Environ Geochem Health (2023) 45:3465–3486

https://doi.org/10.1007/s10653-022-01421-7

ORIGINAL PAPER

Application of Monte Carlo simulation

for carcinogenic and non‑carcinogenic risks assessment
through multi‑exposure pathways of heavy metals of river
water and sediment, India
Suyog Gupta · Sunil Kumar Gupta

Received: 24 August 2022 / Accepted: 14 October 2022 / Published online: 8 November 2022
© The Author(s), under exclusive licence to Springer Nature B.V. 2022, corrected publication 2023

Abstract Heavy metal contamination has severe of water (8.10E-04, 2.36E-04) for adults and children,
detrimental impacts on the entire river ecosystem’s respectively. The analysis of non-carcinogenic risk
quality and causes potential risks to human health. revealed a significantly higher overall hazard index
An integrated approach comprising deterministic and (OHI) for both sediment (adults: 1.26E+02, children:
probabilistic (Monte Carlo simulation) models with 1.11E+03) and water (adults: 3.26E+00, children:
sensitivity analysis was adopted to determine heavy 9.85E+00) than the USEPA guidelines (OHI ≤ 1).
metals’ chronic daily intake (CDI) and their associ- The sensitivity analysis identified that the concentra-
ated health risks from the riverine ecosystem. Both tion of heavy metals was the most influencing input
carcinogenic and non-carcinogenic risks of water factor in health risk assessment. Based on the reason-
and sediment were estimated through multi-exposure able maximum exposure estimate (RME), the study
pathways. The analytical results indicated that the will be advantageous for researchers, scientists, poli-
concentration patterns of heavy metals in sediment cymakers, and regulatory authorities to predict and
(Fe > Mn > Sr > Zn > Cr > Cu > Cd) were slightly dif- manage human health risks.
ferent and higher than in water (Fe > Zn > Cr > Sr > M
n > Cu > Cd). The potential carcinogenic risks of Cr Keywords Monte Carlo simulation · Carcinogenic ·
and Cd in sediment (5.06E-02, 5.98E-04) were sig- Heavy metal · River · Water · Sediment
nificantly (p < 0.05) higher than in water (9.08E-04,
8.97E-05). Moreover, 95th percentile values of total
cancer risk (TCR) for sediment (1.80E-02, 3.37E- Introduction
02) were about 22 and 143 times higher than those
Rivers have ecological and socio-economic impor-
tance for both developed and developing countries.
Supplementary Information The online version These are the prime freshwater source for drink-
contains supplementary material available at https://​doi.​
org/​10.​1007/​s10653-​022-​01421-7.
ing, bathing, irrigation, fish farming, and industrial
activities (Singh & Kumar, 2017; Xiao et al., 2019).
S. Gupta · S. K. Gupta (*) Numerous geogenic and anthropogenic actions dis-
Department of Environmental Science and Engineering, rupt the health of rivers. The main contributors
Indian Institute of Technology (Indian School of Mines),
to the river contamination comprise heavy metals
Dhanbad, Jharkhand 826004, India
e-mail: [email protected] and organic compounds. Among various contami-
nants, heavy metals get a special prominence (Ali
S. Gupta
e-mail: [email protected] et al., 2022; Desai et al., 2021; Joseph et al., 2019;

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 3466 Environ Geochem Health (2023) 45:3465–3486

Khan & Rai, 2022; Man et al., 2020; Ngeve et al., Tana River, Kenya, using multivariate statistical
2015; Ustaoğlu, 2021). Weathering and disintegra- analysis and water quality index method. They found
tion of metal rocks and ores can also release heavy that 26.3% locations recorded HQ > 1 due to high
metals into the river water and sediment (Kumar Mn contamination and also revealed that the children
et al., 2020; Mukherjee et al., 2020). Moreover, rapid were more prone to non-carcinogenic health risks
urbanization, industrialization, mining activities, and than the adults. Ceballos et al. (2021) appraised the
economic growth are the significant causes of heavy human health risk due to the Cr and N ­ O3 contamina-
metals and other hazardous materials in river water tion in the soil and groundwater within the Matanza-
and sediment, leading to ecological and human health Riachuelo River Basin, Argentina. They recognized
hazards (Bonnail et al., 2019; Jiang et al., 2021a; Man the unacceptable carcinogenic and non-carcinogenic
et al., 2021; Xu et al., 2019; Yuan et al., 2021). risks of Cr on both children and adults exposed to
Due to the non-degradability of heavy metals, groundwater and soil via ingestion and dermal con-
they adversely affect humans, animals, and plants tact; however, the non-carcinogenic risk of ­NO3 was
(Kumar et al., 2020; Okereafor et al., 2020). Heavy acceptable. Kumar et al. (2020) reviewed the disper-
metals impair the immune system and cause severe sal and causes of ecological health risks of heavy
carcinogenic and non-carcinogenic diseases (Qiao metals in sediment from India (1979–2017) and found
et al., 2020; Seleem et al., 2021). They accumulate in that mean values of heavy metals (Cr, Cu, Co, Zn, Pb,
human body tissues through adsorption and biomag- As) in Indian sediment were high from the Austral-
nification via direct ingestion, dermal contacts, and ian Interim Sediment Quality Guidelines, World Sur-
inhalation (Mukherjee et al., 2020; Singh & Kumar, face Rock Average, and Threshold Effect Level for
2017). However, the population’s exposure to heavy freshwater ecosystems. Moreover, they also exposed
metals like Cd, Cr, Cu, and Sr is undesirable in the the high carcinogenic risk to the adults and children
river ecosystem due to their adverse effects on the because of the elevated concentration of Cr, As, and
gastrointestinal tracts, kidneys, and nervous system Cd through sediment contaminated food and water.
(Qiao et al., 2020; Singh & Kumar, 2017). Although Accordingly, specific emphasis should be given to the
some heavy metals (e.g., Fe, Mn, and Zn) are required heavy metal-associated health risks in river water and
for humans, the higher concentration (more than sediment.
desirable limits) of Fe produces stomach ache, nau- The previous studies (Ceballos et al., 2021; Gafur
sea, vomiting, heart failure, and fatal damage to the et al., 2019; Mokarram et al., 2020; Kumar et al., 2020;
brain (Rodríguez & Mandalunis, 2018; Seleem et al., Njuguna et al., 2020; Shil & Singh, 2019; Ucun Ozel
2021; Singh & Kumar, 2017), and the symptoms of et al., 2020; Whitehead et al., 2019) were focused on
Mn poisoning are the weak muscles, insomnia, and the health risk assessment mainly by addressing the
parkinsonian syndromes (Okereafor et al., 2020). heavy metal contamination in river water, whereas the
However, Zn poisoning causes cardiovascular, res- studies on exposure assessment in sediment and its
piratory, renal, and hepatobiliary failure (Rodríguez effects on human health are scarce (Ali et al., 2022;
& Mandalunis, 2018). Kumar et al., 2020). Moreover, the health risk assess-
Over the past years, numerous studies have ments relied only on the deterministic approach
been carried out to address the water quality prob- (USEPA, 2011) based on single-point value estimation
lems, heavy metal contamination, and its associ- without considering the uncertainties in the param-
ated impacts on human health (Kumar et al., 2020; eter selection and hazard identification approach (Jiang
Njuguna et al., 2020; Wu et al., 2021). Shil and Singh et al., 2021b; Mukherjee et al., 2020; Rajasekhar et al.,
(2019) investigated the impacts of dissolved heavy 2018). In India, rivers and their tributaries are the major
metals and metalloids in the water of Mahananda source of water for domestic and agricultural activities.
River, India, on human health. They revealed that the However, several industries discharge their untreated
accumulative effect of the heavy metals and metal- effluents directly into rivers (Kumar et al., 2020). Addi-
loids was higher than their guidelines at some sam- tionally, the imperative aspects of heavy metal contami-
pling locations, which impacted both carcinogenic nation and their toxic impacts on human health were
and non-carcinogenic effects on the adults and chil- rarely addressed for the rivers flowing through the coal
dren. Njuguna et al. (2020) explored health risks in mining regions. Therefore, a comprehensive study was

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required for heavy metal-associated human health risks rain-fed river originated from the Khamerpet hill
in river water and sediment considering uncertainties. (elevation: 1068 m), Chota Nagpur Plateau in the
Hence, the tropical rain-fed river Damodar, India, was Palamau district of Jharkhand, India (Verma et al.,
selected for this study, which is a major source of water 2019). Damodar River basin (DRB) is a sub-basin
for domestic and agricultural activities in Jharkhand of the Ganga River basin and covers 11.8% and 8.6%
and West Bengal (Ambade et al., 2021; Gupta & Gupta, of the total geographic area of the Jharkhand and
2021). Based on the 2011 census, the estimated popula- West Bengal, respectively. DRB is the repository of
tion of the study region is over 14,69,000 (Pal & Maiti, about 46% of the Indian coal assets (Gupta & Gupta,
2018). In recent years, this river has witnessed exten- 2021; Verma et al., 2019). The river is approximately
sive contamination due to both regulated and unregu- 541 km long and flows through three major geologi-
lated discharge from coal washeries and several other cal features: granites and the Gondwana tract, viz.
industries like steel and coke industries (Ambade et al., gneisses of the Archaean Age. Finally, the river enters
2021; Verma et al., 2019). West Bengal and meets the Hooghly River near Kol-
In the present study, an integrated approach was kata (Verma et al., 2019). DRB is a coal rich region
applied to explore the heavy metal exposure and its and the experiences hot summers (~ 48 °C) and very
associated health risk in river water and sediment. In mild winters. The average annual rainfall and wind
this approach, the United States Environmental Pro- speed were around 1350 mm and 5 km/h, respec-
tection Agency (USEPA) recommended deterministic tively. More than 80% of the total rainfall occurs in
and Monte Carlo simulation (MCS)-based probabil- monsoon from June to September (Bandyopadhyay
istic health risk models associated with sensitivity et al., 2021, Ghosh et al., 2022; Gupta & Gupta,
analysis were used to achieve a higher degree of accu- 2021). The overall slope of DRB is towards southeast,
racy in the health risk assessment. The application of which varies from > 70° (upper catchment) to < 2°
MCS technique has been proved as the most prom- (lower catchment) (Ghosh et al., 2022).
ising technique for probabilistic uncertainty and risk
investigations in prior studies (Keramati et al., 2018; Sample collection and analytical procedure
Lin et al., 2020; Pham et al., 2019; Rajasekhar et al.,
2018; Tong et al., 2018). However, Seifi et al. (2020) Total 120 samples including water (60 samples) and
also applied Monte Carlo method for evaluating the sediment (60 samples) were collected from ten repre-
groundwater quality at Kerman province plain, Iran. sentative sampling locations along the Damodar River
They concluded that this method was efficient to twice during summer season (March to April, 2022).
identify the uncertainties in the water quality index Triplicate samples for both water and sediment were
evaluation and increased the water quality assess- collected at each location from ¼, ½, ¾ across the
ment’s consistency. The main objectives of this study river width. The water samples were collected from
were to (a) determine the concentration of heavy met- a depth of 30 cm in pre-washed 1 L polypropylene
als (Cd, Cr, Cu, Fe, Mn, Sr, and Zn) in the Damodar bottles. To maintain homogeneity, the water samples
River water and sediment, (b) assess the carcinogenic collected along the width were thoroughly mixed, of
and non-carcinogenic health risks to children and which three replicates (100 mL each) were analyzed
adult populations using both deterministic and proba- and the average values were reported. The collected
bilistic models, and (c) determine the need of reme- samples were filtered through Whatman grade 42
diation techniques for risk management. filter papers to eliminate the undissolved impurities
and acidified (pH < 2) with ultrapure ­ HNO3 (65%,
AR grade, Thermo Fisher Scientific, USA) to pre-
Materials and methods serve the metals in samples and avoid their chemical
alterations, i.e., adsorption and precipitation (APHA,
Description of study area 2017). Samples were cautiously sealed, labeled, and
transported to the laboratory within 24 h for preserva-
Damodar River is located at 26°45′30.48″ N and tion at 4 °C to avoid chemical vacillations.
24°57′29.2″ N latitude and 87°48′17.79″ E and The river sediment samples were collected from
88°26′0.73″ E longitude (Fig. 1). It is a shallow the depth of 0–10 cm using the grab sampler and

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Fig. 1  Map layout of study area and sampling locations

deposited in labelled polyethylene bags of 500 gm reagents (Thermo Fisher Scientific, USA) were used to
capacity. In laboratory, the sediment samples were obtain high accuracy and precision in the analytical pro-
dried in the hot air oven at 105 °C and sieved through cedures. Moreover, reagent blanks, sample triplicates,
a 70-µm sieve. 0.5 gm of the sieved sample was occu- and reiterating experiments were performed to confirm
pied in a Teflon beaker and mixed with HF: ­HNO3 in quality control. Triplicate analyses of standard material
1:2 proportion. The solution was heated till dry, and measured accuracy. The instruments were recalibrated
then 3 ml aqua-regia was added and again heated when the relative percent difference transcended ± 5%.
till everything dissolved. The last step was repeated The limit of detection (LOD) and limit of quantifica-
multiple times to obtain a clear solution. After cool- tion (LOQ) of the target heavy metals were 0.001 mg/L
ing, the solution was filtered and diluted to 50 ml and 0.003 mg/L for Cd, Cr, Cu, Mn, and Zn, while it
with 1% (v/v) ­HNO3 (Raj & Maiti, 2020; Shahbazi was 0.002 mg/L and 0.006 mg/L for Fe, and Sr, respec-
& Beheshti, 2019). The heavy metals in both types tively. In this study, the method for water analysis was
(water and sediment) of river samples were analyzed standardized using NIST 1640a (National Institute of
using Inductively Coupled Plasma-Optical Emission Standards and Technology (NIST), USA) certified ref-
Spectroscopy (ICP-OES; Thermo Fisher Scientific, erence material (CRM). Moreover, the analytical results
USA). of sediment were also verified using MESS-4 (National
Research Council (NRC), Canada) CRM. In order to
Quality control and quality assurance evaluate the analytical accuracy and precision, % recov-
ery of each meatal was estimated by comparing the
To avoid sample contamination and obtain reliable certified and experimental values of CRM. The heavy
data, utmost care was taken during the sample collec- metal recovery percentages with certified reference
tion, preservation and analysis. The analytical grade

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material were in the range of 93.10–102.18% for water n √(

∑ ( i i
)2 ( i i
)2 )
and 97.58–103.57% in the case of sediment (Table S1). TRI = TRIi = CM ∕CTEC + CM ∕CPEC ∕2
i=1
(6)
Statistical analysis
where CM: heavy metal concentration (mg/kg), BM:
background concentration of the heavy metal (mg/
Standard statistical analytics like mean, standard devia-
kg), CRef: concentration of the reference heavy metal
tion, and range were evaluated to describe the heavy
(Fe) (mg/kg), BRef: background concentration of the
metal concentration in water and sediment. The sig-
reference heavy metal (mg/kg), PI: single factor con-
nificant difference between the heavy metal-associated
taminant index (CM/BM) of each target heavy metal,
risks to children and adults through water and sediment
CTEC: threshold effect concentration of the heavy
was analyzed using the t test with 95% confidence lev-
metal (mg/kg), and CPEC: probable effect concentra-
els (Khan et al., 2016). All the statistical analyses were
tion of the heavy metal (mg/kg), n: number of target
accomplished using RStudio integrated development
heavy metals. The background concentration (Taylor
environment (version 2022.07.2-576) for R.
& McLennan, 1985; Turekian & Wedepohl, 1961),
PEC, and TEC values (MacDonald et al., 2000) of
Heavy metal contamination in river ecosystem
heavy metals are given in Tables S2–S3, whereas the
categories of individual and combined heavy metal
In this study, heavy metal contamination in river eco-
contamination are also described in Tables S4–S8.
system was characterized by estimating the geo-accu-
mulation index (Igeo) (Ergin et al., 1991; Muller, 1969),
contamination factor (CF) (Hakanson, 1980; Ahmed Human health risks assessment
et al., 2016), enrichment factor (EF) (Ergin et al., 1991;
Kumar et al., 2020; Zeng et al., 2019), pollutant load Due to physiological and behavioral variances in
index (PLI) (Mandour et al., 2021; Tomlinson et al., the population of diverse age groups, the populaces
1980), metal pollution index (MPI) (Sedeño-Díaz et al., of the study region were separated into two groups,
2019; Singovszka et al., 2017), and toxic risk index i.e., children (1–10 years) and adults (21–70 years)
(TRI) (Zhang et al., 2016). The Igeo (Eq. 1), CF (Eq. 2), (Rajasekhar et al., 2018). Considering these two pop-
and EF (Eq. 3) indicators allowed the assessment of ulation groups enables a clear vision of risk assess-
single element contamination, whereas PLI (Eq. 4), ment differences. The USEPA deterministic (USEPA,
TRI (Eq. 5), and MPI (Eq. 6) determined an integrated 2011) and MCS-based probabilistic models were
assessment of all target heavy metal contamination. adopted to assess the carcinogenic and non-carcino-
genic health risks through direct ingestion and dermal
(1)
( )
Igeo = log2 CM ∕1.5BM absorption exposure pathways for each population
group.
CF = CM ∕BM (2)
Exposure assessment
(3)
( ) ( )
EF = CM ∕CRef ∕ BM ∕BRef
The chronic daily intake (CDI) for each target heavy
metal through direct ingestion ­(CDIIng) and dermal
(4) absorption ­(CDIDer) pathways was evaluated using
√
n
PLI = PI1 PI2 … PIn
Eqs. (7–9) (Gao et al., 2022; Kumar et al., 2020).
(5)
√
n
MPI = CM1 CM 2 … … CMn ( )
CDIIng = CM × IR × EF × ED ∕(BW × AT) (7)

(8)
( )
For water ∶ CDIDer = CM × Kp × SA × Te × EF × ED × Fc ∕(BW × AT)

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(9)
( )
For sediment ∶ CDIDer = CM × Af × SA × Fabs × EF × ED × Fc ∕(BW × AT)

(10)
[( ) ( )]
where CM: heavy metal concentration (mg/L or mg/ CR = CDIIng × SFIng + CDIDer × SFDer
kg), IR: ingestion rate (L/day or g/day), Te: exposure
where CR: cancer risks, ­ SFIng: slope factor for
time (hours/day), EF: exposure frequency (days/year),
ingestion, and ­SFDer: slope factor for dermal expo-
BW: body weight of the human (kg), AT: average
sure of target heavy metal. S ­FIng and S­FDer were
exposure time (days), ED: exposure duration (years),
adopted from USEPA (2021) and Mukherjee et al.
SA: exposed skin area (­cm2), Fc: conversion factor,
(2020). The CR values > 1.00E-06 were consid-
Kp: dermal permeability coefficient (cm/hour), Fabs:
ered for potential carcinogenic health risk (USEPA,
absorption factor, and Af: sediment to skin adherence
2011). The brief classification of CR values could
factor (mg/cm2) as illustrated in Table 1.
be described as: very low risk (CR ≤ 1.00E-06),
low risk (1.00E-06 < CR ≤ 1.00E-04), moderate
Carcinogenic health hazards assessment
risk (1.00E-04 < CR ≤ 1.00E-03), high risk (1.00E-
03 < CR ≤ 1.00E-01), and very high risk (CR > 1.00E-
Exposure to heavy metal contaminated water and sed-
01) (Mukherjee et al., 2020). The total carcinogenic
iment may lead the carcinogenic impacts on human
health risk (TCR) was calculated using Eq. (11).
beings. Among the seven target heavy metals, Cd
and Cr were classified as human carcinogens by the n
∑
International Agency for Research on Cancer (Bal- TCR = CR (11)
ali-Mood et al., 2021). Therefore, the carcinogenic i=1

risks of these two metals for both population groups

(children and adults) were determined through vari-
Non‑carcinogenic health risk assessment
ous exposure pathways. The carcinogenic health risk
associated with target heavy metals of carcinogenic
The method prescribed by USEPA (USEPA, 2011)
nature was evaluated using Eq. (10).
was used to estimate human health hazards in water

Table 1  Input parameters for exposure assessment

Parameter Symbol Unit Value for water samples Value for sediment References
samples
Children Adults Children Adults
* **
Heavy metal concentra- CM mg/L mg/kg Measured values Measured values Present study
tion
Body weight BW kg 15 70 15 70 USEPA (2011); Kumar
et al. (2020)
Ingestion rate IR L/day* g/day** 0.78 2.50 0.20 0.10 USEPA (2011); Kumar
et al. (2020)
Exposure frequency EF day/year 365 365 365 365 USEPA (2011)
Exposure duration ED year 6 30 6 30 USEPA (2011)
Average time AT*** days 2190 10,950 2190 10,950 USEPA (2011)
Exposed skin area SA cm2 12,000 16,600 12,000 16,600 USEPA (2011), Pazhu-
parambil Jayarajan
and Kuriachan (2021)
Sediment to skin adher- AF mg/cm2 – – 0.2 0.7 Kumar et al. (2020)
ence factor
Absorption factor Fabs – – – 0.001 0.01 Kumar et al. (2020)
* ** ***
Unit for water, unit for sediment, AT for carcinogenic health risk: 25,550 days for both adults and children

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and sediment. The health hazards of heavy metals minimum, maximum, and mean values. A range of
were evaluated using Eq. (12). output risk values was obtained instead of point val-
ues by considering the 10,000 iterations with the
(12)
[( ) ( )]
HQ = CDIIng ∕RfDIng + CDIDer ∕RfDDer assurance of numerical stability (Rajasekhar et al.,
2018). It helped to explain the influences of uncer-
where HQ: hazard quotient, R ­ fDIng: oral toxicity ref-
tainty on the performance of risk assessment pro-
erence dose (mg/kg/day), and R ­ fDDer: dermal toxic-
cesses. Moreover, an advanced sensitivity analysis
ity reference dose (mg/kg/day). Both reference doses
was also applied using spider graphs to identify the
for each heavy metal were obtained from USEPA
most influencing heavy metals causing significant
(2011) and Mukherjee et al. (2020). HQ ≤ 1 indicated
risk in the overall risk assessment process (Lu et al.,
the non-occurrence of the detrimental human health
2019). However, the reasonable maximum exposure
effects due to exposure of target heavy metal, whereas
(RME) estimates of risks were assessed and com-
potential non-carcinogenic effects were occurred
pared with USEPA (2011) guidelines for the execu-
when HQ > 1. The assessment of non-carcinogenic
tion of risk management practices. The RME esti-
health hazard risk was intended based on the overall
mates that exceeded the recommended safety risks
hazard index (OHI) method Eq. (13) (Sawut et al.,
suggested the necessity of risk management in the
2018).
contaminated region.
n
∑
OHI = HQi (13)
i=1
Results and discussion
The required values of exposure parameters for
carcinogenic and non-carcinogenic heavy metals are Assessment of heavy metals in water
given in Table 2.
The concentration of heavy metals varied along the
river and was found to be in the order of Fe > Zn > C
Probabilistic risk analysis and risk management
r > Sr > Mn > Cu > Cd (Fig. 2a). However, concentra-
tion of all target heavy metals was within the permis-
Due to point values estimation of risk to the popula-
sible limits (Table S9) except in the case of Cd, Cr,
tion, the health risk assessments are typically asso-
and Fe, where they exceeded their acceptable limits
ciated with uncertainties (Ali et al., 2022; Mukher-
of 0.003 mg/L, 0.05 mg/L, and 0.3 mg/L, respectively
jee et al., 2020; Shil & Singh, 2019). Monte Carlo
(BIS, 2012; Moghal et al., 2019). The higher concentra-
simulation (MCS), a probabilistic technique, was
tion of Fe (0.43 ± 0.04 mg/L) than that of other heavy
applied using Palisade @Risk 8.2 software to remove
metals may be due to effluents from steel plants, mining
these uncertainties. In MCS, the input point values
activities, sponge iron factories, and its natural abun-
were transformed into statistical random variables
dance at the study area (Chakraborty et al., 2021; Gupta
(USEPA, 2011). The probability distribution indi-
& Gupta, 2021). The elevated values of Zn may be due
vidually described the random variables with their
to natural weathering, mining, and smelting activities

Table 2  Values of exposure parameters for carcinogenic and non-carcinogenic heavy metals
HMs Kp (cm/hour) RfDing (mg/kg/day) RfDder (mg/kg/day) SFing (mg/kg/day) SFder (mg/kg/day) References

Cd 1.00E-03 5.00E-04 5.00E-06 3.80E-01 7.60E+00 Mukherjee et al. (2020)

Cr 1.00E-03 3.00E-03 1.50E-05 5.00E-01 1.32E+01 Mukherjee et al. (2020)
Cu 1.00E-03 4.00E-02 1.20E-02 – – Shil and Singh (2019)
Fe 1.00E-03 3.00E-01 4.50E-02 – – Shil and Singh (2019)
Mn 1.00E-03 2.00E-0 2 8.00E-03 – – Shil and Singh (2019)
Sr 1.00E-03 6.00E-01 1.20E-01 – – Mukherjee et al. 2020
Zn 6.00E-04 3.00E-01 6.00E-02 – – Shil and Singh (2019)

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Fig. 2  Dissemination of heavy metal concentration in a water and b sediment

in the region (Kumar et al., 2020), whereas interaction They revealed that mine wastewater discharges were
of carbonate rocks (weathering) with river water may the main source of high heavy metal concentrations.
increase Sr concentration (Peng et al., 2021). The high- Comparatively low flow rate at this location could have
est concentrations of Cd, Cr, and Fe were observed at been another factor for observing elevated concentra-
sampling location S4, which may be attributed to the tions of heavy metals. The higher concentration of Cd
heavy discharge of industrial (coal washeries, steel could be allied with about 250 operating coalmines
plants, thermal power stations, metal smelting plants, actions, industrial activities (electroplating, welding,
and chemical plants), domestic, and fertilizer inten- fertilizer, and pesticide manufacturing), and domestic
sive agricultural (rice crop) effluents on the u/s side wastewater runoff (Goel, 2006; Mondal et al., 2018).
of this location (Chakraborty et al., 2021; Mondal The prime sources of Cr in the region were the coal
et al., 2018). The findings of the present study were in mining activities, steel industries, and waste dumping
agreement with the study by Custodio et al. (2020a) (Chakraborty et al., 2021; Mondal et al., 2018). Leach-
on toxic metals and metalloids in Mantaro River, Peru. ing of Cr from sub-surface soil and parent rocks was

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the most imperative natural source of its entrance into negative impacts of mine water. Both studies revealed
water bodies (Mondal et al., 2018; Ravindra & Mor, similar results as obtained in the present study.
2019). Therefore, better management actions should be
acquired for controlling the industrial activities to pre- Evaluation of heavy metal contamination in river
vent the river contamination (specially at location S4). ecosystem
Kumar et al. (2021) used the indexical and chemomet-
ric methods for a preliminary assessment of heavy met- Both individual and comprehensive contamination
als in Nakuvadra-Rakiraki River, Fiji. They revealed status of the target heavy metals in the river ecosys-
that the concentration of Cr (0.133 ± 0.033 mg/L) and tem was evaluated using Igeo, CF, EF, PLI, TRI, and
Cd (0.003 ± 0.001 mg/L) was higher than the accepted MPI methods. Igeo was applied to quantify the heavy
limits, while Fe (0.198 ± 0.119) was within the guide- metal accumulation in sediment to assess the study
lines of WHO (2011). However, the relatively higher region’s pollution status concerning the background
concentration of Cd and Fe and lower Cr concentration concentration values. Accordingly, Igeo categorized
were observed in the present study than in that region. the sediment quality from Class 0 (uncontaminated)
to Class II (moderately contaminated) due to the aug-
Assessment of heavy metals in sediment mentation of target heavy metals (Fig. 3a). Igeo of Cu
(1.39–1.64) indicted moderate (1 < Igeo ≤ 2) con-
Comparatively higher concentrations of heavy metals tamination, whereas Cd exhibited weakly to moderate
in sediment were observed than in water and found contamination in sediment. Moreover, weak contami-
to be in the order of Fe > Mn > Zn > Cr > Cu > Sr > Cd nation due to Cr (Igeo: 0.48–0.55) was also observed,
(Fig. 2b). The high concentration of Fe may be due while the rest of the metals indicated unpolluted
to the direct enrichment of sediment from weathering (Igeo ≤ 0) sediment quality. The mean CF value of Cu
(disintegration, dissociation, and dissolution) of iron- (4.26) revealed that sediment was considerably con-
rich laterite rocks in the region (Seal et al., 2022). taminated (3 ≤ CF < 6) with this metal, whereas mod-
High Fe concentration may cause organic decomposi- erate contamination (1 < CF ≤ 3) was observed by
tion, which impacts aquatic organisms (Yalcin et al., other metals (Fig. 3b). The mean EF values for the
2008). Moreover, the fine-grained sediment also heavy metals were found in the order: Cu (4.55) > Cd
acted as the sink for heavy metals and performed as (3.19) > Cr (2.28) > Mn (1.54) > Zn (1.00) as shown
a potential carrier of these metals (Ali et al., 2022). in Fig. 3c. EF > 1.5 for all heavy metals except Zn
Subsequently, earth crust formations, mineralogical revealed that the study area was influenced by anthro-
compositions, and anthropological (e.g., mining, resi- pogenic activities (Zhang & Liu, 2002). The EF (2–5)
dential, agricultural, and industrial) activities could values for Cu and Cd indicated moderate enrichment
have intensified the heavy metal concentration in in sediment, whereas EF < 2 for Zn showed its mini-
the river ecosystem (CPCB, 2011; Singh & Kumar, mal enrichment and concentration was due to natural
2017; Genchi et al., 2020). In China, Wu et al. (2020) weathering process (Duncan et al., 2018). The ele-
evaluated the long-term impacts of mining activities vated values of Igeo, CF, and EF for Cu may be attrib-
and natural weathering on heavy metal contamination uted to the arable nature of the basin and the massive
in the sediment of the Diaojiang River basin They utilization of Cu-rich fertilizers and crop-safety prod-
described the cumulative effects of high geologi- ucts in the study region (Świercz et al., 2022).
cal background values and mining activities on the PLI abridged heavy metal pollution data of each
high accumulation of Cd and other heavy metals in monitoring location into a single value, which indi-
the Diaojiang River’s sediment. Similarly, Zakrutkin cated that S4 (1.97) was the most polluted location in
et al. (2020) also assessed the heavy metal pollution the study region, followed by S3 > S10 > S7 > S6 > S
level of the river sediments within the coal mining 8 > S2 > S5 > S9 > S1 (Fig. 3d). It may be due to the
areas of east Donbass (Rostov Region, Russian Fed- massive amount of contaminated influx of domestic
eration). They found the elevated concentration of and industrial effluents from the mining and agricul-
Fe followed by other heavy metals in the sediments tural activities. 1 < PLI ≤ 2 revealed the footprints of
due to high anthropogenic load and disproportionate heavy metal pollution at all the locations in the study
region. TRI was used to estimate the toxic risks of

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 3474 Environ Geochem Health (2023) 45:3465–3486

Fig. 3  Evaluation of sediment contamination using a Igeo, b CF, c EF, d PLI, e TRI, and f MPI

sediment, which categorized the study region with The results were in agreement with previous stud-
no toxic risks except S4 (5 < TRI ≤ 10), which fell ies conducted on the Damodar River and recognized
in the low toxic risk level (Fig. 3e). However, MPI an elevated nature of heavy metal toxicity in the
was observed as 0.06 ± 0.01 for water ­(MPIW) and river ecosystem (Banerjee and Gupta, 2013; Pal and
98.34 ± 4.32 for sediment ­(MPIS) (Fig. 3f). Although Maiti, 2018). However, the findings of present study
MPI did not use any reference concentrations of tar- revealed that the heavy metal contamination in the
get heavy metal, it highlighted the polluted location study region had amplified with the passing years due
by comparing the index values of all monitoring to the influence of anthropogenic activities (urban set-
locations. This indicated that S4 was the most pol- tlements and industrialization) at river basin.
luted location with high heavy metal contamination
­(MPIW: 0.07 and M ­ PIS: 106.72) in comparison with Health risks assessment
other locations in the region. It may be attributed to
the local pollution load of the highly contaminated Carcinogenic health risk assessment
domestic wastewater influenced by dense popula-
tion and multifarious industrial effluents (Banerjee & The carcinogenic health risk through water and sedi-
Gupta, 2013; Verma et al., 2019). ment was evaluated to assess the impact of prolonged

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Environ Geochem Health (2023) 45:3465–3486 3475

exposure to Cd and Cr on children and adults. The However, population of the present study region
cancer risk values of Cd (adults: 6.38E-05–7.42E-05; were less susceptible to the Cr-assisted carcinogenic
children: 1.87E-05–2.17E-05) and Cr (adults: risk through river water than the residents exposed
6.56E-04–7.65E-04; children: 1.91E-04–2.23E-04) in to the Yamuna River water at Delhi region. How-
water for both population groups surpassed the maxi- ever, the study area (mainly S4) was suffered from
mum acceptable risk value (1.00E-06) as per USEPA prolonged contamination (high ­CRW) from the coal
(2011) (Fig. 4). The TCR values of water (adults: mining activities, geological settings, domestic, and
7.20E-04–8.39E-04, children: 2.10E-04–2.45E-04) industrial effluents (Gupta & Gupta, 2021; Seal et al.,
fall under moderate-risk category. They thus indi- 2022; Verma et al., 2019). Seal et al. (2022) also
cated that both metals impose potential carcinogenic reported the potential carcinogenic risk to both adults
health risks to both population groups in the region. and children in this region due to high heavy metal
Therefore, both population groups of the study contamination using a long-term database from 1980
region were highly susceptible to the endometrial, to 2019 of Damodar River basin.
breast, lung, pancreatic, and bladder cancers due to In the case of sediment, the cancer risk values were
the exposure of Cd and Cr (Dong et al., 2020; Abedi significantly higher than in water, i.e., Cd (adults:
Sarvestani et al., 2019). Typically, high Cd expo- 1.79E-04–2.49E-04; children: 3.35E-04–4.66E-04)
sure through water is allied with an increased risk of and Cr (adults: 1.73E-02–1.81E-02; children:
lung cancer (Idrees et al., 2018). However, carcino- 3.22E-02–3.38E-02) and exceeded the maximum
genic risks (specially lung cancer) due to Cr exposure acceptable risk value (Fig. 4). Moreover, the TCR
through consumption of river water were previously values of sediment (adults: 1.74E-02–1.84E-02,
reported in several studies around the globe (Kumar children: 3.26E-02–3.43E-02) were under the cat-
et al., 2022; Rahman et al., 2021; Yang et al., 2015). egory of high risk and thus indicated a considerably
Vulnerability of high carcinogenic risks to the popu- higher potential of cancer risk than the adults. It was
lation due to Cr exposure was also reported at the primarily associated with the fact that children have
Yamuna River, Delhi, India (Kumar et al., 2022). frequent hand-to-mouth behavior in comparison with

Fig. 4  Carcinogenic health risk through water and sediment in children and adults

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 3476 Environ Geochem Health (2023) 45:3465–3486

adults (Mokadem et al., 2022). Khelifi et al. (2022) risks in addition to Cd and Cr. The OHI values in
also evaluated the heavy metal contamination and sediment were significantly (p < 0.05) higher, i.e.,
associated health risks through soil and sediments 38.75 and 112.88 times higher than those of water in
at southern Tunisia. They found that children were adults and children, respectively, and thus indicated
more susceptible to the carcinogenic health risk than comparatively higher potential of non-carcinogenic
adults, which supported the observations of the pre- health risks to both population groups in the region.
sent study. However, chronic exposure of Mn can cause Mangan-
ism and Parkinson’s disease (Obasi & Akudinobi et
Non‑carcinogenic health risk assessment al., 2020). The prolonged high-level Fe exposure can
cause fatigue, joint pain, weight loss, and vomiting. It
The non-carcinogenic health risk of water and sedi- can also cause hemochromatosis and promote DNA
ment was also evaluated to assess the impact of pro- damage, which can harm both heart and liver (Bagchi
longed exposure to heavy metals among children and and Bagchi, 2020). Enduring Cu exposure can cause
adults. The HQ values for heavy metals in river water diarrhea and eyes irritation and damage the liver
followed the order as Cr > Cd > Fe > Mn > Cu > Zn > (Okereafor et al., 2020; Sall et al., 2020). Pathak and
Sr; however, the values were less than 1 for all indi- Gupta (2020) revealed that the elevated Sr uptake can
vidual heavy metals except Cd (adults: 1.09–1.26; produce harmful effects on liver bone tissue, teeth,
children: 2.90–3.36) and Cr (adults: 1.81–2.10; chil- and brain. Sr abnormally impacts the skeleton devel-
dren: 6.06–7.06) (Fig. 5). HQ > 1 of Cd and Cr for opment process of children (Ding et al., 2022). High
children and adults inferred that these metals indi- Zn exposure can lead to anemia, nausea, skin irrita-
vidually pose potential non-carcinogenic risks, while tions, and gastrointestinal exasperation (Singh et al.,
the others had negligible non-carcinogenic effects. 2022).
However, the OHI values in water were significantly
(p < 0.05) higher than 1 for both children and adults Comparative assessment of carcinogenic
and thus indicated that all these metals together and non‑carcinogenic risks of water and sediment
impose substantially higher potential for non-carci- among adults and children
nogenic health risks than individually. Cd exposure
can influence the children’s growth rate of the study The overall analysis of the risk data revealed that
region (Mukherjee et al., 2020). The population of among the target metals, the cancer risk due to Cr was
children in the study area might also be susceptible 10.12 and 84.61 times higher than due to Cd in water
to anemia, kidney malfunction, bronchitis, and oste- and sediment, respectively (Fig. 4). It may be attrib-
oporosis (Bharti & Sharma, 2021; Mukherjee et al., uted to the higher concentration and cancer slope fac-
2020). Moreover, they also suffered from low intel- tor of Cr than Cd. Many researchers (Alvarez et al.,
ligence quotient level due to Cd exposure (Bharti & 2021; Sayadi et al., 2020; Tseng et al., 2019) identi-
Sharma, 2021). However, both children and adults fied cancer mortality and reported a higher risk of Cr
might get affected by Cr exposure, which impacts exposure than Cd in children and adults in their study
the liver, kidney, and gastrointestinal systems and worldwide. Karunanidhi et al. (2022) also reported
also influence the hematological paraphernalia of the the increased vulnerability of cancer risk due to Cd
human body (Alvarez et al., 2021). Cr exposure can and Cr exposure at Noyyal River, India. Relatively
also cause dermatitis and skin ulcers in the popula- higher concentrations of metals found in the sedi-
tion of study region (Mukherjee et al., 2020; Alvarez ment resulted in higher TCR values than in water, i.e.,
et al., 2021). 23.13 and 147.95 times in adults and children, respec-
In sediment, the HQ values for heavy metals fol- tively (Fig. 4). The study revealed that the populations
lowed a slightly different order: Cr > Fe > Mn > Cd > of the study area were more susceptible to the can-
Cu > Zn > Sr from that in water, and the values were cer risk associated with these heavy metals through
more than 1 for all individual heavy metals for adults exposure to sediment than the water. The non-carci-
(except Sr and Zn) and children (Fig. 5). This indi- nogenic risk analysis also revealed similar observa-
cated that in the case of sediment, Cu, Fe, Mn, Sr, and tions for water (Fig. 5). Among various metals, Cr
Zn also contributed to the potential non-carcinogenic and Cd demonstrated potential non-carcinogenic

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Environ Geochem Health (2023) 45:3465–3486 3477

Fig. 5  Non-carcinogenic health risk through water and sediment in children and adults

risks of water individually; however, the risks due values (Kumar et al., 2020; Li et al., 2020). Moreover,
to Cr were higher than others. It may be due to the findings of the present study also revealed that in case
relatively higher concentration and different refer- of sediment, children were highly susceptible to non-
ence doses of Cr than other metals. Indeed, previous carcinogenic risks than adults due to high concentra-
studies also reported the high non-carcinogenic risks tion of all target heavy metals (Kumar et al., 2020).
posed by Cr and Cd due to their lower reference dose

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 3478 Environ Geochem Health (2023) 45:3465–3486

The health risks of water and sediment were com- percentile values of TCR for adults and children were
pared due to the fact that sediment acts not only as 1.80E-02 and 3.37E-02 through sediment, whereas
sink for the heavy metals but also as a potential 8.10E-04 and 2.36E-04, respectively, through water
source of contamination by means of water–sediment (Fig. 6a–d). It was also observed that the TCR val-
interaction, variations in environmental conditions, ues in water and sediment were maintained at 2–4
and anthropogenic disturbances in the region (Lundy orders (100–10,000 times) higher than the acceptable
et al., 2017). The overall investigation inferred that the carcinogenic health risk value (1.00E-06) and could
potential of carcinogenic and non-carcinogenic health cause unacceptable carcinogenic health risks to both
risks due to sediment was comparatively higher than population groups. In the case of non-carcinogenic
that of water for children and adults. This also indi- health risk (Fig. 6e–h), 95th percentile values of OHI
cated that the children were more susceptible to carci- for sediment, i.e., 1.27E+02 and 1.12E+03, were sig-
nogenic risks through sediment than adults (Arisekar nificantly higher than those of water, i.e., 3.37E+00
et al., 2020; Mondal et al., 2021), whereas adults were and 1.02E+01 for adults and children, respectively.
more prone to this risk through the water (Saha et al., The higher OHI (> 1) indicated that both population
2017). It could be attributed to the diverse pattern of groups were susceptible to the potential non-carcino-
ingestion rates for water and sediment in each popula- genic health risk. At each percentile value of the risk
tion group. However, children showed higher suscep- distributions, the carcinogenic and non-carcinogenic
tibility to non-carcinogenic health risks than adults risk levels in children and adults were in agreement
in the region. It could be due to children’s diverse with those observed through a deterministic approach.
physiological and behavioral characteristics than
adults (Desai et al., 2021; Li et al., 2020; Yohannes Sensitivity analysis
et al., 2022). Similar results were observed by Custo-
dio et al. (2020b) in the rivers at a mining influenced An advanced sensitivity analysis was performed using
region Central Andes of Peru. They found the higher spider graphs to identify the influence of input param-
OHI values (> 1) than their threshold value (OHI = 1) eters in risk assessment for each population group
for both adults and children, which indicated the high (Fig. 7). The results described that among all the
non-carcinogenic risks for both population groups. input parameters, the concentration of heavy metal
Moreover, the carcinogenic risks varied from medium (CM) was the most influential parameter, followed by
to high for children, whereas low to high for adults. exposure frequency (EF), ingestion rate (IR), exposed
skin area (SA), and average exposure time (AT). Body
Monte Carlo simulation based probabilistic risk weight (BW) did not show much influence to the total
assessment risk and was found inversely correlated. These results
were consistent with the previous studies on human
Probabilistic risk assessment is an imperative tool health risk assessment (Jiang et al., 2021b; Mukherjee
to achieve a higher accuracy level in the outcomes et al., 2020). It was also observed that heavy metals
of health risk assessment by recognizing the uncer- had various sensitivities to different health risks for
tainties (Rajasekhar et al., 2018). In this study, an both population groups. In this study, Cr was the most
MCS-based probabilistic risk assessment was car- dominant heavy metal causing both carcinogenic and
ried out to simulate the overall non-carcinogenic non-carcinogenic risk, followed by Cd, Mn, and Fe as
and carcinogenic health risk values for both popula- depicted by the steeper line between health risk val-
tion groups through ingestion and dermal absorption ues and input percentiles for children and adults. The
pathways. The simulated health risk values of water contribution of other heavy metals to the absolute risk
and sediment were determined after 10,000 random was almost similar, as shown by collinear lines in the
simulations at certain percentiles (5th, 50th, and sensitivity graph. Sayadi et al. (2020) also reported
95th) and were used to validate the health risk assess- higher cancer risk of Cr exposure than Cd in Eastern
ment outcomes (Fig. 6). The 95th percentile value Iran, which may be attributed to a higher cancer slope
implied the worst-case risk estimate, and the 5th factor and heavy metal concentration. The study sug-
percentile values corresponded to the low-end expo- gested that regular monitoring of the heavy metals
sure risk (Rajasekhar et al., 2018). Accordingly, 95th

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Environ Geochem Health (2023) 45:3465–3486 3479

Fig. 6  Simulated values of

a–d carcinogenic and e–h
non-carcinogenic health
risks through water and
sediment

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 3480 Environ Geochem Health (2023) 45:3465–3486

Fig. 7  Sensitivity analysis of input parameters for health risks assessment of water a: adults, b: children and sediment c: adults, d:
children

should be carried out in the study region to minimize Risk management

the potential human health risk.
The need for execution of remediation was decided
by using the 95th percentile values as a reasonable

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Environ Geochem Health (2023) 45:3465–3486 3481

maximum exposure estimate (RME), which was the most influential parameter, followed by exposure
advised for the risk management decisions (USEPA, frequency (EF), ingestion rate (IR), exposed skin
2011). Accordingly, remediation techniques must be area (SA), and average exposure time (AT), trigger-
adopted if RME exceeds the acceptable risk level. ing the overall health risk. The study outcomes will
Therefore, the 95th percentile value of output risk be advantageous for researchers, scientists, policy-
distribution was taken as an expedient parameter for makers, and regulatory authorities (state and central
the risk management decisions. The RME values of government) to predict and manage human health
overall non-carcinogenic and carcinogenic risks for risks in the future.
both the population groups in water and sediment
exceeded the acceptable limit (Fig. 6). The in situ Acknowledgements The authors acknowledge the Depart-
ment of Environmental Science & Engineering, Indian Institute
and ex situ remediation techniques, i.e., caping, elec- of Technology (Indian School of Mines), Dhanbad, India, for
trokinetic remediation, dredging, phytoremediation, providing the support in carrying out the research work.
bioaccumulation, and translocation, should be incor-
porated in the contaminated region by considering the Author contributions All authors contributed to the study
conception and design. Material preparation, data collec-
socio-economic, political, and geological factors of
tion and analysis were performed by SG. The first draft of the
the study area (Kumar et al., 2020; Rajasekhar et al., manuscript was written by SG, and all authors commented
2018). The regulatory agencies like pollution control on previous versions of the manuscript. All authors read and
boards should exercise strict compliance on heavy approved the final manuscript.
metal monitoring of effluents generated from the vari-
Funding The authors declare that no funds, grants, or
ous industrial activities. other support were received during the preparation of this
manuscript.

Conclusions Declarations

Competing interests The authors have no relevant financial

Heavy metal pollution and associated carcino- or non-financial interests to disclose.
genic and non-carcinogenic risks of water and
sediment of Damodar River basin through differ- Ethical approval The manuscript has not been submitted to
more than one journal for simultaneous consideration.
ent pathways were thoroughly investigated. The
occurrences of high concentrations of Cd, Cr, and Consent to participate This study has not directly involved
Fe were mainly allied to the mining and adjoining humans or animals.
industrial (steel plants, sponge iron factories, ferti-
Consent to publish The manuscript was reviewed, and all
lizer) activities in the study region. TCR to adults authors consented to publish.
(7.20E-04–8.39E-04, 1.74E-02–1.84E-02) and
children (2.10E-04–2.45E-04, 3.26E-02–3.43E-02)
were found under moderate and high carcinogenic
risk category, through water and sediments, respec- References
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