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A R T I C L E I N F O A B S T R A C T
Keywords: Heavy metal concentrations in surface sediments collected from 17 stations samples in Bizerte coastal line were
Heavy metals determined in order to evaluate the contamination status in the region. Heavy metal concentrations (mg/kg) of
Assessment Bizerte coast line followed the decreasing trend of Fe > Pb > Zn > Mn > Cu > Cr > Ni > Co > Cd. The pollution
Sediment
degree of the surface sediment collected from 17 samples station in Bizerte coast line by heavy metals was
Contamination
Bizerte coast line
evaluated on the basis of pollution indices (EF, Igeo, CF, PLI and CD). Results of Igeo, EF, CF, PLI and DC
demonstrated that pollution levels of Pb and Cd were moderate, which should require more attentiveness as main
pollution factors. However, no pollution was found for Zn, Cu, Ni, Cr, Co and Mn. Hierarchical cluster analysis
was used to identify the influence of anthropogenic activities on the surface sediment.
* Corresponding author.
E-mail address: abdelwaheb_2000@yahoo.fr (A. Aydi).
https://doi.org/10.1016/j.marpolbul.2022.114171
Received 11 January 2022; Received in revised form 19 September 2022; Accepted 20 September 2022
Available online 28 September 2022
0025-326X/© 2022 Elsevier Ltd. All rights reserved.
A. Aydi et al. Marine Pollution Bulletin 184 (2022) 114171
Tunisia. Statistical analysis of data was performed, allowing to ascertain to human pressures including agricultural, urban, and industrial activ
relationships between investigated variables in the samples and to ities that generate significant quantities of various types of pollutants
identify the origin of the heavy metal pollution sources of the studied (liquids, solids, and gases) (El Zrelli et al., 2021). Among these pollut
area. The study of their potential contamination refined by application ants, heavy metals are considered the most toxic ones which can lead to
of multi-indicators evaluation methods through the geo-accumulation further pollution in the aquatic environments (Alves Martins et al.,
index, enrichment factor, contamination factor, pollution load index, 2016).
degree of contamination, and principal component analysis. In August 2019, surface sediment samples were collected in triplicate
from 17 stations located along the coastal zone of Bizerte. A Van Veen
2. Materials and methods grab sampler (305 mm x305 mm) was used to take samples of superficial
sediments (5 cm depth).Sediment samples were collected and stored in
The Bizerte coast line, which has an approximate length of 6 km, glass jars at 4 ◦ C before being air-dried at room temperature (25 ◦ C) and
width of 300 m and depth of 12 m was chosen as the research area. It is sieved through a 2-mm mesh.
located between the coordinates 37◦ 15′ 15′′ N - 9◦ 52′ 50′′ E and 37◦ 15′ About 0.2 g of air-dried sediment sample was digested by the
15′′ N - 9◦ 51′ 02′′ E on the northern of Tunisia (Fig. 1). In this area, there dissolution technique using a mixture of concentrated acid (3 ml HCl +
are several urban and industrials activities, as well as fishing boats ac 4 ml HNO3 + 1 ml H2O2 + 0.5 ml HF). After digestion and cooling, the
tivities many of them without a treatment system for their wastewaters. samples completely dissolved were diluted with 3 % HNO3 to 10 ml for
In spite of its regional socio-economic importance, the Bizerte coast line further analysis. Finally, the heavy metals (Pb, Fe, Zn, Cd, Co, Cu, Ni, Mn
has been continuously and increasingly, over the past decades, subjected and Cr) concentrations were analyzedusing Atomic Absorption
Fig. 1. Location map of Bizerte coastline and the localization of surface sediment samples.
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A. Aydi et al. Marine Pollution Bulletin 184 (2022) 114171
Spectrometer Perkin-Elmer Analyst 200. The analytical precision was 1980) for assessing pollution which permits a comparison of pollution
within 10 % of the variability. levels between sites and at different times. The PLI was determined as
the nth root of the product of the n CF:
√̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅)
2.1. Assessment of potential heavy metals pollution PLI = n CF1 × CF2 × …CF3 (4)
To assess the contamination of heavy metals in surface sediment, the Where CF = contamination factor; n = number of heavy metals.
enrichment factor, the contamination factor, Geo-accumulation index as The pollution load index includes the four following classes: no
well as Pollution load index of each sample site was computed. pollution (PLI < 1), moderate pollution (1 < PLI < 2), heavy pollution
(2 < PLI < 3), and extremely heavy pollution (3 < PLI) (Zarei et al.,
2.1.1. Enrichment factor (EF) 2014).
In order to evaluate the magnitude of anthropogenic contribution
related to the abundance of heavy metals in the examined surface sed 2.1.5. Degree of contamination (CD)
iments, the computation of enrichment factor (EF) is required (Dick The degree of contamination (Cd) is defined as the sum of CF for each
inson et al., 1996). The value of EF calculated using the following heavy metals tested according to the following formula (Rehman et al.,
formula (Ergin et al., 1991): 2018):
(Cx /CFe )sample ∑
n
EF = (1) CD = CF (5)
(Cx /CFe )crust or background
i=1
Where (Cx/CFe) sample is the ratio of concentration of heavy metals in the Hakanson (1980) proposed four classes of CD: low degree contami
examined sediments samples (Cx) to that of Fe (CFe) in the sediment nation (CD < 6), moderate degree contamination (6 < CD < 12),
sample and (Cx/CFe)crust or background is the same ratio in unpolluted considerable degree of contamination (12 < CD < 24) and high degree
baseline samples. Accordingly, the degree of enrichment can be classi contamination (CD > 24).
fied as 7 classes(Li et al., 2019): EF < 1 (no enrichment), 1 < EF < 3
(minor enrichment), 3 < EF < 5 (moderate enrichment), 5 < EF < 10 3. Results and discussions
(moderately severe enrichment), 10 < EF < 25 (severe enrichment), 25
< EF < 50 (very severe enrichment) and EF > 50 (extremely severe In Table 1, the concentrations of 9 heavy metals in the 15 surface
enrichment). coastal sediments along the Bizerte coastline has been illustrated.
The mean concentrations of these heavy metals following the
2.1.2. Geo-accumulation index decreasing trend of Fe > (384 mg/kg) > Pb (4.7 mg/kg) > Zn (2.7 mg/
The geoaccumulation index (Igeo) was calculated following the Eq. kg) > Mn (2.3 mg/kg) > Cu (1.1 mg/kg) > Cr (0.6 mg/kg) > Ni (0.5 mg/
(2) (Muller, 1969): kg) > Co (0.1 mg/kg) > Cd (0.03 mg/kg).
( ) The abundance order of total heavy metal concentrations in sam
Cn
Igeo = Log2 (2) pling station was found to be: S3 > S14 > S13 > S15 > S11 > S4 > S12
1.5Bn > S7 > S10" > S2 > S6 > 10’ > S10 > S5 > S8 > S1 > S9. The maximum
levels of heavy metals concentration were found at station S3, due to
Where Cn is the concentration of the element in the enriched samples
high anthropogenic activities in the area.
and Bn is the background concentration of the element in the Earth's
The minima of Cd (0.01 mg/kg), Co (0.02 mg /kg), Fe (113 mg/kg)
crust. The factor 1.5 is used to account possible variations due to
and Mn (0.8 mg/kg) were observed in station S9, the minima of Pb (0.3
lithogenic effects (Ruiz, 2001).
mg /kg), Cu (0.01 mg /kg), Ni (0.20 mg/kg) and Zn (0.77 mg /kg) in
Muller (1969) has categorized Igeo index as follows: unpolluted
station S15 and the minima of Cr (0.3 mg/kg) is recorded in station S11.
(Igeo≤0) (Class 0); unpolluted to moderately polluted (0 < Igeo≤1)
The lowest heavy metals concentrations were recorded at stations S9
(Class 1); moderately polluted (1 < Igeo≤2) (Class 2); moderately to
and S15, due to low anthropogenic activities in the area. The high heavy
heavily polluted (2 < Igeo≤3) (Class 3); heavily polluted (3 < Igeo≤4)
metals concentrations was recorded for iron (955 mg/kg) in station S14
(Class 4); heavily to extremely polluted (4 < Igeo≤5) (Class 5); and
which can be attributed to the discharge of steel scrap plant.
extremely polluted (Igeo≥5) (Class 6).
The variations in the concentrations of heavy metals are mainly to be
related to the variable intensity of various human activities along the
2.1.3. Contamination factor (CF)
coastal line of Bizerte likely agrochemicals from agriculture fields,
For toxicological assessment of surface sediment contamination with
urban, and numerous industrial facilities (such as the Cement Factory of
heavy metals, the Contamination factor (CF) was calculated following
Bizerte, Tunisian Company of Lubricants, and Tunisian Company of
the procedure of Hakanson (1980):
Refining Industries) (El Zrelli et al., 2021). Apart from these, the set
Cn tlements domestic wastes are released directly into the Bizerte coast line
CF = (3)
Bn without being treated feeding this water body with significant quantities
of contaminants.
Where Cn = heavy metal concentration in sediment sample and Bn = Comparison of metal concentration in sediments from other coastal
background concentration of that metal. Based on the level of contam areas, concentrations of Fe, Pb, Zn, Mn, Cu, Cr, Ni, Co and Cd in Bizerte
ination, Hakanson categorized the CF values: CF<1, low contamination cost line surface sediments were illustrated in Table 1. In general, the
factor; 1≤CF<3, moderate contamination factors; 3≤CF<6, consider heavy metals concentration obtained in this study were in the range
able contamination factors; and CF≥6, very high contamination factor recorded in other Mediterranean Sea coast (Table 1), or even lower in
(Ghannem et al., 2014). some cases (Alomary and Belhadj, 2007; Alonso Castillo et al., 2013; El
The background values for Pb, Fe, Zn, Cd, Co, Cu, Ni, Mn and Cr were Nemr et al., 2007; Neşer et al., 2012; Saddik et al., 2021).This finding
70, 35,900, 175, 1, 29, 50, 68,750 and 90 mg/kg, respectively(Hakan can be further validated by the calculation of pollution indices.
son, 1980).
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A. Aydi et al. Marine Pollution Bulletin 184 (2022) 114171
Table 1
Comparison between heavy metal concentrations in the studied surface sediments with those obtained by other worldwide Mediterranean Sea.
Site Cd Co Cr Cu Fe Mn Ni Pb Zn
3.1. Indices of the heavy metal contamination assessment The pollution degrees of heavy metals in surface sediments are
evaluated by the geo-accumulation index (Igeo). The Igeo values ranged
3.1.1. Enrichment factors (EF) from − 8.68 to − 0.46 for Cd (mean of − 4.78), − 9.61 to − 5.69 for Co
The Enrichment Factor (EF) in metals a widely used to assess the (mean of − 7.63), − 8.42 to − 6.30 for Cr (mean of − 7.57), − 12.17 to
presence and intensity of anthropogenic contaminant relative to average − 3.25 for Cu (mean of − 6.42), − 10.41to − 7.19 for Mn (mean of − 9.70),
natural abundance (Ghouma et al., 2022). The mean EF values of Co, Cr, − 8.52 to − 5.56 for Ni (mean of − 7.53), − 6.36 to − 0.71 for Pb (mean of
Cu, Mn and Ni were lower than 1, indicating “no enrichment”, whereas − 6.98) and − 7.95 to − 4.92 for Zn (mean of − 6.93)(Fig. 3). All of the
Pb, Cd and Zn were lower than 3, indicating “minimal enrichment”. The obtained results are below zero (Igeo < 0) indicating that the pollution
EF values for Pb in the surface sediments of this station were 4.9, indi degree with respect to heavy metals is unpolluted. The geo-
cating “moderate enrichment”. The EF value for Cd at station S10' was accumulation index (Igeo) values of the studied heavy metals showed
2.9, indicating “minor enrichment” (Fig. 2). As a whole, the EF values of the decreasing order of Pb > Cd > Zn > Cu > Ni > Cr > Co > Mn.
studied heavy metals in The Bizerte coast line followed a descending The CF is widely used to evaluate the degree of pollution in sediment
order of Pb > Cd > Zn > Cu > Ni > Cr > Co > Mn. by heavy metals (Aydi, 2015). Based on the Muller (1969) classification
Fig. 2. Enrichment factor ofPb, Fe, Zn, Cd, Co, Cu, Ni, Mn and Cr in the surface sediments collected from the 17 samples sites.
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A. Aydi et al. Marine Pollution Bulletin 184 (2022) 114171
Fig. 3. Geoaccumulation index (Igeo)of heavy metals in surfaces sediments along Bizerte coast line.
of CF values, all heavy metal exhibited “low” contamination (CF<1) have been used to identify possible source of heavy metals in surface
along the Bizerte coast line, except for Pb which showed moderate sediments along the Bizerte coast line. Several positive correlations (p <
contamination (1≤CF<3) in stations S4 (2.59), respectively. The higher 0.05) existed between Ni with Co (r = 0.70) and Fe with Co, Mn and Ni
CF value for Pb could be attributed to sewage discharge from fishering with correlation coefficient 0.92,0.75, and 0.70, respectively, indicating
and small boats which use diesel as fuel (Fig. 4). The highest CF value that these heavy metals probably have the same source, which is most
observed in station S4 is due to the reception of sugar refinery water and likely linked to anthropogenic activities. Another positive correlation
beet molasses release, discharge from metal construction factory and was marked between Pb with Cu (r = 0.86) and Zn with Cu and Pb with
urban wastewater discharge. The CF values of examined heavy metals correlation coefficient 0.85 and 0.7, respectively, implying that these
decreased in the following sequence: Pb > Cd > Zn > Cu > Ni > Cr > Co heavy metals have a common sources and exhibited similar geochemical
> Mn, which is closer to what has been observed from Igeo and EF behavior(Wang et al., 2012) (Table 2).
values. Hierarchical cluster analysis was also conducted to further evaluate
The PLI values attributed to heavy metals in the sediments of the those potential correlations between the heavy metals in surface sedi
Bizerte coast line were slightly lower than 1, suggesting no pollution ments samples. Fig. 7 clearly showed two main statistically significant
(Ullah et al., 2019) (Fig. 5). clusters: group 1 (Pb-Mn-Zn-Cu)influenced mainly by industrial sources
The degree of contamination (CD) values for all sampling sites (industrial waste water, stainless manufactory, sugar refinery and agri
ranged from 0.05 to 2.87, which confirmed that the sediment of the cultural activities)(Sungur et al., 2020),group 2 (Cr–Ni) suggested in
Bizerte coast line showed a “low degree contamination” (CD < 6) dustrial sources of contamination (waste water from cement plant),
(Fig. 6). The pollution degree of total heavy metals in sampling station whereas Fe (group 3) mainly have lithogenic origin and group 4 indi
decreased the following sequence: S4 > S3 > S10' > S1 > S7 > S10” > cated Co and Cd are closely related to each other, it can therefore be
S6 > S2 > S10 > S13 > S12 > S5 > S9 > S14 > S8 > S11 > S15. proposed that heavy metals of the fourth group are mainly derived from
In the present study, the Person correlation and the cluster analysis the similar sources.
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A. Aydi et al. Marine Pollution Bulletin 184 (2022) 114171
Fig. 5. Pollution Load index (PLI) values of the surface sediments samples along Bizerte coast line.
Heavy metal concentrations (Pb, Fe, Zn, Cd, Co, Cu, Ni, Mn and Cr) Specific contributions made by each author are as follow:
were examined in surface sediments collected from seventeen sampling - Conceptualization: Abdelwaheb Aydi, Samir Ghannem, Ahmed
station in Bizerte coast line, Northeast Tunisia. This work aimed to assess Nasri, Rania Hessine, Amine Mezni
the heavy metal pollution status based on the multi-indicators evalua - Methodology: Abdelwaheb Aydi, Samir Ghannem, Amine Mezni
tion methods (EF, Igeo, CF, PLI and DC) and identifying the correlations - Analysis and interpretation: Abdelwaheb Aydi, Ahmed Nasri, Rania
between these studied heavy metals. The results showed that the orders Hessine, Amine Mezni
of heavy metals concentration in surface sediments are in the following - Writing original draft, review and revision: Abdelwaheb Aydi,
order: Fe > Pb > Zn > Mn > Cu > Cr > Ni > Co > Cd. Based on the Ahmed Nasri, Rania Hessine, Amine Mezni
indices of the heavy metal contamination assessment from EF, Igeo, CF,
PLI and DC values demonstrated that heavy metals pollution in the
Bizerte coast line was from non-contamination to moderate contami Declaration of competing interest
nation, and the contribution rate of Pb and Cd was largest. Although the
pollution level in the Bizerte coast line was relatively low at present, The authors declare that they have no known competing financial
long-term dynamic oversight of Cd and Pb should be brought out to interests or personal relationships that could have appeared to influence
avoid potential ecosystem risks. the work reported in this paper.
6
A. Aydi et al. Marine Pollution Bulletin 184 (2022) 114171
Fig. 6. The Degree of Contamination (CD) values of the 17 sampling station in Bizerte coast line.
Table 2
Pearson correlations between heavy metals in surfaces sediments samples along the Bizerte coast line.
Cd Co Cr Cu Fe Mn Ni Pb Zn
Cd 1
Co − 0.08 1
Cr 0.13 0.27 1
Cu 0.36 0.06 0.38 1
Fe − 0.15 *0.92 0.43 0.03 1
Mn − 0.10 0.68 0.53 − 0.23 *0,75 1
Ni 0.01 *0.70 0.37 0.59 *0.70 0.2 1
Pb 0.02 0.02 0.44 *0.86 0.06 − 0.12 0.50 1
Zn 0.34 0.09 0.46 *0.85 0.05 − 0.22. 0.58 *0.7 1
Fig. 7. Cluster dendrogram of heavy metal contents in surfaces sediments samples along the Bizerte coast line.
7
A. Aydi et al. Marine Pollution Bulletin 184 (2022) 114171
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