Environmental Nanotechnology, Monitoring & Management 16 (2021) 100524

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Environmental Nanotechnology, Monitoring & Management

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

Quality assessment of freshwaters from a coastal city of southern

Bangladesh: Irrigation feasibility and preliminary health risks appraisal
Md. Abu Bakar Siddique a, *, Rahat Khan b, *, Abu Reza Md. Towfiqul Islam c, Md. Kowsar Alam d,
Md. Shahinur Islam d, Md. Saddam Hossain e, Md. Ahosan Habib f, Md. Ahedul Akbor a,
Ummey Hafsa Bithi g, Md. Bazlar Rashid f, Faisal Hossain h, Ismail M.M. Rahman i,
Iftakhar Bin Elius b, Md. Saiful Islam j
a
Institute of National Analytical Research and Service, Bangladesh Council of Scientific and Industrial Research, Dhanmondi, Dhaka 1205, Bangladesh
b
Institute of Nuclear Science and Technology, Bangladesh Atomic Energy Commission, Savar, Dhaka 1349, Bangladesh
c
Department of Disaster Management, Begum Rokeya University, Rangpur 5400, Bangladesh
d
Department of Physics, Faculty of Science, University of Chittagong, Chittagong 4331, Bangladesh
e
Department of Environmental Science and Resource Management, Mawlana Bhashani Science and Technology University, Tangail 1902, Bangladesh
f
Geological Survey of Bangladesh, Segunbaghicha, Dhaka 1000, Bangladesh
g
Institute of Food Science and Technology, Bangladesh Council of Scientific and Industrial Research, Dhanmondi, Dhaka 1205, Bangladesh
h
Department of Chemistry, Faculty of Science, University of Chittagong, Chittagong 4331, Bangladesh
i
Institute of Environmental Radioactivity, Fukushima University, 1 Kanayagawa, Fukushima City, Fukushima 960-1296, Japan
j
Department of Soil Science, Patuakhali Science and Technology University, Patuakhali 8602, Bangladesh

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

Keywords: The present study was conducted for the first time to appraise the water quality, irrigation feasibility, and human
Coastal region health risk of surface water in heavy industrial and urban establishments from a coastal city of Bangladesh.
Freshwater basins Surface water samples were collected from the hilly terrain comprised of Plio-Pleistocene to Miocene-sediments
Human health risk
throughout the study area. The ranges of pH were 5.35 to 7.58, EC values were 42.3 to 2440 µS cm− 1, and
Irrigation feasibility
turbidity were 2.53 to 1570 NTU, respectively. The overall physicochemical condition of water samples revealed
Toxic elements
Water quality that the water was unsuitable and also unsafe for domestic use. A bias-free systematic sampling and analyzed
parameters invoke that surface water quality is deteriorated by Cr (52.2), Mn (532), Fe (4797), Mg (31445), K
(29213), Co (69.0), Ni (39.5), and Pb (22.4 µg L− 1) contamination and make the surface water unsuitable for
drinking, cooking, fisheries, and other purposes. Anthropogenic activities (e.g., domestic, industrial, agricultural,
etc.) intensified by climate change-induced sea-level rise are mainly responsible for the source apportionment of
metal pollution in the study region. However, the surface waters of the studied sites are allowed to use for ir­
rigations, except for Karnaphuli river due to high alkali hazards. Furthermore, the existence of toxic metal-
induced non-carcinogenic and carcinogenic risks does not allow inhabitants to use this water for household
works.

1. Introduction geogenic (e.g., arsenic contamination) and anthropogenic processes.

Water is an essential environmental compartment that plays a vital
role for all living organisms and forms the ecosystems. Concomitantly,
water quality possesses significant importance due to its versatile uses
such as drinking, household works, industrial purpose, irrigation, etc.,
for which both groundwater and surface water have long been used (Li
and Wu, 2019; Li, 2020). The water quality can be compromised by both
However, geographically the quality of water in the current time of the
world is deteriorating in several ways such as due to industrial pollution,
domestic discharge, and sea-level rise (Ahsan et al., 2019; Seddique
et al., 2019; Alshehri et al., 2021). The unplanned urbanizations, in­
dustrializations, and densely populated demography in many devel­
oping countries are the key components for polluting the water body
(Chowdhury et al., 2017; Ahmed et al., 2021; Alshehri et al., 2021).

* Corresponding authors.
E-mail addresses: sagor.bcsir@gmail.com (Md.A.B. Siddique), rahatkhan.baec@gmail.com (R. Khan).

https://doi.org/10.1016/j.enmm.2021.100524
Received 30 October 2020; Received in revised form 14 June 2021; Accepted 1 July 2021
Available online 3 July 2021
2215-1532/© 2021 Elsevier B.V. All rights reserved.
Md.A.B. Siddique et al.
However, the water quality in the coastal regions is mainly worsened
due to the impact of seawater intrusion (Roy and Zahid, 2021). All kinds
of contaminated water, especially with the persistent excess chemical
elements, have potential human health and environmental implications
(Talukder et al., 2016; Alshehri et al., 2021; Rakib et al., 2013).
As a part of the world’s largest delta, Bangladesh is washed away by a
large number of Himalayan or non-Himalayan rivers which are even­
tually merged with the Bay of Bengal. After identifying arsenic
contamination in the groundwater of the Bengal basin, surface water has
given more priority for the usual usages. However, surface water re­
sources are facing progressive deterioration owing to rapid urbaniza­
tion, industrialization, agricultural run-off, atmospheric depositions,
and so forth (Ahsan et al., 2019; Islam et al., 2020a). Like other devel­
oping countries, Bangladesh has also been experiencing environmental
deterioration on an unprecedented scale by the potentially toxic ele­
ments (PTEs) that originated from anthropogenic activities as well as
geogenic processes (Habib et al., 2019, 2018; Habib and Khan, 2021;
Khan et al., 2021a, 2021b, 2019a, 2018; Begum et al., 2021). In the last
two decades, firstly growing industrial sectors and concomitant un­
planned urbanization have been aggravating the aquatic pollution sce­
nario (Khan et al., 2020). The pollution by PTEs in the aquatic systems
causes irreversible human health damage (Ali et al., 2016; He and Li,
2020) as well as the loss of biodiversity (Zhang et al., 2009) due to its
long persistence and potential toxicity (Hasan et al., 2020). Moreover,
global warming-induced sea-level rise (Ortiz, 1994) may increase the
salinity of the freshwater basin residing in the coastal regions which can
ultimately affect human health (Talukder et al., 2016) and crop yields
(Rawat et al., 2018) in those areas.
Chittagong, a coastal city of Bangladesh, is one of the busiest port
cities in South Asia where more than 2.5 million people live with a
population density of ~ 15,000 km− 2. Rapidly growing industrial ac­
tivities including ship breaking and oil refinery, and unplanned urban
establishments with vulnerable environmental regulations are causing
serious PTEs mediated aquatic pollutions in this area which can poten­
tially induce health risks to humans (Ahmed et al., 2021; Khan et al.,
2017, 2019b, 2019c). Further, the coastal city has been identified as
susceptible due to a significant effect on water quality and quantity from
various aspects of anthropogenic and natural phenomena (Islam et al.,
2017a, 2020d) such as industrial discharge, over population, rise in sea
level, and intrusion of saline water (Ali et al., 2016; Raknuzzaman et al.,
2016; Seddique et al., 2019; Islam et al., 2020b,c; Ali et al., 2021). Thus,
the assessment of anthropogenic pollution with associated human health
risks along with the water-salinity-related irrigation-water feasibility
evaluation is vital for such a coastal city. Several works (Sarwar et al.,
2010; Ali et al., 2016; Raknuzzaman et al., 2016; Bhuyan and Bakar,
2017; Karimet al., 2019; Islam et al., 2020b; Moula et al., 2020) have
been carried out in this region focusing on the evaluation of water
quality based on the physicochemical parameters, trace elements, and
essential elements present in the water body while some works were
limited to the comparison of their results with the permissible limits only
(Ahmed et al., 2010; Sarwar et al., 2010). Most of these studies
considered the water contaminations from industrial, domestic, and
sewage discharge. Only a few studies (e.g., Islam et al., 2020b) evaluated
the water quality considering the seawater intrusion in this region.
However, being a densely populated, industrial, and coastal city, the
degradation of water quality in the city should be considered from all
possible aspects of contamination since it has a potential impact on
human health, crop production, and the environment (Ahmed et al.,
2021; Talukder et al., 2016). Although extensive research has been
carried out in many coastal regions in the world including Bangladesh
(Naidu et al., 2021; Roy and Zahid, 2021; Islam et al., 2020b; Ahmed
et al., 2020; Sehnaz et al., 2020; Seddique et al., 2019; Bhuyan and
Bakar, 2017; Raknuzzaman et al., 2016; Hasan et al., 2021; Kumar et al.,
2021), studies have not hitherto been found which considered a com­
bined impact of seawater intrusion and industrial discharge (with PTEs)
on the overall water quality. Further, most of these studies didn’t
2
Environmental Nanotechnology, Monitoring & Management 16 (2021) 100524
evaluate the human health risks associated with contaminated water.
So, to fill up the gaps, a comprehensive study on index-based water
quality assessment, affiliated health risks evaluation, and irrigation
water feasibility study considering the effects of both seawater intrusion
and industrial discharge have to be carried out urgently to appraise the
overall environmental condition of the study area.
Therefore, the major objectives of the present work are (1) to
determine the elemental and physicochemical parameters in a suit of
systematically collected water samples from the coastal Chittagong City,
(2) to evaluate the distribution and sources of the analyzed water quality
parameters with statistical approaches, (3) to draw a comprehensive
scenario for the evaluation of water quality and irrigation water feasi­
bility, and (4) to assess the associated human health risks for the local
inhabitants who rely on surface water for life and livelihoods. The
outcomes of these multi-disciplinal approaches will have significant
impacts on building the regulation policies for identical study sites
around the globe.
2. Experimental and methodologies
2.1. Studied area
Chittagong (Bangladesh) is one of the important port-city in South
Asia which is surrounded by the Bay of Bengal (west-side), Karnaphuli-
Halda rivers (south and east side), and the Chittagong hill-tracts (north-
side). It locates in the folded-flank Tectonic Element of Bengal Basin
(Khan, 2002). The studied area consists of recent coastal plain sediments
along the west of the eastern coast (Cliff-coast) backed by hilly terrain
comprised with Plio-Pleistocene to Miocene-sediments termed as bed-
rock. Tidal, fluvial-deltaic to estuarine environments were the main
depositional system of this area related to sea-level fluctuations in the
late Quaternary Period.
The region experiences a humid tropical monsoon climate. It enjoys
three distinct seasons, namely monsoon, winter and summer. The
monsoon begins in June and lasts until October. During this time, the sky
is often overcast with dark clouds, and it rains heavily accompanied by
gusty wind and occasionally with a cyclone storm which sometimes
causing extensive damage to the region. The winter season begins at the
end of November and continues towards the end of February with
pleasantly cool, calm, and dry weather. The summer season prevails
between March and May. The average rainfall in the region is about
3000 mm/year (Anon, 2011) and the daily temperature rises from about
13.5 ◦ C in the dry season to 32.5 ◦ C before the onset of the monsoon
(Anon, 2011).
Two types of surface water bodies i.e., stagnant water bodies and
flowing water bodies are found here. There are plenty of small and large
ponds and tanks in this area. These reservoirs are used for domestic and
irrigation purposes throughout the year. The flowing water bodies of the
area consist mainly of rivers and streams. The area is drained by an
extensive network of seasonal, intermittent, and perennial streams and
streamlets. Generally, the streams, locally known as Chara, are dendritic
in the pattern. The Sitakunda hill ranges from a prominent water divide.
Many perennial streams have been observed on the western and eastern
slopes of the hill ranges which join the Sandwip channel and Halda river,
respectively. Consequently, the eastern part of the hills as well as the
Halda valley forms a wide catchment basin. This catchment basin is
drained by the river Halda and the Karnaphuli, which are the main rivers
in the study area (Fig. 1). These two rivers flow south-southwest and
eventually fall into the Bay of Bengal. Halda river is a tributary of the
Karnafuli river. In addition to these, there is a tidal network in the area.
The water in these rivers and tidal channels is salty for shaking in winter
but freshening up in the rainy season.
Considering the potential contamination load, six different locations
of the greater Chittagong City were selected randomly for sampling
which includes Chaktai canal, Karnaphuli river bridge site, Chittagong
Medical College (CMC) area, KDS garments area (Bayejid-Bostami),
Md.A.B. Siddique et al. Environmental Nanotechnology, Monitoring & Management 16 (2021) 100524

Fig. 1. Map showing the sampling points with geomorphological features of Chittagong (Chattogram) area, Bangladesh.

Halda river, and Goolpukur of Chittagong University (CU) (Fig. 1). The wastewater in the nearby large drain, whereas KDS garments mainly
Chaktai canal regularly receives many industrial effluents, domestic discharge a huge amount of untreated or partially treated dark effluents
discharge, and other wastewater around it. The CMC and the nearby beside a canal. All this wastewater ultimately meets the Karnaphuli river
local markets discharge several solids and liquid wastes including polluting the aquatic system. The Halda river site, located on the

3
Md.A.B. Siddique et al.
different side of Karnaphuli river (Fig. 1), is also contaminated by in­
dustrial discharge from several industries such as textile, paper, and
power plant situated in the nearside of the river as well as sewage
discharge (Karim et al., 2019; Moula et al., 2020). Some local people
besides these two rivers are using the water for their domestic, drinking,
and irrigation purposes. Moreover, Halda is the only carp-breeding river
ground in Bangladesh and also in Southeast Asia (Islam et al., 2020c;
Karim et al., 2019). The fishes from both the rivers Halda and Karna­
phuli are regularly consumed by the local inhabitants. Hence, the
contamination of these two water bodies by several near and far con­
nected polluted sites has potential human health impacts. The waste­
water from Chaktai canal, CMC, and KDS garments area are not directly
utilized for drinking, but some very poor people living beside these areas
might use this wastewater sometimes for their washing, bathing, and
other household works as well as for irrigation which might have
considerable health impacts. However, the sampling site Goolpukur is
situated in the central zone of CU which is a completely uncontaminated
site and is considered as the control site of this study.
2.2. Sample collection, processing, and analysis
Total 20 composite surface water samples were collected from six
different sampling stations (St, Fig. 1) of the Chittagong region viz.,
Chaktaicanal (St-1, canal water: W1-3), Karnaphuli river bridge (St-2,
river water: W4-6), Chittagong Medical College (St-3, drainage water:
W7-9), Halda river (St-4, river water: W10-14), Goolpukur of CU (St-5,
pond water: W15-17), and KDS garments (St-6, canal water: W18-20).
Sampling points belong to the same sampling stations are separated
by ~ 250 m from each other. From each of the sampling points, 3–5
replicate samples were initially collected and were mixed to obtain a
representative composite sample. Sample collection, processing, and
preparation for elemental analysis are similar to those of APHA (2012)
and Ahsan et al. (2019, 2018). During sample preparation, analytical
grade concentrated nitric acid (68 % pure) as obtained from Sigma-
Aldrich, and high-quality deionized water (electrical conductivity: 0.2
µS cm− 1, resistance: 18.2 MΩ.cm at 25 ◦ C) were used (Khan et al.,
2015a,b). The accuracy and precession of the analysis were ensured by
the replicate measurements (relative standard deviation < 5 %) of the
NIST (National Institute of Standard and Technology) traceable certified
reference material (Fluka Analytical, Sigma-Aldrich, Germany) as well
as the randomly selected prepared samples with the same identification
number (Siddique et al., 2020; Hasan et al., 2020; Ahsan et al., 2019).
Elemental abundances of Cr, Pb, Cd, As, Mn, Ag, Fe, Ni, Co, Mg, Ca,
Cu, and Zn in the water samples were determined by using atomic ab­
sorption spectrometer (AAS) while K and Na were measured by using
flame photometer (Model: PFP7, Jenway, UK). Lead, Cd, Cr, and Ni
abundances in the water samples were measured by Zeeman-AAS
(Model: GTA 120-AA240Z, Varian, Australia) and the contents of
arsenic in the water samples were measured by electric hydride vapor
generation technique of AAS (Model: SpectrAA 220 equipped with ETC-
60 & VGA-77, Varian, Australia). Other metal concentrations were
estimated by flame-AAS (Model: AA240 FS, Varian, Australia). On the
other hand, physicochemical parameters, e.g., pH, electrical conduc­
tivity (EC), and oxidation–reduction potential (ORP) were measured
insitu at the sampling sites for all samples by a handheld portable
Multiparameter meter (Model: sensionTM156, HACH, USA) by inserting
the electrode of the meter directly into the water (Ahsan et al., 2019).
ORP of the water samples were measured in millivolts (mV), without any
temperature correction of the solution. Turbidity of water samples was
also determined insitu at the collection spots using a portable Turbidity
meter (Model: 2100P, HACH, USA) taking the sample in a small
turbidity measuring glass vial and putting the vial into the sample
measuring compartment of the meter. All the considered water quality
parameters were determined following the standard method (APHA,
2012) and the quality control approaches are essentially the same as
those of our previous works (Habib et al., 2020; Islam et al., 2020a;
4
Environmental Nanotechnology, Monitoring & Management 16 (2021) 100524
Ahsan et al., 2019).
2.3. Indices for water pollution and quality assessment
2.3.1. Heavy metal pollution index (HPI)
HPI index was constructed by establishing a weightage (Wi) for each
desired parameter which is an arbitrary value ranging from 0 to 1,
indicating the relative importance of the specific quality parameter
under consideration and is considered as inversely proportional to the
recommended value (permissible value, Si for each parameter) for the
specific parameter (Mohan et al., 1996; Reddy, 1995; Horton, 1965). In
this work, the recommended limits (i.e., Si: standard permissible value,
and Ii: highest desirable value for each parameter) were adopted from
the WHO (2011) standard and Bangladesh standard (ECR, 1997)
(Table S1). The highest permissive value (Si) for drinking water means
the maximum allowable concentration in drinking water without any
other water sources. The desirable maximum value (Ii) refers to the
standard limits for the same parameters in drinking water (Bhuiyan
et al., 2010).
Assigning a weightage (Wi) for each considered parameter, HPI was
calculated by Eq. (1) (Mohan et al., 1996).
∑n
Wi Qi
HPI = ∑i=1 n (1)
i=1 Wi
where Qi & Wi represent the sub-index and unit weight of the ith
parameter, respectively, and n represents the considered number of
analyzed parameters. Qi was estimated as below.
∑n
Qi =
|Mi − Ii |
× 100 (2)
i=1
Si − Ii
where Mi, Ii, and Si represent the measured metal, ideal, and standard
concentration values of the ith parameter, respectively. Based on the
index value, classifications of HPI as well as the subsequent indices are
tabulated in Table S2.
2.3.2. Heavy metal evaluation index (HEI)
HEI elaborated the overall water-quality regarding the elemental
contents (Edet and Offiong, 2002) and can be expressed as below.
∑
n
Mi
HEI = (3)
Si
i=1
where Mi and Si represent the measured value and maximum admissible
concentration (MAC) of the ith parameter, respectively.
2.3.3. Degree of contamination (CD)
CD showed the collective effects of the water-quality parameters
which are being considered as harmful for the domestic water usages
(Backman et al., 1997) and can be estimated as below.
∑
n
CD = CFi (4)
i=1
CAi
CFi = − 1 (5)
CNi
where CFi, CAi, and CNi are the contamination factor, measured con­
centrations, and upper permissible concentration of ith parameter,
respectively. ‘N’ indicates the ‘normative value’ while CNi is considered
as MAC.
2.3.4. Water quality index (WQI)
The WQI depends on mathematical expressions that convert
measured analytical water-quality parameters into a single number,
which represents the water-quality level (Horton, 1965). The three
Md.A.B. Siddique et al. Environmental Nanotechnology, Monitoring & Management 16 (2021) 100524

stepped WQI calculation processes (Sahu and Sikdar, 2008) are sum­ 1954; Li et al., 2016a), soluble sodium percentage (SSP: Todd, 1980; Li
marized by using Eq. (6) (Islam et al., 2020a) in which the standard et al., 2018b), Kelley’s ratio (KR: Kelley, 1963; Li et al., 2016b), mag­
values were taken from the WHO and Bangladesh standard (Table S1). nesium hazard ratio (MHR: Raghunath, 1987; Zhou et al., 2020), total
[( ] hardness (TH: Raghunath, 1987) and total dissolved solids (TDS: Islam
∑ n ∑n ∑
WQI = SI = (Wi × qi ) =
W Ci
∑i ) × ( × 100) (6) et al., 2018) are used to evaluate the water quality for irrigation by using
i=1 i=1 n Wi
Si the following Eqs. (15)–(20).
Na
where Ci represents the concentration of each variable, Si is standard SAR = √̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅ (15)
values, wi is assigned a weight according to its relative significance in (Ca + Mg)/2
water-quality for ingestion uses (Table S1), qi represents water-quality
rating variable, Wi is the relative weight, and SIi is the sub-index of ith
Na + K × 100
SSP = (16)
parameters. Ca + Mg + Na + K

Na
2.3.5. Entropy water quality index (EWQI) KR = (17)
Ca + Mg
Shannon (1948) demonstrated the concept of entropy as a measure
of information or uncertainty which can predict the output of a proba­ Mg × 100
bilistic event (Guey-Shin et al., 2011). The entropy concept for evalu­ MHR = (18)
Ca + Mg
ating the water quality (Islam et al., 2020a) involves the following steps.
For estimating the entropy weight for m (i = 1, 2, …, m) number of water TH = 2.50 × Ca + 4.12 × Mg (19)
samples with n (j = 1, 2, …, n) number of analyzed parameter, Eigen­
value matrix X can be constructed by Eq. (7) (Li et al., 2018a; Li et al., TDS = EC × 0.64 (20)
2019a; Wang et al., 2020).
In calculating the above indices, all the ionic concentrations were
converted in meq. L− 1, and TDS is expressed as a function of electrical
⎡ ⎤
x11 x12 ⋯ x1n
⎢ x
X = ⎣ ⋮21
x22 ⋯ x2n ⎥
(7) conductivity.
⋮⋱ ⋮ ⎦
xm1 xm2 ⋯ xmn
2.5. Health risk appraisal
To remove the influences of various units and contents of analyzed
parameters, the efficiency type (Eq. (8)) normalization approach (Li For the evaluation of health risks induced by trace elements in water,
et al., 2010) was adopted to convert the Eigenvalue matrix (X) into a direct oral and dermal absorption by the skin is generally considered
standard grade matrix (Y) (Eq. (9)). (Zeng et al., 2015). According to USEPA (2004), the exposure doses for
( ) direct ingestion (ADDingestion) and dermal absorption (ADDdermal) are
Xij − Xij min
Yij = ( ) ( ) (8) expressed as bellow.
Xij max − Xij min
Cw × IR × Absg × EF × ED
⎡ ⎤ ADDingestion = (21)
y11 y12 ⋯ y1n BW × AT
⎢ y21 xy22 ⋯ y2n ⎥
Y=⎣ (9)
⋮ ⋮⋱ ⋮ ⎦ Cw × SA × Kp × EF × ET × ED × 10− 3
ADDdermal = (22)
ym1 ym2 ⋯ ymn BW × AT
Then, the ratio of the analyzed parameter index (Pij), information where Cw, IR, EF, SA, ET, ED, BW, AT, Absg, and Kp represent the con­
entropy (ej), and entropy weight (ωj) can be calculated by Eqs. (10–12). centrations of trace elements (μg L− 1), ingestion rate (L day− 1), exposure
Yij frequency (days year− 1), exposed skin area (cm2), exposure time (h
Pij = ∑m (10) day− 1), exposure duration (in years), body weight (in kg), average time
i=1 Yij
for non-carcinogens (days), gastrointestinal absorption factor, and
1 ∑ m dermal permeability coefficient (cm h− 1), respectively. The values of
ej = − (Pij ×lnPij ) (11) each parameter (USEPA, 2004; Zeng et al., 2015; Schecter and Li, 1997;
ln(m) i=1
Tripathee et al., 2016; Xiao et al., 2019; Wu et al., 2009; Iqbal and Shah,
1 − ej 2013; Wang et al., 2017; Rodriguez-Proteau and Grant, 2005; Qu et al.,
ω j = ∑m (12) 2018) are presented in Table S3. Then, the non-carcinogenic risk (NCR)
j=1 (1 − ej )
can be estimated from the hazard quotients (HQ) for both ingestion and
The quality rating scale for the analyzed parameter (j) can be dermal pathway from Eqs. (23) and (25) as follows.
calculated from the obtained data (Cj) and the standard data (Sj) by Eq.
ADDingestion
(13). HQingestion = (23)
Rf Dingestion
Cj
qj = × 100 (13)
Sj ADDdermal
HQdermal = (24)
Rf Ddermal
From Eqs. (12) and (13), EWQI can be calculated by Eq. (14).
∑
n Rf Ddermal = Rf Dingestion × Absg (25)
EWQI = ωj qj (14)
j=1 where RfDingestion and RfDdermal are the reference doses for individual
According to the EWQI value, water samples can be categorized into elements (µg kg− 1 day− 1). Hence the total potential NCR can be evalu­
five ranks as described in Table S2. ated from the hazard index (HI) as follows.
∑
n
( )
2.4. Irrigation indices HI = HQingestion + HQdermal (26)
i=1

Irrigation indices such as sodium adsorption ratio (SAR: Richards, Non-carcinogenic health hazards can be considered, only when the

5
Md.A.B. Siddique et al.
values of HQ and HI are > 1 (USEPA, 2004). On the other hand, carci­
nogenic risks (CR) for individual elements can be calculated by Eq. (27).
CR = ADD × SF (27)
− 1
where, SF is the oral cancer slope factor (mg/kg/day) . In this work,
the CR was estimated for Cd, Cr, and As; and the SFs are 0.0015,
0.00038, and 0.041 (mg/kg/day)− 1 for ingestion intake, respectively
whereas dermal SF for As is 0.00366 (mg/kg/day)− 1 (Saha et al., 2017;
De Miguel et al., 2007; Gao et al., 2019). The acceptable ranges (1 ×
10− 6 to 1 × 10− 4) of the CR values were adopted from USEPA (2004).
2.6. Statistical analyses
The monitored data were evaluated statistically by SPSS-software
(Version-20, IBM-Corporation, Armonk, NY, USA). Multivariate statis­
tical methods, e.g., principal component analysis (PCA) and cluster
analysis (CA) are the most commonly used method in water-quality
assessment (Ahsan et al., 2019; Wu et al., 2020; Islam et al., 2020a).
PCA with a Varimax rotation method was utilized to demonstrate the
degree of metal pollution and for possible sources identification (Ahsan
et al., 2019). CA was performed with Ward algorithmic method and
rescaled linkage distance of similarity measurement was implemented to
know the sample groups of similar elemental contents (Li et al., 2019b).
Pearson correlation analysis was executed to show the relevant associ­
ations among the analyzed parameters (Wu et al., 2014; Islam et al.,
2019). For the comparison of data of different sampling stations and to
see the variation between samples and within samples (Ostertagova and
Ostertag 2013), one-way ANOVA was performed in this work at the
statistical significance level (p < 0.05).
3. Results and discussion
3.1. Water characterization
The results of physicochemical parameters e.g., pH, oxida­
tion–reduction potential (ORP), electrical conductivity (EC), and
turbidity of water samples are tabulated in Table 1. The highest and
lowest pH value of 7.58 and 5.35 were recorded at St-5 (Goolpukur of
CU) and St-1 (Chaktai canal), respectively. The mean values of water pH
of almost all samples in the studied areas were within the permissible
limits recommended by ECR (1997), WHO (2004), EPA (2001), BIS
(1991) (Table 1). An average pH of 7.89 in the nearby Karnaphuli river
was recorded (Ali et al., 2016), and the measured pH value in the Halda
river was ranged from 7.03 to 8.60 (Ahmed et al., 2010). The pH of the
nearby water system where the waste materials being dumped was
significantly affected by industrial or municipal waste materials. The
highest and lowest value of EC were found at St-2 (Karnaphuli river) and
St-5 (Goolpukur of CU), respectively. EC values of St-1 (Chaktai canal),
St-2 (Karnaphuli river), and St-3 (Chittagong Medical College: CMC)
were comparatively higher than the permissible limit of EU (1998) that
reflected the water pollution in these three regions. However, EC values
were within the allowable level at St-4 (Halda river), St-5 (Goolpukur of
CU), and St-6 (KDS garments) according to EU (1998). The higher EC
values were probably due to the contribution of ionic pollutants from
industrial and municipal activities. The measure of ORP of water sam­
ples in all sampling stations except for St-2 was mostly negative, indi­
cating the presence of substances with reducing properties. The positive
value of ORP in St-2 indicates an oxidizing nature of the water samples.
The highest (950 NTU) and lowest (2.79 NTU) mean turbidity value was
observed at St-1 and St-5, respectively. All the sampling stations, except
for St-5, showed much higher turbidity values than the standard values
of 10 NTU (ECR, 1997) and 5 NTU (WHO, 2004). Sarwar et al. (2010)
recorded the mean turbidity of 31 NTU at the Karnaphuli river, ranging
from 14 to 50.1 NTU. The overall physicochemical condition of water
samples in the study areas revealed that the water except for Goolpukur
of CU (St-5) was unsuitable and also unsafe for domestic use.
6
Environmental Nanotechnology, Monitoring & Management 16 (2021) 100524
The concentration of metals in the tested water samples from the six
different stations as provided in Table 1, indicating significant fluctu­
ated conditions among the sampling stations except for Cd, As, Ag, Co,
and Ni, where the variations in concentrations were not too high. The
highest metal concentrations were found to be at St-1 in which the
concentrations of most of the metals exceeded the maximum permitted
limit (Table 1). The mean level of Fe at St-1 was about 32 times higher
than the standard limit (Table 1) which is probably due to the contri­
bution from Fe-enriched waste waters of metallurgical industries,
especially steel rerolling mills beside the sampling point. The measured
Fe concentration in all the sampling locations was significantly higher
than the permissible level of drinking-water set by national and inter­
national laws (Table 1). Kazi et al. (2009) stated that metals usually
possess unique distribution in all the samples as exchangeable Fe cor­
relates typically to the adsorbed metals, which can easily be re-
mobilized into the water-system (Ikem et al., 2003). Krishna et al.
(2009) reported that the anthropogenic contribution of Fe in surface
water varied from 42.0 to 1886.0 µg L− 1 (mean: 161.8 µg L− 1) and
effluent waters are mainly accountable for such high concentration of Fe
in the water body. Aesthetic nuisances, including staining of laundry,
unpleasant taste, and odor, have resulted from the major undesirable
effects of high Fe contents in water (Gardner and Gunn, 1991). Nickel
concentration (131 µg L− 1) was slightly higher than the permissible
limit. Nickel can cause respiratory problems and lung cancer. Further­
more, the concentration of Cr at St-1 was nearly 3 times higher than both
the national and international water quality guidelines (ECR, 1997;
WHO, 2004; WHO, 2011; EU, 1998; EPA, 2001; BIS, 1991) (Table 1).
Chromium may cause several acute and chronic diseases including skin
and mucous membrane irritation, asthma, lung tumors, lung cancer,
respiratory problem, chronic bronchitis, corrosion, hemorrhagic diath­
esis, kidney, and liver damage, male reproductive system damage, and
chronic ulceration (Asaduzzaman et al., 2002). The concentration of Mn
at stations 1, 2, 3, and 6, respectively, were nearly about 15, 4, 12, and
13 times higher than the acceptable limit proposed by EU (1998), and
EPA (2001) (Table 1). The mean concentrations of Cr, Mn, Fe, and K in
most of the sampling stations (except for Mn concentration at St-4) were
exceeded the maximum permissible level (Table 1) indicating significant
pollutions and that water from these sites were not safe for domestic use
(Ali et al., 2016). Comparison of the results of the present work (Table 1)
with the guidelines for drinking water according to ECR (1997), WHO
(2004), WHO (2011), EU (1998), EPA (2001), and BIS (1991) demon­
strated that the concentrations of Pb, As, Cd, Ag, Ni, Co, Cu, Na, and Zn
were found to be below the permissible limit in almost all the studied
areas, except for Ni at St-1. The mean concentration of Mg was 121950.3
and 43480 µgL− 1 at St-1 and St-2, respectively, which were much higher
than the water quality standards. The concentration of K was signifi­
cantly higher at stations 1, 2, 3, and 6. However, Ca concentration was
only evident at St-3. The level of some essential metals such as Ca, Na, K,
Zn, Cu, and Mg indicated that the surface water in the studied areas was
dominated by Mg and Na type (Table 1). Copper and Zn were the least
dominant metals. The contributions of these metals are probably due to
the drainage from municipal and other anthropogenic activities around
the study area. It was demonstrated that elevated consumption of ionic
salts, mainly NaCl, may sometimes be very critical for hypertension,
stroke, asthma, renal stones, left ventricular hypertrophy, and osteo­
porosis (McCarty, 2004).
In Table 1 and Table S4, the analyzed parameters of the studied sites
are compared to previous literature studies. Elemental abundances of
Mn, Fe, and Co are significantly higher in the studied sites than those in
the water samples around the globe (Table 1). Whereas the metal con­
centrations in surface water from several parts of Bangladesh and some
Asian countries are compared comprehensively in Table S4. The study
will give a reasonable idea about surface water pollution in the Asian
region. Briefly, Pb content in the surface water of this study (22 ± 9 µg
L− 1) was comparable to some of the areas of Bangladesh. Only the sur­
face water from the Dhaka region showed exceptionally high Pb
 Md.A.B. Siddique et al.
Table 1
Analytical data of the measured parameters of water samples collected from different locations of the Chittagong region, Bangladesh.
Stations Sample ID pH EC ORP Turbidity Na Mg K Ca Cr Mn Fe Co Ni Cu Zn Ag Pb As Cd
1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1
µScm− mV NTU µgL− µgL− µgL− µgL− µgL− µgL− µgL− µgL− µgL− µgL− µgL− µgL− µgL− µgL− µgL−

St-1 W-01 7.06 1308 − 2.5 82 90,000 19,580 30,500 55,150 37 462 4881 <15 8 141 700 16.3 14.3 2.05 5
W-02 6.92 1396 2.2 1570 130,000 247,485 60,000 82,000 242 3055 15,795 61 222 650 1058 25.1 71.3 1.9 5.11
W-03 7.01 1367 − 2.5 1198 111,000 98,786 43,400 69,260 189 885 7879 77 163 243 888 19.3 45.7 2.29 6.23
Mean (n = 3) 7.00 1357 − 0.93 950 110,333 121,950 44,633 68,803 156 1467 9518 69 131 345 882 20.2 43.8 2.08 5.45
SD (1σ) 0.07 45 2.71 774 20,008 115,705 14,789 13,431 106 1391 5639 11.3 111 269 179 4.5 28.5 0.2 0.68
RSD (%) 1 3.3 − 290.7 81.5 18.1 94.9 33.1 19.5 68.2 94.8 59.2 16.4 84.4 78.1 20.3 22.3 65.2 9.5 12.5

St-2 W-04 6.83 1356 7.3 790 150,000 31,300 40,000 29,850 12 189 503 <15 <5 128 308 11.2 7.71 1.6 3.09
W-05 6.91 1496 2.6 530 145,000 41,800 16,500 29,550 45 258 11,045 <15 13 133 191 19.3 13.8 1.45 3
W-06 6.77 1917 10.9 1180 185,000 57,340 19,000 34,750 30 158 7085 <15 6 134 153 26.3 11.2 1.45 1.12
Mean (n = 3) 6.84 1590 6.93 833 160,000 43,480 25,167 31,383 29 202 6211 9.5 132 217 18.9 10.9 1.5 2.4
SD (1σ) 0.07 292 4.16 327 21,794 13,101 12,907 2919 16.5 51 5325 4.9 3 81 7.6 3.1 0.09 1.11
RSD (%) 1 18.4 60 39.3 13.6 30.1 51.3 9.3 57 25.4 85.7 52.1 2.4 37.2 40 28 5.8 46.3

St-3 W-07 7 2440 − 2.9 98 110,000 17,820 80,000 79,800 45 433 5020 <15 7 167 651 31.2 13.8 1.15 2
W-08 5.35 1968 96.5 430 100,000 26,780 120,000 91,450 55 604 12,860 <15 17 250 558 31.3 24.4 1.15 4.16
W-09 7.09 1632 − 7.9 107 70,000 13,700 65,000 147,800 63 692 3088 <15 20 221 954 26 24.3 3 4
Mean (n = 3) 6.48 2013 28.6 212 93,333 19,433 88,333 106,350 54.3 576 6989 14.7 213 721 29.5 20.8 1.77 3.39
SD (1σ) 0.98 406 58.9 189 20,817 6688 28,431 36,366 9 132 5175 6.8 42 207 3 6.1 1.07 1.2
RSD (%) 15.1 20.2 206.1 89.4 22.3 34.4 32.2 34.2 16.6 22.9 74 46.4 19.8 28.7 10.3 29.4 60.5 35.5

St-4 W-10 7.15 137 − 11.9 113 9000 6005 5500 12,950 29 73 582 <15 7 136 247 <10 <5 2.25 3.12
W-11 7.03 143 0.6 370 10,000 6275 5500 11,100 29 87 786 <15 <5 122 140 <10 <5 1.6 1.17
W-12 7.01 138 − 2.5 129 10,000 6720 5000 14,800 25 94 4290 <15 <5 120 167 <10 <5 1.9 2.19
W-13 7.02 138 − 1.4 117 8500 6240 6000 12,200 20 96 4460 <15 16 134 173 <10 <5 1.7 2
W-14 7.03 137 − 3.4 106 10,500 5315 5000 8300 25 72 3220 <15 <5 127 155 <10 <5 1.55 <1.00
7

Mean (n = 5) 7.05 139 − 3.72 167 9600 6111 5400 11,870 25.6 84.4 2668 11.5 128 176 1.8 2.12
SD (1σ) 0.06 2 4.81 114 822 515 418 2408 3.7 11.4 1874 6.4 7 41 0.29 0.8
RSD (%) 0.8 1.8 − 129.3 68.1 8.6 8.4 7.7 20.3 14.5 13.5 70.2 55.3 5.5 23.4 15.8 37.8

St-5 W-15 7.55 43.7 − 35.6 2.88 4500 1630 2400 6625 8 <50 278 <15 <5 126 309 <10 <5 1.4 2.15
W-16 7.5 42.3 − 30.5 2.53 4230 1428 2138 6793 7.16 <50 253 <15 <5 113 289 <10 <5 1.65 2.31

Environmental Nanotechnology, Monitoring & Management 16 (2021) 100524

W-17 7.58 43.8 − 37.8 2.96 3766 1693 2583 6689 8.87 <50 289 <15 <5 131 315 <10 <5 1.32 1.65
Mean (n = 3) 7.54 43.2 − 34.6 2.79 4165 1584 2374 6702 8.01 273 123 305 1.46 2.04
SD (1σ) 0.04 0.9 3.7 0.23 371 138 224 85 0.86 18 9 14 0.17 0.34
RSD (%) 0.5 2 − 10.8 8.2 8.9 8.7 9.4 1.3 10.7 6.7 7.5 4.5 11.8 16.9

St-6 W-18 6.98 931 − 1.4 59 65,000 13,825 24,000 56,850 57 654 4860 <15 7 151 560 12.1 12.8 2.7 1.03
W-19 7.01 993 − 3.2 49 60,000 11,970 26,500 48,400 49 543 3975 <15 16 143 497 15.1 13.8 2.6 1.17
W-20 7.03 997 − 3.3 58.7 63,500 13,215 25,230 49,325 68 689 4798 <15 12 156 523 13.7 15.4 2.88 1.53
Mean (n = 3) 7.01 974 − 2.63 55.6 62,833 13,003 25,243 51,525 58 629 4544 11.7 150 527 13.6 14 2.73 1.24
SD (1σ) 0.03 37 1.07 5.7 2566 945 1250 4635 9.5 76 494 4.5 7 32 1.5 1.3 0.14 0.26
RSD (%) 0.4 3.8 − 40.6 10.2 4.1 7.3 5 9 16.4 12.1 10.9 38.7 4.4 6 10.9 9.1 5.2 20.7

pH EC ORP Turbidity Na Mg K Ca Cr Mn Fe Co Ni Cu Zn Ag Pb As Cd
1 1 1 1 1 1 1 1 1 1 1 1 1 1 1 1
µScm− mV NTU µgL− µgL− µgL− µgL− µgL− µgL− µgL− µgL− µgL− µgL− µgL− µgL− µgL− µgL− µgL−

This work
Mean (n=20) 6.99 931 − 1.34 350 67,000 31,445 29,213 42,682 52.2 532 4797 69.0 39.5 176 442 20.6 22.4 1.88 2.74
SD (1σ) 0.44 774 26.5 468 58,339 55,987 31,358 37,378 59.4 703 4352 11.3 69.1 118 287 7.19 18.4 0.57 1.53
RSD (%) 6.3 83.1 1986 134 87 178 107 88 113.8 132 90.7 16.4 175 67.2 65.0 35.0 82.1 30.2 55.7
Median 7.015 995 − 2.50 110 64,250 13,458 21,500 32,300 33.5 433 4375 69.0 13.0 135 312 19.3 14.1 1.675 2.19
Min. 5.35 42.3 − 37.8 2.53 3766 1428 2138 6625 7.16 72.0 253 BDL BDL 113 140 BDL BDL 1.15 1.03
Max. 7.58 2440 96.5 1570 185,000 247,485 120,000 147,800 242 3055 15,795 77.0 222 650 1058 31.3 71.3 3 6.23

Literature Data
(continued on next page)
 Md.A.B. Siddique et al.
Table 1 (continued )
ECRa 6.5–8.5 10 200,000 30,000 12,000 75,000 50 100 300 100 1000 5000 20 50 50 5
WHOb 50 70 2000 10 10 3
EUc 250 50 50 200 20 2000 10 10 5
EPAd 6.5–9.5 2500 200,000 50 50 200 20 2000 10 10 5
BISe 6.5–8.5 50 100 300 50 1500 5000 50 50 10
Huaihe river, Chinaf 8.0 12,027 23.1 49.02 440.7 42.5 46.2 52.3 10,504 155 61.7
MKSTPR river, 7.62 10,160 3680 2610 11,060 24.9 233.8 2476 13.5 53.2 12.4 6.53 6.24
Bangladeshg
Halda river, Bangladeshh 30 160 10 410 100 350 30 40
Karnaphuli river, 7.89 78.2 13.3 28.9 8.55
Bangladeshi
Chittagong port, 5.30 8.30 9.0 20.3 5.50 2.60 2.30 0.006
Bangladeshj
Gomati river, Indiak 4.80 115 2028 1.99 7.0 7.34 16.9 4.29 2.25 0.96
Manchar lake, Pakistanl 8.14 5650 351,900 151,760 21,480 224,560 7.64 72.56 2960 38.94 34.96 18.9 730.4 82.42 80.8 5.30
Houjing river, Taiwanm 35 128 401 2 475 ND 2
Surface water, Chinan 8.46 225042.9 112942.9 87.1
Ground water, Vietnamo 4.80 1.0 3300 2.00
Surface water, Koreap 7.40 5645 1,076,000 129,000 49,500 56,000
8

Tap drinking water, Iranq 11.34 5014 30.38 21.0

Guayas River, Ecuadorr 7.70 200 9.8
Atoyac River, Mexicos 8.23 1020 12.6 146.8
Oum Er Rbia River, 8.13 1575 538.8
Morocco t
Nile river, Egyptu 7.83 699,250 57,730 20,690 11,530 38,410

Environmental Nanotechnology, Monitoring & Management 16 (2021) 100524

Drinking water, Nigeriav 5.92 50,771 9586 7332 44,160 329.3 162.8 136 91.48
Shahr Chai river, Iranw 8.45 311.2 63.5 11,183 10,917 1733 34,900 117

Parameters for EWQI

Standard data (Sj) 7.62g 250c 10 a 200000a 30,000 a
12,000 a 75,000 a
50 a 100 a 300 a 50x 100 a 1000 a 5000 a 20 a 50 a 50 a 5a
Information entropy (ej) 0.980 0.850 0.756 0.839 0.685 0.804 0.827 0.802 0.724 0.849 0.228 0.456 0.709 0.849 0.752 0.700 0.897 0.858
Entropy weight (ωj) 0.004 0.034 0.055 0.036 0.071 0.044 0.039 0.045 0.062 0.034 0.174 0.123 0.066 0.034 0.056 0.068 0.023 0.032
a
ECR: The Environment Conservation Rules, Bangladesh (1997); bWHO: World Health Organization (2004, 2011); cEU: European Union, (1998); dEPA: Environmental Protection Agency, Ireland (2001); eBIS: Bureau of
Indian Standards (1991); fWang et al. (2017); gMKSTRP: Meghna, Korokoya, Shitolokha, Teesta, Pasur & Rupsa river (Islam et al., 2020a); hBhuyan and Bakar (2017); iAli et al. (2016); jRaknuzzaman et al. (2016): polluted
coastal area of Bangladesh; kJigyasu et al. (2020); lKazi et al. (2009); mVu et al. (2017); nHe and Li (2020): surface water in the Middle Chinese Loess Plateau; oNguyen et al. (2020); pVenkatramanan et al. (2017); qFakhri
et al. (2018); rDamanik-Ambarita et al. (2016); sMartinez-Tavera et al. (2017); tBarakat et al. (2016); uEl-Sayed et al. (2020); vEgbueri et al. (2020); wZeinalzadeh and Rezaei (2017); xWHO: World Health Organization
(1993).
Md.A.B. Siddique et al. Environmental Nanotechnology, Monitoring & Management 16 (2021) 100524

concentration. Pakistan, China, Cambodia, South Korea, and Laos had

lower Pb content in the surface water than Bangladesh, while Srilanka
and Nepal had much higher Pb content in their surface water bodies.
This study found the most moderate amount of Cd concentration (3.0 ±
0.7 µg L− 1) than any other studies done from several areas of
Bangladesh. A survey from Cambodia found the minimum amount of Cd,
which is 300-fold less than our study. Except for Dhaka, Bangladesh, this
report revealed a higher Cr concentration (55 ± 24 µg L− 1) than all other
parts of the country. The Cr concentration of Bangladesh was higher
than all the Asian countries in the world (He and Li, 2020). Arsenic (As)
contamination is a widespread scenario in Bangladesh. This study
revealed the lowest amount of As than the other parts of the country but
higher than any other Asian country. The amount of Mn in the surface
water sample was comparable in almost every region of the country. All
the other Asian countries listed had much less Mn concentration in their
surface water than Bangladesh. Notably, Thailand had 1475-fold less Mn
than the water from Bangladesh. The surface water from Sylhet,
Bangladesh, contains 13.6-fold Fe than found in Chittagong. While there
was a fluctuation of Fe content in the surface water in several Asian
countries of the world. Cambodia and Pakistan contained a much higher
concentration of Fe than the other countries listed. The lowest Fe con­
tent was observed in India (9 ± 5 µg L− 1). The Co in surface water was
found in the case of only Cambodia and Bangladesh. Cambodia still
contained 30-fold less Co than Bangladesh. Nickel contamination was
much in Dhaka and Chittagong than in the rest of the studied Asian
countries. This study revealed that surface water in Bangladesh has at
least 13-fold more Ni content than China. Except for research from
Pakistan, all other Asian countries had much less Cu concentration than
that of Bangladesh. The lowest Cu concentration was found in Thailand
(0.5 ± 0.4 µg L− 1). Zn content was also found highest than any other
country. But the Zn concentration in our study was much higher than in
most of the Asian countries. Based on the above comparison, it is
alarming that almost all of the elements in the surface-water of
Bangladesh were found in much higher concentration than any other
Asian countries. It suggests that the contamination of surface water is
threatening in Bangladesh, and proper measures should be taken
immediately.
3.2. Spatial distribution of analyzed parameters
The results of one-way ANOVA (Table S5) of analytical data indicate
that all the measured parameters except for pH, ORP, Fe, and Cu showed
significant (p < 0.05) variations in their values with different sampling
points of the studied region (Ostertagová and Ostertag, 2013). Further,
the results of post-hoc multiple comparisons and effect size (r) (Table S6)
demonstrated that EC and K showed significant variations (p < 0.05,
larger r-value) in the concentration at stations 3, 4, and 5. In contrast,
Pb, Cd, Zn, and Na concentration varied significantly (p < 0.05, larger r-
value) at St-2, 4, 5 and 6. The level of Cr showed significant variations (p
< 0.05) at St-2 (r = 3.10), St-4 (r = 3.18), and St-5 (r = 3.61) while Co
and Ni showed their concentration variations over the whole studied
region (St-2 to 6). Among all metals, Na demonstrated the highest sig­
nificant variations in the concentration at St-5 (r = 7.74), while Mn
showed the lowest significant variations at St-5 (r = 2.61) concerning St-
1 indicating a highly fluctuating nature of these two associated param­
eters (Ostertagová and Ostertag, 2013). The significant differences or
variations in the concentrations of the concerned water quality param­
eters are probably due to the different types of contamination sources (e.
g., industrial activities, medical waste, anthropogenic activities, etc.)
associated with the sampling locations.
On the other hand, discriminated pattern of distribution of the
analyzed water quality parameters among the six sampling stations is
shown in Fig. 2. The pattern shows a clear clustering and separation of
the sampling stations as defined by the discriminant functions. Most of
the water quality parameters were generally available in all six stations
and these were employed for canonical discriminant analysis (CDA).
Fig. 2. Discrimination plot according to the analyzed parameters for the sur­
face water samples from Chittagong region, Bangladesh.
However, only eleven parameters (pH, EC, Cd, As, Ag, Fe, Zn, Na, Mg, K,
and Ca) have been identified which were responsible for the separation.
The sampling stations were categorized based on the concentrations of
the analyzed parameters of 100 % samples with cross-validated samples
of 95 % by 5 discriminant-functions as shown in Table S7 along with
affiliated statistical parameters. Function-1 (F-1) signifies 95.4 % of total
variance with a canonical correlation value of 1.0 providing the main
separation and the Function-2 (F-2) contributed 2.9 % of total variance
by second correlation of 0.998 (Table S7). Among the analyzed vari­
ables, EC and Zn showed 1st and 2nd highest discriminant function
coefficient and positive correlation values, respectively with F-1 indi­
cating the greater discriminating ability, whereas pH and Na lead to F-2.
Hence, according to the test of equality of group means in SPSS-output,
the order of potential for grouping is EC > Zn > pH > K > Na > Ca > As
> Ag > Fe > Mg > Cd (Table S7). The horizontal and vertical zero-line of
discrimination-plot creates a subdivision representing four clusters
corresponding to the hydrological feature of the sampling stations. In
Fig. 2, Chaktai canal (St-1) and KDS garments (St-6) constitutes one
domain, Halda river (St-4) and Goolpukur of Chittagong University (St-
5) comprised of another domain, whereas Karnaphuli river bridge (St-2)
and Chittagong Medical College (St-3) represent a single domain.
3.3. Source apportionment
The level of pollutant contamination and their probable sources were
identified by PCA. PCA extracted four controlling factors from the
analytical datasets of water quality parameters of surface water with
Eigenvalues > 1 (Fig. 3a). The scree plot (Fig. 3a) is commonly used to
identify the number of principal components (PCs) of the datasets
(Ahsan et al., 2019; Siddique et al., 2020) and sorted the Eigenvalues in
descending order as a function of the PC number. The observed factor
loadings and the percentage of cumulative and variance explained by
the factors are shown in Table S8. The initial data dimensions of the
samples are reduced by the factors without considerable loss of data and
about 89.17 % of the total variance is explained by whole factors.
The PC1 which accounted for 41.91 % of the total variance,
demonstrated the high and robust positive loadings of the factors mainly
due to Turbidity, Pb, Cr, Mn, Co, Ni, Cu, and Mg; and moderate positive
loadings of Cd, Fe, and Zn. The positive loading of Turbidity is attributed

9
Md.A.B. Siddique et al.
Fig. 3. (a) Principal component analysis of the analyzed water quality pa­
rameters by scree plot of the characteristic roots (eigenvalues), and component
plot in rotated space. (b) Dendrogram obtained by hierarchical clustering
analysis for measured water quality parameters.
to the massive amounts of colloidal solids, natural weathering, and
human activities in the study sites, whereas the aforementioned
elemental loadings are corroborated to the anthropogenic influences,
urban activities, and an increasing number of households as well as
industrial wastes in the studied areas. The PC2 explained 18.36 % of the
total variance, which represented respectively the strong positive and
negative loadings of ORP and pH, whereas moderate positive loadings of
Ag, Fe, and K indicating their common source of origin in the water. The
moderately favorable loading of Fe in both PC1 and PC2 revealed that Fe
was present also at the contamination source(s) in the studied areas in
addition to the anthropogenic contribution of Fe in surface water (Sid­
dique et al., 2020). PC3 accounted for 16.90 % of total variance with the
strong positive loadings of EC and Na, and moderate positive loading of
Ag. Strong positive loading of EC and Na on PC3 indicate anthropogenic
sources of pollutions, such as effluents of domestic origin, septic tanks,
application of fertilizers in agriculture (Chapagain et al., 2010; Islam
et al., 2017b). The PC4, explaining 12.00 % of the total variance, showed
a strong positive loading of As and moderate positive loadings of Zn, and
Ca. The mineral contents in the water body may tend to lead, under the
reduced condition, the processes of dissolution of geological formation
releasing As in water (Islam et al., 2019). Moderate positive loadings of
Zn and Ca in PC4 indicate the contribution of domestic wastewater as
10
Environmental Nanotechnology, Monitoring & Management 16 (2021) 100524
well as urban run-off that contaminated the water. The overall study of
PCA depicts that the water in the studied regions is mainly polluted from
anthropogenic activities of municipal, domestic, and industrial origin.
Based on the information derived from PCA, hierarchical cluster
analysis (CA) was employed to detect spatial similarities in the chemical
composition of water samples of different sources (Ahsan et al., 2019)
and to classify the analyzed water-quality parameters based on the
chemical similarities (Rahman and Gagnon, 2014; Wu et al., 2020). Two
main clusters can be differentiated in the dendrogram retained from the
CA employed on the parameters measured with Ward’s method and the
Euclidean distance as a measure of similarity (Fig. 3b). Cluster-1
included the elements, K, Ca, Na, and Mg, which were identified in
PCA as contaminants of anthropogenic origin. Cluster-2, which con­
tained Fe, Zn, EC, Turbidity, Cu, Mn, ORP, Co, Cr, Ni, Ag, Pb, pH, As, and
Cd are also generated from anthropogenic influence, including urban
activities, household sources, industrial wastes as well as chemical
weathering of some minerals containing metals. Overall, different
anthropogenic activities (e.g., domestic, industrial, agricultural, etc.)
and economic developments in the studied regions are mainly respon­
sible for various sources of elemental pollution (Li et al., 2011).
Pearson’s correlation matrices were utilized to identify the associa­
tions among analyzed parameters (Tamim et al., 2016), and the results
are presented in Table S9. The inter-parameter relationship empowers
the results found from PCA. Turbidity, Pb, Cr, Mn, Co, Ni, Cu, Mg, Cd, Fe,
and Zn which were loaded positively on PC1, also showed a significant
positive association in the correlation analysis. ORP, Ag, Fe, and K
loaded positively on PC2 showed a positive correlation among them but
showed a significant negative correlation with pH (loaded negatively on
PC2). No significant positive correlation between pH and any other trace
elements was observed. EC, Na, and Ag were significantly and positively
correlated and were loaded positively on PC3. Zn, As, and Ca were
showing positive loading on PC4, also showed a significant positive
correlation with each other. Moreover, Na, Mg, K, and Ca, which showed
similarities in cluster analysis (Cluster-1), also showed similar associa­
tion in the correlation analysis. The strong and significant correlations
among the parameters indicate their common sources of origin(s).
3.4. Water pollution and quality assessment
The water quality standard used in the water quality indices calcu­
lation is given in Table S10, and the results of PTEs evaluation indices
with mean concentrations of every station are shown in Table S11. To
evaluate the water-quality and to compare the pollution load in the
studied regions, pollution indices such as HPI, HEI, and CD were
determined separately for each sampling locations (Table S11). The HPI
was calculated using the ECR (1997) and WHO (2011) standards. The
HPI values in the selected areas were in the range of 1.43–159. The
highest value of HPI (159) was observed at St-1 (Chaktai canal), which
was the only value above the critical index limit, indicating the most
significant pollution loading due to industrial waste and domestic
sewage (Milivojevic et al., 2016). Index calculations revealed that HPI
values for all stations, except for St-1, were lower than the critical limit
(100) for drinking water (Prasad and Jaiprakas, 1999; Prasad and Bose,
2001). Moreover, the CD was utilized as a reference for determining the
metal pollution extent (Al-Ani et al., 1987). The ranges of CD values
were as 0.37–111.60, and except for St-5 (Goolpukur of CU), the CD
values for all the sampling stations are more than 3, which indicates that
water samples from those sampling stations are highly polluted
(Table S2; Edet and Offiong, 2002). Whereas, HEI values varied from
2.53 to 88.87, and according to HEI criteria (Table S2; Edet and Offiong,
2002), all the stations, except for St-5, exceeded the critical limit,
however, St-4 (Halda river) showed a moderate pollution level. The CD,
HEI, and HPI showed an almost similar pattern of changes in their values
in all the sampling points (Table S11).
However, estimated values of HEI and HPI associated with the water
quality of the analyzed samples are contradictory and differ
Md.A.B. Siddique et al.
significantly. Therefore, the criteria for pollution indices were normal­
ized using HEI (Edet and Offiong, 2002). Different approaches for HEI
values were developed for surface-water considering their associated
average concentrations, and a multiple of their mean values expresses
the different pollution levels in the water. The proposed HEI-criteria for
the surface-water samples are low (HEI < 10), medium (HEI = 10–20),
and high (HEI > 20). Existing schemes of water-quality for HPI and CD
were also modified according to the approaches of mean concentrations
as HEI, and obtained results are shown in Table S12. Hence, it was
evident that, among all the sampling points, St-5 (Goolpukur of CU)
showed a low level of pollution (Table S12), and St-4 (Halda river)
showed a moderate level of pollution. Considering HPI and CD, 5 sta­
tions (St-1, 2, 3, 4, and 6) were found to show a high level of pollution
(Table S12), which exceeded the critical limit of the proposed criteria
(Edet and Offiong, 2002).
The Pearson correlation matrix was performed to determine the
contribution of metals to the calculated indices (HPI, CD, and HEI),
which showed the associations among variables describing the overall
contribution of the obtained dataset (Table S13). For surface water, four
elements, Pb, Cr, Mn, and Cu showed significantly strong positive cor­
relations (p < 0.01) with all the indices. Iron possesses a strong positive
correlation with CD and HEI at a significant level of p < 0.01 and HPI (p
< 0.05). Cd, Ni, Zn, and Mg also showed a strong positive correlation
with CD (p < 0.05) and HEI (p < 0.05) and with HPI (p < 0.01). The
strong correlation of Pb, Cr, Mn, Cu, Fe, Cd, Ni, Zn, and Mg with the
pollution indices (Table S13) suggested that these elements are the
major parameters contributing significantly to the surface water pollu­
tion in the studied regions. HPI showed strong significant positive cor­
relations (p < 0.01) with CD and HEI; CD and HEI also showed a strong
(p < 0.01) correlation with each other. Results of HEI and the modified
category of CD and HPI are comparable; and the HEI method may be
utilized as a simple criterion for evaluating the surface water quality in
the study area. Hence, St-5 (Goolpukur of CU) may be considered as
uncontaminated, whereas station-1, 2, 3, 4, and 6 are moderate to highly
polluted by elemental contaminants.
To obtain a comprehensive evaluation of water-quality, contribu­
tions of all measured parameters (elements and physicochemical pa­
rameters) should be considered. In doing so, weightage-based WQI and
stochastic information-oriented statistics-based entropy water quality
index (EWQI) were used in this study. The calculated results of the WQI
using the concentrations of the measured physicochemical parameters
and chemical elements in water samples from contaminated and fresh
areas of Chittagong City are presented in Table S13. The WQI model can
be classified as shown in the supplementary Table S2. It can be seen that
all water samples of the studied regions have WQI ranged from 35 to 494
(Table S13) reflecting a “good” to “unsuitable” categories of water-
quality. The results showed different qualities of water samples at
different sampling sites and an unsuitable nature of a very large majority
of the samples. The minimum value of WQI was observed 35 for the
water sample W-17 (St-5: Goolpukur of CU) which was considered an
unpolluted station from all other stations. The maximum value of WQI
was found for the water sample W-02 (St-1: Chaktai canal). This might
be attributed to the fact that the anthropogenic inputs, surface run-off
from adjacent urban areas, upstream water flow, and storm water
drains may cause this abnormal distribution of WQI values as well as the
high stream water flow in this station.
Evaluation of water-quality based on WQI is the foremost such
attempt in different areas of Chittagong City. Therefore, the results of
this study can render as a baseline environmental data benchmark for
monitoring the build-up of physicochemical parameters and chemical
elements in the study areas. The baseline data generated in this inves­
tigation can empower the understanding regarding the water-quality
status of socio-economically important fluvial systems, and the factors
affecting the overall water quality.
The findings of this work can be compared with the comparable
previous works around the globe (Wang et al., 2017; Ramakrishnaiah
11
Environmental Nanotechnology, Monitoring & Management 16 (2021) 100524
et al., 2009; Bora and Goswami, 2016; Chakraborty et al., 2007) which
can eventually establish the usefulness of WQI. Wang et al. (2017)
conducted a study on Huaihe river, Anhui, China, and found that the
WQI showed a wide range of WQI values; varied from 9.40 to 2204.90
for water samples with varying depths (0–8 m), respectively. However,
groundwater quality of West Bengal, India in terms of WQI values
(range: 68–621) demonstrated ‘very poor’ and ‘water unsuitable for
drinking’ status for 26 % and 17 %, respectively of the analyzed samples
(Chakraborty et al., 2007). Water-quality needs to be protected by
implementing some effective measures like proper treatment of indus­
trial effluents before discharge, halting inflows of raw sewerage from the
household, preventing direct release from stormwater drains, and un­
abated dumping of solid waste to the ambient aquatic systems.
However, in WQI model calculation, usages of consensus-based
weightage of analyzed parameters may introduce less-acceptable un­
certainties. Thus, to get a justified water quality index relative to the
internationally recognized standards, entropy water quality index
(EWQI) is introduced which can identify the weight of every analyzed
parameter (Li et al., 2010) instead of introducing consensus-based
weightage. In explaining the water quality in terms of EWQI, esti­
mated values of information entropy (ej) and entropy weight (ωj) are two
vital parameters that are tabulated in Table 1. Analytical parameters
with larger ωj and minimal ej value possess the major impacts on general
water quality (Islam et al., 2020a; Gorgij et al., 2017). Depending upon
the ej and ωj values, the effects of analyzed parameters on the overall
water quality showed the following order: Co > Ni > Mg > Pb > Cu >
Mn > Ag > Turbidity > Cr > K > Ca > Fe > Zn > Na > EC > Cd > As in
the studied site. Therefore, Co, Ni, and Pb concentrations are mostly
degraded the water quality. Mean (n = 3 to 5) values of EWQI for each
sampling stations are 858 (St-1: Chaktai canal), 606 (St-2: Karnaphuli
river), 331 (St-3: Chittagong Medical College), 148 (St-4: Halda river),
22.9 (St-5: Goolpukur of CU) and 171 (St-6: KDS garments) with a
descending order of St-1 > St-2 > St-3 > St-6 > St-4 > St-5. According to
the EWQI ranking water samples from St-1, St-2, and St-3 are catego­
rized as ‘extremely poor’ whereas water samples from St-4 and St-6 are
categorized as ‘poor’ for drinking. Although all the studied surface water
samples from the port city of Chittagong are unsuitable for drinking,
only the water sample from St-5 (Goolpukur of CU) possesses an
‘excellent’ ranking for drinking.
3.5. Irrigation feasibility study
The rankings of irrigation water available for agricultural purposes
have significant impacts on crops and their yields. The potentiality of
sea-level rise (Ortiz, 1994) due to climate change may introduce an extra
load of salinity to the freshwater basins of the coastal and estuarine
zone, which invoke the study of irrigation water ranking. Irrigation
water with high salinity can alter the physical and chemical properties of
agricultural soil by the accumulation of excess Na+, which can affect the
crop’s quality and yields by (1) soil structure degradation followed by
reduction of water permeability and aeration of the soil, (2) excess Na+
toxicity in plant physiology, and (3) depleting K+ and Ca2+ in agricul­
tural fields (Rawat et al., 2018). In this study, irrigation indices such as
SAR, SSP, KR, MHR, TH, and TDS were used to evaluate the water
quality for irrigation. Sampling station-wise mean (n = 3 to 5) irrigation
indices with their uncertainties (standard deviations, 1σ) are plotted in
Fig. 4 with their associated rankings (by dotted lines).
SAR is a primary estimation of potential Na+ accumulation by agri­
cultural soil at the expense of K+, Mg2+, and Ca2+ as a consequence of
sodic-water usage for irrigation purposes. SAR values for all the sam­
pling stations were less than 10 (Fig. 4a) which indicates little or no
adverse effect on irrigation. However, SSP ranges from 33.9 (St-4) to
59.9 (St-2) which is positioned between ‘good’ to ‘doubtful’ region
(Fig. 4b) among which only St-2 (Karnaphuli river) is significantly
(considering the SD) ranked as ‘doubtful’ source of irrigation water.
Similarly, KR is more than 1 only for St-2 (Karnaphuli river water) which
Md.A.B. Siddique et al. Environmental Nanotechnology, Monitoring & Management 16 (2021) 100524

Fig. 4. Irrigation quality indices including (a) sodium adsorption ratio (SAR), (b) soluble sodium percentage (SSP), (c) Kelley’s ratio (KR), (d) magnesium hazard
ratio (MHR), (e) total hardness (TH), and (f) total dissolved solids (TDS) for the water samples collected from Chittagong region, Bangladesh.

is attributed to its direct interaction with the Bay of Bengal (Fig. 1). depicted in Fig. 5, the water samples from St-2 (Karnaphuli river bridge)
Further, the water classification by the United States Salinity Laboratory fall in the category of C3S4 of high salinity and very high alkalinity
(USSL) was introduced (Fig. 5) to evaluate the suitability of the water (SAR). Only one sample from St-3 (CMC) belongs to the C4S3 category
samples of the study area for irrigation purposes (Xiao et al., 2020). As representing water with very high salinity and high alkalinity while

Fig. 5. Water quality of the study area based on the sodium and salinity hazards of the analyzed samples for irrigation purposes.

12
Md.A.B. Siddique et al.
most of the water samples (St-1, 3, and 6) are partitioned in the zone of
C3S2 of high salinity and medium SAR showing their similar nature and
almost same types of pollution sources. Thus, the water samples from St-
1, 2, 3, and 6 are entirely unsuitable for irrigation use and proper
drainage systems are recommended to mitigate this issue. However, the
water samples collected from St-4 (Halda river) are found with a low
salinity and alkalinity (C1S1 category) indicating the most suitable na­
ture of water for irrigation. The water samples from St-5 (Goolpukur of
CU) are obtained free from salinity and alkalinity as expected.
Though Mg and Ca are associated with soil aggregation and fria­
bility, both of these alkaline earth metals are treated as the essential
nutrients for plants (Rawat et al., 2018). However, higher Mg and Ca
contents in irrigation water can raise the soil pH with a consequential
decrease in phosphorous availability (Al-Shammiri et al., 2005). Thus,
the excess concentration of Mg in irrigation water increases the soil
alkalinity and decreases the crop’s yield (Singh et al., 2013). Consid­
ering the uncertainties (SD: 1σ) from a repeated estimation of MHR, only
Karnaphuli river (St-2) is not recommended for irrigation. On the other
hand, water samples from all the studied sites are soft (Fig. 4e) and water
from St-4 (Halda river) and St-5 (Goolpukur of CU) possess the best
irrigation quality in terms of TDS (Fig. 4f).
3.6. Potential health risks evaluation
3.6.1. Non-carcinogenic health risks
Hazard index (HI) is used in this study to state the overall potential
health risks originated from elemental abundances in used water, which
is the sum of hazard quotients (HQs) estimated for all possible pathways
of elemental exposure. HQ and HI values for specific elements due to
ingestion and dermal contacts for adults and children are tabulated in
Table 2. Overall, the HI values for non-carcinogenic risks (for Cr and Co)
for both age groups exceeded the safe limits (> 1) for St-1 (Chaktai
canal), indicating that surface-water from this site possesses a clear
potential health risk. Chromium and Co were the main contributors to
the ingestion and dermal exposures, while the other trace elements of
this study were relatively less important. Industrial activities like elec­
troplating, metallic cleansing, dyeing processing, and cement
manufacturing are the significant sectors that play a pivotal role in
discharging Cr into the environment. At high concentrations, Cr is toxic,
mutagenic, carcinogenic, and teratogenic (Belay, 2010). Skin contact
with compounds containing Cr causes rashes and allergic contact
dermatitis (SCHER, 2015). On the other hand, Co can cause potential
non-carcinogenic risks to human health despite its low contents in water
owing to its very low reference dose (RfD) (Wang et al., 2017) over
which Co can be linked to allergic dermatitis and rhinitis (Fang et al.,
2014).
Element-specific predominant contributions on HI (> 10− 1) values
followed the order of Co > Cr > Mn > As > Cu > Pb, for both adults and
children, where HI of Co and Cr exceeded 1 which can cause severe
health risks to the residents. Although Mn is necessary for human health,
long-lasting exposure to a very high level of Mn in drinking water may
cause neurological disorder (WHO, 2011). The results showed that the
HI values of As for adult and child was also higher and the potential
pollutant in the water. Symptoms of chronic arsenicism, including
dermal lesions such as hypopigmentation and hyperpigmentation, skin
cancer, peripheral neuropathy, peripheral vascular disease, and bladder
& lung cancers were observed in populations ingesting arsenic-
contaminated drinking water (WHO, 2011).
However, estimation of such health risks consists of uncertainties
due to (1) potential dissimilarities of RfD values (recommended by
USEPA, 2004) to the population of Bangladesh, (2) variation of exposure
frequencies and ages, and (3) modification of risk elements by in­
teractions with physicochemical characteristics of aquatic media (Wu
et al., 2009). Therefore, this study presents a preliminary health risk
assessment, and more accurate evaluations for the trace metals should
be carried out.
13
Environmental Nanotechnology, Monitoring & Management 16 (2021) 100524
3.6.2. Carcinogenic health risk
Cadmium, Cr, and As are the toxic elements among the measured
elements that can cause carcinogenic risks (CR) which values are tabu­
lated in Table 2. CRingestion values of As (for both adults and children)
followed the decreasing order as St-6 (adults: 1.15 × 10− 4, children:
1.19 × 10− 4) > St-1 (adults: 8.75 × 10− 5, children: 9.10 × 10− 5) > St-4
(adults: 7.57 × 10− 5, children: 7.87 × 10− 5) > St-3 (adults: 7.43 × 10− 5,
children: 7.72 × 10− 5) > St-2 (adults: 6.31 × 10− 5, children: 6.56 ×
10− 5) > St-5 (adults: 6.12 × 10− 5, children: 6.37 × 10− 5). Similarly, the
CRdermal values of As followed by the identical trend. On the contrary,
the CRingestion values of Cr in surface-water for both adults and children
represented high cancer risk with the following order: St-1 > St-5 > St-6
> St-3 > St-2 > St-4. The CRingestion values of Cd (for both age groups)
followed the decreasing order as St-1 > St-3 > St-2 > St-4 > St-5 > St-6.
The results demonstrated that the CRingestion values of Cr were signifi­
cantly higher than those of Cd and As for adults and children. Moreover,
the CRingestion values of As were also larger compared to the CRdermal
values which are concomitant with those of previous studies (Gao et al.,
2019; Islam et al., 2017a, 2017b). These findings invoke that As can
cause detrimental risk to the local inhabitants via water intake. Lower
CRdermal values compared to the permissible limit (1 × 10− 6) implied
insignificant health risks of carcinogenicity through dermal exposure.
However, CRingestion values of Cr in all studied areas were greater than
the permissible limit (1 × 10− 6 to 1 × 10− 4) of cancer risk suggested by
the USEPA (2004), except for the control site (St-5: Goolpukur of CU).
Earlier studies (Jia et al., 2018; Xiao et al., 2019; He and Li, 2020; Kabir
et al., 2021) demonstrated that long-term exposure to elevated con­
centrations of Cr can cause adverse cancer risk in the human body. Thus,
the elevated concentrations of Cr in the studied sites may induce high
carcinogenic risk. Therefore, regular evaluations of the sampling areas
with higher hazard index values are suggested to avoid the accumula­
tion of Cr and other potentially toxic elements of this study that could
induce severe health problems.
4. Conclusions
In the present investigation, the value of EC, Fe, Pb, Mn, Cr, and Ni in
water samples were higher than the recommended values, which sug­
gests that the studied water bodies are contaminated by metals that
might cause adverse effects on these coastal riverine ecosystems in
Bangladesh and revealed that surface water from the studied sites is
unsuitable for drinking as well as domestic and industrial uses without
proper treatment. One-way ANOVA test followed by post-hoc multiple
comparisons test results revealed that EC, K, Pb, Cd, Zn, Na, Cr Ag, Mn,
Mg, Ca, Co, and Ni showed significant (p < 0.05) variations in their
concentrations due to the variation in sampling locations with different
pollution sources. Water pollution indices HPI, HEI, and CD showed
similar fashion of differences for all points and revealed that most of the
sampling points were highly polluted (except for Goolpukur of CU) due
to intensive industrial and municipal wastes. Furthermore, the water
quality index and entropy water quality index also identified the similar
pollution scenario of the studied sites. Multivariate statistical analysis
identified the water pollution sources, which could be attributed mostly
to anthropogenic activities exacerbated by climate change-induced sea-
level rise. Irrigation indices recommended that Karnaphuli river water is
unsuitable for agricultural purposes. The non-cancer risks related to
individual element exposure through water ingestion and dermal con­
tact pathways showed a low risk for both adults and children except for
Cr and Co which showed considerable risks. The carcinogenic risks from
Cd, Cr, and As at all sites were in acceptable ranges. But the concern is
that long-term exposure to these elements can pose cancer risks for both
adults and children. Therefore, it is recommended that a proactive
approach from the Bangladesh government will be required to evaluate
the role of potentially responsible parties (PRPs) for causing the rapid
rise in elemental contamination in the associated water bodies in
Bangladesh and also make new laws to stop the unregulated discharges
Md.A.B. Siddique et al. Environmental Nanotechnology, Monitoring & Management 16 (2021) 100524

Table 2
Non-carcinogenic risks based on hazard quotient (HQ) and hazard index (HI) of each analyzed element as well as carcinogenic risks for Cd, Cr, and As in the surface
water samples collected from the Chittagong region, Bangladesh.
St-1 St-2 St-3 St-4 St-5 St-6

Adult Child Adult Child Adult Child Adult Child Adult Child Adult Child

Non-carcinogenic risks indices

HQ
(ingestion)
Pb 1.08 × 1.12 × 2.69 × 2.80 × 5.14 × 5.34 × 3.45 × 3.59 ×
10− 1 10− 1 10− 2 10− 2 10− 2 10− 2 10− 2 10− 2
Cd 1.61 × 1.67 × 7.09 × 7.37 × 9.99 × 1.04 × 6.26 × 6.51 × 6.01 × 6.25 × 3.67 × 3.82 ×
10− 2 10− 2 10− 3 10− 3 10− 3 10− 2 10− 3 10− 3 10− 3 10− 3 10− 3 10− 3
Cr 5.83 × 6.06 × 1.08 × 1.13 × 2.03 × 2.11 × 9.57 × 9.95 × 2.99 × 3.11 × 2.17 × 2.25 ×
10− 2 10− 2 10− 2 10− 2 10− 2 10− 2 10− 3 10− 3 10− 3 10− 3 10− 2 10− 2
Mn 1.08 × 1.13 × 1.49 × 1.55 × 4.25 × 4.42 × 6.23 × 6.47 × 4.64 × 4.82 ×
10− 1 10− 1 10− 2 10− 2 10− 2 10− 2 10− 3 10− 3 10− 2 10− 2
Fe 5.62 × 5.84 × 3.67 × 3.81 × 4.12 × 4.29 × 1.57 × 1.64 × 1.61 × 1.68 × 2.68 × 2.79 ×
10− 3 10− 3 10− 3 10− 3 10− 3 10− 2 10− 3 10− 3 10− 4 10− 4 10− 3 10− 3
Co 1.36 1.41
Ni 7.73 × 8.04 × 5.61 × 5.83 × 8.65 × 9.00 × 6.79 × 7.06 × 6.88 × 7.16 ×
10− 3 10− 3 10− 4 10− 4 10− 4 10− 4 10− 4 10− 4 10− 4 10− 4
Cu 1.45 × 1.51 × 5.54 × 5.76 × 8.94 × 9.30 × 5.37 × 5.59 × 5.19 × 5.39 × 6.31 × 6.56 ×
10− 1 10− 1 10− 2 10− 1 10− 2 10− 2 10− 2 10− 2 10− 2 10− 2 10− 2 10− 2
Zn 1.73 × 1.80 × 4.27 × 4.44 × 1.42 × 1.47 × 3.47 × 3.61 × 5.99 × 6.23 × 1.04 × 1.08 ×
10− 2 10− 2 10− 3 10− 3 10− 2 10− 2 10− 3 10− 3 10− 3 10− 3 10− 2 10− 2
Ag 4.77 × 4.96 × 4.46 × 4.64 × 6.96 × 7.24 × 3.22 × 3.34 ×
10− 3 10− 3 10− 3 10− 3 10− 3 10− 3 10− 3 10− 3
As 1.94 × 2.02 × 1.40 × 1.46 × 1.65 × 1.72 × 1.68 × 1.75 × 1.36 × 1.42 × 2.55 × 2.65 ×
10− 1 10− 1 10− 1 10− 1 10− 1 10− 1 10− 1 10− 1 10− 1 10− 1 10− 1 10− 1

HQ (dermal)
Pb 1.60 × 3.30 × 4.00 × 8.22 × 7.64 × 1.57 × 5.14 × 1.06 ×
10− 2 10− 2 10− 3 10− 3 10− 3 10− 2 10− 3 10− 2
Cd 3.36 × 6.89 × 1.48 × 3.04 × 2.09 × 4.29 × 1.31 × 2.68 × 1.25 × 6.30 × 7.66 × 1.57 ×
10− 1 10− 2 10− 2 10− 2 10− 2 10− 2 10− 2 10− 2 10− 2 10− 3 10− 3 10− 2
Cr 9.61 × 1.97 1.79 × 3.67 × 3.35 × 6.88 × 1.58 × 3.24 × 4.93 × 1.01 × 3.57 × 7.34 ×
10− 1 10− 1 10− 1 10− 1 10− 1 10− 1 10− 1 10− 2 10− 1 10− 1 10− 1
Mn 2.35 × 4.84 × 3.24 × 6.65 × 9.25 × 1.90 × 1.35 × 2.78 × 1.01 × 2.07 ×
10− 1 10− 1 10− 2 10− 2 10− 2 10− 1 10− 2 10− 2 10− 1 10− 1
Fe 1.05 × 2.15 × 6.83 × 1.40 × 7.69 × 1.58 × 2.93 × 6.03 × 3.01 × 6.18 × 5.00 × 1.03 ×
10− 2 10− 2 10− 3 10− 2 10− 3 10− 2 10− 3 10− 3 10− 4 10− 4 10− 3 10− 2
Co 7.08 × 1.46
10− 1
Ni 1.01 × 2.07 × 7.32 × 1.50 × 1.13 × 2.32 × 8.86 × 1.82 × 8.98 × 1.85 ×
10− 1 10− 1 10− 3 10− 2 10− 2 10− 2 10− 3 10− 2 10− 3 10− 2
Cu 4.42 × 9.09 × 1.69 × 3.47 × 2.73 × 5.61 × 1.64 × 3.37 × 1.58 × 3.25 × 1.93 × 3.96 ×
10− 3 10− 3 10− 3 10− 3 10− 3 10− 3 10− 3 10− 3 10− 3 10− 3 10− 3 10− 3
Zn 1.36 × 2.79 × 3.34 × 6.87 × 1.11 × 2.28 × 2.72 × 5.58 × 4.69 × 9.64 × 8.11 × 1.67 ×
10− 3 10− 3 10− 4 10− 4 10− 3 10− 3 10− 4 10− 4 10− 4 10− 4 10− 4 10− 3
Ag 2.08 × 4.27 × 1.94 × 3.99 × 3.03 × 6.22 × 1.40 × 2.87 ×
10− 3 10− 3 10− 3 10− 3 10− 3 10− 3 10− 3 10− 3
As 1.12 × 2.31 × 8.11 × 1.67 × 9.55 × 1.96 × 9.73 × 2.00 × 7.87 × 1.62 × 1.47 × 3.03 ×
10− 3 10− 3 10− 4 10− 3 10− 4 10− 3 10− 4 10− 3 10− 4 10− 3 10− 3 10− 3

HI
Pb 1.24 × 1.45 × 3.09 × 8.22 × 5.90 × 1.57 × 3.97 × 1.06 ×
10− 1 10− 1 10− 2 10− 3 10− 2 10− 2 10− 2 10− 2
Cd 4.96 × 8.57 × 2.19 × 3.04 × 3.09 × 4.29 × 1.93 × 2.68 × 1.86 × 6.30 × 1.13 × 1.57 ×
10− 2 10− 1 10− 2 10− 2 10− 2 10− 2 10− 2 10− 2 10− 2 10− 3 10− 2 10− 2
Cr 1.02 2.04 1.89 × 3.67 × 3.55 × 6.88 × 1.67 × 3.24 × 5.23 × 1.01 × 3.79 × 7.34 ×
10− 1 10− 1 10− 1 10− 1 10− 1 10− 1 10− 2 10− 1 10− 1 10− 1
Mn 3.44 × 5.96 × 4.72 × 6.65 × 1.35 × 1.90 × 1.98 × 2.78 × 1.47 × 2.07 ×
10− 1 10− 1 10− 2 10− 2 10− 1 10− 1 10− 1 10− 2 10− 1 10− 1
Fe 1.61 × 2.74 × 1.05 × 1.40 × 1.18 × 1.58 × 4.51 × 6.03 × 4.62 × 6.18 × 7.68 × 1.03 ×
10− 2 10− 2 10− 2 10− 2 10− 2 10− 2 10− 3 10− 3 10− 4 10− 4 10− 3 10− 2
Co 2.07 2.87
Ni 1.09 × 2.15 × 7.88 × 1.50 × 1.22 × 2.32 × 9.53 × 1.82 × 9.67 × 1.85 ×
10− 1 10− 1 10− 3 10− 2 10− 2 10− 2 10− 3 10− 2 10− 3 10− 2
Cu 1.49 × 1.60 × 5.70 × 3.47 × 9.21 × 5.61 × 5.54 × 3.37 × 5.34 × 3.25 × 6.50 × 3.96 ×
10− 1 10− 1 10− 2 10− 3 10− 2 10− 3 10− 2 10− 3 10− 2 10− 3 10− 2 10− 3
Zn 1.87 × 2.08 × 4.61 × 6.87 × 1.53 × 2.28 × 3.74 × 5.58 × 6.46 × 9.64 × 1.12 × 1.67 ×
10− 2 10− 2 10− 3 10− 4 10− 2 10− 3 10− 3 10− 4 10− 3 10− 4 10− 2 10− 3
Ag 6.85 × 9.23 × 6.40 × 3.99 × 9.99 × 6.22 × 4.61 × 2.87 ×
10− 3 10− 3 10− 3 10− 3 10− 3 10− 3 10− 3 10− 3
As 1.95 × 2.04 × 1.41 × 1.67 × 1.66 × 1.96 × 1.69 × 2.00 × 1.37 × 1.62 × 2.56 × 3.03 ×
10− 1 10− 1 10− 1 10− 3 10− 1 10− 3 10− 1 10− 3 10− 1 10− 3 10− 1 10− 3

(continued on next page)

14
Md.A.B. Siddique et al. Environmental Nanotechnology, Monitoring & Management 16 (2021) 100524

Table 2 (continued )
St-1 St-2 St-3 St-4 St-5 St-6

Adult Child Adult Child Adult Child Adult Child Adult Child Adult Child

Carcinogenic risks indices

HQ
(ingestion)
Cd 3.05 × 3.18 × 1.35 × 1.40 × 1.90 × 1.97 × 1.19 × 1.24 × 1.14 × 1.19 × 6.97 × 7.25 ×
10− 6 10− 6 10− 6 10− 6 10− 6 10− 6 10− 6 10− 6 10− 6 10− 6 10− 7 10− 7
Cr 7.17 × 7.46 × 1.33 × 1.39 × 2.50 × 2.60 × 1.18 × 1.22 × 3.68 × 3.83 × 2.67 × 2.77 ×
10− 3 10− 3 10− 3 10− 3 10− 3 10− 3 10− 3 10− 3 10− 4 10− 4 10− 3 10− 3
As 8.75 × 9.10 × 6.31 × 6.56 × 7.43 × 7.72 × 7.57 × 7.87 × 6.12 × 6.37 × 1.15 × 1.19 ×
10− 5 10− 5 10− 5 10− 5 10− 5 10− 5 10− 5 10− 5 10− 5 10− 5 10− 4 10− 4

HQ (dermal)
As 1.17 × 2.41 × 8.46 × 1.74 × 9.96 × 2.05 × 1.01 × 2.08 × 8.21 × 1.69 × 1.54 × 3.16 ×
10− 6 10− 6 10− 7 10− 6 10− 7 10− 6 10− 6 10− 6 10− 7 10− 6 10− 6 10− 6

of contaminants in the coastal riverine ecosystems in Bangladesh. Be­
sides, the information obtained from the present study could be useful
for environmental agencies to monitor aquatic systems and for the
management of human health practices, and also in evaluating legacy
environmental insurance claims.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgments
The authors are grateful to the Institute of National Analytical
Research and Service (INARS), Bangladesh Council of Scientific and
Industrial Research (BCSIR), Dhaka, Bangladesh for providing labora­
tory facilities and other logistic support during the research period. We
are also grateful to the staff of the analytical chemistry laboratory at
INARS for the laboratory assistance.
Appendix A. Supplementary material
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.enmm.2021.100524.
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