the experiment.
The soil was predominantly illitic clay with loss on ignition
2.5%, sulfur content up to 4 g/kg and pH 7-7.5 (1 g soil in
10 mL water) (16).
Electrokinetic Experiments. Electrokinetic experiments
were conducted in a 46 × 10 × 10 cm3 plastic box (Figure
1). Graphite plate electrodes were placed at the ends of the
FIGURE 1. The experimental setup.
VOL. 37, NO. 1, 2003 / ENVIRONMENTAL SCIENCE & TECHNOLOGY 9 177
TABLE 1: Approximate Mass-Balance of Several Elements in TABLE 2: Metals Mobilized by Selective Leaching of the
the Soil Sample at 4 cm from the Anode Compartment after
Electrokinetic Treatmenta
Zn Pb Cu Ni Fe Cd Ca Mg Mn
fraction A B C D E
initial concn 608 375 174 47 42000 6 16121 8373 2286
(mg/kg) Ca (mg/kg) start 4150 139 6726 6919 8060
after 182 days 851 377 273 128 48000 4 7396 6824 2501 182 days 63 0 0 128 365
(mg/kg) Mn (mg/kg) start 1 0 693 1024 1143
recovered from 140 100 160 270 110 67 46 82 110 182 days 0 0 0 9 60
the soil (%) Fe (g/kg) start 0 0 2.4 15 21
182 days 0 0 1 2 9
Ni (mg/kg) start 0 0 0 20 24
box in electrode compartments, separated from the soil by 182 days 13 7 15 15 16
a polypropene geotextile. 2 kg soil was placed in the middle Cu (mg/kg) start 0 32 52 81 87
182 days 4 8 7 11 18
compartment. The total length of the soil column was 27 cm. Zn (mg/kg) start 0 32 183 450 304
The solutions in the electrode compartments were stirred 182 days 0 0 0 7 31
continuously. Each electrode compartment was connected Pb (mg/kg) start 0 20 114 207 188
182 days 35 0 32 35 112
to a water tank by a siphon to reduce soil desiccation. An
electric field of 30 V was applied for 182 days. a Metal amounts as they were analyzed in the leachant, without

The solution in the electrode compartments and in the
connecting tanks consisted of 0.01 M NaCl at the start.
Solution was added regularly in order to replace water that
was lost by evaporation. Final chloride concentrations of
0.08 M Cl at the anode and 0 M Cl at the cathode were
obtained. The smell of chlorine gas was noticed near the
anode.
Analysis. The pH and voltage gradients in the soil were
measured in-situ at regular intervals during the experiment.
The current between the electrodes was measured as well.
The initial soil pH was measured in a suspension of 1 g of
soil and 10 mL of 18MΩ water.
After 9, 40, and 79 days, soil samples were taken at the
pH shift and on both sides of the pH shift. After 126 and 182
days, samples were taken over the whole soil column. The
soil samples were taken by pushing a cut plastic syringe, 8
mm in diameter, into the soil, while maintaining the syringe
plunger at the soil surface. Thus, the soil was not compacted
during sampling. The samples were dried for 24 h at 40 °C
and extracted by microwave assisted digestion in aqua regia
(leachant E, see selective leaching). The total content of cop-
per, zinc, lead, nickel, iron, calcium, magnesium, and chro-
mium was determined by ICP-AES. Soil samples after 182
days were also subjected to selective leaching. The same ele-
ments without chromium and magnesium were determined.
Solution samples were taken from the electrode com-
partments and the same metals were analyzed. Chloride was
measured by titration.
Selective Leaching. The dried soil samples were subjected
to selective leaching according to a procedure adapted from
Lifvergren (16). 1 g of dried soil was shaken with 20 mL of
one of the following solutions:
A. 1 M sodium chloride for 24 h. Weakly adsorbed and
readily mobilized metals were recovered from the super-
natant.
B. 1 M sodium hydroxide for 7 d. The alkaline conditions
mainly extracted metals associated to humic matter.
C. 0.1 M hydrochloric acid for 5 h and selected samples
for 5 days. Fraction A plus metals mobilized by acid conditions
were extracted. These metals were mainly associated with
carbonates and iron- and manganese oxides.
D. 5 mL of hydrogen peroxide and 15 mL of concentrated
nitric acid at 60 °C for 3 h. In addition to metals mobilized
in fraction A, B, and C, the extraction oxidized organic matter
and secondary sulfide precipitates from the soil.
E. 1 g of dried soil was digested by open focused microwave
extraction with 20 mL aqua regia. This procedure yielded the
total content of metals (17).
Centrifugation and analysis of the supernatants followed.
New soil was taken for each extraction, so that each extraction
step was independent of the steps before. Three replicates
were made for each leachant on the soil before treatment.
correction for weaker extraction steps.
Sampling volumes from the soil after 182 days permitted
only 1 soil sample for each leachant.
In the figures presented in the next section, the leached
amounts have been corrected so that they represent the
fraction that was mobilized in excess of the weaker leachant
that came before, since the diagrams give the visual impres-
sion of being cumulative. Thus, fraction C denotes the results
from leachant C minus leachant A; fraction D the results
from leachant D minus leachant C; fraction E the results
from the total extraction minus leachant D. The result of
leachant B is reported without correction, since only few
metals (copper, lead, and nickel) are extracted by leachant
B, and leachant B does not overlap with leachants C, D, and
E. In Table 2, the amounts have not been adjusted.
Results and Discussion
Time Series. The current through the soil was between 2 and
15 mA except for occasional short-lived peaks when mea-
surements disturbed the zone of high resistance at the pH-
shift. The voltage gradient in the soil was directly proportional
to pH. This can be explained by the domination of hydroxide
ions and protons to the electric conductivity of the soil
solution (1).
A shift in pH developed within 9 days. Hydrogen ions
produced at the anode moved into the soil, as did hydroxide
ions produced at the cathode. Water formed where the hy-
drogen and hydroxide ions met. The conductivity of the soil
solution is much decreased at this zone, as could be seen
from an increase in current when the zone was disturbed by
measurements. The pH-shift was between 16 and 20 cm from
the anode geotextile after 40 days, around 20 cm after 79
days, and between 20 and 25 cm after 126 days (Figure 2).
Almost all the soil was acid at the final sampling after 182
days. Thus, the pH-shift moved slowly toward the cathode.
The shift from pH 3 to pH 10 occurred within approximately
5 cm.
Calcium, magnesium, nickel, zinc, manganese, copper,
and chromium were released from the soil in the region of
low pH (Figure 2). This is probably due to the decreasing pH
in the soil (18). The elements were transported toward the
cathode, and thus were in cationic form. The elements
accumulated where pH shifted from acidic to alkaline (Figure
2). Higher pH lowered the mobility of the cations and they
associated with the soil.
The zone of metal accumulation moved together with
the pH-shift toward the cathode. When the pH-shift moved
closer to the cathode, the elements moved as well. They
remobilized with the successive acidification of the soil and
precipitated closer to the cathode where pH continued to be
high. The precise location of the accumulation zone in

178 9 ENVIRONMENTAL SCIENCE & TECHNOLOGY / VOL. 37, NO. 1, 2003

FIGURE 2. Distribution of pH, calcium, zinc, iron, and lead during the electrokinetic experiment. Magnesium, manganese, nickel, copper,
and chromium were very similar to zinc (see Figure 1 Supporting Information). [ start, O 40 days, × 79 days, 4 126 days, b 182 days.
relation to the pH-shift differed between the metals. Calcium
accumulated on the alkaline side of the pH-shift, copper on
the acidic side. The order of the metals followed the order
of hydrolysis constants for the elements, i.e., Ca > Mg >Ni
≈ Zn ≈ Mn > Cu > Cr (19, 20). High hydrolysis lead to
remobilization at high pH, so that calcium moved closest to
the cathode and chromium nearest the anode (Figure 2).
An approximate mass-balance for the soil after 182 days
was calculated (Table 1). Each soil sample after 182 days was
assumed to represent the soil section around the sample.
The limits of each section were halfway between the sampling
points. Thus, each sample represented a section 6-7 cm
long. This resulted in a coarse approximation of reality since
the spatial distribution of the concentrations showed high
variability near the maximum concentrations. Therefore, the
mass balance has low precision. However, there are some
aspects of the approximate mass-balance that deserve
attention.
The recovery from the soil of most elements was > 100%
(Table 1). This shows that metals were not removed from the
soil, only redistributed. This is not true for calcium. Around
half of the original calcium was recovered in the soil. As seen
in Figure 2, calcium was the element that moved furthest
toward the cathode. Calcium was also found in precipitates
in the cathode compartment. These precipitates were not
included in the mass-balance because it was difficult to
ascertain the total amount of precipitate. The high calcium
content of the precipitate in the cathode compartment
showed that calcium has migrated into the cathode com-
partment and has been removed from the soil.
Selective Leaching. The results from the selective leaching
are shown in Figure 3. Before the electrokinetic treatment,
50% of the initial calcium content was extractable by leachant
A, and the calcium was mobilized by the electric field. Some
copper, zinc, and lead were extracted by leachant B, which
is expected due to their high affinity for organic matter (21,
22). Leachant A and B extracted less than 2% of manganese,
iron, and nickel (Table 2).
Acid leaching (C) or acid and oxidizing leaching (D) did
generally mobilize the metals in the start soil. Leachant C
and D resemble the conditions near the anode, i.e., acidic
and oxidizing. As expected from the selective leaching, the
VOL. 37, NO. 1, 2003 / ENVIRONMENTAL SCIENCE & TECHNOLOGY 9 179

FIGURE 3. Extraction of zinc, copper, calcium, iron, and lead by
selective leaching after 182 days of electrokinetic treatment.
Manganese and nickel were similar to zinc (see Figure 2 Supporting
Information).
metals were released from the soil near the anode during the
electrokinetic treatment.
After 182 days of electrokinetic treatment, leachant A
extracted less than 4% of copper, zinc, manganese, and
magnesium at all locations in the experiment. The exception
was nickel: up to 80% of nickel near the anode was extracted
with leachant A (Table 2). Thus, nickel near the anode is
more available for transport by electromigration. However,
nickel behaved similar to copper, zinc, and manganese as
evidenced by the time series and by the leaching charac-
teristics at other locations in the experiment.
The metals near the cathode were expected to be
hydroxide precipitates, since they were immobilized by the
high pH. This is also proposed by several other publications
(1, 2, 14). If this was the case, the metals should be released
by acidic leaching (leachant C) (9, 16). However, leachant C
extracted only up to 65% of copper, zinc, lead, nickel, calcium,
and iron. It is possible that the extraction with leachant C for
5 h was too short to dissolve all hydroxides. The extraction
was originally developed for soils that are not treated with
an electric field. Since electromigration can transport ions
through micropores in the soil, hydroxides could have
precipitated in these micropores. Dissolution of hydroxides
could then be controlled by the diffusion of ions in the
micropores. This would make the extraction slower for
hydroxides in micropores than for hydroxides that can be
reached directly by the extracting solution.
To test whether kinetics played a major role, the 2 soil
samples closest to the cathode were leached for 5 days with
leachant C. These samples were the most likely to contain
hydroxides, since these locations had been most alkaline.
The 5-day leaching did not extract more metals that the 5-h
leaching. Either the 5-hour extraction mobilized all metals
associated with hydroxides, or hydroxides were not leached
even after 5 days. A surprisingly large amount of the metals
(> 50%) was present in a form that was not leachable with
acid within 5 days.
The metals that were difficult to leach were transported
by the electric field. They were not near the cathode at the
start of the experiment. For example, the zinc concentration
180 9 ENVIRONMENTAL SCIENCE & TECHNOLOGY / VOL. 37, NO. 1, 2003
throughout the soil before the experiment was 300 ppm.
After treatment, 1170 ppm zinc was found near the cathode.
640 ppm of these 1170 ppm was extracted by leachant E
only. New zinc was therefore present in fraction E. The
elements that had been transported toward the cathode were
difficult to mobilize despite the short time (less than 182
days) since their arrival.
The low mobility of the metals could be explained by the
role of soil micropores. Electrokinetic transport uses micro-
pores more than does hydraulic transport (1, 2). Metals that
were transported into micropores by electromigration, and
that either adsorbed to the soil or precipitated as hydroxides,
could be difficult to extract using agitation. These metals
would of course also have low mobility under natural
conditions.
Calcium was only extracted by leachant D. This excludes
calcium hydroxide or carbonate as the final form, since these
would be extracted by leachant C. A possibility is the presence
of calcium as calcium sulfate. The sulfur content of the soil
was quite high, up to 4 g/kg, due to the industry’s use of
elemental sulfur to produce sulfuric acid. Calcium sulfate is
one of the few sulfates that has low solubility and may thus
be limiting for the mobility of calcium. Calcium sulfate would
be extracted by leachant D and not by leachant C, which is
in agreement with the observations.
Even near the anode the availability of the elements was
low (Table 2). Typically over 60% of the remaining metals
were found in fraction E. The selective leaching results near
the anode can be compared with results from Ribeiro et al.
(11) and Kim and Kim (13), since both these publications
concern studies where the entire studied soil is acidic. Both
Ribeiro et al. and Kim and Kim report that metals moved
from the intermediate fractions to the fractions that were
more easily extracted. Metals were also removed from the
residual fraction (E) in both the present study and the study
reported by Kim and Kim. However Ribeiro et al. found no
removal of copper from the fraction corresponding to fraction
E in the present study (“strongly bound” fraction), despite
a treatment time of 125 days.
Only copper and nickel were associated with low mo-
lecular weight organic material. 40-50% of the total copper
and nickel was extracted by an alkaline solution (leachant
B) near the anode. This is probably due to the high affinity
of copper and nickel for organic molecules, which are
extracted by leachant B (21, 22).
The most available metals were found adjacent to the
anode side of the pH-shift (19 cm, Figure 3). Leaching results
were typically A 15%, B 0%, C 45%, D 80%. The elements
were in the process of remobilization and transport toward
the cathode.
Iron and lead behaved somewhat differently from the
other metals (Figure 2). The iron in the soil was transported
slowly toward the cathode, but the process was not dominated
by pH. No relation between iron transport and the position
of the pH-shift was evident from the data. Possibly iron was
transported as a cation in solution. An alternative explanation
is electroosmotic or electrophoretic transport of iron-
containing colloids.
Initially, iron was mobilized by leachants D and E (acid
and oxidizing and total content, respectively, Figure 3). This
mobilization occurred near the anode, since conditions were
oxidizing and acidic. After 182 days, the iron was found in
fraction E near the cathode. Immobilization may have
occurred due to reduction or by the higher pH. The migrated
iron was insoluble.
Some lead moved toward the cathode, and this cationic
lead behaved very similar to the elements described earlier
(Figure 2). Most lead however moved toward the anode. This
might be explained by an anionic lead complex, such as lead
chloride or sulfate. Model calculations using Mineql+ (23)
show that 0.1 M chloride, which was the highest chloride
concentration that was measured during the experiment, is
not sufficient to cause the presence of a considerable amount
of anionic lead chloride complexes. Less than 1% of lead
would be present as PbCl3- or PbCl42-. Sulfate may also form
complexes with lead. Analysis has shown up to 4% sulfur in
the soil (16), and if even a tenth of the sulfur was oxidized,
concentrations of sulfate may locally exceed 1 M. At a sulfate
concentration of 0.1 M, 20-30% of lead may be in the form
of Pb(SO4)22-. The lead sulfate complex has the highest
stability constant of the metals, and lead is the only metal
for which an anionic complex with two sulfates is reported
(24), which may explain why the other metals showed no
anionic behavior while lead did. Anions are scarce near the
cathode, since they migrate toward the anode. Therefore
lead was present as a cation near the cathode.
The cationic lead was extracted by leachant C, D, and E,
similar to the metals discussed above (Figure 3). The anionic
lead was also difficult to extract. Half of the lead was
extractable by oxidizing conditions (leachant D), while the
remaining half was residual (Figure 3).
Common to all the discussed elements was their strong
attachment to the soil after the treatment with the electric
field. Metals were removed from the acidic part of the soil.
The sequential extraction showed that these metals were
removed from all soil fractions. Most metals concentrated at
the pH-shift. The formation of metal hydroxide is an unlikely
explanation, in view of the low extraction by an acid solution.
The low potential for remobilization of the metals shows
that both mobilization and immobilization by electric fields
could be feasible methods for the remediation of contami-
nated soil.
Acknowledgments
The authors gratefully acknowledge the help of Hanna Ericsen
at Sydkraft SAKAB with the chloride analysis. This work was
financially supported by MISTRA, as a part of the program
soil remediation in a cold climate (COLDREM) and the
Knowledge foundation.
Supporting Information Available
Distribution of magnesium, manganese, nickel, copper, and
chromium and the sequential extraction of manganese and
nickel, which are similar to metals shown in the text. This
material is available free of charge via the Internet at http://
pubs.acs.org.
Literature Cited
(1) Acar, Y. B.; Alshawabkeh, A. N. Environ. Sci. Technol. 1993, 27,
2638-2647.
(2) Probstein, R. F.; Hicks, R. E. Science 1993, 260, 498-503.
(3) Hansen, H. K.; Ottosen, L. M.; Kliem, B. K. J. Chem. Technol.
Biotechnol. 1997, 70, 67-73.
(4) Li, Z.; Yu, J.-W.; Neretnieks, I. Environ. Sci. Technol. 1998, 32,
394-397.
(5) Lageman, R. Environ. Sci. Technol. 1993, 27, 2648-2650.
(6) Ho, S. V.; Athmer, C.; Sheridan, P. W.; Hughes, B. M.; Orth, R.;
McKenzie, D.; Brodsky, P. H.; Shapiro, A. M.; Sivavec, T. M.;
Salvo, J.; Schultz, D.; Landis, R.; Griffith, R.; Shoemaker, S.
Environ. Sci. Technol. 1999, 33, 1092-1099.
(7) Haus, R.; Zorn, R.; Aldenkortt, D. In 2nd symposium Heavy Metals
in the Environment and Electromigration Applied to Soil
Remediation; Technical University of Denmark: Denmark, 1999;
pp 165-170.
(8) Alshawabkeh, A. N.; Yeung, A. T.; Bricka, M. R. J. Environ. Eng.
1999, 125, 27-35.
(9) Tessier, A.; Campbell, P. G. C.; Bisson, M. Anal. Chem. 1979, 51,
844-851.
(10) Saouter, E.; Campell, P. G. C.; Ribeyre, F.; Boudou, A. Intl. J.
Environ. Anal. Chem. 1993, vol. 54, 57-68.
(11) Ribeiro, A.; Villumsen, A.; Réfega, A.; Vieira e Silva, J.; Bech-
Nielsen, G. In 16th world congress of soil science; Montpellier,
France, 1998.
(12) Ribeiro, A. B.; Mexia, J. T. J. Haz. Mater. 1997, 56, 257-271.
(13) Kim, S.-O.; Kim, K.-W. J. Haz. Mater. 2001, B85, 195-211.
(14) Reddy, K. R.; Xu, C. Y.; Chinthamreddy, S. J. Haz. Mater. 2001,
B84, 279-296.
(15) Suèr, P.; Allard, B. Accepted for publication in Water, Air, Soil
Pollut. 2002.
(16) Lifvergren, T. Ph.D. Thesis, Örebro Studies in Environmental
Science 1, Örebro University: Örebro, Sweden, 2001.
(17) Lifvergren, T.; Suèr, P.; Wievegg, U. In 11th Annual International
Conference on Heavy Metals in the Environment; Nriagu, J., Ed.;
University of Michigan, School of Public Health, Ann Arbor, MI,
USA (CD-ROM), 2000; p Contribution #1367.
(18) Alloway, B. J., Ed. Heavy metals in soils; 1st ed.; Blackie and Son
Ltd.: London, 1990.
(19) Allard, B. In Trace elements in natural waters; Salbu, B., Steinnes,
E., Eds.; CRC Press: 1995; Chapter 157, pp 151-176 .
(20) Appelo, C. A. J.; Postma, D. Geochemistry, groundwater and
pollution; A. A. Balkema: Rotterdam, 1996.
(21) Asami, T.; Kubota, M.; Orikasa, K. Water, Air, Soil Pollut. 1995,
83, 187-194.
(22) Morera, M. T.; Echeverria, J. C.; Mazkiaran, C.; Garrido, J. J.
Environ. Pollut. 2001, 113, 135-144.
(23) Schecher, W. D.; McAvoy, D. C. MINEQL+ A chemical equi-
librium modeling system; 4.0 for Windows ed.; Environmental
Research Software: Hallowell, 1998.
(24) Lindsay, W. L. Chemical equilibria in soils; Wiley and Sons, Inc.:
Canada, 1979.
Received for review September 6, 2001. Revised manuscript
received October 14, 2002. Accepted October 14, 2002.
ES010226H
VOL. 37, NO. 1, 2003 / ENVIRONMENTAL SCIENCE & TECHNOLOGY 9 181