Environ Monit Assess (2014) 186:5033–5040

DOI 10.1007/s10661-014-3757-y

Soil contamination by heavy metals in landfills: measurements

from an unlined leachate storage basin
Fethi Bouzayani & Abdelwaheb Aydi & Tarek Abichou

Received: 25 August 2013 / Accepted: 21 March 2014 / Published online: 12 April 2014
# Springer International Publishing Switzerland 2014

Abstract Landfills are sources of groundwater and soil Keywords Landfills . Heavy metal contamination . Soil
pollution due to the production of leachate and its mi- and water contamination . Pollution management
gration through refuse. This study was conducted in
order to determine the extent of soil pollution within
and around the Jebel Chakir landfill, located in the Tunis
Introduction
City, Tunisia. The main objective was to characterize
soil samples of an unlined storage basin in relation to
The disposal of waste from anthropogenic activity has
heavy metal concentrations in the Jebel Chakir landfill
been done by landfilling for centuries (Lopez et al.
to the southwest of Tunis, Northern Tunisia. Twenty-
2004). This technique of waste disposal provides an
four soil samples taken from different locations around
efficient and cost-effective methodology of the urban
the storage basin were analyzed by atomic absorption
waste elimination (Khattabi et al. 2002). However, this
spectrophotometry for Cr, Cu, Ni, Pb, and Zn investiga-
technique suffers from many imperfections such as
tion. Our results indicated high concentrations of Cr
odors, biogas, and especially leachate. Leachate is gen-
(54.4–129.9 mg/kg of DM), Zn (4.1–81.8 mg/kg of
erated by rainwater percolation through wastes, chemi-
DM), Ni (15.1–43.9 mg/kg of DM), Pb (5.6–16.1 mg/kg
cal and biological processes in waste, and the inherent
of DM), and Cu (0.2–1.84 mg/kg of DM). These results
water content of wastes themselves (Reinhart and Grosh
suggested that contaminant migration is controlled by
1998; Tazi 2001; Chofqi et al. 2004). Furthermore,
an active clay layer acting as an insulating material in
landfill leachate generation remains continuous when
the landfill. It is therefore necessary to set a treatment
water comes in contact with the solid waste. Landfill
system for the landfill leachates and place a liner under
leachate usually contains four groups of contaminants,
the storage basin to reduce the pollution threat.
including dissolved organic matters, inorganic com-
pounds (e.g., ammonium, calcium, magnesium, sodium,
F. Bouzayani potassium, iron, sulfates, chlorides), heavy metals (e.g.,
SISGEO, Borj Louzir, Ariana 2073, Tunisia cadmium, chromium, copper, lead, zinc, nickel…), and
xenophobic organic substances, the discharge of which
A. Aydi (*)
causes serious environmental threats to the surrounding
Laboratory of Water, Energy and Environment, National
School of Engineers, SfaxPB: 1173-3038, Tunisia soil, groundwater, and even surface water (Kjeldsen
e-mail: [email protected] et al. 2003). Contaminants carried in leachate are de-
pendent on solid waste composition and on the simul-
T. Abichou
Department of Civil and Environmental Engineering,
taneously occurring physical, chemical, and biological
FAMU-FSU College of Engineering, 2525 Pottsdamer Street, activities within the landfill (Adeyemi et al. 2007).
Tallahassee, FL 32310, USA Hazardous metals like Pb, Zn, and Cd take part in the
5034 Environ Monit Assess (2014) 186:5033–5040

biogeochemical cycles, and their mobility depends was determined according to the standard NF M03-002
strongly on their chemical forms rather than total ele- (MODECOM Méthode de caractérisation des ordures
ment concentration (Garcia et al. 2005). Thus, heavy ménagères 1993). Each 2-kg MSW sample was oven-
metals present in leachate can migrate away from the dried at 105 °C for 24 h until constant mass was
disposal site boundaries and may constitute a serious achieved.
pollution threat for the water table and the soil around After the placement of each 2-m layer of waste, the
the landfill (Yoshida et al. 2002; Zairi et al. 2004). The waste layer is cover by a 30-cm sand layer. An approx-
impact of landfill leachate on surface and groundwater imately 1.8-m-thick soil layer is used as a final cover
has been extensively studied in recent years (Yoshida above the waste layer.
et al. 2002; Chofqi et al. 2004; Marzougui and Ben The average leachate collected with high-density
Mammou 2006). polyethylene pipes (diameter 160 mm) and stocked in
To control environmental impact of solid waste, the storage basins without any treatment was about
Tunisian government rehabilitated uncontrolled 342 m3/day, which is relatively high. This large amount
dumpsites and constructed sanitary landfills similar to can be attributed to the large fraction of organic matter
the Jebel Chakir landfill (which was the first to be set and moisture remaining in the waste-stream-to-leachate
and has been receiving the domestic waste of Tunis City formation. The generated leachate is usually collected
since May 1999). Leachate generated by the site is by a network of wells and pipes (diameter 160 mm) and
stored in nine storage basins, but not lined with material stored in nine storage basins (B1 (11,000 m3), B2
to prevent leachate percolation into the ground water (11,000 m3), B3 (11,000 m3), B4 (11,000 m3), B5
and soil. (11,000 m3), B6 (11,000 m3), B7 (14,000 m3), B8
The stored leachate in-earth basin with high pollutant (20,000 m3), and B9 (2,000 m3). These storage basins
load may be the main source of soil and groundwater were covered with lined material to prevent leachate
contamination. That is why the assessment of potential percolation to ground water and soil. In addition, the
environmental threatening of soil by heavy metals is- leachate has to be stocked because of its threat to the
sued from the active, Jebel Chakir landfill located in the surrounding area of fauna and flora (Tizaoui et al. 2007).
southwest Tunis, Tunisia, is necessary. This paper stud- The soil stratigraphy of Jebel Chakir landfill consists
ies the possibility of vertical and lateral percolation of of clay intercalated with clay gypsum or chalky. This
the pollutants by evaluating the degree of the substratum impermeable clay layer plays an important role in
contamination from the storage basin. Some remedial protecting the underlying confined aquifer from leachate
measures were also suggested to further reduce contam- infiltration.
ination of soil and water via leachate percolation. Figure 1 depicts the monthly average quantities of
leachate collected and waste deposited from 1999 to
2010. The climate in Tunis City is typically
Materials and methods Mediterranean, characterized by dry and warm summers
(from June to August) and cool, wet winters (from
Site description December to February) with an annual precipitation of
about 480 mm, an annual temperature 19 °C (minimum
The Jebel Chakir landfill is located 10 km southwest of in January with 12 °C and maximum in August with
Tunis City. It has a capacity of about 7 million tons of 27 °C), and an average evaporation rate of 129 mm/
municipal solid wastes (MSW) and a global area of month. The predominant wind blows northward with an
31 ha. The landfill opened in 1999 and closed in 2010. average speed of 5 m/s.
The composition of MSW received in the Jebel
Chakir landfill showed an organic fraction (65 %; com-
posed mainly of food waste), followed by papers–card- Samples and analysis
board (12 %), fines (8 %), plastics, leather and rubber
(7 %), metals (4 %), textiles (3 %), and glass and Leachate samples were collected from 1 m depth at the
ceramic (1 %) (Aydi et al. 2009). The average moisture storage basins (L1 in B5 and L2 in B8) in December
content of the waste received in the landfill is around 2006 (T=19 °C). Due to technical constraints, it was not
70 % on wet mass (Aydi et al. 2009). Moisture content possible to take samples from other storage basins.
Environ Monit Assess (2014) 186:5033–5040 5035

Leachate generation waste input

5000 60000

Leachate collection (m )
50000

3
4500

Waste disposal (m )
3
40000
4000
30000
3500
20000
3000 10000

2500 0
Fe a ry

Month

A y

r
pt st
il
ry

ch

D ber
ne

O er
ay

N ber

be
l
pr

u
Ju

b
ua

Ju
ar

ug
nu

em
em
A

em

cto
M
br
Ja

ec
ov
Se
Fig. 1 Monthly average quantities of leachate collected and waste deposited from 1999 to 2010

Twenty liters of leachate was stored at 4 °C for heavy and sieved through a 2-mm mesh. Then, they were
metal analysis by atomic absorption spectroscopy. leached according to the NF 12457 methodology; heavy
Field investigations were conducted in December metals and total organic carbon (TOC) were estimated.
2006 concerning the impact of dumping waste on soil. The dosage of the TOC is achieved by coulometry with
During this survey, four excavations have been under- the help of the device Coulomat 702 (Herrmann and
taken using a digger around the leachate storage basins Knake 1973).
(Fig. 2). Excavation depth was extended up to 4 m depth The electrical conductivity (EC), salinity, and pH
because of technical constraints of exploitation (drains, were measured in situ by using a multi-parameter
wells). conductimeter (WTW Windaus LF 538, Inolab.,
Soil sampling was performed on a dry basis. In this Germany) and a pH meter (WTW Windaus pH 538
way, 24 soil samples were collected from the four exca- Inolab., Germany with combine electrode) for
vations. Initially, all samples were stored in glass jars at leachate samples. The concentration of sodium
4 °C before being air-dried at room temperature (25 °C) (Na), chloride (Cl), sulfate (SO4), and magnesium

N
Platform sorting

Water gutters pluvial Bi: Leachate storage basins

B1 B2
B9 E3
B3 B4
Alveolar
Alveolar Cell C4
B5 B6 B7 B8
E4
Cell C2 Cell C3
Cell C1 E1
E2
Concrete
basin
Direction
Main entry
Transfer Basin

0 100m

Fig. 2 Localization of excavations points

5036 Environ Monit Assess (2014) 186:5033–5040

(Mg) were determined by NFT 90-003 AFNOR consisted of biologically degradable dissolved organics
methods (AFNOR 1999). COD was measured fol- whereas COD described chemically oxidizable compo-
lowing the MA-315 COD-1.0 (Centre d’expertise nents in leachate and reflected the amount of O2 that is
en analyse environnementale du QUEBEC 2003) required by the bacteria to metabolize the existing or-
for leachate samples. ganic substrate as well as the O2 required by other
The biochemical oxygen demand (BOD5) was mea- oxidizable chemical compounds.
sured by using a BOD meter (BSB-controller Model The two leachate samples were characterized with
620 T (WTW), Germany). Total nitrogen was deter- high COD values (21,480 mg O2/l) and low BOD5
mined using (NT) titrimetric method EN 25663 for (5,490 mg O2/l). In the literature, there has been reported
leachate samples. Aliquots of soil samples were digested a considerable variation in the quality of leachate pro-
in HF-NO3-HCLO4 and stored at 4 °C prior to chemical duced from different landfills in the world (Zayen et al.
analysis. Heavy metal (i.e., Fe, Cr, Zn, Cu, Cd, Ni, Pb, 2010). The COD value is much higher than that of
and Mn) concentrations were determined using an atom- domestic wastewater, and it is higher than the Tunisian
ic absorption spectrometer (Perkin-Elmer Analyst 200 Standards for discharge in public sewer (NT 106 002:
Inc., Japan) (Pinta et al. 1980). COD=1,000 mg/l and BOD5 =400 mg/l); therefore, a
discharge into the sewer is not permitted.
The BOD5/COD ratio is considered as an indicator of
Results and discussion the organic matter biodegradability and the maturity of
leachate and landfill (Chofqi et al. 2004). For a young
Characterization of leachate landfill, where biological activity corresponds to the
acid phase of anaerobic degradation, the BOD5/COD
The data in Table 1 showed the physicochemical prop- ratio reached 0.85 and decreased to 0.05 for other land-
erties of the studied leachate, indicating an alkaline fills (El Jadida, Alger, and Belfort) for which active
mixture of dark color. The electrical conductivity of methane production is recorded (Kerbachi and
leachate ranged from 36.5 to 42.8 ms/cm, which is Belkacemi 1994; Khattabi et al. 2002; Chofqi et al.
higher than the domestic wastewater and those reported 2004). For the Jebel Chakir landfill, the BOD5/COD
in literature (15 ms/cm) (Blight et al. 1999). This pa- ratio of 0.25 indicated a mature landfill. The yearly
rameter indicates the high mineral contents. BOD transient evolution of the COD, BOD5, and BOD5/

Table 1 Physical and biochemical properties of Jebel Chakir leachate landfill

Parameters L1 L2 Mean (L1 and L2) NT 106 002a

pH 8.25 8.15 8.20 6.5–9

Electric conductivity (ms/cm) 42.80 36.50 39.65 NA
COD (mg O2/l) 20,500 22,460 21,480 1,000
BOD5 (mg O2/l) 5,780 5,200 5,490 400
BOD5/COD 0.28 0.23 0.25 0.4
Fe (mg/l) 20,500 22,460 21,480 5
Cr (mg/l) 1.22 1.12 1.17 0.5
Zn (mg/l) 0.72 0.77 0.745 5
Cu (mg/l) 0.81 0.78 0.795 1
Cd (mg/l) 0.042 0.047 0.044 0.1
Ni (mg/l) 0.22 0.25 0.23 2
Pb (mg/l) 0.4 0.3 0.35 1
Mn (mg/l) 0.048 0.051 0.046 1

NA not available
a
Norm for the wastewater drained to public sewer, Tunisia
Environ Monit Assess (2014) 186:5033–5040 5037

COD parameter is clearly evidenced for the Jebel Chakir pollutants, but more in organic materials (ADEME
landfill of an important decrease (Table 1). These values 1996).
suggest that leachate from the Jebel Chakir landfill is
significantly stabilized with the highest possible pol- Site lithology
lution and that this landfill is at present in the inter-
mediate phase of anaerobic degradation (DBO 5 / In order to characterize the migration of heavy metals in
DCO=0.25), indicating an important proportion of soil at the Jebel Chakir landfill, four excavations have
inert matter. been conducted near storage basins (Fig. 2). The phys-
The results shown in Table 2 clearly indicate the ical properties of the soil profile at the four excavations
important metallic load of Jebel Chakir landfill leachate (E1–E4) were described as follows (Fig. 3):
in comparison with other landfills in the Alger area
(Kerbachi and Belkacemi 1994), El Jadida region – E1 (36° 44′ 17″ N/10° 04′ 29″ E, excavated 20 m
(Chofqi et al. 2004), and in the Belfort area (Khattabi away from the storage basins B6 at a depth of 3 m)
et al. 2002). Heavy metal concentrations showed the showed topsoil and a layer of brownish and green-
following sequence: Fe>Cr>Cu>Zn>Pb>Ni>Mn> ish compact clay (2.2 m) followed by another thin
Cd. The average concentrations of Zn, Cu, Cd, Pb, Ni, layer of brown clay (0.7 m).
and Mn were well below the Tunisian regulations for – E2 (36° 44′ 15″ N/10° 04′ 31″ E, distant of 60 m of
discharge in a public sewer whereas Fe and Cr exceeded the leachate basin storage B7 with a final depth of
the permissible limits of Tunisian regulations. 3 m): After the topsoil, 1.3 m greenish clay was
Generally, the metallic load of studied leachate found. Then, yellow compact clay layer reached
corresponded to a typical composition of leachate gen- 1.1 m thick, whereas greenish clay with traces of
erated by urban landfill nationally and internationally gypsum was located at a depth of 0.2 m. Finally,
(Table 2). brown and yellow clays were found up to 3 m
The relatively low concentration of the studied heavy depth.
metals coupled with high BOD, COD, and nitrogen – E3 (36° 44′ 18″ N/10° 04′ 33″ E, 10 m from the
concentration further confirmed the high organic con- storage basin B7): After the topsoil, a greenish
tent of the waste deposited in the Jebel Chakir landfill compacted clay layer was found between 1.3 and
(Zairi et al. 2004). As compared to European norm 3 m depth.
relative to controlled landfills, the effluents of the Jebel – E4 (36° 44′ 14″ N/10° 04′ 37″ E, 30 m from the
Chakir landfill appear much less loaded in mineral storage basin B8): It consisted mainly of greenish

Table 2 Comparison of metal concentrations of Jebel Chakir landfill leachates in relation to others national and international landfills

Concentration Landfill of El Jebel Landfill of El Landfill of Landfill of Variation of metal

of heavy metals Chakir (Tunisia) Jadida (Morocco)a Alger (Algeria)b Etueffont (France)c concentrations of urban
in leachates landfill leachatesd

Fe (mg/l) 21,480 24 12.3 2.63 3–5,500

Cr (mg/l) 1.17 0.156 0.500 0.27 0.02–1.5
Zn (mg/l) 0.745 0.747 0.700 0.74 0.03–1,000
Cu (mg/l) 0.795 0.158 0.450 0.27 5–10
Cd (mg/l) 0.044 0.034 – 0.1 0.0001–0.4
Ni (mg/l) 0.23 0.134 0.250 0.21 0.15–13
Pb (mg/l) 0.35 – – – –
Mn (mg/l) 0.046 1.257 0.400 – 0.03–1,000
a
Chofqi et al. 2004
b
Kerbachi and Belkacemi 1994
c
Khattabi et al. 2002
d
Christensen et al. 2001
5038 Environ Monit Assess (2014) 186:5033–5040

Fig. 3 Geological cross section showing lithologic succession near the basins storage of the landfill of Jebel Chakir

clay with gypsum (0.9 m) and then brown clay The metal values found in soil samples varied over a
(1.6 m). The final depth of E4 was 3 m. wide range as follows: from 0.2 to 1.8 mg/kg of DM
(Cu), from 5.6 to 16.1 mg/kg of DM (Pb), from 15.1 to
This survey has been undertaken to show the impor- 43.9 mg/kg of DM (Ni), from 4.1 to 81.8 mg/kg of DM
tant role of different clay levels of different aspects (Zn), and from 54.4 to 129.9 mg/kg of DM (Cr). The
(tuffaceous in top and compacted to the basis) with a highest value of Cr (129.9 mg/kg of DM) was recorded
depth of 3 m that usually followed by topsoil in the at excavation E3 implanted to a nearest distance of the
study area. storage basin, probably because of metal-processing and
Those excavations reached 3 m depth, but could not textile industries, tanneries, treatment of surfaces,
exceed this depth because of technical constraints of sprays, and mineral wastes dumped in the Jebel Chakir
exploitation (drains, wells). They showed a little change landfill.
in color: brownish, yellow, and greenish (Fig. 3). The The average metal leaching values found in this study
permeability tests were carried out in laboratory on were also compared with values reported from other
natural clay samples collected at the bottom of four studies. For almost all the samples, the heavy metal
excavations (ASTM 2434 2006); our results showed contents are close to or even less than those measured
an average permeability varying from 3×10−12 to 8.4× values in the Greek and the Ivoirian landfills (Kouame
10−10 cm/s, confirming that the bottom of the storage et al. 2006; Kasassi et al. 2008).
basins could be considered as impermeable. Quality control of the soil in the studied areas was
performed according to the limit values given by the
Geochemical study European norm. It was obvious that at the Jebel Chakir
landfill, the average of heavy metal values was lower
In order to evaluate the contaminated levels by heavy than the critical values given by the European norm
metals, a geochemical study of air-dried soil samples (Table 3).
was performed. The distribution of the different heavy Excavations E1 and E4 showed a decrease of heavy
metals versus depth showed low concentrations of Cu, metals and of TOC from a depth of 2 m to the bottom.
Pb, and Zn and high concentration of Ni and Cr of air- This is probably due to the insulated clay being at a high
dried soil samples. Cadmium was not detected in all level. In fact, E2 and E3 showed an increase (near
samples (Fig. 4). Furthermore, heavy metal concentra- storage basins B7). It is also important to notice that
tions recorded in the gypsum level were lower than the heavy metals and total organic carbon were recorded
those of the clay levels, confirming the retention of these in excavation E3 (10 m to the storage basin B7) and
compounds by clayey soils. were higher than in the excavation E2 (60 m to the
Environ Monit Assess (2014) 186:5033–5040 5039

Excavation E1 Excavation E2
mg/Kg of DM mg/Kg of DM
0 50 100 150 0 50 100 150
0m 0 0m 0
Cu Cu
0,5 Pb 0,5 Pb
Ni Ni
1m 1 Zn 1m 1 Zn
Depth (m)

Depth (m)
1,5 Cr 1,5 Cr
COT COT
2m 2 2m 2
2,5 2,5
3m 3 3m 3
3,5 3,5

Excavation E3 Excavation E4
mg/Kg of DM mg/Kg of DM
0 50 100 150 0 50 100 150
0m 0 0m 0
Cu Cu
0,5 Pb 0,5 Pb
1m Ni 1m 1 Ni
1

Depth (m)
Zn
Depth (m)

Zn
1,5 Cr 1,5
Cr
COT 2 COT
2m 2 2m

2,5 2,5
3m 3
3m 3
3,5
3,5

Topsoil Glaygypsum Clay Chalk

Fig. 4 Variation of heavy metals and total carbon (TOC) contents with the depth on four excavations (E1, E2, E3, and E4)

storage basins B7), which proved that lateral migration assimilated solid waste of the great City of Tunis since
of pollutants was less important than the vertical one. May 1999 with an average of 1,800 tons/day. This
landfill produced a highly polluted leachate with an
average of 342 m3/day in anaerobic degradation. The
main pollution source in the Jebel Chakir landfill is
Conclusions linked to the infiltration of leachate that conveys a strong
polluting load and to the direct contact of the leachate
The Jebel Chakir landfill was the first controlled dump- with the soil substratum.
ing site in Tunisia. It received the municipal and Based on the results of investigation works, the
pollutants migrate vertically rather than laterally,
Table 3 Comparison of concentrations of the heavy metals of the whereas the site presents high clay levels accumu-
soil of the landfill of Jebel Chakir with the European norms
lating heavy metals and organic matter. So, to pre-
Parameters Concentrations of the Limit values in soil vent further potential pollution of soil and water, it
(mg/kg of DM) heavy metals of the European norm is recommended to:
landfill of Jebel Chakir (86/278/EEC) (mg/kg
(mg/kg of DM) of DM) (Fras 2006)
– Stop immediately the storage of leachate in earth
Chromium 54.4–129.9 50–140 basins
Zinc 4.1–81.8 150–300 – Set an insulated barrier under storage basins
Nickel 15.1–43.9 30–75 reaching the geological substratum
Lead 5.6–16.1 50–300 – Build a concrete basin to store leachate and to
Copper 0.2–1.84 50–140 guarantee the protection of the substratum
– Set a system of treatment of landfill leachates
5040 Environ Monit Assess (2014) 186:5033–5040

– Set a piezometer to control the groundwater quality sedimentären Gesteinen. Zeitschrift für Analytische Chemie,
266, 196–201.
and survey its evolution with time and space.
Kasassi, A., Rakimbei, P., Karagiannidis, A., Zabanitou, A.,
Tsiouvaras, K., Nastis, A., et al. (2008). Soil contamination
by heavy metals: Measurement from a closed unlined land-
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