Analytical Letters

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Assessment of Heavy Metal Pollution and

Ecological Risk of Roadside Soils in Tlemcen
(Algeria) Using Flame-Atomic Absorption
Spectrometry

Soumia Ramdani, Amina Amar, Kamal Belhsaien, Souad El Hajjaji, Said

Ghalem, Abdelmjid Zouahri & Ahmed Douaik

To cite this article: Soumia Ramdani, Amina Amar, Kamal Belhsaien, Souad El Hajjaji, Said
Ghalem, Abdelmjid Zouahri & Ahmed Douaik (2018) Assessment of Heavy Metal Pollution
and Ecological Risk of Roadside Soils in Tlemcen (Algeria) Using Flame-Atomic Absorption
Spectrometry, Analytical Letters, 51:15, 2468-2487, DOI: 10.1080/00032719.2018.1428985

To link to this article: https://doi.org/10.1080/00032719.2018.1428985

Published online: 23 Apr 2018.

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ANALYTICAL LETTERS
2018, VOL. 51, NO. 15, 2468–2487
https://doi.org/10.1080/00032719.2018.1428985

ENVIRONMENTAL ANALYSIS none defined

Assessment of Heavy Metal Pollution and Ecological Risk of

Roadside Soils in Tlemcen (Algeria) Using Flame-Atomic
Absorption Spectrometry
Soumia Ramdania, Amina Amara, Kamal Belhsaienb,c, Souad El Hajjajib, Said Ghalemd,
Abdelmjid Zouahric, and Ahmed Douaikc
a
Condensed Matter and Sustainable Development Laboratory, University of Sidi Bel Abbès, Sidi Bel Abbès,
Algeria; bLS3M2E-CERNE2D, Department of Chemistry, Faculty of Sciences, Mohammed V University, Rabat,
Morocco; cResearch Unit on Environment and Conservation of Natural Resources, National Institute of
Agricultural Research, Rabat, Morocco; dLaboratory of Natural Products and Bioactives, Aboubekr Belkaid
University of Tlemcen, Tlemcen, Algeria

ABSTRACT ARTICLE HISTORY

In Algeria, few studies have been conducted on the evaluation of Received 10 December 2017
roadside soil pollution. A total of 34 soil samples (28 roadside and 6 Accepted 14 January 2018
off-road) was obtained at 0–20 cm depth along the RN 35 national KEYWORDS
road. Heavy metal (Cd, Cr, Cu, Fe, Ni, Pb, and Zn) contents were Algeria; atomic absorption
extracted using aqua regia digestion and determined using atomic spectrometry (AAS);
absorption spectrometry. Background values of heavy metal contents ecological risk; heavy metal;
were determined using the robust statistical method of median plus pollution; roadside soil
two times the median absolute deviation. Single- and multi-element
pollution and ecological risk indices were calculated. The results
showed that background values were 2.5 � 0.3, 64.9 � 8.1, 28.0 � 4.1,
29371.5 � 4403.0, 32.9 � 4.4, 72.2 � 12.8, and 445.1 � 62.9 mg/kg for
Cd, Cr, Cu, Fe, Ni, Pb, and Zn, respectively. The results were all higher
than their corresponding median values. Single-element pollution
indices (enrichment factor and geoaccumulation index) showed that
the pollution is primarily due to Pb and Zn. Multi-element pollution
index (Nemerow index) indicated that only 3% of the soil samples are
strongly contaminated, whereas 23% are seriously contaminated. The
potential ecological risk index showed that Cd is the most harmful
element, followed by Pb and Zn. 65% of the soil samples had
moderate potential ecological risk, while only 3% had considerable
potential ecological risk. This study may be used as a baseline for
future monitoring and as a tool for decision-making regarding
environmental protection policies and sustainability of this semiarid
agroecosystem.

Introduction
The ever-increasing world population put more pressure on the soil to produce more food.
This pressure leads to the intensification of agriculture using more fertilizer and pesticides
(Josephson, Ricker-Gilbert, and Florax 2014). Although agriculture intensification allows
improved crop production, it may result in the degradation of the quality of the soil due
to erosion, salinization, and contamination (Tilman et al. 2001).

CONTACT Ahmed Douaik ahmed_douaik@yahoo.com Research Unit on Environment and Conservation of Natural
Resources, National Institute of Agricultural Research, PO Box 6356, Rabat, Morocco.
© 2018 Taylor & Francis
 ANALYTICAL LETTERS 2469

Furthermore, the current economic development model, based on the industrialization

and urbanization, contributes to exacerbate soil pollution, especially from heavy metals
(Zhang et al, 2013). In particular, urban traffic is a main source of heavy metal pollutants
for urban and roadside soils (Werkenthin, Kluge, and Wessolek 2014). These pollutants are
emitted by different parts of vehicles and road materials (Legret and Pagotto 2006). For
example, cadmium is released by vehicle tires and the burning of vehicle fuels (Zhang
et al. 2015); zinc is released by lubricating oils and tire abrasion (Smolders and Degryse
2002); copper may result from brake linings and tires (Hjortenkrans, Bergback, and
Haggerud 2007); lead can be emitted from leaded fuels (Van Bohemen and Van de Laak
2003); while chromium is released from abrasion of tires and brake pads and also from
oil residues (Zehetner et al. 2009).
Most of the time, heavy metals originating from road traffic (vehicles and road
materials) are suspended under the atmosphere in the form of dust. They may be deposited
into the soil following any rainfall event. These heavy metals can be unevenly distributed
in space due to many factors like wind (Piron-Frenet, Bureau, and Pineau 1994), rainfall,
traffic type and intensity, condition of road, and land use types (Liu et al. 2016).
Since heavy metals are not degradable, they reside in soils for a long time. Consequently,
they contribute to the damage of soil living organisms and to the toxicity of plants as they
migrate from roots to shoots and other parts of plants (Wang et al. 2013). This toxicity can
also be a main threat to the health of humans and animals.
Once the heavy metal contents are determined in the laboratory, the pollution and the
ecological risk can be measured. The pollution is assessed using either single- (one heavy
metal) or multi-element (many heavy metals) indices. Among the most used single-element
indices are the enrichment factor (EF), the geoaccumulation index (Igeo), and the
contamination factor (CF). Regarding multi-element indices, the most common ones are
the pollution load index, the modified degree of contamination (mCd), the Nemerow
pollution index (NI), and the modified Nemerow pollution index (mPI). The ecological
risk can be evaluated using either single-element index like the monomial potential
ecological risk (Er) or multi-element index like the potential ecological risk index (PERI).
Cai et al (2015) compared seven single- and multi-element pollution and ecological risk
indices and found that the best were ranked as follows: Igeo > NI > EF > PERI
(Papaioannoua et al. 2017). These four indices are used in this research work.
All of the pollution and ecological risk indices require definition of a local reference of
background value for each of the heavy metals (Tume et al. 2017). These background values
are considered to be the heavy metal contents for unpolluted soils, meaning the natural
contents without the human influences (Salminen and Gregorauskien 2000). There are
basically two methods for determining background value. These are empirical geochemical
or direct methods and the statistical or indirect methods (Dung et al 2013). Moreover,
these two methods can also be combined resulting in a third kind of methods: the
integrated ones.
Many studies on roadside soil pollution have been undertaken in different parts of the
world (Akbar et al. 2006; Aktas and Kocabas 2010; Aslam, Khan, and Khan 2013; Kluge,
Werkenthin, and Wessolek 2014). However, in Algeria, very little work has been done
regarding roadside soil pollution (Bouras et al. 2010). Moreover, no work has been done
in the neighborhood of the city of Tlemcen, Northwest of Algeria. The RN 35 national
road, linking the cities of Maghnia and Remchi in the Willaya of Tlemcen, is an important
2470 S. RAMDANI ET AL.

transportation way for these two cities which are experiencing fast economic and
demographic growth.
The objectives of the present research work are to determine the concentrations and the
background concentrations of seven heavy metals in the soil around the RN 35 national
road; to evaluate the degree of pollution in the roadside soils using different single- and
multi-element pollution indices; and to assess the ecological risk to humans and animals
using potential ecological risk indices.

Materials and methods

Study area
The study area belongs administratively to the province of Tlemcen in Northwest
Algeria (Figure 1). The RN 35 national road links the cities of Maghnia and Remchi across
43 km from coordinates 34° 500 35.46″ N and 1° 420 26.90″ W to 35° 050 03.32″ N and 1° 260
14.49″ W. It is the main road of the city of Maghnia in its exchanges with other
municipalities in the province of Tlemcen and neighboring cities. This is a busy road with
a traffic rate of 21600 vehicles/day in both directions for 2013 with 12% for trucks and 88%
for light vehicles (Public Works Department 2013). Agriculture is the only economic
activity in the region with no industries. There is a gas station along the road between
the S5 and S7 soil samples at the crossing of RN 35 and RN 98 roads (Figure 1). The climate
is characterized by a cold winter and a very hot summer. The annual rainfall varies between
400 and 600 mm (Public Works Department 2014). The RN 35 road crosses the following
geological formations (Public Works Department 2014): quaternary alluvial and limestone
crusts; pliocene stony calcareous alluvial lake districts; and miocene marl, clay, sandstone,
and conglomerate.

Figure 1. Sampling sites of roadside soils along the RN 35 National Road, Tlemcen, Algeria.
 ANALYTICAL LETTERS 2471

Soil sampling
A total of 34 soil locations was sampled along the RN 35 national road. Among them, 28 sites
(S1 to S28) were sampled in the spring of 2014, in both directions, 2 m from the edge of the
roadway and at a depth of 0–20 cm (Figure 1). Each sample consists of five subsamples taken
from the same depth. Also, six other samples were taken from remote control soils (T1 to T6),
500 m apart from the roadside, in both directions. All soil samples were collected using a stain-
less steel hand auger. They were stored in polyethylene bags and transported to the laboratory.
The samples were dried in the open air and then at 40°C for 24 h and sieved to remove large
debris and stones. The samples were manually crushed in a porcelain mortar before being
sieved to 2 mm. After these pretreatments, samples were stored until analysis.

Soil heavy metal analysis

Heavy metals of soil samples were extracted using the hot aqua regia digestion method
according to the Norme Française International Organization for Standardization (1995)
11,466 protocol (1995) and their total concentrations were determined. The widespread
use of the hot aqua regia digestion method is due to its simplicity and adaptability as a
routine procedure (Siaka, Owens, and Birch 1998). Nitric (HNO3) and hydrochloric
(HCl) acids were used for the mineralization of soil. A total of 3 g of soil sample was treated
with 21 mL of HCl and 7 mL of HNO3 and was kept at room temperature for 24 h. The
samples were next heated in a sand bath on a hot plate to 50°C for 5 h and refluxed at
130°C for 3 h. The samples were filtered, washed with doubly distilled water, and placed
in 50-mL volumetric flasks.
The heavy metal concentrations were determined using atomic absorption spectrometry
on a Perkin Elmer Analyst Instrument 300 Atomic Absorption Spectrometer device using
hollow cathode lamps with flame and electrothermal atomization. The results are reported
as mg/kg of dry matter.

Background value
As pointed out in the introduction, the calculation of pollution indices requires the
knowledge of background levels. These values are used for distinguishing between natural
or geogenic origin and the non-natural or anthropogenic influences (Baise and Sterckeman
2001; Reimann and Garret 2005; Galuszka 2007).
Background values are determined using either the geochemical, also called empirical or
direct, approach (Dung et al. 2013; Matschullat et al. 2000) or the statistical or indirect
approach (Matschullat et al. 2000; Mrvic et al. 2011). The former approach is criticized
and the latter is recommended (Reimann and De Caritat 2000; Reimann, Filzmoser, and
Garret 2005).
There are many statistical methods for determining background values ranging from
univariate to multivariate and from parametric to nonparametric, and currently data
mining approaches are used. The oldest is a parametric univariate method based on mean
� 1, 2, or 3 times standard deviation assuming a normal distribution which is rather the
exception than the rule in geochemistry (Reimann and Filzmoser 2000). A first solution
was to do an iterative approach, deleting the outliers until a normal distribution was
obtained (Roca, Pazos, and Bech 2012). A better approach is to use graphical tools like
2472 S. RAMDANI ET AL.

estimated or calculated cumulative distribution function (CDF), probability plots (Karim,

Qureshi, and Mumtaz 2014), or robust or nonparametric methods that are resistant to
outliers. For example, median �2 times median absolute deviation (MAD) (Reimann,
Filzmoser, and Garret 2005; Rothwell and Cooke 2015) or exploratory data analysis like
the box plot (Hoaglin, Mosteller, and Tukey 2000; Bounessah and Atkin 2003) may be
used. In this study, we used the robust or nonparametric statistical method, i.e., the median
and the MAD (Reimann, Filzmoser, and Garret 2005, Zinkute et al. 2017).

Pollution indices
Enrichment factor
The enrichment factor (EF) is the oldest single-element pollution index (Turekian and
Wedepohl 1961). It was defined, originally, as the ratio of the concentration of a metal
to the concentration of an immobile element for a given sample divided by the same ratio
for a reference sample (Abrahim and Parker 2008; Arab et al. 2015):
ðCi =Cie ÞS
EF ¼ ð1Þ
ðCi =Cie ÞRS
where (Ci/Cie)S is the ratio of the concentration of the ith heavy metal to that of an
immobile element in a given sample and (Ci/Cie)RS the same parameter for the reference
sample. Examples of immobile elements are iron and aluminum. The average earth crust
content was considered to be the background. This definition has some intrinsic flaws
(Reimann and De Caritat 2000). The EF was redefined, following the new definition of
background value (Sutherland et al. 2000; Mmolawa, Likuku, and Gaboutloeloe 2011;
Lar, Ngozi-Chika, and Ashano 2013):
ðCi ÞS
EF ¼ ð2Þ
½medianðCi ÞB þ 2� MADðCi ÞB �
with (Ci)S being the concentration of a given heavy metal in any one of the roadside and
background soil samples, median(Ci)B is the median concentration of an element in the
background soil samples, and MAD is a robust indicator of variation around the median
defined as (Reimann, Filzmoser, and Garret 2005, 2017):
MAD ¼ 1:48� median½ðCi ÞS medianðCi ÞS � ð3Þ
Sutherland (2000) defined five contamination categories based on the EF:
EF < 2: minimal enrichment; 2 � EF < 5: moderate enrichment; 5 � EF < 20: significant
enrichment; 20 � EF < 40: very high enrichment; and EF ≥ 40: extremely high enrichment.

Geoaccumulation index
The second old single-element pollution index is due to Muller (1969). It is called Igeo and it
compares the present (any sample) and past (background) heavy metal concentrations (Iqbal
and Shah 2011; You et al. 2015; Giri, Singh, and Mahato 2017). It is defined, in its original
form, as log2 of the ratio between the concentrations of the ith heavy metal to 1.5 times that
of the same metal from the background sample. Later, following the new definition of back-
ground value, Igeo was defined to be (Mmolawa, Likuku, and Gaboutloeloe 2011):
Igeo ¼ log2fðCi ÞS =½1:5� medianðCi ÞB �g ð4Þ
 ANALYTICAL LETTERS 2473

Muller (1969) and Sutherland (2000) distinguished seven classes for the Igeo: Igeo �0:
uncontaminated; 0 < Igeo � 1: slightly contaminated; 1 < Igeo � 2: moderately
contaminated; 2 < Igeo � 3: moderately to heavily contaminated; 3 < Igeo � 4: heavily
contaminated; 4 < Igeo � 5: heavily to extremely contaminated; and Igeo > 5: extremely
contaminated.

Nemerow pollution index

The Nemerow pollution index (NI) is defined as (Nemerow, 1991):
p�
ðCFMax Þ2 þ ðCFAve Þ2
�
NI ¼ ð5Þ
2
where CFMax is the maximum among the contamination factor (CF) values of the n heavy
metals for a given sample and CFAve is the arithmetic mean of these CF values. The CF is
defined to be (Mmolawa, Likuku, and Gaboutloeloe 2011):
� �
ðCi ÞS
CF ¼ ð6Þ
medianðCi ÞB
where (Ci)S and median(Ci)B are defined as above.
The Nemerow pollution index is, probably, the most used multi-element pollution index
with examples from different countries and different supports or media: Mohammed et al.
(2012) for Australia, Ma et al. (2015) for China, and Giri, Singh, and Mahato (2017) for
India.
Seven categories can be distinguished for the NI (Giri, Singh, and Mahato 2017): NI < 1:
uncontaminated; 1 � NI < 2: slightly contaminated; 2 � NI < 3: moderately contaminated;
3 � NI < 5: strongly contaminated; and NI ≥ 5: seriously contaminated.

Potential ecological risk index

The three former indices are indicators of the level of pollution. To assess the ecological
risk of heavy metals, Hakanson (1980) defined the PERI as the sum of the monomial
potential Er factors:
PERI ¼ ð1=nÞREr for n heavy metals ð7Þ
with Er ¼ CF/Tr where CF is as defined above and Tr are the “toxic response” factors
specific to each heavy metal. For our case study, Tr has the values 30, 2, 5, 5, 5, and 1
corresponding to Cd, Cr, Cu, Ni, Pb, and Zn, respectively (Hakanson, 1980).
Hakanson (1980) distinguished four categories for PERI. However, as for Er, he used
eight elements (PCB and seven heavy metals: Hg, Cd, As, Cu, Pb, Cr, and Zn). The sum
of their Tr is 133 rounded to 150 (Saeeidi et al. 2014; Wu et al, 2017; Liu et al, 2018) which
is the threshold for the first class for PERI, the other thresholds are found just by doubling
the former threshold: 300 and 600. In our study, we have only six heavy metals for which
the sum of Tr is 48 that is rounded to 50. Thus, the original thresholds from Hakanson’s
(1980) work were adapted (Zhu, Bian, and Li 2008) to give 50, 100, and 200: PERI < 50:
low potential ecological risk; 50 � PERI < 100: moderate potential ecological risk;
100 � PERI < 200: high potential ecological risk; and PERI ≥200: significantly high
potential ecological risk.
2474 S. RAMDANI ET AL.

Statistical analyses
First of all, the distribution of heavy metal contents was checked to test the normality of the
distribution, either graphically using histogram or box plot or numerically by computing
the skewness and using the formal Shapiro–Wilk test. In the affirmative, descriptive
statistical parameters like the arithmetic mean, the standard deviation, the minimum,
the maximum, and the coefficient of variation (CV) were considered. When the hypothesis
of normality was rejected, robust or nonparametric descriptive statistical parameters like
median, MAD, and robust CV were used.
The geochemical background threshold values (GBTV) were computed for each heavy
metal as the median þ2 * MAD after an iterative procedure. In addition, main descriptive
statistical parameters (mean, standard deviation, minimum, and maximum) were computed
for the different single-element and multi-element pollution and ecological risk indices.
All statistical computations were done using the Microsoft Excel and the IBM SPSS
Statistics.

Results and discussion

Heavy metal contents
The histograms (Figure 2) and the skewness coefficients (Table 1) show that all seven heavy
metals, except Cd, were either negatively (Cr and Fe) or positively (Cu, Ni, Pb, and Zn)
skewed. This skewness implies that only the distribution of Cd is symmetric, whereas
the distribution of the other six heavy metals is asymmetric; this asymmetry being clearly
more pronounced for Pb and Zn, since they have the strongest skewness coefficients (2.94
and 2.04, respectively). In addition, the box plots (Figure 3) show the presence of some
abnormally low or high (circles) or even some extreme (stars) values. Moreover, the CDFs
(not shown) show that only Cd has a normal distribution, whereas all the other six heavy
metals do not follow a normal distribution as is usually the case in the environmental
geochemistry (Reimann and Filzmoser 2000). The either normal or non-normal
distribution is confirmed by the Shapiro–Wilk test with probability ≥0.05 and <0.05,
respectively (Table 1). The non-normality of the heavy metal distributions is illustrated
by the large discrepancies between the mean and median values, for example, 373.2 against
126.8 mg/kg for Zn or 57.3 against 41.4 mg/kg for Pb.
According to their median values, heavy metals can be ordered as Fe > Zn > Cr > Pb >
Ni > Cu > Cd with 17787.5, 126.8, 45.3, 41.4, 22.4, 16.1, and 1.9 mg/kg. Range values were
1.2–3, 10.8–60.3, 5.5–39.8, 53.8–27675, 7.8–47.3, 5.5–301.3, and 52.5–1952.5 mg/kg for Cd,
Cu, Cr, Fe, Ni, Pb, and Zn, respectively. Based on the robust coefficient of variation,
defined as the ratio between the MAD and the median (Reimann and De Caritat 2005;
Reimann et al. 2008), the most variable heavy metals were Zn (71.4%) and Pb (51.4) which
show high variability (Qing, Yutong, and Shenggao 2015), followed by Cu (29.8%), Fe
(24.8%), and Ni (22.3%) showing moderate variability, whereas the least variable ones were
Cd (18.8%) and Cr (18%) which show low variability. Based on these values, it is expected
that Cd, Cu, Cr, Fe, and Ni are dominated by natural sources, whereas Pb and Zn are likely
to be affected by anthropogenic sources (Manta et al. 2002). Also, the high coefficient of
variation values of Pb and Zn contents and their wide ranges suggest a multiplicity of their
sources (Yongming et al. 2006).
 ANALYTICAL LETTERS 2475

Figure 2. Histograms of the soil heavy metals with fitted theoretical probability distributions.
2476 S. RAMDANI ET AL.

Table 1. Descriptive statistics of soil heavy metals.

Probability
Robust corresponding
Coefficient coefficient to the
Median of of Shapiro–Wilk
Standard absolute variation variation test of
Element Mean Median deviation deviation (%) (%) Minimum Maximum Skewness normality
Cd 1.9 1.9 0.4 0.4 19.9 18.8 1.2 3.0 0.55 0.541
Cr 44.2 45.3 10.7 8.1 24.2 18.0 10.8 60.3 −1.47 0.001
Cu 16.9 16.1 6.7 4.8 39.6 29.8 5.5 39.8 0.98 0.048
Fe 16668.0 17787.5 7266.7 4403.0 43.6 24.8 53.8 27675.0 −1.13 0.001
Ni 24.4 22.4 8.2 5.0 33.7 22.3 7.8 47.3 1.08 0.004
Pb 57.3 41.4 60.0 21.3 104.8 51.4 5.5 301.3 2.94 0
Zn 373.2 126.8 510.7 90.5 136.8 71.4 52.5 1952.5 2.04 0

Background levels of heavy metals

The GBTV were calculated, for each heavy metal, as Median þ2 * MAD (Table 2). Since all
the heavy metals except Cd did not follow the normal distribution, the calculations were
done on the raw data for Cd but using the logarithmic scale for the remaining six heavy
metals. Then, for the latter, background levels were transformed back to get these levels
on the original scale. The highest GBTV is for Fe (29371.5 mg/kg) and the lowest is for
Cd (2.5 mg/kg). The ranking from the highest to the lowest GBTV is Fe > Zn > Pb > Cr >
Ni > Cu > Cd. The same ranking was observed for the median values with the exception
of the inversion of the ranks for Cr and Pb. The median values of the seven heavy metals
(Table 1) were all lower than their corresponding regional background values (Table 2).
Any heavy metal value lower than the corresponding GBTV is considered to be the
geochemical background representing the geogenic or natural origin and that higher values
than the GBTV can be assumed as outliers coming from anthropogenic origin (Figures 2
and 4).
There were no outliers for Cr and Fe and all 34 samples can be considered as natural or
geogenic, while there were one, two, four, five, and seven outliers for Cu, Cd, Ni, Pb, and
Zn, respectively, representing the anthropogenic contribution which represents 2.9, 5.9,
11.8, 14.7, and 20.6% of the total samples (Table 2 and Figure 4). The outliers were not
always found for the same soil samples, but it was the case for some heavy metals: S13
and S27 for Cd; S3 for Cu; S4, S6, S13, and S16 for Ni; S3, S11, S12, S13, and S16 for
Pb; and S5, S7, S8, S15, S24, S25, and S28 for Zn. More attention should be given to the
recurrent samples S3 for Cu and Pb; S13 for Cd, Ni, and Pb; and S16 for Ni and Pb.
As there is no industry in the study area, the origin of Cd in roadside soils may be due to
lubricating oils and the wearing of tires and brake pads (Okunola, Uzairu, and Ndukwe
2007; Yan et al. 2013; Aryal et al. 2017). High levels of Cd can be also attributed to
agriculture, mainly the use of agrochemicals (fertilizers and pesticides) that are potential
sources of various metals (Bhatti et al. 2017), in particular the phosphatic parent rock
(Mortvedt 1996; Savci 2012).
According to Addo et al. (2012), most of the Cu particles are released from vehicle
components more than from exhaust gas, and from the corrosion of metallic parts, in diesel
which deposit in the topsoil close to the road edge (Lu et al. 2009). The Fe contents were
found to be significantly higher than other metals due to their abundance in parent rock
material (Bhatti et al. 2017). The source of Ni in roadside dust is believed to be due to
 ANALYTICAL LETTERS 2477

Figure 3. Box plots of the soil heavy metals.

2478 S. RAMDANI ET AL.

Table 2. Geochemical background threshold value (mg/kg), number, and percentage of outliers
detected using the median absolute deviation criterion with comparison with two worldwide examples
from Hawaii and Poland. The nonassessed heavy metals are marked by NA (not applicable).
Element Cd Cr Cu Fe Ni Pb Zn
Geochemical background threshold value 2.5 64.9 28.0 29371.5 32.9 72.2 445.1
Number of outliers 2 0 1 0 4 5 7
Percentage of outliers 5.9 0 2.9 0 11.8 14.7 20.6
Manoa, Hawaii (Sutherland et al, 2000) NA NA 114.0 113800.0 310.0 14.0 141.0
Sadecki Beskid Mts, Poland (Kicinska, 2016) 0.6 30.0 NA NA 17.0 39.0 158.0

corrosion of vehicular parts (Lu et al. 2009). The contamination of soil with Ni compounds
modifies the physicochemical properties of soil.
Pb is a highly toxic element to humans, with urban areas characterized by a higher
contamination. There is a relationship between road traffic and lead contamination of
roadside soils (Nabulo, Oryem-Origa, and Diamond 2006; Radziemska and Fronczyk
2015), since Pb is found on roads as a result of vehicle emissions from the combustion
of gasoline containing tetraethyl lead (Mielke et al. 1983).
Wear and corrosion of vehicle parts (brakes, tires, radiators, bodies, and engine parts)
might be one of the potential sources of Zn (Adachi and Tainosho 2004; Councell et al.
2004). However, since Tlemcen is located in a mountainous region at a high altitude,
the oxygen rate in the atmosphere, decreasing with increasing altitude, may influence
the efficiency of gas consumption and vehicle emission mechanism. Previous studies
showed that vehicle emissions at high altitude may be much higher than that observed
at the sea level (Bishop et al. 2001).
Our GBTVs were compared to other published papers where they were computed using
the same robust statistical method that we used (median plus two times MAD) for soils
along roads (Table 2). Our Cd and Cr GBTV (2.4 and 64.9 mg/kg, respectively) were higher
(four times and twice, respectively) than those found in Poland (Kicinska, 2016), whereas
our Cu and Fe GBTV were much lower (four times for both) than those for Hawaii
(Sutherland et al, 2000). Our Ni GBTV (32.9 mg/kg) was not really different from that from
Poland (17 mg/kg) whereas it was lower (10 times) than that from Hawaii (310 mg/kg).
Also, our Pb GBTV was higher (twice) than that from Poland and much higher (five times)
than that from Hawaii. Finally, Zn GBTV from Poland and Hawaii were similar and
differed clearly (three times) than from our study. The differences between the three study
areas may be attributed to different natural sources (mainly parent material, climate, and
wet and dry deposition of atmospheric salts).

Pollution indices
Enrichment factor
The EF for the seven heavy metals were calculated using Eq. (2), their statistical descriptive
parameters are summarized in Table 3, and their box plots are displayed in Figure 5,
left side.
The maximal EF values (Table 3) were found for Zn and Pb (4.39 and 4.17) showing that
the roadside soils were mainly contaminated by these two heavy metals. Moreover, Figure 5
confirms this and shows some high to extreme EF values (samples S3 and S13 for Pb and
S5, S7, S8, S24, S25, and S28 for Zn). This is in agreement with what was found from the
 ANALYTICAL LETTERS 2479

Figure 4. Background upper limits (geochemical background threshold value: horizontal line) and soil
sample distribution for the heavy metals.
2480 S. RAMDANI ET AL.

Table 3. Statistical summary of the enrichment factor of the soil heavy metals.
Element Minimum Maximum Mean Standard deviation
Cd 0.48 1.19 0.77 0.15
Cr 0.17 0.93 0.68 0.16
Cu 0.20 1.42 0.61 0.24
Fe 0.00 0.94 0.57 0.25
Ni 0.24 1.44 0.74 0.25
Pb 0.08 4.17 0.79 0.83
Zn 0.12 4.39 0.84 1.15

Figure 5. Box plots of two single-element pollution indices: (a) enrichment factor and
(b) geoaccumulation index. Horizontal lines represent the different class thresholds.

box plot of the original heavy metal contents (Figure 3). The former cited samples can be
considered as having moderate enrichment, whereas all remaining samples for Pb and Zn
and all 34 samples for the other five heavy metals are minimally enriched (Table 4).

Geoaccumulation index
The Igeo values were calculated for the seven heavy metals using Eq. (4). Their summary
statistics are given in Table 5 and their box plots are shown in Figure 5 on the right side.
Again, as for EF, Zn, and Pb have the highest Igeo values (3.48 and 2.45), confirming
the pollution of roadside samples with Pb and Zn, whereas Cr has a negative maximal value
(−0.17), while Cd and Fe have almost zero values for maximal Igeo indicating that there is
no pollution of roadside soil samples with Cd, Cr, and Fe.

Table 4. Number (percentage) of soil samples in each category of two single-element pollution indices
(enrichment factor and geoaccumulation index).
Element Classes Cd Cr Cu Fe Ni Pb Zn
Enrichment factor <2 34 (100) 34 (100) 34 (100) 34 (100) 34 (100) 32 (94) 29 (85)
2–5 2 (6) 5 (15)
Geoaccumulation index <0 33 (97) 34 (100) 31 (91) 32 (94) 30 (88) 23 (68) 19 (56)
0–1 1 (3) 3 (9) 2 (6) 4 (12) 7 (20) 8 (23)
1–2 2 (6) 0 (0)
2–3 2 (6) 5 (15)
3–4 2 (6)
 ANALYTICAL LETTERS 2481

Table 5. Statistical summary of the geoaccumulation index of the soil heavy metals.
Element Minimum Maximum Mean Standard Deviation
Cd −1.24 0.08 −0.58 0.29
Cr −2.66 −0.17 −0.68 0.51
Cu −2.13 0.73 −0.62 0.61
Fe −8.96 0.05 −1.37 2.38
Ni −2.09 0.52 −0.51 0.49
Pb −3.33 2.45 −0.46 1.24
Zn −1.74 3.48 0.16 1.52

Figure 5 shows the presence of some high Igeo values for Pb and Zn (especially samples
S3 and S13 for Pb). However, there are also some noticeably low Igeo values, particularly
for Fe (samples S4, S6, S13, and S16), Cr (samples T5 and T6), and Ni (sample T6). The
entire 34 soil samples can be considered either not or slightly contaminated regarding
the heavy metals except for Pb and Zn (Table 4). For Pb, 88% of the samples is either
not or slightly contaminated, while 12% is moderately to heavily contaminated. Regarding
Zn, these classes include 79 and 21% of the samples, respectively.

Nemerow pollution index

Based on the CF, all 34 samples can be considered either of low or moderate contamination
regarding all heavy metals, except for Pb and Zn. For these two latter metals, in addition to
88 and 79% of the samples that have low to moderate contamination, there are 6% of the
samples that have considerable contamination and 6% having very high contamination for
Pb (samples S3 and S13). For Zn, there are 21% of the samples that belong to the very high
contamination (samples S5, S7, S8, S15, S24, S25, and S28).
The NI was calculated using Eq. (5). The results are reported in Tables 6 and 7 and
displayed in Figures 6 and 7. The soil samples are classified, in average, as strongly
contaminated based on the mean value of 3.05 (Table 6). Nevertheless, the maximal value
(12.02) indicates that samples can also be considered as strongly and even seriously
contaminated. Effectively, if there are only 3% uncontaminated, 56% slightly contaminated,
and 15% moderately contaminated samples, there are also 3% strongly and 23% seriously
contaminated samples (Table 7).
All of the off-road samples are either uncontaminated (T6) or slightly contaminated (all
the remaining five samples), whereas the strongly (S3) and the seriously contaminated (S5,
S7, S8, S13, S15, S24, S25, and S28) samples are roadside (Figure 7). Again, samples S5 and
S8 should be carefully inspected and monitored (Figure 6).

Potential ecological risk index

Based on the mean monomial potential Er factors, the ranking of the heavy metals from the
most to the least harmful is Cd > Pb > Ni > Cu > Zn > Cr. All the 34 samples are classified
as having low potential ecological risk regarding Cr, Cu, and Ni. Regarding Zn, there are
only two samples (6%, S5 and S8) that belong to the moderate potential ecological risk

Table 6. Statistical summary of the Nemerow index and the potential ecological risk index of the soil
heavy metals.
Index Minimum Maximum Mean Standard deviation
Nemerow index 0.70 12.02 3.05 2.95
Potential ecological risk index 24.62 108.43 54.55 15.17
2482 S. RAMDANI ET AL.

Table 7. Number and percentage of soil samples in each category of

Nemerow index and potential ecological risk index.
Index Classes Number Percentage
Nemerow index <1 1 3
1–2 19 56
2–3 5 15
3–5 1 3
>5 8 23
Potential ecological risk index <50 11 32
50–100 22 65
100–200 1 3

Figure 6. Box plots of (a) Nemerow index and (b) potential ecological risk index.

category, all of the remaining samples (94%) belong to the low potential ecological risk. For
Pb, 30 samples (88%), 2 samples (6%, S11 and S12), and 2 samples (6%, S3 and S13) are
classified as having low, moderate, and considerable potential ecological risk, respectively.
Finally, regarding Cd, there is no sample in the low potential ecological risk category, while
16 (47%) and 18 samples (53%) belong to moderate and considerable potential ecological

Figure 7. Class limits of (a) Nemerow index and (b) potential ecological risk index and soil sample
distribution for the heavy metals.
 ANALYTICAL LETTERS 2483

risk categories, respectively. In summary, Cd is the most harmful followed by Pb and, to a

lower extent, Zn. Regarding Cr, Cu, and Ni, there is only low potential ecological risk.
Based on the thresholds from Table 6, the mean PERI of 54.55, calculated based on
Eq. (7), classifies the study area as having a moderate potential ecological risk. Looking
deeper in the PERI values, it is noted that 11 samples (32%) have a low potential ecological
risk, while 22 samples (65%) and 1 sample (3%, S13) have moderate and considerable
potential ecological risk, respectively (Table 7). These overall potential ecological risks
are primarily linked to Cd and Pb, and secondarily to Zn as was noted for Er values.

Conclusion
This work had the primary goal of evaluating the pollution of agricultural soils along the
RN 35 national road in northwestern Algeria. The background values were all higher than
their corresponding median values. For Cr and Ni, none of the samples were above the
background value, whereas some samples were above their corresponding background
values for the remaining heavy metals. This is likely due to the anthropogenic activities,
including road materials and traffic.
The single-element pollution indices showed that the pollution is mainly due to Pb and
Zn with a moderate enrichment and a heavily contamination. The multi-element Nemerow
pollution index indicated that some samples are either strongly or seriously contaminated.
For the single-element potential ecological risk, Cd is the most harmful followed by Pb and
Zn. The multi-element potential ecological risk showed that some samples had moderate or
considerable potential ecological risk.
This study can be considered as a baseline for the assessment of heavy metal pollution
and ecological risk of roadside agricultural soils in northwestern Algeria. Specific attention
should be given to samples that showed high pollution and ecological risk indices. This
baseline may be used as a reference for future monitoring of the study area and also
as a tool for helping in decision-making regarding environmental protection policies,
sustainability of this semiarid agroecosystem, and safeguard the health of human beings,
animals, and plants.

Acknowledgments
The authors are thankful to Mr. Rabie Ghoul for his help in preparing Figure 1. The first author
would also thank the University of Sidi Bel Abbès for the financial support that allowed her to
visit Morocco, especially INRA, and this manuscript is the output of this Algerian–Moroccan
collaboration. We thank also Dr Mohamed Karrou, former Head of Department of Agronomy in
INRA and former Senior Research Scientist with ICARDA, for helping us to improve the quality
of the English language of the manuscript.

ORCID
Ahmed Douaik http://orcid.org/0000-0001-7374-4674

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