Marine Pollution Bulletin 160 (2020) 111649

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Marine Pollution Bulletin

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Baseline

Heavy metal contamination and ecological risk assessment in water and T

sediments of the Halda river, Bangladesh: A natural fish breeding ground
Mohammad Amirul Islama, , Biplob Dasb, Shamshad Begum Quraishic, Rahat Khana,
⁎

Kamrun Nahera, Syed Mohammod Hossaina, Shanjib Karmakerd, Shaikh Abdul Latife,
Mohammad Belal Hossenb
a
Reactor and Neutron Physics Division, Institute of Nuclear Science & Technology, AERE, Bangladesh Atomic Energy Commission, Ganakbari, Ashulia, Dhaka 1349,
Bangladesh
b
Department of Physics, Chittagong University of Engineering & Technology, Chittagong 4349, Bangladesh
c
Chemistry Division, Atomic Energy Centre, Bangladesh Atomic Energy Commission, 4 Kazi Nazrul Islam Avenue, Dhaka, Bangladesh
d
Nuclear Power and Energy Division, Bangladesh Atomic Energy Commission, E-12/A Agargaon, Sher-e-Bangla Nagar, Dhaka 1207, Bangladesh
e
Department of Nuclear Engineering, Faculty of Engineering, King Abdul Aziz University, Jeddah 21589, Saudi Arabia

ARTICLE INFO ABSTRACT

Keywords: This study reports the mass fractions of Al, Cr, Mn, Fe, Co, Zn, As, Ni, Cu, Cd, Hg, and Pb in water and sediments
Heavy metal and metalloid of the Halda river, Bangladesh, and studies the distribution, contamination, and potential ecological risks of the
Water and sediment contamination metals and metalloid. The average mass fractions of As, Cd, and Pb are relatively higher in sediments compared
Ecological risk assessment to those in background values, whereas Al, Fe, Mn, and Pb concentration fractions in water are higher than the
Halda river
international guideline values. The results of the different contamination indices indicate that Halda river se­
Multivariate statistical analysis
Neutron activation analysis
diments are minorly contaminated by As and Pb and moderately to considerably contaminated by Cd. The
ecological risk assessments indicate considerable to high ecological risk due to Cd. Multivariate statistical
analysis reveals the origin of the contaminants in the river, and indicate that Cr, Zn, Pb, and Cd are from
anthropogenic activities while the other metals originate from natural lithogenic actions.

Rapid urbanization and industrial activity have introduced many
pollutants, including heavy metals, to marine environments worldwide.
Heavy metal contamination in the marine ecosystem resulting from
natural and anthropogenic inputs pose serious threats due to their cu­
mulative behavior and toxicity (Singh et al., 2005; Zhu et al., 2017;
Gopal et al., 2018). The heavy metals move into the sediments, mainly
through geogenic and anthropogenic processes (Romic and Romic, 2003;
Tang et al., 2010; Hossain et al., 2016). Bioaccumulation in and effects of
heavy metals on marine biota depend indirectly on their type and mass
fraction in marine ecosystems (Edem et al., 2008; Kibria et al., 2016;
Islam et al., 2017). Therefore, the accumulation of heavy metals in the
water and sediments often induces harmful effects on marine biota when
the mass fraction limit exceeds certain threshold values (Macfarlane and
Burchettt, 2000; Vinodhini and Narayanan, 2008; Yi and Zhang, 2012).
To assess the contamination of sediments by toxic metals, various con­
tamination indices have been developed based on the metals' total content,
speciation, bio-availability, and toxicity (Yu et al., 2011; Yang et al., 2009).
Geo-accumulation index (Igeo), enrichment factor (EF), and contamination
factor (CF) are generally used for single metal contamination assessment.
On the other hand, to evaluate the combined risk of multiple metals in
sediments, the pollution load index (PLI), potential ecological risk index
(PERI), and sediment pollution index (SPI) have also been developed
(Huang et al., 2013; Islam et al., 2017).
In recent years, heavy metal contamination has become an issue of
major concern in fast-growing countries like Bangladesh (Latif et al., 2009;
Islam et al., 2015; Bhuiyan et al., 2015; Rahman and Islam, 2019; Khan
et al., 2019). The Halda river is one of the most important rivers in Ban­
gladesh as it is a natural breeding ground and a major source of eggs of
freshwater fishes. Indian major carps spawn naturally in this river, making
it a unique heritage of this country (Tsai et al., 1981; Kabir et al., 2013). As
a tidal river, this is the only one of its kind in the world where fishermen
directly collect fertilized fish eggs. This river also plays a pivotal role in the
local and national economy by providing means of navigation, drinking
water supply, sand quarrying, and irrigation. However, the river is being
polluted daily (Hossain et al., 2015; Bhuyan and Bakar, 2017). As this river
passes through the industrial zone of Chittagong, it receives a huge
amount of untreated effluents from various industries. Therefore, mon­
itoring programs are very important for assessing and identifying the

⁎
Corresponding author.
E-mail addresses: amirul.islam@baec.gov.bd, liton80m@yahoo.com (M.A. Islam).

https://doi.org/10.1016/j.marpolbul.2020.111649
Received 30 March 2020; Received in revised form 25 August 2020; Accepted 5 September 2020
Available online 24 September 2020
0025-326X/ © 2020 Elsevier Ltd. All rights reserved.
M.A. Islam, et al.
Fig. 1. Location map and sampling points in the Halda river, Bangladesh.
distribution of heavy metals and their toxic effects on the biota of this river
so that the natural fish breeding ground may be preserved. A few pre­
liminary studies have been conducted on metal pollution at a few specific
points of this river and these indicate an alarming situation (Hossain et al.,
2015). Therefore, it is important to characterize the water and sediments
over a wide range of the river to elucidate the metal pollution status. The
objectives of this study are to (i) assess the mass fractions and spatial
distributions of selected heavy metals/metalloid in surface sediments and
water of the Halda river; (ii) assess the degree of the metal contamination
and potential ecological risks on the biota of the river; and (iii) identify the
sources of the metals through multivariate statistical analyses.
Sediment samples were collected from 20 sampling points, and
water samples were collected from 5 points of the 20 sediment sample
collection points of the river (Fig. 1). The surface sediment (0–5 cm)
samples were collected using an acrylic pipe sampler during ebbs. In
this study, for each sediment sample, three replicate sediment samples
collected from each point are mixed into a composite sample. The
collected samples were dried in an electric oven at 45 °C until they
attained constant weight, and ground into powder by agate mortar and
pestle. For water sample collection, 2 L of surface water sample was
collected from each site. Each water sample was immediately acidified
with nitric acid (pH ~ 2) and transferred to the laboratory. Analytical
grade chemicals and reagents were used throughout the study.
The sediment sample analysis procedures using neutron activation
analysis (NAA) and atomic absorption spectrometry (AAS) techniques
2
Marine Pollution Bulletin 160 (2020) 111649
were the same as by Islam et al. (2017). NAA is considered to be a primary
method of measurement and possesses a versatile applicability (Greenberg
et al., 2011; Islam et al., 2011; Islam and Ebihara, 2017). For metal ana­
lysis in the sediment samples by NAA, approximately 50 mg of each dried
powder sediment sample and three reference materials—IAEA-Soil-7,
IAEA-SL-1 (Lake Sediment), and NIST-1633b were analyzed. For the re­
lative standardization approach of NAA, the samples and standards were
irradiated using a pneumatic transfer (rabbit) system (thermal neutron
flux of ~1013 cm−2·s−1) at the 3 MW TRIGA Mark–II research reactor of
the Bangladesh Atomic Energy Commission. In this study, the mass frac­
tions of Ni, Cu, Cd, Hg, and Pb in sediment samples were determined using
AAS following the standard procedure (Islam et al., 2017), and the mass
fractions of the rest of the studied metals were determined using NAA. For
the determination of mass fractions of Al in the sediment samples by NAA,
the interferences from 28Si(n,p)28Al and 32P(n,α)28Al reactions were cal­
culated and corrected following the procedure published earlier (Islam
et al., 2017). One gram of sediment subsamples and the same standards
used for NAA were digested for AAS. The mass fractions of the metals in
sediment and water samples were determined by AAS (Varian Analytical
Instruments, Models AA DUO 240 FS and AA 280 Z).
To assess metal pollution levels of the sediments of the Halda river,
EF and Igeo (Abrahim and Parker, 2008), CF (Hakanson, 1980), and PLI
(Tomlinson et al., 1980) were used. To calculate these environmental
indices, metal abundances of upper continental crust (UCC: Rudnick
and Gao, 2014) were used as the baseline data. The PERI (Hakanson,
M.A. Islam, et al. Marine Pollution Bulletin 160 (2020) 111649

Table 1
Mass fractions of the metals/metalloid (mg/ kg or indicated) in the surface sediments of the Halda river.
Sample Al (%) Cr Mn Fe (%) Co Ni

HR-1 6.71 ± 0.22 114 ± 5 652 ± 20 3.25 ± 0.11 13.8 ± 0.7 34.8 ± 0.6
HR-2 7.38 ± 0.23 98.2 ± 4.1 723 ± 23 3.83 ± 0.13 15.0 ± 0.7 40.0 ± 0.7
HR-3 6.64 ± 0.21 85.9 ± 3.7 586 ± 18 3.32 ± 0.12 13.2 ± 0.7 32.1 ± 0.2
HR-4 7.18 ± 0.23 112 ± 5 803 ± 25 4.43 ± 0.15 18.7 ± 0.9 47.6 ± 0.3
HR-5 6.66 ± 0.21 92.5 ± 3.9 643 ± 20 3.19 ± 0.11 13.5 ± 0.7 32.9 ± 0.4
HR-6 6.71 ± 0.21 84.5 ± 3.6 631 ± 20 3.07 ± 0.11 12.6 ± 0.6 38.1 ± 1.5
HR-7 6.12 ± 0.19 86.0 ± 3.7 550 ± 17 2.79 ± 0.10 11.5 ± 0.6 33.8 ± 0.4
HR-8 5.94 ± 0.19 56.7 ± 2.6 529 ± 17 2.00 ± 0.07 8.12 ± 0.4 30.2 ± 0.7
HR-9 7.21 ± 0.23 90.7 ± 3.9 638 ± 20 3.41 ± 0.12 13.1 ± 0.6 46.5 ± 0.5
HR-10 7.58 ± 0.24 90.7 ± 3.9 809 ± 25 3.48 ± 0.12 14.3 ± 0.7 45.7 ± 0.3
HR-11 5.50 ± 0.17 76.1 ± 7.1 485 ± 17 2.78 ± 0.15 13.0 ± 1.3 28.6 ± 0.1
HR-12 7.01 ± 0.22 120 ± 11 674 ± 23 3.54 ± 0.20 17.2 ± 1.8 38.7 ± 0.6
HR-13 7.29 ± 0.23 74.9 ± 7.0 705 ± 24 2.77 ± 0.15 13.8 ± 1.4 43.1 ± 0.6
HR-14 7.46 ± 0.23 111 ± 10 729 ± 25 4.36 ± 0.24 20.3 ± 2.1 46.5 ± 0.5
HR-15 6.58 ± 0.21 83.1 ± 7.8 566 ± 20 3.41 ± 0.19 16.7 ± 1.7 36.3 ± 0.6
HR-16 7.07 ± 0.22 87.7 ± 8.1 715 ± 24 3.61 ± 0.20 16.8 ± 1.7 41.2 ± 0.6
HR-17 6.76 ± 0.21 75.2 ± 7.1 391 ± 14 2.55 ± 0.14 14.1 ± 1.4 35.1 ± 0.1
HR-18 5.55 ± 0.17 103 ± 10 504 ± 17 1.48 ± 0.08 9.21 ± 1.0 30.6 ± 0.5
HR-19 6.79 ± 0.21 93.2 ± 8.7 702 ± 24 3.08 ± 0.17 13.8 ± 1.4 41.4 ± 0.1
HR-20 3.27 ± 0.10 70.9 ± 6.7 529 ± 18 1.69 ± 0.10 7.27 ± 0.8 26.6 ± 0.3
DL 0.005 17.7 4.31 0.10 0.86 0.83
Min 3.27 56.7 391 1.48 7.27 26.6
Max 7.58 120 809 4.43 20.3 47.6
Mean 6.57 90.7 628 3.10 13.8 37.0
SD 0.99 16.0 110 0.77 3.3 6.4
RSD,% 15.1 17.8 17.4 24.7 23.6 17.1
UCC 8.15 92 775 3.92 17.3 47
Shale 8.00 90 850 4.72 19 68
WHO, 2008 0.1 0.5 0.05
WHO, 2004 25.0 20.0
USEPA, 1999 25.0 30.0 16.0
FAO, 1985 5.0 0.1 0.2-10 0.05 0.2

Sample Cu Zn As Cd Hg (μg/kg) Pb

HR-1 18.70 ± 0.06 58.0 ± 0.2 7.16 ± 0.24 0.35 ± 0.01 49.2 ± 0.2 19.2 ± 0.9
HR-2 20.10 ± 0.20 70.3 ± 0.3 7.01 ± 0.24 0.50 ± 0.01 85.5 ± 3.0 21.2 ± 0.6
HR-3 14.45 ± 0.12 57.8 ± 0.4 6.02 ± 0.21 0.40 ± 0.01 18.0 ± 0.5 17.2 ± 0.1
HR-4 29.85 ± 0.03 62.0 ± 0.4 9.32 ± 0.32 0.58 ± 0.01 53.0 ± 3.5 25.2 ± 0.5
HR-5 16.28 ± 0.07 52.8 ± 0.8 6.48 ± 0.22 0.40 ± 0.01 34.5 ± 1.5 17.2 ± 0.3
HR-6 17.68 ± 0.09 44.0 ± 0.1 6.53 ± 0.23 0.40 ± 0.03 25.2 ± 0.4 18.0 ± 0.4
HR-7 14.75 ± 0.04 43.1 ± 0.2 5.08 ± 0.18 0.38 ± 0.01 34.0 ± 0.4 16.5 ± 0.4
HR-8 12.93 ± 0.09 54.6 ± 0.8 4.36 ± 0.16 0.35 ± 0.02 15.0 ± 0.1 14.7 ± 0.1
HR-9 20.20 ± 0.12 46.0 ± 0.8 6.50 ± 0.23 0.50 ± 0.02 28.7 ± 1.1 21.0 ± 1.6
HR-10 23.83 ± 0.05 41.7 ± 0.2 7.46 ± 0.26 0.43 ± 0.01 18.2 ± 0.6 20.5 ± 1.1
HR-11 12.75 ± 0.17 44.6 ± 0.1 5.12 ± 0.20 0.28 ± 0.01 44.5 ± 1.2 14.5 ± 0.1
HR-12 17.75 ± 0.07 61.8 ± 0.1 6.95 ± 0.27 0.40 ± 0.01 40.5 ± 0.5 19.2 ± 0.4
HR-13 20.08 ± 0.14 60.9 ± 0.1 5.54 ± 0.21 0.43 ± 0.01 26.5 ± 0.9 19.5 ± 0.4
HR-14 24.28 ± 0.02 67.1 ± 0.7 9.40 ± 0.36 0.48 ± 0.03 35.2 ± 1.6 20.5 ± 0.5
HR-15 15.88 ± 0.06 52.9 ± 0.9 6.41 ± 0.25 0.45 ± 0.02 40.7 ± 0.9 17.2 ± 1.0
HR-16 19.48 ± 0.08 58.5 ± 0.3 6.92 ± 0.27 0.43 ± 0.01 41.2 ± 2.6 19.5 ± 0.2
HR-17 16.95 ± 0.10 53.2 ± 0.1 8.31 ± 0.32 0.43 ± 0.02 28.0 ± 1.5 15.5 ± 0.3
HR-18 12.10 ± 0.07 43.8 ± 0.7 4.92 ± 0.20 0.38 ± 0.01 37.2 ± 1.4 14.0 ± 0.8
HR-19 18.18 ± 0.24 60.9 ± 0.3 6.33 ± 0.25 0.53 ± 0.03 43.2 ± 2.4 19.2 ± 0.4
HR-20 10.28 ± 0.13 36.9 ± 0.1 4.46 ± 0.18 0.35 ± 0.01 19.0 ± 0.1 13.7 ± 0.1
DL 0.60 15.3 0.63 0.2 10 1.5
Min 10.28 36.9 4.36 0.28 15.0 13.7
Max 29.85 70.3 9.40 0.58 85.5 25.2
Mean 17.8 54.5 6.51 0.42 35.9 18.2
SD 5.2 9.0 1.41 0.07 15.9 2.90
RSD,% 26.0 17.3 21.7 16.7 44.3 15.9
UCC 28 67 4.8 0.09 50 17
Shale 45 95 13 0.3 400 20
WHO, 2008 5
WHO, 2004 123 6
USEPA, 1999 110 0.6 40
FAO, 1985 0.2 2 5

Individual uncertainties with mass fractions measured by INAA are due to total uncertainties estimated in INAA for single measurement.
RSD = relative standard deviation; UCC = upper continental crustal average.

3
M.A. Islam, et al. Marine Pollution Bulletin 160 (2020) 111649

Table 2
The concentration fractions (μg/L) of the metals in water of the Halda river and their comparison with international standards.
Metal W1 W2 W3 W4 W5 Mean ECR, 1997 WHO, 2004, 2006 USEPA, 2006

Al 650 ± 30 710 ± 40 940 ± 50 1220 ± 60 1230 ± 65 950 ± 273 200 – –

Cr < 11.0 < 11.0 < 11.0 < 11.0 14.4 ± 1.6 – 50 50 100
Mn 77.0 ± 2.5 84.4 ± 3.4 91.0 ± 5.0 90.3 ± 4.6 160 ± 8 100 ± 34 100 400
Fe 1940 ± 10 2410 ± 30 3460 ± 40 3550 ± 14 5230 ± 80 3320 ± 1270 300–1000 300a –
Co 5.80 ± 0.17 6.23 ± 0.85 5.20 ± 0.36 6.55 ± 0.75 9.00 ± 0.83 6.56 ± 1.46 – 4a –
Ni 9.52 ± 0.25 8.85 ± 0.24 9.23 ± 0.26 9.40 ± 0.28 10.2 ± 0.3 9.44 ± 0.49 100 20 –
Cu 6.91 ± 0.03 7.52 ± 0.05 6.50 ± 1.35 5.71 ± 0.02 92.4 ± 12.1 23.8 ± 38.3 1000 2000 13
Zn 19.6 ± 0.3 16.8 ± 0.8 20.8 ± 3.2 23.7 ± 0.3 39.1 ± 3.9 24.0 ± 8.8 5000 5000a 120
Cd 0.65 ± 0.07 0.69 ± 0.08 0.96 ± 0.09 0.70 ± 0.28 1.60 ± 0.14 0.92 ± 0.40 5 3a 2.5
Pb 24.0 ± 2.0 20.0 ± 1.4 19.5 ± 3.5 23.0 ± 1.4 36.0 ± 2.6 24.5 ± 6.7 50 10 2.5

Concentration fractions of As (< 2.0 μg/L) and Hg (< 0.3 μg/L) were below detection limits.
a
Data from WHO, 2006.

1980) and sediment quality guidelines (SQGS: MacDonald et al., 2000;
Long and Morgan, 1991) were used to assess ecological risks posed by
the metals in the sediments. Methodologies and mathematical expres­
sions for EF, Igeo, CF, PLI, and PERI were essentially the same as those of
our previous studies (Islam et al., 2017; Tamim et al., 2016). In this
study, Statistica 8.0 for Windows (StatSoft Inc. STATISTICA, 2008) was
used to calculate the Pearson correlation matrix and principal compo­
nent analysis (PCA).
To ensure reported data quality, repeated analyses of reference
materials IAEA-SL-1 and NIST-1633b were performed along with the
sediment samples (Supplementary data: Table S1). To ensure data
quality of water samples, NIST-SRM-1643e (water) was also analyzed
(Table S1). For the metals determined in sediments by AAS, mass
fractions of Ni, Cu, Cd, Hg, and Pb in method blanks were 0.034, 0.0,
0.022, 0.0016, and 0.14 mg.kg−1, respectively. The spike recoveries
were from 88 to 99%.
The mass fractions of 11 metals and 1 metalloid in the surface sedi­
ments of the Halda river are given in Table 1. Among the studied metals,
Al, Cr, Mn, Fe, Co, Zn, and As were determined by NAA, whereas Ni, Cu,
Cd, Hg, and Pb were determined by AAS. In Table 1, descriptive statistics
of the metal mass fractions, relative standard deviations (RSDs,%),
available international guideline values (WHO: World Health Organiza­
tion and USEPA: Environmental Protection Agency, USA; FAO: Food and
Agricultural Organization), literature data for the UCC (Rudnick and
Gao, 2014), and average shale values (ASV: Turekian and Wedepohl,
1961) for the respective metals are also given. According to RSD values,
it is observed that metal contents of Fe, Co, Cu, As, and Hg values vary
over a wide range (RSD: 21.7–51.0%), whereas the rest of the metal
contents do not vary over a wide range (RSD < 20%). The anthro­
pogenic stresses, point/non-point sources, and geochemical processes in
the area may be the causes for this spatial variation of the metals
(Jonathan et al., 2010; Bhuyan and Bakar, 2017). In Table 1, it is also
observed that mean mass fractions (n = 20) of As, Cd, and Pb show
elevated values relative to background (UCC) values, whereas mass
fractions of Cd only show elevated values relative to ASV value. In this
study, the elevated values of Cd in the Halda river sediments can be
attributed to the pollution from industrial and domestic sewage of the
Chittagong municipal area (Zhang et al., 2008). When average mass
fractions of the metals in the Halda river sediments are compared with
available international guideline values, it is observed that Cr, Mn, Co,
and Ni mass fractions are higher than the WHO, 2004 and WHO, 2008
and USEPA, 1999 values (Table 1), whereas the mass fractions of Zn and
Cd are below the WHO, 2004 limits and Pb is below the USEPA, 1999
value. The mean mass fractions of the metals in sediment samples from
this study are compared with available literature data of this river as well
as other rivers of Bangladesh (Saha and Hossain, 2011; Banu et al., 2013;
Islam et al., 2013; Islam et al., 2014; Rahman et al., 2014; Hassan et al.,
2015; Mohiuddin et al., 2015; Islam et al., 2016) in Table S2. It is ob­
served that most of the metal contents in the Halda river sediments,
except for Zn, are higher than those of the previous study (Bhuyan and
Bakar, 2017). This indicates the progressive deterioration of the sediment
quality of this river. Comparison of metal mass fractions in sediments of
this river with those of other rivers indicates that the Al content in the
sediments is remarkably high while other metals had values comparable
to many other rivers of Bangladesh.
The levels of toxic metals play a significant role in the water en­
vironment. In this study, concentration fractions of 10 metals in water
samples are tabulated in Table 2 along with mean, standard deviation
(1σ), and guideline values by ECR (Environmental Conservation Rules,
Bangladesh), WHO, and USEPA. The concentration fractions of the
metal/metalloid As (< 2.0 μg/L) and Hg (< 0.3 μg/L) are below the
detection limits under the present experimental conditions. From
Table 2, it is observed that metal concentration fractions at point W5 are
relatively higher than the other points of the Halda river. When con­
centration fractions of the studied metals are compared with interna­
tional guideline values, it is observed that Al and Fe concentration
fraction at all sampling points, and Mn at W5, are higher than the ECR
(1997) standard values whereas, for other metals, concentration fraction
values are within the guideline values of ECR (1997). The concentration
fractions of Pb at all sampling points are higher than the WHO (2004)
and USEPA (2006) guideline values, whereas Cu at W5 is higher than the
USEPA (2006) value. The mean metal mass fractions of the water sam­
ples from this study are compared with available data of this river as well
as other rivers of Bangladesh (Mokaddes et al., 2013; Bhuiyan et al.,
2015 ; Ahmed et al., 2009; Rashid et al., 2012; Zakir et al., 2012; Islam
et al., 2013) in Table S3. In this study, the concentration fractions of most
of the studied metals in the water of the Halda river are comparable to
the previously reported values (Bhuyan and Bakar, 2017), except for Al,
Ni, Cu, and Zn, whose concentration fractions in the present study are
lower than the data reported in the previous study (Table S3).
In this study, the EF values of the Halda river varies from 0.41 (for Hg
at HR10) to 11.0 (for Cd at HR18). The mean EF, Igeo, and CFs for twenty
samples with their associated uncertainties (standard deviation (n = 20),
1σ) for the studied metals are plotted in Fig. 2(a, b, c). The EF values of Cr,
As, and Pb indicate minor enrichment, whereas those of Cd indicate
moderate to severe enrichment in sediments of the Halda river. The rest of
the metals do not show any significant enrichment in the river sediments.
The Igeo values for the studied metals range from −2.06 (for Hg at HR3) to
2.09 (for Cd at HR4). The Igeo values for the studied metals indicate that
the Igeo values of Cd (1.03 to 2.09 with mean 1.62 ± 0.24) are sig­
nificantly higher than unity and that the Igeo values for the rest of the
metals/metalloid are less than or equal to unity (Fig. 2b). According to the
criteria of Igeo, sediments of the Halda river are moderately contaminated
by Cd. The relatively high content of Cd in sediments of the Halda river
can be attributed to anthropogenic sources including chemical fertilizers
and pesticides used in agricultural fields, and municipal wastes discharged
into the river with Cd-containing batteries, pigments, and anti-corrosive
metals (Siegel, 2002; Ghrefat et al., 2011). The calculated CF values of the
studied metals also indicate that Halda river sediments are moderately
contaminated by Cr, As, and Pb, but are considerably contaminated by Cd

4
M.A. Islam, et al. Marine Pollution Bulletin 160 (2020) 111649

8.0 Table 3
(a) Results of PLI and potential ecological risk assessment for toxic metals/me­
7.0 talloid in surface sediments of the Halda river.
Sample Er PERI PLI
6.0 Severe
Cr Mn Ni Cu Zn As Cd Hg Pb
Enrichment Factor

5.0 HR-1 2.48 0.84 3.70 3.34 0.87 14.9 117 39.4 5.66 188 1.47
HR-2 2.14 0.93 4.26 3.59 1.05 14.6 167 68.4 6.25 268 1.59
Moderate HR-3 1.87 0.76 3.41 2.58 0.86 12.5 133 14.4 5.07 175 1.32
4.0
HR-4 2.44 1.04 5.07 5.33 0.93 19.4 192 42.4 7.43 276 1.88
HR-5 2.01 0.83 3.50 2.91 0.79 13.5 133 27.6 5.07 190 1.38
3.0 HR-6 1.84 0.81 4.06 3.16 0.66 13.6 133 20.2 5.29 183 1.37
Minor HR-7 1.87 0.71 3.59 2.63 0.64 10.6 125 27.2 4.85 177 1.23
2.0 HR-8 1.23 0.68 3.21 2.31 0.82 9.09 117 12.0 4.34 150 1.05
HR-9 1.97 0.82 4.94 3.61 0.69 13.5 167 23.0 6.18 221 1.50
HR-10 1.97 1.04 4.86 4.25 0.62 15.5 142 14.6 6.03 191 1.56
1.0 HR-11 1.65 0.63 3.05 2.28 0.67 10.7 91.7 35.6 4.26 150 1.08
HR-12 2.61 0.87 4.12 3.17 0.92 14.5 133 32.4 5.66 198 1.53
0.0 HR-13 1.63 0.91 4.59 3.58 0.91 11.5 142 21.2 5.74 192 1.36
HR-14 2.41 0.94 4.95 4.33 1.00 19.6 158 28.2 6.03 226 1.70
Al Cr Mn Fe Co Ni Cu Zn As Cd Hg Pb
HR-15 1.81 0.73 3.86 2.83 0.79 13.4 150 32.6 5.07 211 1.35
HR-16 1.91 0.92 4.39 3.48 0.87 14.4 142 33.0 5.74 206 1.47
2.0 HR-17 1.64 0.50 3.73 3.03 0.79 17.3 142 22.4 4.56 196 1.25
HR-18 2.23 0.65 3.25 2.16 0.65 10.3 125 29.8 4.12 178 1.21
(b) HR-19 2.03 0.91 4.40 3.25 0.91 13.2 175 34.6 5.66 240 1.52
1.5
HR-20 1.54 0.68 2.83 1.83 0.55 9.30 117 15.2 4.04 153 1.09
Tr 2.0 1.0 5.0 5.0 1.0 10 30 40 5.0
Geo-accumulation Index

1.0

0.50 Different SQGs (mg/kg)a References

TEL 52.3 15.9 18.7 124 7.24 0.68 130 30.2 CCME, 1999
0.0 PEL 160 42.8 108 271 41.6 4.2 700 112 CCME, 1999
ERL 81 20.9 34 150 8.2 1.2 150 46.7 NOAA, 2012
ERM 370 51.6 270 410 70 9.6 710 218 NOAA, 2012
-0.50

-1.0 Percentage of the samples based on SQGs

< TEL 0.0 0 60 100 80 100 100 100

-1.5 TEL-PEL 100 75 40 0 20 0 0 0
< ERL 25 0 100 100 85 100 100 100
-2.0 ERL-ERM 75 100 0 0 15 0 0 0
Al Cr Mn Fe Co Ni Cu Zn As Cd Hg Pb Tr = toxic response factor; TEL = threshold effects level; PEL = probable ef­
fects level; ERL = effect range low; ERM = effect range medium.
a
6.0 SQG for Hg in μg/kg.
(c)
In this study, the ecological risk factors (Er) and PERI along with
5.0
different SQGs are tabulated in Table 3. The Er values for all studied
metals and metalloid at all sampling points are less than 40, which
represents low ecological risks, except for Cd and Hg. For Cd, Er values
Contamination Factor

4.0
Considerable
vary from 80 to 160 (considerable) for most of the sampling points,
except at H2, H4, H9, and H19 where risk is considered to be high
3.0 (Er˃160). For Hg, Er values at H2 and H4 are considered to be moderate
(40˂Er˂80), whereas at other points, Er values are less than 40 (low
Moderate ecological risk). The high contents of Cd in the sediments of the Halda
2.0 river result in biochemical changes in fish metabolism (Vinodhini and
Narayanan, 2008), which will affect the natural breeding of fish in this
river. The estimated comprehensive PERI values considering all studied
metals at all sampling points are moderate (150˂PERI˂300) (Table 3).
1.0

To assess the potential biological effects of heavy metals in sedi­

0.0
Al Cr Mn Fe Co Ni Cu Zn As Cd Hg Pb
Fig. 2. Environmental contamination indices- (a) enrichment factor, (b) geo-
accumulation index, and (c) contamination factor of the Halda river sediment
samples.
(Fig. 2c). The calculated PLI values at the sampling points vary from 1.05
to 1.88 with mean 1.39 ± 0.21 (Table 3). The estimated PLI values
greater than 1.0 indicate the deteriorated surface sediment quality at all
sampling points of the Halda river.
ments of the Halda river, different SQGs were also used. According to
the threshold effect level (TEL) and probable effect level (PEL) SQGs,
any site is considered to be contaminated if 10% of the values exceed
TEL. In this study, Cr, Ni, Cu, and As contents in Halda river sediments
have more than 10% of the values above TEL. For Cr, 100%; Ni, 75%;
Cu, 40% and As, 20% of the samples have values between TEL and PEL,
while no metal mass fractions are above PEL (Table 3). On the other
hand, according to effect range low (ERL) and effect range medium
(ERM) SQGs, only Cr (75%), Ni (100%), and As (15%) fall between ERL
and ERM values. Therefore, the results of sediment classification ac­
cording to different SQGs suggest that Zn, Cd, Hg, and Pb are not

5
M.A. Islam, et al.
expected to cause adverse biological impacts on the biota of the Halda
river because the obtained values are below TEL and ERL (Table 3).
However, surface sediments at most of the studied points are expected
to pose a threat to the organisms of the river due to the high mass
fractions of Cr, Mn, and Ni.
Correlation among metals reflects the origin and transport behavior
of the metals in a river system. Pearson correlation matrices among the
studied metals indicate that most of the metals in sediments have sig­
nificant correlations among them (Tables S4 and S5). Strong positive
correlations of Al with other metals in sediments indicate their asso­
ciation with clay minerals like silicate/alumino-silicate minerals.
Mercury (Hg) shows poor correlations with the studied metals which
indicates the unique behavior of this metal in sediments or its origin
from a separate source(s) compared to those of other metals. The strong
positive correlations of Fe with Mn, Co, Ni, and Pb in sediments and
water indicate their similar behavior and their same origin, which is the
lithogenic sources (Tamim et al., 2016; Varol, 2011). The metalloid As
in sediments also shows positive correlations with Cr (0.61), Cu (0.84),
and Cd (0.64), which indicates the common origin of these metals. The
strong positive correlations of Pb with Cr (0.59), As (0.73), and Cd
(0.80) in sediments suggests a potential common source of these ele­
ments such as anthropogenic sources. All detectable metals in water are
significantly positively correlated with each other (Table S4).
The principal component (PC) analysis was performed by applying
varimax rotation on the normalized data of the metals to determine the
influencing factors and potential sources of the pollutants in sediments
and water of the Halda river (Tables S6 and S7). For sediment samples,
PC1 (first principal component) shows the highest loadings for Al, Mn,
Fe, Ni, Cu, Cd, and Pb, and it explains 67% of the variance. Among these
metals, Al, Mn, Fe, Ni, and Cu are controlled by the geological back­
ground (Islam et al., 2017; Boruvka et al., 2005; Sajn et al., 2011)
whereas Pb and Cd are related to the transportation and agricultural
activities (Miguel et al., 1997). Cadmium (Cd), the most toxic metal with
high ecological risk, is related to agricultural sources like pesticides and
chemical fertilizers (Green-Ruiz and Páez-Osuna, 2001; Maanan et al.,
2014). Therefore, PC1 represents both rock materials as well as anthro­
pogenic activities. PC2 shows the highest loadings of Cr, Zn, and Hg and
explains 9.9% of the variance. These metals are related to traffic activ­
ities; in particular, Zn is a marker for fuel oil burning and untreated dying
industrial wastes (Khan et al., 2020; Fu et al., 2014; Imperato et al.,
2003). Khan et al., 2020 is not in same format like others (last name first)
at refererence list. Please correct this format. This component accounts
for metals from anthropogenic activities. PC3 explains 5.6% variance and
has high loadings for Al, Fe, Co, and As. For water samples, the principal
components with eigenvalues > 0.68 reduced the number of variables to
two principal components which account for 94.1% of the variance for
all variables. Here, the first component (PC1) shows the highest loadings
of most of the metals except Al and Fe. This component explains 86.2%
of the total variance of the data of metal concentration fractions in water.
The second component (PC2) shows the highest loadings of Al and Fe
and it explains 7.9% of the variance of the data. A strong positive cor­
relation between Al and Fe was also observed in the previous section.
The highest loadings of Al and Fe in the second component and the
uncontaminated status of these metals likely originated from natural
sources. R. Khan et al., 2020 is not in same format (last or family am at
first). it can not be corrcted. Please correct this in rference list.
This study depicted the spatial distribution, contamination, ecolo­
gical risks, and sources of 11 metals and 1 metalloid in water and se­
diments of the Halda river. From these findings, it can be concluded
that effective management and restoration work should be conducted to
preserve the natural breeding ground of freshwater fishes by decreasing
ecological risks due to toxic metal pollution.
CRediT authorship contribution statement
All co-authors approved and contributed to the article.
6
Marine Pollution Bulletin 160 (2020) 111649
Declaration of competing interest
The authors declare that they have no conflict of interest.
Acknowledgments
The authors thank the technical personnel of RNPD and Analytical
Chemistry Laboratory of AECD of BAEC for their help during sample
preparation and analysis. The CRR of BAEC is gratefully acknowledged
for neutron irradiation of the samples.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://
doi.org/10.1016/j.marpolbul.2020.111649.
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