Journal of Water Process Engineering 42 (2021) 102165

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Journal of Water Process Engineering

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Prediction of Trihalomethanes in water supply of Chattogram city by

empirical models and cancer risk through multi-pathway exposure
F. Khan a, M.F.R. Zuthi a, *, M.D. Hossain b, M.N.I. Bhuiyan c
a
Department of Civil Engineering, Chittagong University of Engineering and Technology, Chittagong, Bangladesh
b
Department of Civil Engineering, Bangladesh University of Engineering and Technology, Dhaka, Bangladesh
c
Institute of Food Science and Technology, Bangladesh Council of Scientific and Industrial Research (BCSIR), Dhaka, Bangladesh

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

Keywords: This study predicts the possible occurrence of trihalomethanes (THMs) in water supply of Chattrogram city in
Disinfection Bangladesh, and life time cancer risk from multi-pathway intakes of the trihalomethanes (THMs) to the city
Drinking water dwellers. A total of 11 water samples were collected from the distribution network of the city, and few water
Disinfection by-products
quality parameters were analyzed in the study. Three empirical models developed by Amy et al. (1998), Rathbun
Model
Cancer risk
(1996), and Malcolm Pirnie (1993) were used to estimate the level of THMs from measured water quality data,
and were denoted as MODEL1, MODEL2 and MODEL3, respectively in the study. Lifetime cancer risk was
estimated using predicted chronic daily intakes (CDI) of THMs’ species for different exposure routes (ingestion,
inhalation and dermal). The total concentrations of THMs ranged between 20 and 440 μg/L, 95–215 μg/L and
162–249 μg/L were predicted by MODEL1, MODEL2 and MODEL3, respectively. An average lifetime cancer risk
was predicted as 1.4 × 10− 4, 1.1 × 10− 4 and 2.9 × 10− 4 for oral, inhalation and dermal exposure, respectively
from the water supply of the city. Percent contribution to total lifetime cancer risk were predicted as 50, 40
and10 for oral ingestion, inhalation and dermal absorption, respectively. The study revealed that lifetime cancer
risk values were higher than minimum risk level set by United States Environmental Protection Agency. The
findings of possible occurrence of THMs in the water supply and associated cancer risk might be beneficial as
baseline data for further investigation, and help the decision makers regarding the formulation of standards and
legislations of THMs.

1. Introduction haloacetic acids (HAAs), haloacetonitriles (HANs) and haloketones

Water disinfection has been practiced worldwide as an essential step
in water treatment process to minimize the microbial pathogenic
infection. Formation of disinfection by-products (DBPs) occurs for the
chemical reaction of disinfectants and natural organic matter present in
water [1–3]. In municipal water supply system, from treatment plant to
consumer tap, various classes of DBPs may be formed at any point of the
distribution line depending upon the availability of precursors and the
disinfectant [4,5]. Chlorine is the most widely used disinfectants
worldwide and in municipal water supply facilities, residual chlorine
reacts with the organic and inorganic precursors to form carcinogenic
chlorinated disinfection byproducts (DBPs) [6,7].
The study of DBPs’ in water took the interest of the researchers for
their carcinogenicity and adverse health effects. [1,8–11]. Various
classes of DBPs’ compounds include: Trihalomethanes (THMs),
(HKs). THMs’ compounds are the most studied and abundant group of
DBPs in water supply. THMs’ species include chloroform (CF), bromo­
dichloromethane (BDCM), dibromochloromethane (DBCM) and bro­
moform (BF). The sum of these four chemical substances refers to as
total trihalomethanes (TTHMs) [2,3,13]. Natural organic matter (NOM)
concentration level of raw water plays the critical role in the formation
of DBPs [13,14]. Different water quality parameters such as pH, tem­
perature, ammonia, carbonate alkalinity, bromide, operational condi­
tions such as disinfectant dose, contact time are identified as the
important influential factors as well [1,5,12,13,14 ]. The USEPA [15]
has established the threshold level of 0.08 mg/L (80 ppb) for total THMs.
The current regulations in China for chloroform (CF), bromodichloro­
methane (BDCM), dibromochloromethane (DBCM) and bromoform (BF)
are 60, 60, 100, 100 μg/L, respectively [14]. The WHO guidelines (100
ppb for TTHMs) are currently adopted by many countries and regions

* Corresponding author.
E-mail addresses: fzuthi@yahoo.com (M.F.R. Zuthi), delwar@ce.buet.ac.bd (M.D. Hossain).

https://doi.org/10.1016/j.jwpe.2021.102165
Received 14 March 2021; Received in revised form 17 May 2021; Accepted 25 May 2021
Available online 10 June 2021
2214-7144/© 2021 Elsevier Ltd. All rights reserved.
F. Khan et al.
[16]. Bangladesh standard for water quality parameters has set the
standard 90 ppb for chloroform (trichloromehane, CHCl3) only [17].
However, no drinking water quality guideline exists for total or other
DBPs’ species in the country.
Exposure pathways of THMs’ species for the people may be catego­
rized into three: oral ingestion, inhalation and dermal absorption.
Showering, bathing, washing swimming are the regular indoor activities
by which people are exposed to THMs through inhalation and dermal
absorption [2,5,9,18]. DBPs in drinking water have positive association
with cancer and potential adverse reproductive effects. Numerous
studies found that DBPs that have been associated with several adverse
health effects from long-term exposure, including bladder and colorectal
cancer and adverse birth outcomes [8–10,16]. Few studies have been
investigated the relationship between chlorination of drinking water
and cancer mortality through toxicological laboratory studies [19–22].
A linkage between exposure to chlorinated drinking water and the
development of urinary bladder cancer is detected [9,10,21]. Moreover,
kidney, liver and intestinal tumorigenesis are also found to be associated
with chronic ingestion of THMs [22,23]. To control DBPs formation,
various pretreatment technologies are applied before chlorination in
developed countries. Removal of precursors is the most effective way to
reduce the formation of DBPs [1,3,5]. To ensure limited DBPs formation
in distribution line, the water works of these countries adjust the oper­
ational parameters and influencing factors of DBP through monitoring
DBPs concentration level regularly [5]. However, there is no strategy or
plans to control DBPs in water treatment plants in Bangladesh.
Monitoring of THMs’ is a time consuming and laborious work, which
involves, complex process for sample extraction and expensive instru­
ment [24–26]. Hence, particular interest has been directed on devel­
opment of models to estimate the formation of THM which may be an
alternative of THMs measurement in the field [26,27–29]. Adaptation of
empirical models (linear or log linear) available in the literature can be a
simplified solution to meet the primary interest in the field of THMs’
research [28–30]. A significant number of mathematical models have
been developed to predict DBPs’ in drinking water [18,21,27,30]
incorporating water quality parameters as well the operational condi­
tions of the water treatment plants in the past three decades. DBPs
models can be roughly classified into two types. First type is based on
empirical relationships and the second type is based on kinetics involved
during chlorine reaction [21]. Multiple linear and non-linear regression
techniques are found to be the most common in developing DBPs’ pre­
dictive models. Other methods like ridge, logistic regression and artifi­
cial neural networks have also been employed. Most of the predictive
models are based on laboratory-scaled studies, but very few models have
been proposed based on real water taken from distribution network
[27]. Chowdhury et al. [30] and Sadiq et al. [31] reviewed existing
static models with their advantages and limitations. Both the studies
discussed the development of models for total THMs (TTHMs or THMs’
species) demonstrating that several of the models were capable of
generating linear correlations (R2) > 0.90 based on results from their
respective studies. However, majority of the models were formulated for
total (TTHMs), and there is limited models evaluating individual THMs’
species, bromide ion and ammonia‑nitrogen. The explanatory variables,
considered in many models, such as fulvic acid, chlorophyll a, fluores­
cence, geographic region, seasons, kinetic rate constants, flow rate and/
or tank volume, or any of several dummy variables are not easy to
investigate. Moreover, it is not possible to convert the mole based unit
(μmol/L) to mg/L without knowing the DBPs speciation. Beside this, it
becomes uncertain how much free chlorine would be available in the
presence of ammonia for reactions leading to formation of THMs [32].
Chattogram is the major port city and financial center in the south­
eastern Bangladesh. Chattogram Water Supply and Sewerage Authority
(CWASA) is the responsible authority for supplying water to its city
dwellers. CWASA is mostly using surface water to meet water demand of
about 2.1 million people [33]. Chlorination is done at the last step of
treatment process by the treatment plants of CWASA to disinfect the
2
Journal of Water Process Engineering 42 (2021) 102165
supply water. Chlorine is used as it is cheap in price and has strong
oxidizing ability. A minimum level of chlorine residual is maintained
throughout the distribution system to protect against microbial recon­
tamination despite of its potential to form carcinogenic DBPs. In
Bangladesh, the research on the occurrence and formation of DBPs in
water supply, developing models aiming at the development of policies
is still at rudimentary level and national standards are yet to set for DBPs
in drinking water despite of its acute and chronic effects to human
health. Khan et al. [34] first worked on the possibility of THMs forma­
tion on chlorinated textile wastewater. This study investigated the
THMs’ level of chlorinated effluent of treated textile waste for different
chlorine dose. The study shows that chlorination of textile waste does
not produce significant amount of THMs (below USEPA limit) as textile
waste contains negligible amount of fulvic and humic acid. Suchana
[32] studied the presence of THMs in the water supply of Dhaka city, and
proposed a modified mathematical model including ammonia as an
influencing parameter based on limited bench scale data. Ahmed et al.
[35] conducted risk assessment for chloroform species in water supply
for few locations of Dhaka city and found that the people are at risk due
to be exposed to chloroform species. The other species of THMs proved
to be carcinogenic to human health should also be investigated along
with the chloroform species. To focus on the issues associated with
THMs formation including health effects and regulatory compliance is a
pressing demand in Bangladesh. It has been a completely new field of
research for Chattogram city to predict the possible presence of potential
DBPs’ using mathematical models in drinking water and associated
health risk to the city dwellers. The modeling study on Dhaka city [35]
was conducted from limited bench-scale data, and modeling study on
field level data for DBPs’ compounds is completely lacking.
The present study, therefore, aims to predict the total trihalomethaes
(TTHMs) and THMs’ species concentration utilizing available THMs’
empirical models from physico-chemical properties of supplied water
collected from different sampling points of CWASA’s distribution line.
Three empirical models developed by Amy et al. [36], Rathbun [37],
and Malcolm Pirnie [38] will be applied to assess the presence of THMs
in the water supply of the city. These models allow the direct utilization
of numerous influential factors as inputs data and are readily available
for predicting disinfection by-products (DBPs). Necessary water quality
data from 11 points of distribution network of Chattogram city were
obtained in the study. Based on the predicted concentrations of THMs’
species cancer risk assessment will be carried out for different exposure
pathways. It is expected that the predictive values of the study would
develop a baseline data for further investigations of the concentration of
THMs in CWASA’s water supply and can preliminary be used to estimate
the human health risks associated with THMs exposure.
2. Materials and methods
2.1. Study area and sampling locations
CWASA draws surface water from Halda and Karnafully river flowing
around the city and supplies water to the city dwellers after conducting
treatment in their treatment plants. It has three surface water treatment
plants and one ground water treatment plant which is basically for iron
removal. The study has considered the Mohra surface water treatment
plant (MSWTP). This plant uses water from Halda river, and several
physico-chemical processes are being performed in the plant as well as
disinfection process. Post-chlorination is followed here using chlorine as
a disinfectant in chlorine contact chamber at a concentration of 2–2.5
mg/L to disinfect water with contact time 30 min in chlorination
chamber at 90 M liters per day (MLD). Karnafully Service Area (KSA) of
CWASA’s distribution network was selected for the study. KSA delivers
treated water to 22 wards fully and 4 wards partially out of 41 wards in
Chattogram city Fig. 1(a). Water samples were collected from water
supplies distribution network which included consumer taps from 11
different locations of Chattogram city as shown in Fig. 1(b), and only
F. Khan et al.
Fig. 1. Sampling sites from existing water supply distribution map of CWASA.
one sample from each location were taken. Five samples were collected
in January 2020 (winter) and six were collected in June 2020 (summer).
The locations of sample collections are as follows: Bohaddarhat (area-1),
Bohaddarhat (area-2), Muradpur (area-1), Muradpur (area-2), 2 No.
Gate (area-1), 2 No. gate (area-2), General Electric Company (GEC)
Circle, Lalkhan Bazar, Wasa, Agrabad and Halishohor. In this study these
sample collection areas are represented as locations 1 to 11,
respectively.
2.2. Characterization of water samples
Water samples were collected from the distribution network of
CWASA at 11 sampling points by one of the authors of this study. The
collected samples were analyzed for a number of water quality param­
eters following standards methods [39]. Ammonia‑nitrogen, NH3-N was
measured by Salicylate method in Spectrophotometer (Model: HACH,
DR6000U), and total organic carbon, TOC measurements were done
using Shimadzu TOC-5000 analyzer.A chlorine dose (D) of 2.5 mg/L was
used in model equations as per the applied dose in the MSWTP. A 6 h
contact time (t) was assumed starting from chlorine contact chamber to
the point of consumer tap. As both the Br− ion concentration and UV254
were not analyzed in the study, value of Br- ion concentration and UV254
were taken as 50 μg/L and 0.144, respectively from a study by Suchana
[32] on the treated water of six water treatment plants located outside
Dhaka city of Bangladesh.
2.3. Selection of predictive models for the estimation of THMs’ species in
supplied water
A thorough literature review has been done prior to the selection of
the available DBPs’ models for this study. Three models were selected to
predict the concentration for all individual THMs’ species with different
explanatory variables. Among the selected models, two are DOC-based
3
Journal of Water Process Engineering 42 (2021) 102165
models developed by Amy et al. [36] denoted as MODEL 1 and Rat­
bun [37] which is denoted as MODEL 2. The third one, MODEL 3 which
is developed by Malcolm Pirnie Inc. [38], is also a DOC-based model but
it includes NH3-N as one of the explanatory variables. Amy et al. [36]
developed the model on data generated from the most comprehensive
bench-scale study for TTHMs/THMs species. This database (hereafter
referred to as the EPA [40] database) was primarily used to develop DBP
models. The model used DOC and UV254 as indicators of natural organic
matter (NOM) in their original works of Amy et al. [36]. Another model
developed by Rathbun [38] for low bromide water, and this model
developed multiple regression models for predicting THMs’ species
formation using water samples from the Mississippi, Missouri and Ohio
Rivers in USA. Water samples were collected during the summer and fall
of 1991 and spring of 1992 at 12 locations. These models were devel­
oped at a constant temperature of 25 ◦ C and constant reaction time of 7
days and showed good predictability. The root mean square of the model
predictions and experimental data were found good. As the service area
receives water from the Halda River which might have bromide, iodine,
salinity due to tidal effect of the Bay of Bengal. Moreover, the root mean
square of the model predictions and experimental data were found good.
Malcolm Pirnie Inc. [38] is the model that incorporated ammonia ni­
trogen with other parameters in modeling THMs’ species in chlorinated
water. In Bangladesh, ammonia content of surface waters is considerably
high, particularly during the dry season which might affect the forma­
tion of THMs in the presence of bromide ion. Moreover, the treatment
plant of the city uses chlorine as their disinfectant, and reactions be­
tween chlorine and ammonia may result in the formation of chlora­
mines, potentially suppressing formation of THMs. Thus, it is necessary
to assess and quantify the effect of ammonia on the formation of THMs
during the chlorination of water containing organic matter as well as
ammonia. The selected models have been shown in Table 1:. In this
paper these three models are expressed as MODEL1, MODEL2,
MODEL3 for Amy et al. [37], Rathbun [36] and Malcolm Pirnie Inc.
F. Khan et al. Journal of Water Process Engineering 42 (2021) 102165

Table 1
Selected models to estimate the conc. of THMs’ species in CWASA’s water supply.
Models Model description Unit R2 Ref.
1.617 0.094 0.175 0.607 1.403 0.306
Model1 CHCl3 = 10 (DOC)
–1.205
(Cl2) (Br )
−
T (pH) (t) (μg/L) 0.93 [36]
CHBrCl2 = 10− 2.874(DOC)0.901 (Cl2)0.017 (Br− )0.733 T0.948(pH)1.511 (t)0.199 0.87
− 0.226 0.108 − 1.81 0.512 2.212
CHBr2Cl = 10 –5.649
(DOC) (Cl2) (Br ) T (pH) (t)0.146 0.90
CHBr3 = 10–7.83(DOC)− 0.983(Cl2)0.804 (Br− )1.765 T0.754(pH)2.139(t)0.566 0.61
Model2 CHCl3 = 0.442 (pH)2 (D)0.229 (DOC)0.912 (Br− )− 0.116 (μg/L) 0.97 [37]
CHBrCl2 = 17.5(pH)1.01(D)0.0367 (DOC)0.228 (Br− )0.513 0.86
CHBr2Cl = 26.6 (pH)1.80 (D)-0.0928 (DOC)− 0.758 (Br− )1.2 0.94
CHBr3 = 0.29 (pH)3.51 (D)− 0.347 (DOC)− 0.330 (Br− )1.84 0.78
Model3 CHCl3 = 0.997 (TOC)0.580 (UV254)0.580(D)0.814(t)0.278 (Br− + 1)− 4.27(T)0.569 (pH-2.6)0.759 (μg/L) [38]
CHBrCl2 = 4.05 (TOC)0.567 (UV254)0.567(D-7.6 × NH3-N)− 0.351(t)0.366 (Br− + 1)0.291 (T)0.568 (pH - 2.6)0.568 –
CHBr2Cl = 22.9 (TOC)0.253 (UV254)0.253(D-7.6 × NH3-N)− 0.352(t)− 0.292 (Br− + 1)1.04(T)0.491 (pH-2.6)0.325
CHBr3 = 1.28 (TOC)− 0.167 (UV254)− 0.167(D-7.6 × NH3-N)− 2.22(t)0.294 (Br− + 1)1.48(T)0.553 (pH-2.6)0.19

Nomenclature: CHCl3 (Chloroform,CF); CHBrCl2 (Bromo-dichloro-methane, BDCM); CHBr2Cl (Dibromo-chloromethane, DBCM); CHBr3 (Bromoform, BF); DOC =
dissolved organic carbon (mg/L); Br− = concentration of bromide ion (mg/L); t = reaction time (hr); T = temperature (◦ C); TOC = total organic carbon (mg/L); UV254
= ultraviolet absorption at 254 nm wavelength (cm− 1); D = chlorine dose (mg/L); t = reaction time (hour); Br − =bromide ion concentrations (mg/L); NH3–N =
ammonia nitrogen (mg/L).

[38], respectively.
2.4. Risk assessment approach
Cancer risk assessment was conducted based on the predicted con­
centrations of THMs’ species for multi-pathway exposure. United States
Environmental Protection Agency (USEPA) guidelines (USEPA, 1986,
1999, 2002) [40–42] were followed which had been adopted in scien­
tific studies in this area [33,18,22,24]. Assessment of cancer risk was
carried out for oral ingestion, inhalation and dermal exposure pathways
through chronic daily intake (CDI). Risk analysis was carried out by
Integrated Risk Information System [43] and Risk Assessment Infor­
mation System [44] with input parameters for the human risk analysis as
summarized in Table 2. Chronic daily intakes through different exposure
pathways were estimated by the equations.
where CDIingestion is the chronic daily intake via ingestion (mg/kg/day);
Cw is the concentration of THMs in drinking water (mg/L); IR is the
drinking water ingestion rate (L/day); EF is the exposure frequency
(days/year); ED is the exposure duration (year); BW is the body weight
(kg) and AT is the averaging time (days); CF is the mass conversion
factor.
Cw × SA × F × PC × ET × EF × ED × CF
CDIdermal (mg/kg − day) =
BW × AT
(2)
where CDIdermal is the chronic daily intake via dermal contact (mg/kg/
day); CW is the chemical concentration in water, mg/L, SA, the skin-
surface area available for contact, cm2, PC, the chemical-specific
dermal permeability constant (cm/h), ET is the exposure time, h/day
or h/event.

Cw × IR × EF × ED × CF Cair × IR × EF × ED × CF
CDIingestion (mg/kg − day) = (1) CDIinhalation (mg/kg − day) = (3)
BW × AT BW × AT

Table 2
Input factors and abbreviations for multi-exposure risk assessment.
Input parameter Notation Units Values References

THM concentration in water supply Cw mg/L As per the measured value This study
Exposure time ET min/day− 1 35 [18]
Exposure frequency EF days/year− 1 365 [18]
Exposure duration ED Year 70 [33]
Conversion factor CF L/m− 3 0.001 [46]
Body weight BW kg 70 [46]
Average exposure time AT days 70 × 365 [46]
Ingestion rate IR L day− 1 4.01 [35]
Skin surface area SA m2 1.8 [47]
Fraction of skin in contact with water F % 90 [46]
Permeability coefficient PC cm/h− 1 Chloroform 6.8 × 10− 3; BDCM 4.20 × 10− 3 [45]
DBCM 2.89 × 10− 3; bromoform 2.35 × 10− 3
THMs’ concentration in air Ca mg/ L Derived by little’s Model
[47]
1
Overall mass transfer coefficient KoLA L min− Chliorform 7.4; BDCM5.9; DBCM 6;
Bromoform3.7 [47]
Henry’s law constant at 40 ◦ C H 0.25 (chloroform); 0.124 (BDCM); 0.0526 (DBCM); 0.0501 (bromoform) [47]
− 1
Air flow rate QG L min 50 [47]
Water flow rate QL L min− 1 5 [47]
Bathroom volume Vs m3 10 [47]
Absorption efficiency AE % 50 [18]
Ventilation rate VR m3 h− 1 0.83 [46]
1
Carcinogenic slope factor (oral) CSForal (mg⋅kg − day− 1)− 1
Chloroform 6.10 × 10− 2; BDCM 6.20 × 10− 2 [44]
DBCM 8.40 × 10− 2; bromoform 7.90 × 10− 3
− 1
Carcinogenic slope factor (dermal) CSFder (mg⋅kg day− 1)− 1
Chloroform 3.05 × 10− 2; BDCM 6.33 × 10− 2 [44]
DBCM 1.40 × 10− 2; bromoform 1.32 × 10− 2
− 1
Carcinogenic slope factor (inhalation) CSFinh (mg⋅kg day− 1)− 1
Chloroform 8.05 × 10− 2; BDCM 6.20 × 10− 2 [45]
DBCM 8.40 × 10− 2; bromoform 3.85 × 10− 3

4
F. Khan et al. Journal of Water Process Engineering 42 (2021) 102165

where CDIinhalation is the chronic daily intake via inhalation (mg/kg/ Table 4
Physico-chemical properties of the studied water samples.
day); where Cair is the contaminant concentration in air, mg/m3, IR, the
inhalation rate (m3/h). Sampling station pH Temperature DOC NH3-N
(◦ C) (mg/L) (mg/L)
To calculate the inhalation exposure two resistance theory by Little
[47] was used in this study. Concentration of THMs’ species in air, Cair Location 1 7.16 21.8 1.805 0
can be estimated by the following equations using two resistance theory Location 2 6.50 28.02 5.79 0.015
Location 3 7.36 22 1.705 0
[47]. Location 4 6.50 28.01 5.86 0.013
Cair = (C0 + Ct) / 2, where Co is initial concentration of THMs’ and Ct Location 5 7.25 22 1.791 0
is concentration at any time t. This study assumed C0 = 0 and Ct has been Location 6 6.98 28.03 5.12 0.014
calculated by the following equation. Location 7 7.30 21.4 0.783 0
Location 8 7.15 21.9 1.7 0
Ct = [1 − exp( − bt) ] (a/b) (4) Location 9 6.90 28.03 4.69 0.015
Location 10 6.92 28.2 5.25 0.011
b = [(QL /H) (1 − exp( − N) ) + QG ]/Vs (5) Location 11 7.05 28.04 4.03 0

a = [(QL ⋅CW )⋅(1 − exp( − N) ) ]/Vs (6)

N = [KoL A/QL ];
where N is a dimensionless coefficient, QL = Water flow rate in liter per
minute, t = time of contact, a and b are factors.
locations 1, 3, 5, 7, 8 and 11 was zero. The water containing NH3-N
value shows higher DOC value except the location 11. This might be
(7)
ascribed to the fact that water containing high TOC may accelerate the
nitrification process, and therefore increase the level of NH3-N in the
studied water.

Total cancer risk = CDIingestion × CSForal + CDIInhalation × CSFInhalation + CDIDermal × CSFDermal (8)

3.2. Occurrence of TTHMs in the supplied water

CSF is the carcinogenic slope factor ([mg/kg/day]− 1) for the Total trihalomethanes (TTHMs) concentration were estimated by
mentioned three exposure pathways. summing up the concentration of four individual THMs’ species pre­
dicted by the three models used in the study. Fig. 2 shows that in many
3. Results and discussions cases the predicted concentration of TTHMs is higher than USEPA limit
(80 ppb). Total THMs concentration (TTHMs) at 11 sampling points
3.1. Physico-chemical properties of the supplied water varied between 20 and 440 μg/L, 95- 215 μg/L and 162–249 μg/L pre­
dicted by MODEL 1, MODEL 2, MODEL 3, respectively.
A statistical summary of the collected data and details of the physico- MODEL1 estimated TTHMs beyond regulatory limit at 6 locations,
chemical properties of the collected water samples are presented in whereas TTHMs’ exceeds the limit at all the sampling points estimated
Table 3 and Table 4 respectively. The observed pH value ranged from by MODEL2 and MODEL3. The average TTHMs concentration by these
6.5 to 7.36 and the observed temperature of the water samples are from models was found to be around 233, 146 and 211 μg/L, respectively.
21.4 to 28.4 ◦ C. This variation in pH and temperature might be due to TTHMs estimated by MODEL1 are 1.5 times higher than MODEL2 which
the fact that the samples were collected at various time of the year. might be ascribed to the varying explanatory variables taken in the two
Literature shows that increased pH and T values have a positive effect on models. Model 2 has considered DOC, Dose, pH and Br− . The tempera­
the formation of THMs’ [2]. The TOC content of the water samples are ture (25 ◦ C) and reaction time (7 h) were kept constant during the
found between 0.783 and 5.86 mg/L. It is noteworthy to mention that development of the model. On the other hand, MODEL1 considers
the TOC values are taken as DOC in this study as no suspended solids temperature, contact time in addition to the parameters of Model 2 as
were found in the studied water samples. It is observed that higher DOC the important factors. The THMs’ formation may increase with the in­
value (around 4–5 mg/L) has generally been observed at higher tem­ crease of temperature because of the faster reaction kinetics, and contact
perature (around 28 ◦ C) in the study. It is found in literature that in time might significantly impact the formation. Moreover, MODEL2 was
summer, a favorable condition for bacteria and algal growth in source developed using low bromide source waters, and this study has taken
water can cause a contribution to DOC and UV254 [25,48]. However, considerable levels of bromide and thereby MODEL2 underestimate the
there is no specific relation cannot be drawn between pH and DOC based THMs’ formation as the studied water samples has varying temperature,
on the observed results of the study. On the other hand, NH3-N, one of different contact time. MODEL1 predicted the highest TTHMs of 440 ppb
the influencing parameters to the THMs formation, are observed be­ at location 4 and lowest of 20 ppb at location 7. Highest TTHMs of 215
tween 0.011 and 0.015 mg/L although that of the water samples from ppb is estimated at location 10 by MODEL2 and lowest 95 ppb at loca­
tion 7. MODEL3 (the NH3 based model), estimated the highest TTHMs of
249 ppb at location 10 and lowest 162 ppb at location 7. TTHMs esti­
Table 3 mated by these three models vary over a wide range. These results also
Statistical summary of the collected data.
highlight the need for actual measurement of THMs’ at distribution
Parameters Number of data and Minimum Maximum Mean network. The estimated concentrations vary due to the fact that specific
sampling station
data sources are used to derive these models. Cristiana Di Cristo et al.
pH 11 6.5 7.36 7.00 [49] compared the performances of the 18 selected empirical models for
Temperature 11 21.4 25.23 25.23 predicting THMs formation in a real water supply system, and found that
(◦ C)
DOC (mg/L) 11 0.783 5.86 3.502
some of them were not able to make good prediction. The study how­
NH3-N (mg/L) 11 0 0.0062 0.015 ever, suggests that an error of this magnitude of predicted concentration

5
F. Khan et al. Journal of Water Process Engineering 42 (2021) 102165

Fig. 2. Predicted concentrations of total THMs (TTHMs) at studied locations by three different models. (a) MODEL1 (b) MODEL2 (c) MODEL3.

Fig. 3. Concentrations of TTHMs’ and THM species predicted by MODEL1 (The cross sign denotes the average concentration).

Fig. 4. Concentration of chloroform (CF), predicted at different locations by (a) MODEL1, (b) MODEL2 and (c) MODEL3.

6
F. Khan et al.
level is accepted for practical situation in which the most important
aspect is to understand whether the regulation limits are respected in all
nodes of the systems. However, in current study, MODEL1 shows good
prediction sensitivity with pH, temperature and TOC concentration. It
estimated the highest average TTHMs concentration (233 μg/L). Other
hand water supply content negligible amount of NH3-N (Table 4).
Therefore, THMs’ species concentration estimated by MODEL1 (Fig. 3)
will be used in risk assessment analysis.
3.3. Variability in concentrations of THMs, species with different models
with varying explanatory variables
Chloroform, CHCl3 (CF) was found to be the dominant THMs species
formed in all 11 measurement nodes, accounting for 60% to 80% of the
total THMs expressed on a μg/L concentration basis except MODEL3
(Fig. 4). CWASA mostly uses surface water and due to tropical weather
and excessive vegetation surface water in Bangladesh may contain a
higher amount of organic load. CF is formed in the distribution network
as this source water with higher organic load is being disinfected with
chlorine [32].
BDCM was the main THM species estimated by MODEL3 (Fig. 5) as
this model considers NH3-N as an explanatory parameter. Presence of
ammonia reduces the availability of free chlorine to form CF [32].
Available chlorine reacts with ammonia when organic matter present in
water, and this reaction results the formation of chloramines, potentially
suppressing formation of THMs. Bromodichloromethane (BDCM) was
found in all samples in concentration ranging from 2 to 40 μg/L esti­
mated by MODEL 1 and MODEL2 whereas MODEL3 estimated BDCM
ranging 126–167 μg/L. Dibromochloromethane (DBCM) and Bromo­
form (BF) were estimated in a negligible amount by MODEL1 and
MODEL2. MODEL3 estimated considerable amount of DBCM (ranging
10 to 18 μg/L) and Bromoform ranging from 2 to 3 μg/L. This might be
due to fact that models developed by MODEL1 and MODEL2 are chlorine
based DOC model whereas MODEL3 is ammonia based model.
4. Cancer risk assessment
As described before, concentrations of THMs species predicted by
MODEL1 have been used in risk assessment analysis. However, all the
models showed that bromoform (BF) had negligible contribution to
TTHMs. The risk due to the presence of BF was not calculated due to its
low predicted concentration (less than 0.1 μg/L). Through stepwise
application of Eqs. (1)–(8), the total lifetime cancer risk levels were
predicted from multi-pathway exposure routes (oral ingestion, inhala­
tion and dermal) for 11 locations of Chattogram city. A 70 years of
exposure duration (ED), average life expectancy in Bangladesh, with 35
Fig. 5. Contribution of CF, BDCM, DBCM and BF to total THM predicted by (a) MODEL1, (b) MODEL2 and (b) MODEL3.
7
Journal of Water Process Engineering 42 (2021) 102165
min/day exposure time (ET) and 365 days per of exposure frequency
(EF) were assumed (Table 2). Other parameters such as conversion
factor (CF); body weight (BW); average exposure time (AT) are listed in
Table 2. An average lifetime cancer risk level of TTHMs of CWASA’s
water supply for the studied areas of Chattogram city was found 2.8 ×
10− 4 which is higher than the minimum prescribed risk level 1.0 × 10− 6
by USEPA [50]. The highest cancer risk was predicted 5.2 × 10− 4 at
location 4 and 3.6 × 10− 5 at location 7. As expected, the predicted re­
sults show that risk level is proportional to the concentration of THMs.
Oral ingestion accounts 50% of the total cancer risk. Dermal contact and
inhalation imparted 40% and 10% contribution to the total cancer risk.
4.1. Cancer risk evaluation via oral route
Fig. 6 shows the estimated cancer risk through oral ingestion for all
11 study locations. The predicted life time cancer risk levels via oral
exposure were found in between 2.23 × 10− 5 to 2.3 × 10− 4. The highest
cancer risk for oral ingestion was estimated at location 4 (2.3 × 10− 4).
As predicted by MODEL1, THMs’ concentrations in location 4 were the
highest. Chronic daily intake for oral ingestion (CDI oral) values increase
with the increased concentration of THMs. Wang [51] reported that
boiling of supply water reduces the concentration of THMs specially CF
and therefore reduces the risk. In this study, the risk estimation is based
on the predicted concentration of THMs. However, in real life cases
boiling of drinking water reduces the concentration of THMs’ species.
Chloroform imparted the highest contribution to total cancer risk for
oral ingestion followed by BDCM and DBCM. An average lifetime cancer
risk of the studied areas due to oral ingestion was predicted 1.4 × 10− 4
for the water supply of Chattogram city.
4.2. Cancer risk evaluation via inhalation pathway
The boiling point of chloroform (CF) is very low and it may be
assumed that during regular activities like washing, bathing showering
etc. CF is the major compound to which people are exposed to [19]. In
closed bathroom or shower room people breathe accumulated air
enriched with THMs’ species (mainly CF) during inhalation. Models
developed by Little [46] were applied to calculate the THMs’ species
concentration in air (Cair). Different parameters of these models such as
overall mass transfer coefficient (KoLA); Henry’s law constant at 40 ◦ C
(H); air flow rate (QG); water flow rate (QL); bathroom volume (Vs) etc.
are tabulated in Table 2. It was predicted that approximately 3.8% of CF,
0.129% of BDCM and 0.055% of DBCM were evaporated from water
which indicates a negligible concentration of other THMs’ species in air
other than CF. Chronic daily intake for inhalation (CDI Inhalation) of
THMs’ species were predicted by Eq. (4). An average exposure time (t) of
F. Khan et al.
Fig. 6. Lifetime total cancer risk of THMs of CWASA’s water supply.
25 min was taken. Other additional parameters such as ingestion rate
(IR) etc. are listed in Table 2. Chronic daily intake for inhalation
(CDIInhalation) of THMs’ species increases with the increased concentra­
tion of Cair. CDIinhalation of Chloroform (CF) was found to be highest in
value as expected. An average lifetime cancer risk of the studied areas
due to inhalation was predicted 1.1 × 10− 4 for the water supply of
Chattogram city. Chloroform is the major contributor (above 99%) to
the total cancer risk for inhalation. The findings are consistent with the
previous study [21,22,52] found in literature.
4.3. Cancer risk evaluation via dermal contact
In case of dermal contact, penetration of THMs’ species into body
through skin depends on the permeability of different THMs’ species.
Chronic daily intake for dermal exposure (CDIdermal) of THMs’ species
Fig. 7. Cancer risk due to multi pathway exposure. (a) Oral ingestion. (b) Inhalation pathway. (c) Dermal absorption.
8
Journal of Water Process Engineering 42 (2021) 102165
(Eq. (3)) varies mainly for two parameters: permeability co-efficient
(PC) and species’ concentration (Cw) in water as the value of other
parameters are kept same. Based on PC value, THMs’ species can be
arranged as CF > BDCM > DBCM > BF (Table 2). As expected highest
cancer risk value for dermal exposure was found for chloroform (CF)
because of its high predicted concentration (Cw) in water supply and
permeability co-efficient (PC). Total lifetime cancer risk level from
exposure to THMs’ through dermal contact were found from 3.2 × 10− 6
to 5.5 × 10− 5, higher than prescribed risk level 1.0 × 10− 6(Fig. 7(iii)).
CF is the major contributor (up to 99.3%) to life time cancer risk due to
dermal exposure. In comparing oral and dermal exposure, Jo et al. [53]
demonstrated that daily dermal intakes were approximately 32.5% of
oral intakes. Dermal intakes from THMs daily were 40–70% of daily
ingestion doses, as demonstrated by Cleek and Bunge [54]. However,
this study did not consider the variability in parameters in predicting the
F. Khan et al.
risk level. For more accurate prediction variability in different param­
eters such as exposed area, exposure duration may be incorporated.
5. Risk minimization by controlling THMs levels
Although the study is based on very limited data and used empirical
models, the findings indicate the probable occurrence of TTHMs in
drinking water of Chattogram city and the city dwellers might face
various health diseases due to the consumption of toxic DBPs. Ozone,
UV-ray etc. as alternative disinfectants are being used in many countries
of the world to avoid the adverse health effects of DBPs. Chlorine is,
however, being used in the developing countries especially in
Bangladesh because of its availability and cost-effectiveness. Special
attention should, therefore, be paid to manage these by-products safely.
Removal of precursor is the most effective strategy to control the levels
of DBPs in chlorinated drinking water. In developed countries, various
pretreatment technologies have been exploited prior to chlorination to
reduce the generation of DBPs. Appropriate mathematical model could
be useful tool for controlling precursors which will help to manage DBP
at the water utility scale. Development of a viable DBPs’ formation
model for water supply distribution network of CWASA is now a pressing
demand evaluating the required reduction in precursors. The existing
DBPs/THMs models differ in origin and structure and developed for
different quality of source water and operational parameters. The model
based on field-scale data, with specific water source and treatment
process, could be used for predicting the formation and changes of
THMs’ species in water distribution network. The predicted concentra­
tion of THMs may guide the water supply authority to adjust different
water quality parameters to minimize THMs levels in drinking water as
well as human health risk.
6. Conclusions
The study of disinfection-by-products is a new field of research for
water supply of Chattogram city and no field data is available to focus on
DBPs’ associated with human health. The study has been conducted to
assess the possible occurrence of THMs, one of the potential DBPs, in
water supply of Chattogram city. Three predictive models, denoted as
MODEL1, MODEL2, MODEL, have been used to estimate the concen­
tration of THMs from measured water quality data of water samples
taken from the city’s distribution network. It is observed that concen­
tration of THMs is higher than USEPA limit (80 ppb) at six locations out
of 11 studied locations as per MODEL1 while the predicted values of
MODEL2 and MODEL3 exceed the acceptable limit at all the locations.
Chloroform (CHCl3) is found dominant form followed by bromo-
dichloromethane (CHBrCl2) among the four THMs species according
to MODEL 1 and MODEL 3 whereas BDCM is the main THMS species
estimated by MODEL3. Variation in estimated THMs’ species estimated
by the three models might be ascribed to the varying explanatory vari­
ables consideration in the models and the water quality and operational
parameters taken in the study. The results, however, highlight the need
for actual measurement of THMs at distribution network. Lifetime
carcinogenic health risk is also assessed based on the predicted levels of
THMs. The city dwellers might be at cancer risk due to multi-pathway
exposure of THMs’ species. An average lifetime cancer risk posed by
TTHMs of CWASA’s water supply for the studied area of Chattogram city
is found to be 2.8 × 10− 4 which is more than 100 times higher than
minimum risk level of USEPA guidelines. Chloroform imparted the
highest cancer risk through the pathway of oral ingestion. However,
during the calculation of risk assessment variability of various input
parameters were not considered and incorporation of variability may
improve the accuracy of risk assessment. The predicted value of THMs in
water supply of Chattogram city and associated cancer risk through the
consumption of the water may be used to obtain baseline data for further
investigations in details to ensure safety to human health.
9
Journal of Water Process Engineering 42 (2021) 102165
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.
Acknowledgment
Research grant for the project (CUET/DRE/2019-20/CE/036) enti­
tled as “Assessment of risk of supply water contamination by disinfec­
tion by-product (DBPs) in Chattogram City” of ‘Chittagong University of
Engineering and Technology (CUET)’, Bangladesh supported for the
fund of the study.
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