Marine Pollution Bulletin 179 (2022) 113730

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Marine Pollution Bulletin

journal homepage: www.elsevier.com/locate/marpolbul

A risk assessment by metal contamination in a river used for public

water supply
Jucelino B. da Silva Junior a, b, c, *, Vanessa S. de Carvalho a, b, Daniele S. Sousa c,
Ivanice F. dos Santos a, b, d, Geysa B. Brito e, Antônio F.S. Queiroz c, Sérgio L.C. Ferreira a, b, *
a
Instituto Nacional de Ciência e Tecnologia, INCT, de Energia e Ambiente, Universidade Federal da Bahia, 40170-115 Salvador, Bahia, Brazil
b
Universidade Federal da Bahia, Instituto de Química, Campus Ondina, 40170-270 Salvador, Bahia, Brazil
c
Universidade Federal da Bahia, Instituto de Geociências, Campus Ondina, 40170-270 Salvador, Bahia, Brazil
d
Universidade Estadual de Feira de Santana, Departamento de Ciências Exatas, 44036-900 Feira de Santana, Bahia, Brazil
e
Universidade Regional do Cariri (URCA), 63105-000 Crato, Ceará, Brazil

A R T I C L E I N F O A B S T R A C T

Keywords: Aquatic ecosystems provide habitats for many organisms. Historically, riverbanks have always been inhabited
Metal pollution and exploited for subsistence and navigation. The present study evaluates the contamination and ecological risks
Pollution indexes caused by potentially toxic elements in surface sediments of the Paraguaçu River, Bahia, Brazil. Seven sediments
Ecological risk indexes
samples were collected, and eight heavy metals were determined employing inductively coupled plasma spec­
Paraguaçu River
Todos os Santos Bay
trometry mass (ICP-MS). The concentrations range as (mg kg− 1) found were 6.78–18.68 for lead, 14.21–42.16 for
Multivariate analysis zinc, 27.61–48.63 for nickel, 2.03–6.50 for chromium, 6.06–12.90 for vanadium, 5.99–13.33 for cupper,
1.25–3.19 for cobalt, and 79.52–286.08 for manganese. Nickel showed significant enrichment (EF: 5.75; 7.62,
and 14.11), followed by zinc, which showed moderate enrichment (EF: 2.16; 2.19, and 4.52). These enrichment
levels are possible of anthropogenic origin. When the pollution index (PI) was evaluated, the elements V, Ni, Zn,
Mn, Co, and Cu were strongly polluted (PI ≥3). In general, the pollution index (PI), geoaccumulation index (Igeo),
enrichment factor (EF), and potential ecological risk indices (Er and PERI) show that contaminated sediments
have adverse effects on aquatic environments, especially for o Mn, Ni, Pb, V, and Zn.

1. Introduction and Pavlovsky, 2017).

The contamination of metals and metalloids in soils and sediments
Pollution indices are tools often employed to classify and identify occurs mainly by anthropogenic activities, among which are: disposal of
possible contamination sources, divided into two groups: single indices solids, liquids, and gases from industrial activities, use of fertilizers and
and total complex indices. The single indices used as indicators of soil herbicides in agriculture (Jiao et al., 2015; Nziguheba and Smolders,
pollution are Geoaccumulation Index (Igeo), Enrichment factor (EF), 2008), gaseous emissions from vehicular traffic (Berghman and Goos­
Pollution Index (PI), and Contamination Factor (CF). All these indices sens, 2021; Zhang et al., 2016), disposal of domestic sewage in urban
are calculated by the concentrations of each chemical element in the areas, improper disposal of metallic objects in seas and rivers due to
sediments and soils. The total complex indices are based on single leisure activities, etc. (Patel et al., 2018; Weissmannova and Pavlovsky,
indices. However, they are calculated as multi-element that are 2017). Nziguheba and Smolders investigated the employment of phos­
described as: Pollution Load Index (PLI), Degree of Contamination phate fertilizers on agricultural soils from European countries. This work
(Cdeg), Modified Contamination Factor (mCdeg), Sum of Pollution Index involved the determination of heavy metals in 196 phosphate fertilizers
(PIsum), Average Pollution Index (PIAvg), Integrated Pollution Index samples from 12 countries. The average contents expressed as mg kg− 1
(IPI), Integrated Threshold Pollution Index (IPIT), New Pollution Index found were 2.9 for lead, 7.4 for cadmium, 7.6 for arsenic, 14.8 for nickel,
(PIN), Nemerow Pollution Index (PINemerow), and indices of ecological and 89.5 for chromium. In addition, the metals concentrations found
risk (Cai et al., 2015; Chen et al., 2022; Rani et al., 2021; Weissmannova were positively correlated with the phosphor contents, which confirmed

* Corresponding authors at: Instituto Nacional de Ciência e Tecnologia, INCT, de Energia e Ambiente, Universidade Federal da Bahia, 40170-115 Salvador, Bahia,
Brazil.
E-mail addresses: [email protected] (J.B. da Silva Junior), [email protected] (S.L.C. Ferreira).

https://doi.org/10.1016/j.marpolbul.2022.113730
Received 28 March 2022; Received in revised form 29 April 2022; Accepted 30 April 2022
Available online 7 May 2022
0025-326X/© 2022 Elsevier Ltd. All rights reserved.
J.B. da Silva Junior et al. Marine Pollution Bulletin 179 (2022) 113730

that the rocks phosphate are the major source of the metals (Nziguheba arsenic contents varied from 0.29 to 333.04 mg kg− 1 of sediment,
and Smolders, 2008). Jiao et al. assessed the metal contamination in significantly correlated with the lead and mercury concentrations. The
river sediments and background soils from Northeast China impacted by contamination factor and geoaccumulation index were used to evaluate
agriculture. The results showed that the agricultural activities developed the level of contamination (Han et al., 2019). Total concentrations of
for 40 years in this region induced the accumulation of the metals: lead, cadmium, mercury, copper, manganese, lead, vanadium, zinc, chro­
cadmium, copper, zinc, chromium, and nickel in river sediments with mium, and iron were determined, and several single and complex
average concentrations 1.23–1.71 times higher than local soil back­ indices were employed to evaluate the pollution and environmental risk
ground values (Jiao et al., 2015). Zhang et al. evaluated the Vehicular of the area. In the industrial region of Ostrava, Czech Republic, the total
traffic effect on the concentrations of metals and metalloids in water and concentrations of cadmium, mercury, copper, manganese, lead, vana­
sediments from Lake Pontchartrain along the I-10 Bridge. The results dium, zinc, chromium and iron were determined, in addition to several
obtained show that the concentrations of arsenic, cadmium, chromium, simple and complex indices to assess pollution and environmental risk in
lead, zinc, nickel, and copper increased in the sediments collected near the area (Weissmannova et al., 2019). In addition, pollution indices
the bridge. Also, it was observed that in summer, the high temperature evidenced contamination by anthropogenic sources in the studied re­
allows the release of the metals from sediments, increasing the con­ gion, from strong to moderate levels. The potential ecological risk index
centrations of these in water (Zhang et al., 2016). Berghman and varied and indicated a moderate ecological risk, having some regions
Goossens determined 13 chemical elements in urban street sediments with high ecological risk. Conclusions for carcinogenic health risks were
collected in 77 locations from Leuven City, Belgium with different traffic estimated and worrying for lead, cadmium, and chromium (Weissman­
conditions. The results demonstrated that high pollution was found for nova et al., 2019).
copper, antimony, lead, and zinc, being that these elements are related In this work, seven sediment samples were collected from the river,
to brake wear and tire wear, respectively (Berghman and Goossens, and the metals: lead, zinc, nickel, chromium, vanadium, copper, cobalt,
2021). Shi et al. used the enrichment factor, the pollution load index, and manganese were quantified employing ICP-MS. Geoaccumulation
and the potential ecological risk index to evaluate the contamination index, Enrichment factor, Single pollution index, Pollution load index,
levels and the ecological risk of chemical elements in sediments of an and Ecological risk were utilized to evaluate the region’s pollution level
industrial park from northwest China. The results of the indexes and ecological risk.
demonstrated that all metals have moderate contamination in the sed­
iments and a low ecological risk level for barium, cobalt, chromium, 2. Methodological approach
copper, manganese, nickel, lead, vanadium, and zinc (Shi et al., 2018).
Nickel, vanadium and lead were determined in sediments from the 2.1. Region setting and sampling
Lagoa dos Patos estuary (RS, Brazil), which is impacted by petroleum
derivatives and antifouling paints. Surface sediments were sampled in The Paraguaçu River (− 11◦ 11′ a -13◦ 42′ S/-38◦ 48′ a -42◦ 07′ ) is
summer and winter in oil refinery regions, marinas, shipyards and located between the cities of São Félix and Cachoeira, Bahia, Brazil,
control station. The geoaccumulation indices (Igeo) were calculated, which is in the western portion of the BTS. This estuary is the largest
and the results showed that nickel and vanadium can be used as in­ source of fresh water in the region, with a drainage area of 56,300 km2
dicators of contamination of human sources by antifouling paints and (Hatje et al., 2010), that offers several services to the population, such as
petroleum derivatives (Pereira et al., 2018). Recent studies have eval­ public and domestic supply to some cities, including Salvador, Bahia. In
uated cadmium and arsenic contamination in a region of China with addition, the Pedra do Cavalo dam is responsible for supplying the
38 years of rice production (Gao et al., 2021). Fertilization processes textile and cellulose industries, mineral processing, and fishing activities
were carried out using inorganic nitrogen, phosphorus, and potassium in several locations.
(NPK), without fertilizer (CK), manure (M) and NPK plus resulting Also, domestic and industrial sewage can be found in some points of
manure (NPKM). The single-factor pollution index, the geoaccumulation this basin (Brito et al., 2020). This river is close to the city of Santo
index, and the risk assessment code were employed to evaluate the Amaro, which for over three decades had a lead processing industry, that
pollution due to the long-time fertilization. The results demonstrated released a large amount of contaminated material into the environment
that the treatments using M, NPK, and NPKM significantly increased the (da Silva Junior et al., 2020; Hatje et al., 2010).
total and available contents of cadmium and arsenic of the soils; cad­ Seven samples of surface sediment (0–5 cm) were collected using a
mium originated from cattle manure, while arsenic from phosphate stainless steel Van Veen dredger in a period of high rainfall of the river.
fertilizer (Gao et al., 2021). An operating Chlor-alkali plant in the Baikal The collected sediments were packed in hermetically sealed plastic bags
region of Russia released 1327 tons of mercury into the environment. and later placed for conservation in thermal boxes at approximately
Continuous monitoring revealed that this metal’s concentration in the 4 ◦ C. Physical and chemical parameters (pH, ORP, OD, salinity) were
sediments has decreased from 2.03 to 0.79 mg kg− 1 in the last 20 years measured in situ using a multiparameter probe (model HI9829,
due to decreased plant operations and environmental awareness. How­ HANNA).
ever, mercury concentrations are still higher than the mercury back­
ground level. The sediment transport rate and water availability 2.2. Laboratory analysis
contributed to the deposition of Hg in the sediment (Pastukhov et al.,
2019). In 2019, a study was published which investigated the contam­ The samples were lyophilized and then disaggregated with a rubber
ination of chromium, copper, nickel, lead, and zinc caused by leaching tipped piston in order not to interfere with the original grain size.
and industrial discharge, spills of chemical products and wastewater The samples destined for the granulometric analysis were sieved
effluents in marine sediments and mangroves (Avicennia marina) in the (500 μm) to remove plastics, roots, among others. All samples were
region from Yanbu in Saudi Arabia (Alharbi et al., 2019). The method­ homogenized, quartered, and destined for analysis. Particle size (parti­
ologies: geo-accumulation index, contamination factor, pollution load cle size analysis) was determined using the Laser Diffraction Particle
index, potential ecological risk index, potential toxicity response index, Analyzer (model 1064, Cilas), while the size classes are named after
bioaccumulation factor, and translocation factor were employed to (Folk, 1980). The organic carbon content was determined by the
evaluate the contamination and the ecological risks. The results elemental analyzer CHN (CN-628/S, LECO). The determination of the
demonstrated that these metals severely contaminate the region chemical elements was performed after acid digestion using 0.5 g of
(Alharbi et al., 2019). A national macro project in China investigated the sediment sample, 5 mL of concentrated HNO3 (Merck – Darmstadt,
arsenic contamination in sediments caused by the discharge of untreated Germany), and 5 mL of ultrapure H2O (Milli-Q system), employing a
domestic and industrial wastewater from ten main river basins. The microwave oven (Milestone Ethos 1600 Microwave Labstation; Sorisole,

2
J.B. da Silva Junior et al. Marine Pollution Bulletin 179 (2022) 113730

Italy). Then the extracts were filtered and diluted. The metal concen­

13.33 ± 0.01

11.26 ± 0.01
10.01 ± 0.34
trations were determined using Plasma Source Mass Spectrometry – ICP

6.36 ± 0.01
5.99 ± 0.01
9.81 ± 0.01
6.08 ± 0.01
6.07 ± 0.01
7.08 ± 0.01
MS (model Xseries II, Thermo, Germany).

112.49
The concentrations of the chemical elements were expressed in mg

197.0
0.51
35.7
Cu
kg− 1 of dry sediment. All plastics, quartz and glassware used in the
analysis were bathed in HNO3 (10%) (Merck – Darmstadt, Germany) for
at least 24 h and rinsed repeatedly with ultrapure water. The Quality

0.01
0.01
0.01
0.01
0.01
0.01
0.01
0.01
Assurance/Quality Control (QA/QC) procedures involved the use of
standard reagents and the analysis of NIST 1646a Certified Reference

2.98 ±
3.07 ±
3.19 ±
2.42 ±
1.25 ±
2.10 ±
1.57 ±
4.06 ±

81.20
0.69
Material (estuarine sediment). The results of the analysis of the certified

(5)
Co

–
–
reference sediment are presented in Table 1.

2.3. Statistical analysis

134.13 ± 0.18
177.90 ± 0.14
255.77 ± 0.31
286.08 ± 6.03
220.23 ± 1.15
193.07 ± 0.18

241.62 ± 0.01
79.52 ± 0.07

234.5 ± 2.8
Major and trace element interrelations, together with grain-size pa­

103.04
rameters and organic carbon contents were studied by Factor Analysis,

0.61
Mn
FA. Prior to the analysis, data were transformed (Karageorgis et al.,

–
–
2009) to meet the requirements of normality (Reimann et al., 2002).
Subsequently, Principal Factor Analysis (PCA) with Varimax rotation

18.68 ± 0.01
was conducted to group clay, organic carbon, and geochemical

9.51 ± 0.01
8.12 ± 0.01
6.78 ± 0.01

8.77 ± 0.05
7.12 ± 0.01
9.34 ± 0.01
12.7 ± 0.01
11.7 ± 1.2
elements.

108.55
0.24
35.0
91.3
Pb
2.4. Accumulation and pollution indices

The frequently used indices can be divided into simple and complex

40.86 ± 0.03
22.21 ± 0.01
37.25 ± 0.02
42.16 ± 0.03
22.92 ± 0.20
14.21 ± 0.01
34.80 ± 0.02
indices of accumulation and pollution and ecological risk indices

49.3 ± 0.05
48.9 ± 1.6
(Weissmannova and Pavlovsky, 2017). The single indices as sediment

100.82
11.93
123.0
315.0
accumulation and pollution indicators comprise several indices such as

Zn
Geoaccumulation Index - Igeo, Enrichment Factor - EF, and Pollution
Index - PI. These indices are calculated from the content of each
potentially toxic element individually in sediment, and different classes

0.06
0.06
0.02
0.05
0.03
0.02
0.04
0.02
can be used to classify the sediment according to the degree of accu­
mulation and/or pollution (Abdullah et al., 2020; da Silva Junior et al.,
48.63 ±
48.63 ±
36.70 ±
40.98 ±
39.84 ±
27.61 ±
53.36 ±
25.71 ±

111.78
2020; Hakanson, 1980; Loska et al., 1997; Rahman et al., 2014; Tang

0.37
18.0
36.0
(23)
Ni

et al., 2022).
Igeo is commonly used to assess sediment pollution by potentially
toxic elements. This index is formulated by:
6.50 ± 0.01
3.06 ± 0.01
2.67 ± 0.01
5.68 ± 0.01
2.57 ± 0.01
2.03 ± 0.01
4.42 ± 0.01
39.2 ± 0.01
40.9 ± 1.9
Cx
Igeo = log2

95.84
0.50
37.3
90.0
1.5 × CB
Cr

where Cx is the concentration of the element in the sediment; CB is the

background concentration of the element in the corresponding sediment
11.18 ± 0.02

12.90 ± 0.01
42.39 ± 0.03
44.84 ± 0.76

or sediment.
Mean concentrations of potentially toxic elements in tropical river sediment.

8.06 ± 0.01
8.36 ± 0.02
9.11 ± 0.01
6.71 ± 0.04
6.06 ± 0.01

The constant 1.5 is used for the state of natural fluctuations of metals
in the environment and detection of minor anthropogenic impacts (Brito
94.54
1.45

et al., 2020; Loska et al., 2004; Lu and Bai, 2010). The geoaccumulation
V

–
–

index is composed of seven degrees.

The EF is given by the standardization of an analyzed element
38◦ 58′ 15.28”
38◦ 58′ 08.87”
38◦ 57′ 59.74”
38◦ 57′ 59.75”
38◦ 57′ 49.94”
38◦ 57′ 44.40”
38◦ 57′ 27.65”

against a reference metal with low variability of occurrence (Sc, Mn, Ti,
Longitude W

Al, Fe, and Ca); however, the most used are Mn, Al, and Fe (Almeida
et al., 2020; Reimann and De Caritat, 2000). EF has five classes
(Sutherland, 2000). The equation that expresses the EF in sediment
–
–
–
–
–
–

samples is given by
( )
Global position

12◦ 36′ 15.81”

12◦ 36′ 08.24”
12◦ 36′ 14.05”
12◦ 36′ 20.59”
12◦ 36′ 31.30”
12◦ 36′ 31.09”
12◦ 36′ 59.65”

Cx
Latitude S

Cref
Sample
EF = ( )
Cx
Cref
–
–
–
–
–
–

Background

where Cx is the potentially toxic element, and Cref is the reference

element. In this paper, the reference element used for the EF calculations
% Recovery (CRM)

was Mn.
CRM analyzed

Single PI often uses multiple reference values of metals in sediments,

NIST 1646a

such as pre-industrial level, middle crust level, background level, base­

Location
Table 1

TEL*
PEL*

line values, criteria, or pollution limit values (Caeiro et al., 2005). Total
LOQ
#1
#2
#3
#4
#5
#6
#7

complex indices of pollution are calculated as multielement indices

3
J.B. da Silva Junior et al. Marine Pollution Bulletin 179 (2022) 113730

based on single pollution indices (Gong et al., 2008). Each type of total #5, and #7 showed values above the probable effects level – PEL. Nickel
complex pollution indices can be composed of the mentioned single has a greater tendency to form complexes and therefore less mobility.
indices separately. The integrated pollution indices will be described in Nickel and cobalt, both in seawater and in freshwater, are mainly in the
this paper by Pollution Load Index - PLI and Modified Contamination form of aqueous ions or carbonate complexes (Xu et al., 2015).
Factor - mCdeg. Cobalt, manganese, and vanadium do not have sediment guidelines
quality established by the TEL and PEL.
Cx
PI = The geoaccumulation index (Igeo) was calculated for Cu, Cr, Co, Mn,
CB
Ni, Pb, Zn, and V. In Table 2, these elements were classified using
√
n
̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅ characteristics of a decontaminated environment (Class 0) at extremely
PLI = CF 1 × CF 2 × … × CF i
high contaminated (Class 6). In general, the samples were decontami­
nated or moderately contaminated (Class 0 to 2) for the analyzed ele­
1∑ n
mCdeg = CF i ments. In particular, Ni, Zn, and Mn showed different characteristics. Mn
n i=1
appeared as a moderately to strongly contaminating agent in stations #3
and #4. The geoaccumulation indices calculated for Ni showed that the
where n is the number of elements evaluated and CF is the contamina­
element is a strong contaminating agent, corroborating the evaluation
tion factor for each element (i) individually (Abrahim and Parker, 2008;
described above when compared with TEL and PEL. The geo­
Liu et al., 2016; Venkatramanan et al., 2015).
accumulation index calculated for Zn showed that the environment is
The ecological risk indices are calculated and evaluated individually
moderate to heavily contaminated.
(Er) and integrated (PERI) as
To compensate for the natural variability of elements in the sedi­
Er = Cx × Tr ments, normalization of the metal to Mn was performed so that any
∑ anthropogenic contributions of metal could be detected and quantified.
PERI = Er Table 3 describes the variation in the enrichment factor (Kelepertzis)
of potentially toxic elements in the sediments on the banks of the Par­
The toxic response factors of individual metals are Pb (5), Cd (30), Cr aguaçu River. The high enrichment factor in terms of mean values in the
(2), Cu (5), Zn (1), Ni (5), and Mn (1). Its classification is given in three sediment was observed in the order of
classes (Hakanson, 1980; Tzoraki and Papadopoulou, 2022; Xu et al., Ni > Zn > V > Mn > Cr > Cu > Co > Pb. It is noted, as well as the values
2015). assumed for Igeo, that Ni and Zn are elements that characterize a mod­
erate to severe enrichment of the aquatic environment.
2.5. Unsupervised methods of analysis: PCA and HCA It is worth mentioning that in determining the pollution index (PI)
the reference values inserted in the equation are related to pre-industrial
With the help of pattern recognition methods, one can identify the concentrations for each element, individually (Brady et al., 2015). Thus,
origin or difference between different samples. The tools used for the the pollution indices shown in Table 4 show high values for Ni, Zn and
pattern recognition method have been widespread in geochemistry, Mn; while Co and Cu present moderate pollution and Cr and Pb low
environmental chemistry, and engineering. potential for pollution.
Principal Component Analysis (PCA) is a method used to project The complex indices, PLI and mCdeg, (Table 5) used to assess the
multivariate data into a smaller dimensional space, thus reducing the quality of the sediment in the Paraguaçu River show that the aquatic
dimensionality of the original space of the data set without affecting the environment of the Paraguaçu River is not polluted when a total context
relationships between samples (Bahrami et al., 2020; Correia and Fer­ of potentially toxic elements is approached. This shows that an indi­
reira, 2007). vidualized assessment for each element is relevant, as it becomes
Hierarchical Cluster Analysis (HCA) is an agglomerative technique, possible to identify the sources of pollution.
which assumes a priori that each sample represents a separate group. In The values of Er and PERI presented in Table 6 denote low ecological
this context, the application of HCA is interesting because it can risk for the elements Cr and Cu, while Zn and Pb showed moderate and
graphically represent in a two-dimensional scheme the hierarchical considerable values of risk for the aquatic biota of the Paraguaçu River.
grouping of multidimensional data (de Carvalho et al., 2021; Poletti When evaluating the ecological risk in an integrated way, the PERI, only
et al., 1997). station #4 showed a moderate ecological risk. Lead and zinc are ele­
PCA and HCA performed the multivariate analysis of the data to ments that appear interconnected in various anthropogenic activities
evaluate the relationship between the concentrations of the potentially such as metallurgy and lead recycling plants, as well as metallic pipes
toxic elements in the sediment samples. and gasoline additives.
Statistical analyzes were performed using the STATISTICA® 6.0 for Generally, industrial effluents are composed of high concentrations
Windows (StatSoft, Inc. 1984–2004, Tusla, USA). of potentially toxic elements such as Cd, Ni, Pb, Zn, Co, Cr, Cu, and Mn.
The species and level of these elements in soils and sediments are
3. Results and discussion influenced by the origin and distance from sources; they also depend on
site-specific conditions, as all solid particles from atmospheric deposi­
3.1. Geochemical and ecological risk indexes applied in sediment quality tion are eventually stored on land or water (Chen et al., 2005; Yu et al.,
assessment 2016). The application of Cu, Zn, Fe, and Mn as important and essential
elements for plant growth is common practice to correct metal de­
Table 1 presents the limits of quantification (LOQ) and contents of ficiencies in soils (Gavrilescu et al., 2009; Kelepertzis, 2014; Toth et al.,
potentially toxic chemical elements analyzed in certified reference ma­ 2016). Many chemicals used in agricultural applications contain Cu, Zn,
terial (CRM) and in sediment samples collected in the Paraguaçu River, and Mn. Applications of phosphate fertilizers increase the concentration
Bahia, Brazil. This table also contains NOAA sediment guidelines quality of Cd, As, Pb and Hg. On the banks of the Paraguaçu River, it is possible
(SGQs). The average concentrations of the analyzed elements allowed to identify places where agriculture is practiced. Possibly these point
the following relationship: Mn > Ni > Zn > Pb > V > Cu > Cr > Co. sources contribute to the increase of Cu, Zn, Mn, and Pb levels deter­
The contents of Cu, Cr, Pb, and Zn were below the threshold effects mined in the sediments. This is because, although the application of
level – TEL. thus indicating that there are no deleterious effects on the correctives and fertilizers occur in the soil, these elements will be
aquatic biota of the Paraguaçu River. However, Ni levels, for all sam­ leached from the same and carried to the banks of the Paraguaçu River.
pling stations, remained higher than TEL, and points #1, #2, #3, #4, Another relevant factor that contributes to the insertion of solid

4
J.B. da Silva Junior et al. Marine Pollution Bulletin 179 (2022) 113730

Table 2
Classification of the geoaccumulation index (Igeo) for the potentially toxic elements determined in sediment from the Paraguaçu River.
Location V Cr Ni Zn Pb Mn Co Cu Classification Igeo

#1 2 0 5 4 0 2 0 1 Class 0: Uncontaminated
#2 2 1 5 3 0 2 0 0 Class 1: Uncontaminated to moderately contaminated
#3 2 0 4 4 0 3 0 0 Class 2: Moderately contaminated
#4 2 0 4 4 1 3 0 1 Class 3: Moderately to strongly contaminated
#5 2 0 4 3 0 2 0 0 Class 4: Strongly contaminated
#6 2 0 4 2 0 2 0 0 Class 5: Strongly to extremely contaminated
#7 3 0 5 4 0 1 0 0 Class 6: Extremely high contaminated

In bold, moderately to highly polluting elements are highlighted (classes 3. 4. and 5).

Table 3
Enrichment Factor (EF) for the potentially toxic elements determined in sediment from the Paraguaçu River.
Location V Cr Ni Zn Pb Mn Co Cu Classification EF

#1 1.84 0.33 7.62 4.52 0.28 1.00 0.41 0.81 EF < 2: Deficiency to minimal mineral enrichment
#2 1.00 0.38 5.75 1.85 0.18 1.00 0.32 0.29 EF ¼ 2–5: Moderate enrichment
#3 0.72 0.23 3.02 2.16 0.11 1.00 0.23 0.19 EF ¼ 5–20: Significant enrichment
#4 0.70 0.44 3.01 2.19 0.26 1.00 0.16 0.28 EF ¼ 20–40: Very high enrichment
#5 0.67 0.26 3.80 1.55 0.16 1.00 0.11 0.22 EF > 40: Extremely high enrichment
#6 0.69 0.23 3.01 1.09 0.15 1.00 0.20 0.26
#7 3.58 1.22 14.11 6.50 0.47 1.00 0.37 0.72

In bold, moderately to severely enriched environments are highlighted.

Table 4
Pollution Index (PI) in the Paraguaçu River.
Location V Cr Ni Zn Pb Mn Co Cu Classification PI

#1 6.01 1.07 24.94 14.80 0.93 3.27 1.36 2.64 PI < 1: Unpolluted. low level of pollution
#2 4.33 0.50 24.94 8.05 0.80 4.34 1.40 1.26 1 ≤ PI ≤ 3: Moderate polluted
#3 4.50 0.44 18.82 13.50 0.66 6.24 1.45 1.19 PI ≥ 3: Strong polluted
#4 4.90 0.94 21.02 15.28 1.83 6.98 1.10 1.95
#5 3.61 0.42 20.43 8.30 0.86 5.37 0.57 1.21
#6 3.26 0.33 14.16 5.15 0.70 4.71 0.95 1.20
#7 6.94 0.73 27.37 12.61 0.92 1.94 0.71 1.41

In bold, moderately to severely contaminated environments are highlighted.

in the Paraguaçu River sediments. Cd was removed from the multivar­

Table 5
iate analysis as it presented values below the LQ for most sampling
Integrated indices of pollution: PLI and mCdeg.
points. Thus, the data matrix used comprised 21 (rows) samples and
Location PLI mCdeg Classifications PLI Classification mCdeg eight elements (columns).
#1 0.39 1.12 PLI > 1: Polluted mCdeg ≤ 1.5: Very low PC1, PC2, and PC3 were selected for data characterization because
PLI ¼ 1: Baseline contamination they presented eigenvalues >1, corresponding to 4.0 for PC1, 1.7 for
#2 0.30 0.88 levels of pollution 1.5 ≤ mCdeg ≤ 2: Low PC2, and 1.1 for PC3. The first three components together described
PLI < 1: Not polluted contamination
#3 0.31 0.91 2 ≤ mCdeg ≤ 4: Moderate
85% of the total variance. Loading factors are shown in Table 7 and
contamination Fig. 1. PC1 explained 50.1% of the total variance and the dominant
#4 0.41 0.96 4 ≤ mCdeg ≤ 8: High variables were Cr, Cu, Zn, V, Ni and Pb, which presented the highest
contamination absolute loading factors. In comparison, Co and Mn have low loading
#5 0.25 0.68 8 ≤ mCdeg ≤ 16: Very high
factors in the PC1. Cr, Cu, Zn, V, Ni, and Pb have the same signs and they
contamination
#6 0.22 0.65 16 ≤ mCdeg ≤ 32: Extremely are positively correlated. However, Mn shows opposite signs to the other
high contamination elements. Thus, Mn is negatively correlated with the other elements.
#7 0.30 1.13 32 ≤ mCdeg: Ultra high This inverse correlation suggests different contamination sources for
contamination Mn. PC2 explained 21.8% of the total variance. Mn indicated strong
In bold, moderately to severely contaminated environments are highlighted. loading factor and it was the dominant variable. PC3 explained 13.2% of
the total variance and Co indicated strong loading factor, and it was the
particles containing potentially toxic elements into the Paraguaçu River dominant variable. The results obtained in the three main components
is related to the high turnover of motor vehicles (Pb, Ni, V, Cr, Co, Zn, indicate different sources of contamination of the elements studied.
Hg) and the metallic corrosion process that occurred on the Ponte Dom HCA was also applied using the Single Linkage and 1-Pearson r dis­
Pedro II (Cu, Pb, Cr, Ni, Co). tance as similarity measures. It maximized heterogeneity between
groups.
3.2. Multivariate data analysis: application of unsupervised methods Moreover, consequently, it allowed better visualization of the clus­
(PCA and HCA) terings between the elements. Fig. S1 shows the dendrogram, and it was
possible to observe the formation of three main clusters (Mn, Co and Pb-
Principal component analysis (PCA) and Hierarchical cluster analysis Zn-Cu-Cr-Ni-V), at linkage distances between 0.400 and 0.650. These
(CA) were employed to verify the correlation between the elements and clusters correspond to the dominant variables observed in PC1, PC2 and
elucidate possible sources of contamination of potentially toxic elements PC3. The first cluster was formed by the elements Pb-Zn-Cu-Cr-Ni-V

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J.B. da Silva Junior et al. Marine Pollution Bulletin 179 (2022) 113730

Table 6
Ecological Risk Singular (Er) and Complex (PERI) in the Paraguaçu River.
Location Er(Cr) Er(Zn) Er(Pb) Er(Cu) PERI Er < 40: low ecological risk

#1 12.99 40.86 47.53 26.65 128.03 40 < Er ≤ 80: moderate ecological risk
#2 6.12 22.21 40.60 12.72 81.65 80 < Er ≤ 160: considerable ecological risk
#3 5.34 37.25 33.89 11.98 88.45 160 < Er ≤ 320: high ecological risk
#4 11.37 42.16 93.38 19.62 166.54 Er > 320: serious ecological risk
#5 5.14 22.92 43.85 12.16 84.06 PERI < 150: low ecological risk
#6 4.07 14.21 35.61 12.15 66.04 150 < PERI ≤ 300: moderate ecological risk
#7 8.83 34.80 46.72 14.17 104.52 300 < PERI ≤ 600: high ecological risk
Tria 2 1 5 5 PERI > 600: serious ecological risk

In bold, moderately to severely contaminated environments are highlighted.

a
Hakanson, 1980.

contamination to i) Pb are agricultural activities using insecticide, her­

Table 7
bicide and fungicide, or untreated domestic sewage discharges (Aly
Loadings of the variables (8) for the first three principal components.
et al., 2013; Gu et al., 2021); ii) Zn, Cu and Cr are discharges resulting
PC1 PC2 PC3 from metallurgy and electroplating (Naveedullah et al., 2014; Wang
V − 0.842 0.407 − 0.007 et al., 2018); iii) Ni are electroplating, mining processes and metal
Cr − 0.968 − 0.122 − 0.069 casting, alloy steel melting and shaping; iv) V are emitted to the envi­
Ni − 0.706 0.513 0.014
ronment especially from combustion of fossil fuels (Soldi et al., 1996).
Zn − 0.868 − 0.258 0.050
Pb − 0.554 − 0.549 − 0.532
Fig. 1 shows the graph of scores for PC1 to PC2. It was possible to
Mn 0.202 − 0.877 − 0.047 observe two groups of the samples in PC1. The triplicate of samples #2,
Co − 0.255 − 0.365 0.868 #3, and #5 were in the positive scores. While triplicates of samples #1,
Cu − 0.835 − 0.171 0.098 #4 and #7 were in the negative scores. Comparing the score graph,
Eigenvalues 4.00 1.74 1.10
samples #1, #4 and #7 have been presented with the highest average
Total variance (%) 50.1 21.8 13.2
Cumulative variance (%) 71.9 85.1 values for the elements Cr, Cu, Zn, V, Ni and Pb.
The average concentration obtained for the #1 were 6.50 μg g− 1 to
Cr; 13.3 μg g− 1 to Cu; 40.9 μg g− 1 to Zn; 11.2 μg g− 1 to V; 48.6 μg g− 1 to
corresponding to PC1. The second cluster was formed by the element Co Ni; 9.50 μg g− 1 to Pb. For #4 were 5.68 μg g− 1 to Cr; 9.81 μg g− 1 to Cu;
correspond to PC3. At the same time, the third cluster was formed by the 42.2 μg g− 1 to Zn; 9.11 μg g− 1 to V; 41.0 μg g− 1 to Ni; 18.7 μg g− 1 to Pb.
element Mn, corresponding to PC2. The observed clusters reaffirm the For #7 were 4.42 μg g− 1 to Cr; 7.08 μg g− 1 to Cu; 34.8 μg g− 1 to Zn;
different sources of contamination for these potentially toxic elements. 12.9 μg g− 1 to V; 53.4 μg g− 1 to Ni; 9.34 μg g− 1 to Pb. The separation of
A low similarity of Mn in relation to the other elements was samples #4.1 and 4.2 was observed in PC2. This was attributed to the
observed, at linkage distances 0.675. Furthermore, it confirms that Mn high concentrations of Mn observed for these samples. They corre­
has a different source of contamination in relation to the other elements. sponded to 384.3 μg g− 1 to #4.1 and 380.1 μg g− 1 to #4.2.
The small linkage distance separating Mn and Co indicates high
similarity. While the large linkage distance (0.375–0.665) separating Co 4. Conclusions
and Pb-Zn-Cu-Cr-Ni-V indicates that they have low similarity. This
suggests that Mn and Co can be from similar sources of contamination. This study showed that most potentially toxic chemical elements
In contrast, Co and Pb-Zn-Cu-Cr-Ni-V can be from different sources of showed low variation in the distribution of metals in sediments, indi­
contamination. Thus, it is probable that Pb Pb-Zn-Cu-Cr-Ni-V emanated cating similar and limited sources of pollution. Based on the results of
from anthropogenic activities. At the same time, the contents of Mn and Igeo, EF, and PI values, the main contaminants in sediments from the
Co may be attributed to natural geological processes. Paraguaçu River were Mn, Ni, V, and Zn. Co and Cu showed moderate
Pb-Zn-Cu-Cr-Ni-V still forms three subgroups by Pb, Zn-Cu-Cr and pollution power. Although it has no potential contaminant in the envi­
Ni–V, at linkage distances 0.20. Possible sources of anthropogenic ronment, Pb presented a moderate ecological risk. However, because of

Fig. 1. Principal Component Analysis (PCA) applied chemical variables: (a) scores; (b)loadings.

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J.B. da Silva Junior et al. Marine Pollution Bulletin 179 (2022) 113730

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