Journal of Environmental Management 299 (2021) 113611

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Journal of Environmental Management

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

Pesticide residues in drinking water, their potential risk to human health

and removal options
Ibrahim El-Nahhal a, Yasser El-Nahhal b, *
a
Université de Toulon - CS, 60584, France
b
Dept. of Earth and Environmental Science Faculty of Science, The Islamic University, Gaza, Palestine

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

Keywords: The application of pesticides in agricultural and public health sectors has resulted in substantially contaminated
Contaminated water water resources with residues in many countries. Almost no reviews have addressed pesticide residues in
Pesticide residues drinking water globally; calculated hazard indices for adults, children, and infants; or discussed the potential
Health risk
health risk of pesticides to the human population. The objectives of this article were to summarize advances in
Health hazards
Pesticide removal options
research related to pesticide residues in drinking water; conduct health risk assessments by estimating the daily
intake of pesticide residues consumed only from drinking water by adults, children, and infants; and summarize
options for pesticide removal from water systems. Approximately 113 pesticide residues were found in drinking
water samples from 31 countries worldwide. There were 61, 31, and 21 insecticide, herbicide, and fungicide
residues, respectively. Four residues were in toxicity class IA, 14 residues were in toxicity class IB, 55 residues
were in toxicity class II, 17 residues were in toxicity class III, and 23 residues were in toxicity class IV. The
calculated hazard indices (HIs) exceeded the value of one in many cases. The lowest HI value (0.0001) for
children was found in Canada, and the highest HI value (30.97) was found in Egypt, suggesting a high potential
health risk to adults, children, and infants. The application of advanced oxidation processes (AOPs) showed
efficient removal of many pesticide classes. The combination of adsorption followed by biodegradation was
shown to be an effective and efficient purification option. In conclusion, the consumption of water contaminated
with pesticide residues may pose risks to human health in exposed populations.

1. Introduction various residues.

1.1. Water
Clean water is an important part of ecosystems and plays an
important role in the sustainability of life on earth. It is a well-
established fact that access to clean water is a fundamental human
right and vital to sustain healthy life. Water contamination may pose a
risk to many types of organisms, including humans. There is great
concern about water contamination from pesticide residues.
Several efforts have been broadly applied to protect water bodies.
Some have succeeded in some countries and failed in others due to the
growing demand for food due to population growth.
To date, the growing demand for food has resulted in the intensive
use of pesticides in agricultural systems for insect, weed, and fungal
control. Despite the success that pesticide application achieves in terms
of food security, it results in contamination of water systems with
It is well documented in the literature that contamination-free water
is an essential part of a healthy, balanced diet because the body relies on
it to function properly. The human body consists of approximately
50–80% water. All chemical processes that take place in the human body
occur in water. Human bodies need contamination-free water to digest
food, absorb nutrients, remove waste metabolites, and maintain the
human body at an isometric body temperature.
Water systems may receive anthropogenic pollution in several ways,
such as from chemical industry discharge (Cho et al., 2020; Posthuma
et al., 2020), wastewater discharge (Gómez-Sanabria et al., 2020;
El-Nahhal et al., 2020), agricultural wastes (Wu et al., 2020; Hodomihou
et al., 2020; Garrido et al., 2020; Natasha et al., 2020; Zhi et al., 2020)
and pesticide residues (Chowdhury et al., 2012; Flores-García et al.,
2011; Varca, 2012; Donald et al., 2007; Teklu et al., 2015; Wan et al.,
2019, 2021; Tröger et al., 2021; Mahai et al., 2021).

* Corresponding author. Gaza, P. O. Box 108, Palestine.

E-mail address: y_el_nahhal@hotmail.com (Y. El-Nahhal).

https://doi.org/10.1016/j.jenvman.2021.113611
Received 7 March 2021; Received in revised form 13 August 2021; Accepted 23 August 2021
Available online 6 September 2021
0301-4797/© 2021 Elsevier Ltd. All rights reserved.
I. El-Nahhal and Y. El-Nahhal
1.2. Occurrence of pesticide residues in water
Pesticide residues may become present in water through one or more
of the pathways described in the following sections.
1.2.1. Pesticide residues in agricultural ecosystems
Pesticides are used in agriculture to control insects, nematodes, ro­
dents, weeds, and fungi. Currently, more than 1100 pesticides (in­
secticides, acaricides, herbicides, fungicides, and rodenticides) are
marketed in European countries (Jeong et al., 2012; Affum et al., 2018;
Lu et al., 2017; Burri et al., 2019) for public use.
The public health sector (PHS) uses permethrin, malathion, piper­
onyl butoxide, and isododecane in homes, schools, offices and stores to
control insects of public health importance (Giddings et al., 2016;
Ankley and Collyard, 1995; Rubin et al., 2002; Markowitz, 1992; Cen­
ters for Disease Control and Prevention, 2011; Liu et al., 2018; Buhl
et al., 2010; Health Consultation, 2010). Additionally, the PHS uses
indoxacarb, dinotefuran, and cyantraniliprole outdoors to control house
flies (Zahn et al., 2019) and mosquitos (Hustedt et al., 2020; Rohani
et al., 2020).
Although pesticide application is necessary to achieve high yields of
products, its application has resulted in food and water contamination
(El-Nahhal 2004, 2020) and continuous damage to ecosystems because
more than 90% of applied pesticides do not reach the target species
(Llorent-Martínez et al., 2011).
Water is an important component of public health, and the failure to
supply safe drinking water results in a substantial health burden on
humanity (van der Kooij, 2014).
1.2.2. Aerial application of pesticides
The aerial application of pesticides may contaminate surrounding
areas with macrodroplets and/or microdroplets (drift) of pesticide res­
idues. Several authors have demonstrated that pesticide sprayers influ­
ence pesticide deposition and distribution far from spraying sites. For
instance, Suarez-Lopez et al. (2020) indicated that pesticide drift caused
acetylcholine esterase inhibition in children living within 1000 m of a
greenhouse. An et al. (2020) detected myclobutanil and tebuconazole in
soil samples 5 m away from the application site. Wang et al. (2020)
indicated that wind speed and droplet size play a critical role in the drift
contamination potential of water resources. Furthermore, the applica­
tion of ultralow-volume aerosols of insecticides to control mosquitoes
results in contaminated water resources (Britch et al., 2018; Chasko­
poulou et al., 2018; Zhang et al., 2015; Mount, 1998).
1.2.3. Indoor and outdoor application
Indoor and outdoor application of pesticides causes critical
contamination of water bodies.
For instance, Lu et al. (2020) revealed cascading effects caused by
fenoxycarb in freshwater systems dominated by Daphnia carinata and
Dolerocypris sinensis. Bao et al. (2020) found that a low concentration of
carbendazim in water systems negatively affected zebrafish (Danio
rerio).
1.2.4. Soil erosion
Soil contains clay minerals, organic matter, and colloidal particles
that can determine the fate of pesticides. These materials can actively
adsorb pesticides from the aqueous phase in soil (El-Nahhal et al., 1998;
Nir et al., 2000). Dry conditions may result in soil erosion and the
transfer of soil particles from one place to another, resulting in the
transfer of the soil components that adsorb pesticides to aquatic systems.
Rheinheimer Dos Santos et al. (2020) have found five herbicides (2,4-D,
atrazine, desethyl-atrazine, simazine, and nicosulfuron), three fungi­
cides (carbendazim, epoxiconazole, and tebuconazole), and one insec­
ticide (imidacloprid) in epilithic biofilms due to high rainfall rates and
inadequate soil use. Ukalska-Jaruga et al. (2020a, 2020b) identified a
wide range of organochlorine pesticides (OCPs) (0.01–21,888 μg/kg) in
2
Journal of Environmental Management 299 (2021) 113611
soil samples collected from areas around previous pesticide storage fa­
cilities and in arable soils of Central and Eastern European countries. In
addition, He et al. (2020) found considerable concentrations of
dichlorodiphenyltrichloroethane (DDT) and hexachlorocyclohexane
(HCH) in the sediments of the Meijiang River Basin. Bento et al. (2019)
found that glyphosate and aminomethylphosphonic Acid (AMPA) con­
tents were 1.1–17.5 times higher in water-eroded sediment than in soil.
1.2.5. Dust fall
Dust comprises fine solid particles composed of organic and inor­
ganic molecules. Dust may have a variety of shapes and sizes and can be
carried by winds to different distances based on its size and wind speed
and direction. Dust can carry pesticide residues due to adsorption forces.
Seven insecticides (carbaryl, propoxur, chlorpyrifos, diazinon, cyflu­
thrin, cypermethrin, and permethrin), five herbicides (2,4-dichlor­
ophenoxyacetic acid [2,4-D], chlorthal, dicamba, mecoprop, and
simazine), and one synergist (piperonyl butoxide) were identified in
≥25% of carpet dust samples (Deziel et al., 2015). Additionally, five
insecticides (chlorpyrifos, diazinon, permethrin, allethrin, and cyper­
methrin) and one synergist (piperonyl butoxide) were identified in
household and urban dust samples (Quirós-Alcalá et al., 2011). Addi­
tionally, six insecticides (carbaryl, chlorpyrifos, chlorthal-dimethyl,
diazinon, iprodione, and phosmet) and one herbicide (simazine) were
identified in carpet dust samples collected within 1250 m of 89 resi­
dences in California (Gunier et al., 2011). Moreover, insecticides used in
urban settings, such as fipronil, have been determined in urban dust (Lin
et al., 2009) and in indoor and outdoor dust (Mahler et al., 2009; Shi
et al., 2020). Therefore, dust can be additional source of drinking water
contamination. To date, pyrethroid insecticides have been detected in
dust from the driveway, curb gutter and street at rates of 53.5–94.8%,
with median concentrations of 1–46 ng/g (Richards et al., 2016). Urban
and residential concrete surfaces are often treated with pesticides to
control ants (Jiang et al., 2014).
1.2.6. Rainfall
Rainfall and runoff characteristics can affect pesticide export from
small headwater catchments due to factors such as pesticide application
dose and timing and the variation in pesticide stocks in soil and soil type.
Intense rainfall-runoff events, which can fragment soil, control the
export of simazine and tetraconazole (Imfeld et al. (2020). Heavy
rainfall enhances the release of rodenticides from baited sewer
systems and outdoor surfaces into receiving streams (Regnery et al.,
2019, 2020). Additionally, water irrigation contributes to pesticide
losses from agricultural lands to water systems (Whelan et al., 2020).
1.2.7. Runoff
Storm water runoff infiltration systems may deteriorate the quality of
groundwater. In fact, storm water runoff contains suspended particulate
matter and many ionic organic molecules, such as pesticides and de­
tergents, that can contaminate groundwater. For instance, in one study,
concentrations of carbendazim, diuron, fluopyram, imidacloprid, and
lamotrigine significantly increased in groundwater impacted by infil­
tration, indicating that storm water runoff infiltration systems
contribute to groundwater contamination (Pinasseau et al., 2020). In
addition, concentrations of diuron, metolachlor, chlorpyrifos, simazine,
galaxolide, and triallate were found to have increased in storm water
recycled via aquifers (Page et al., 2014). Similarly, in another study,
concentrations of desethylatrazine, simazine, atrazine, terbuthylazine,
diuron, metolachlor, and diazinon increased in artificial recharge of
aquifers used for drinking water production in many countries (Kuster
et al., 2010). Moreover, high concentrations of 3,4-dichloroaniline,
molinate, desethylatrazine, dimethoate, simazine, atrazine, metola­
chlor and chlorpyrifos are present in the Ebro River basin area (Claver
et al., 2006). Additionally, considerable concentrations of terbutryn,
diuron, imidacloprid, 2,4-D, and diazinon have been identified in agri­
cultural runoff (García-Galán et al., 2020). Furthermore, considerable
I. El-Nahhal and Y. El-Nahhal
concentrations of four pyrethroids (bifenthrin, permethrin, cyfluthrin,
and cyhalothrin) and fipronil were detected in wash-off water from
concrete surfaces, indicating an additional source of water contamina­
tion (Jiang et al., 2010). Additionally, urban surface runoff has been
found to be contaminated with considerable concentrations of fiproles
and their degradation products (Cryder et al., 2019).
1.2.8. Air pollution
Pesticides that have high volatility may move via air systems and
substantially contaminate water systems. For instance, Kim et al. (2020)
found higher concentrations of total (Σ3) endosulfan (50.3–611 pg/m3,
mean: 274 pg/m3) in air samples than in water and soil samples during
summer.
Similarly, Jeon et al. (2019) determined the concentration of hex­
abromocyclododecanes (HBCDs) in air, water, soil, and sediment sam­
ples in South Korea and found that the Ʃ3 HBCDs were 22–133 pg/m3,
10–128 ng/g, 0.2–151 ng/L, and 0.5–552 ng/g for these samples,
respectively. However, Zhou et al. (2020) determined various levels of
neonicotinoid insecticides in respirable fine particulate matter (PM2.5),
suggesting risk factors for human health.
1.3. Potential health risk associated with contaminated water
It has been shown that exposure to pesticide residues may cause
reproductive toxicity to both men and women (El-Nahhal, 2020),
disruption in the endocrine system (Miranda-Contreras et al., 2013),
enhancement of human breast cancer (Yang et al., 2020) and prostate
cancer (Pardo et al., 2020), Parkinson’s disease (Pouchieu et al., 2018),
and cardiovascular toxicity (El-Nahhal and El-Nahhal, 2021).
1.4. Pesticide residue removal options
Method for removing pesticide residues from water include physical,
chemical and/or biological methods. For instance, physical methods
include adsorption and/or filtration using clay and organoclay (Boyd
et al., 1988; Boyd and Jaynes, 1992; Nir et al., 2000; El-Nahhal and Safi,
2010), activated carbon (Alves et al., 2019; Gamboa-Carballo et al.,
2016), nanoparticles (Brooks et al., 2012), and plant materials (El-Ba­
kouri et al., 2007). Chemical methods include photochemical reactions
or zerovalent iron that produce hydrogen peroxide radicals that strongly
interact with organic pollutants and convert them to nontoxic fragments
(Buxton et al., 1988; Munter, 2001; Stefan, 2017). Additionally, bio­
logical methods use living plants, fungi and/or bacteria to remove
pesticide residues from contaminated water (Escoto et al., 2019 Lucas
et al., 2008).
Furthermore, Snow et al. (2020) detected high concentrations of
γ-HCH, p,p’-DDE, and dieldrin in water samples collected from the Syr
Darya River. Li et al. (2020) detected the concentration profiles of
organochlorine pesticides in surface seawater and lower atmosphere gas
samples between 18◦ N and 40◦ S in the open Pacific Ocean in
2006–2007. They found higher concentrations of α-HCH, γ-HCH,
trans-chlordane, and cis-chlordane in the Northern Hemisphere than in
the Southern Hemisphere in both the air and water phases. Wu et al.
(2020) found high concentrations of HCHs and low concentrations of p,
p’- and o,p’-DDT in near east Antarctica and in the Ross Sea.
A few reviews have focused on pesticide residues in drinking water
samples at a global level. For instance, Morrissey et al. (2015) reviewed
global surface water contamination with neonicotinoids and character­
ized the associated risk to aquatic invertebrates, where they recom­
mended a threshold of 0.013–0.067 μg/L for imidacloprid, which is
quite different from the USEPA 2017 recommendations.
Bruce-Vanderpuije et al. (2019) characterized the status of persistent
organic pollutants, whereas Mohammed et al. (2019) reviewed insecti­
cide residues in different matrices in Ghana. Elibariki and Maguta
(2017) characterized the status of pesticide pollution in Tanzania. Li and
Jennings (2017) reviewed the worldwide regulations of standard values
3
Journal of Environmental Management 299 (2021) 113611
of pesticides for human health risk control. Recently, Olisah et al. (2020)
reviewed the occurrence of organochlorine pesticide residues in bio­
logical and environmental matrices in Africa. These reviews focused on
narrow scales and locations, and they did not evaluate the health risk
among adults, children, and infants or discuss the potential health risks
of pesticide residues found in water. The objectives of this article are to
summarize the advances in research related to pesticide residues in
drinking water; estimate the daily intake and health hazards of pesticide
residues consumed only from drinking water by adults, children, and
infants; and summarize pesticide removal options from water systems.
2. Methodology
2.1. Data collection
Following the procedure reported by Prosser et al. (2020) with slight
modification, an extensive search of scholarly databases, such as Scopus,
Web of Science, Science Direct, PubMed, BMC, Research Gate, and
Google Scholar, was conducted using the following specific keywords:
‘pesticide residues in drinking water’, ‘insecticide residues and drinking
water’, ‘fungicide residues and drinking water’, ‘herbicide residues and
drinking water’, ‘water and pesticide contamination’ [(organochlorine
insecticides and water) (organophosphate residues and drinking
water)], ‘water contamination and pesticides’, ‘human health effect­
s/impacts/risks’ and ‘pesticides and health risk’.
2.2. Inclusion and exclusion criteria
The full texts of the articles were downloaded and carefully
reviewed. Articles that identified pesticide residues in drinking water
samples collected from different locations in a country, on different
continents, and in different drinking wells/or well survey processes in a
country were considered relevant to this review and included in the
study. Articles that developed analytical methods and validated them for
pesticide monitoring programs were considered relevant to the review
and included in the study. Review articles on pesticides and water were
considered relevant and included. Articles that developed and validated
analytical methods and/or techniques to determine pesticide residues in
water samples in the laboratory were excluded. Articles that surveyed
pesticide residues in agricultural water systems, rivers, and/or lakes
were considered irrelevant and excluded.
2.3. Data processing and calculations
Pesticide residue information was collected from the included arti­
cles and classified into insecticide, herbicide and fungicide residue
groups.
The majority of the collected articles presented pesticide residues as
averages, whereas the minority of articles presented pesticide residues
as a range, minimum, maximum, 25th percentile, 50th percentile and
75th percentile. The presented averages in the majority of articles were
used to estimate the optimal daily intake (ODI). This value was denoted
as the optimal scenario.
Some articles presented data as minima, maxima and/or percentiles
(the minority of articles), and the average was calculated from the
presented data.
The average concentration of pesticide residue presented as mg/L
was multiplied by 1000 as a conversion factor to convert it to μg/L.
2.4. Health risk assessment and estimation of pesticide daily intake
The health risk assessment was conducted by estimating pesticide
intake from drinking water using data on average pesticide residue ob­
tained from the literature and water consumption for adults, children,
and infants. Hazard quotients (HQs) and hazard indices (HIs) were
calculated based on equations (1)–(3).
I. El-Nahhal and Y. El-Nahhal
2.4.1. Optimal daily intake (ODI)
The ODI of the pesticide residue was estimated according to equation
(1),
[ODI] = ([APS] × Q)/BW (1)
where [APS], Q, and BW are the average concentration of a pesticide
residue found in a drinking water sample (μg/L), the amount of water
consumed by a person and body weight (kg), respectively. Water con­
sumption equals 2, 1.5 and 0.75 L for adults, children and infants,
respectively, and the BW of adults, children and infants is 60, 15 and 5
kg, respectively (WHO, 2017).
2.5. Characterization of HQ and HI
HQ was estimated according to equation (2):
HQ = [ODI]/ARfD (2)
where HQ is the health quotient and ARfD is the acute reference dose of
pesticide residue expressed in μg/L/day. The use of ARfD was previously
reported (Bommuraj et al., 2019; US EPA, 2000). The value of ARfD was
obtained from the Pesticides Properties DataBase (PPDB) (2007) and its
updates.
When a water sample contains more than one pesticide residue, the
HQ is calculated individually for each sample. HI values ≥ 1 indicate
additive effects and a high risk, whereas values < 1 indicate low or
negligible health risk (US EPA, 2000).
HI=HQ1+HQ2+ HQ3+HQ4+HQ5+ … HQn (3)
When a sample contains only one pesticide residue,
HI=HQ (4)
In fact, the HQ was added to equation (3) because a mixture of
pesticide residues in which each individual residue is present in the
mixture at a level approximating the no observed effect level elicits a
measurable response denoted as a joint additive effect. Thus, the sum­
mation of individual effects is given in equation (3). This is in accor­
dance with the US Environmental Protection Agency (EPA) (2000) and
Tinwell and Ashby (2004), who emphasized the joint additive effects of
chemical mixtures.
2.6. Prediction of HI due to repeated consumption
Using the equations mentioned above, the HI was estimated at 1, 10,
25, 50 and 75 times the consumption of drinking water during the year
by multiplying the ODI by a factor of 10, 25, 50, and 75, respectively.
Then, the HI was calculated according to the equations mentioned
above. This approach provided useful information to predict the future
HI due to the consumption of contaminated water.
2.7. Meta-analysis of pesticide residues
2.7.1. Concentration groups
Concentrations of pesticide residues found in the water samples were
subdivided into three groups. Group 1 included concentrations above
the ARfD value, denoted as high concentrations. Group 2 included
concentrations equal to or five times lower than the ARfD value, denoted
as medium concentrations, and group 3 included concentrations below
those in group 2, denoted as diluted concentrations.
2.7.2. Classification of pesticide residues according to toxicity class and
function
The pesticide residues found in the water samples from a country
were subdivided into three groups according to their functions: insec­
ticide, fungicide, and herbicide residues. Each group was subdivided
into four toxicity classes (Ia, Ib, II, III and IV) according to the World
4
Journal of Environmental Management 299 (2021) 113611
Health Organization (WHO) guidelines (2009).
2.7.3. Statistical analysis of pesticide residue means
Based on recently published studies and other modifications
(El-Nahhal, 2020), the reference average (Ref Aver) of the insecticide,
herbicide or fungicide concentrations (μg/L) was calculated by summing
the corresponding concentrations (e.g., insecticide residues) in all
countries and dividing them by the corresponding total number of res­
idues (e.g., insecticide residues).
The country average insecticide, herbicide or fungicide concentra­
tion (μg/L) was calculated by summing the corresponding concentra­
tions (e.g., insecticide residues) in a country (e.g., Lebanon) and
dividing them by the number of insecticides detected in the water
samples. The calculation mentioned above was used for insecticides,
herbicides, and fungicides. The relative average (Rel Aver) in each
country was calculated according to equation (5).
Country average
Rel Aver = (5)
Reference average
Based on the results of equation (5), water samples from different
countries were subdivided into four groups as follows:
Group 1 included countries with Rel Aver values below 0.01, group 2
included countries with Rel Aver values between 0.01 and 0.1, group 3
included countries with Rel Aver values between 0.11 and 0.5, and
group 4 included countries with Rel Aver values ≥ 0.51.
To estimate the significant differences between the Rel Aver values of
various countries, the reference standard deviation (Ref Stdev) was
calculated from the general formula of the calculation. Then, the relative
standard deviation of a country was calculated according to equation
(6):
Country Stdev
Rel Stdev = (6)
Reference Stdev
Then, the Rel Stdev value was used to estimate the relative standard
error (Rel Std Error) from equation (7) as follows:
Rel Stdev
Rel Std Error = √ ̅̅̅ (7)
2
n
where n is the number of pesticide residues used to calculate the Rel
Aver and/or Rel Stdev in a country. The Rel Std Error values were used
to indicate the error bars in the figures. The overlapping error bars
indicate no significant difference in the relative means at a p-value ≤
0.05, whereas no overlap indicates a significant difference in the Rel
Aver in the studied countries.
3. Results and discussion
Approximately 39 articles that detected pesticide residues in 31
countries were included in this review. These articles were published
during 2000–2021, except two articles published in the 1990s. More
than one relevant article from some countries, such as China, India,
Portugal and the USA, was included in this review to integrate the
collected information and to obtain a clear picture of the data. The
countries included in the study were Brazil, Burkina Faso, Canada, China
(4); Co^te d’Ivoire, Egypt, Ethiopia, France, Germany, Ghana (2); India
(2); Iran (2); Ireland, Japan, Lebanon, Luxembourg, Mexico, Nicaragua,
Nigeria, Philippines, Portugal (2); Slovenia, South Africa, Spain,
Thailand, Togo (Africa), Turkey, USA, Vietnam, and West Bengal. The
number in brackets indicates the included articles from a country.
3.1. Pesticide residues in drinking water
3.1.1. Organochlorine (OC) insecticide residues
The average concentrations of the OC residues found in water sam­
ples in several countries are shown in Table 1. Approximately 1116
I. El-Nahhal and Y. El-Nahhal Journal of Environmental Management 299 (2021) 113611

Table 1
Average concentration of insecticide residues in drinking water.
3
RN CF ARfD μg/L Average daily intake ng/g *10− HQ AS DR Cn Au
μg/L
Ad Ch In Ad Ch In

α-HCH 0.01 6.00 0.20 0.59 0.88 0.00 0.00 0.00 27 14 China Wu et al. (2014)
β-HCH 0.01 6.00 0.48 1.45 2.18 0.00 0.00 0.00
γ-HCH 0.01 0.30 0.29 0.88 1.32 0.00 0.00 0.00
δ-HCH 0.01 6.00 0.49 1.46 2.18 0.00 0.00 0.00
p, p′ -DDE 0.05 0.50 1.56 4.68 7.02 0.00 0.01 0.01
p, p′ -DDD 0.00 0.50 0.03 0.10 0.16 0.00 0.00 0.00
p, p′ -DDT 0.00 0.50 0.15 0.46 0.70 0.00 0.00 0.00
Heptachlor 0.02 0.50 0.73 2.20 3.30 0.00 0.00 0.01
Heptachlor- epo 0.01 0.50 0.41 1.23 1.85 0.00 0.00 0.00
HCB 0.02 6.00 0.55 1.65 2.48 0.00 0.00 0.00
Aldrin 0.03 0.03 0.92 2.76 4.14 0.03 0.09 0.14
Dieldrin 0.01 0.05 0.45 1.34 2.01 0.01 0.03 0.04
Endrin 0.01 0.30 0.38 1.15 1.73 0.00 0.00 0.01
Endrin aldehyde 0.01 0.30 0.21 0.62 0.92 0.00 0.00 0.00
HI 0.05 0.15 0.22
α-HCH 0.002 6.00 0.07 0.21 0.31 0.00 0.00 0.00 17 8 China Liu et al. (2016)
β-HCH 0.003 6.00 0.09 0.27 0.40 0.00 0.00 0.00
γ-HCH 0.001 0.30 0.05 0.15 0.22 0.00 0.00 0.00
δ-HCH 0.000 6.00 0.00 0.00 0.01 0.00 0.00 0.00
p,p’-DDE 0.002 0.50 0.06 0.19 0.29 0.00 0.00 0.00
p,p’-DDD 0.000 0.50 0.01 0.03 0.05 0.00 0.00 0.00
o,p’-DDT 0.001 0.50 0.04 0.11 0.16 0.00 0.00 0.00
p,p’-DDT 0.001 0.50 0.04 0.12 0.18 0.00 0.00 0.00
0.001 0.003 0.005
α-HCH 0.11 6 3.50 10.50 15.75 0.00 0.00 0.00 5 7 China Li et al. (2012)
β-HCH 0.52 6 17.33 52.00 78.00 0.00 0.01 0.01
γ-HCH 2.65 0.3 88.33 265.00 397.50 0.29 0.88 1.33
δ-HCH 0.17 6 5.67 17.00 25.50 0.00 0.00 0.00
o,p’-DDT 0.02 0.5 0.75 2.25 3.38 0.00 0.00 0.01
p,p’ -DDD 0.05 0.5 1.67 5.00 7.50 0.00 0.01 0.02
p,p’-DDT 0.03 0.5 0.92 2.75 4.13 0.00 0.01 0.01
HI 0.31 0.92 1.37
α-HCH 0.004 6 0.14 0.41 0.61 0.000 0.000 0.000 27 13 China Zhou et al. (2008)
β-HCH 0.018 6 0.60 1.81 2.71 0.000 0.000 0.000
γ-HCH 0.003 0.3 0.09 0.26 0.40 0.000 0.001 0.001
δ-HCH 0.008 6 0.28 0.84 1.26 0.000 0.000 0.000
Heptachlor 0.012 0.5 0.40 1.21 1.81 0.001 0.002 0.004
Aldrin 0.007 0.03 0.23 0.68 1.02 0.008 0.023 0.034
Heptachlor epoxide 0.012 0.5 0.39 1.18 1.77 0.001 0.002 0.004
p,p’-DDE 0.002 0.5 0.07 0.20 0.30 0.000 0.000 0.001
Diedrin 0.003 0.05 0.12 0.35 0.52 0.002 0.007 0.010
Endrin 0.002 0.3 0.08 0.23 0.34 0.000 0.001 0.001
p, p’-DDD 0.001 0.5 0.03 0.08 0.11 0.000 0.000 0.000
o, p’-DDT 0.001 0.5 0.02 0.07 0.11 0.000 0.000 0.000
p, p’-DDT 0.004 0.5 0.13 0.39 0.59 0.000 0.001 0.001
HI 0.013 0.038 0.057
3
RN CF ARfD μg/L Average daily intake ng/g *10− HQ AS DR Cn Au
μg/L
Ad Ch In Ad Ch In

α-HCH 0.01 6 0.40 1.20 1.80 0.00 0.00 0.00 38 11 India Kaushik et al. (2012)
γ-HCH 0.07 0.3 2.32 6.95 10.43 0.01 0.02 0.03
β-HCH 0.20 6 6.79 20.36 30.54 0.00 0.00 0.01
α-Endosulfan 0.18 6 5.86 17.57 26.36 0.00 0.00 0.00
β-Endosulfan 0.24 6 7.86 23.59 35.39 0.00 0.00 0.01
o,p′ -DDT 0.03 0.5 1.04 3.12 4.68 0.00 0.01 0.01
p,p′ -DDT 0.32 0.5 10.70 32.09 48.13 0.02 0.06 0.10
o,p′ -DDE 0.03 0.5 0.91 2.72 4.08 0.00 0.01 0.01
p,p′ -DDE 0.17 0.5 5.54 16.63 24.95 0.01 0.03 0.05
o,p′ -DDD 0.04 0.5 1.48 4.43 6.65 0.00 0.01 0.01
p,p′ -DDD 0.34 0.5 11.49 34.48 51.71 0.02 0.07 0.10
HI 0.07 0.22 0.33
α-HCH 0.09 6 3.11 9.32 13.98 0.00 0.00 0.00 60 12 India Mohapatra et al. (1995)
β-HCH 0.06 6 2.01 6.04 9.06 0.00 0.00 0.00
γ-HCH 0.07 0.3 2.32 6.97 10.45 0.01 0.02 0.03
pp’ DDT 0.18 0.5 5.95 17.85 26.78 0.01 0.04 0.05
op’-DDT 0.08 0.5 2.61 7.83 11.75 0.01 0.02 0.02
pp’-DDT 0.02 0.5 0.73 2.20 3.30 0.00 0.00 0.01
Op’-DDE 0.01 0.5 0.23 0.70 1.05 0.00 0.00 0.00
α-Endosulfan 0.03 6 1.10 3.30 4.95 0.00 0.00 0.00
β-Endosulfan 0.01 6 0.34 1.03 1.54 0.00 0.00 0.00
(continued on next page)

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I. El-Nahhal and Y. El-Nahhal Journal of Environmental Management 299 (2021) 113611

Table 1 (continued )
3
RN CF ARfD μg/L Average daily intake ng/g *10− HQ AS DR Cn Au
μg/L
Ad Ch In Ad Ch In

Aldrin 0.09 0.03 3.01 9.03 13.55 0.10 0.30 0.45

Dieldrin 0.02 0.05 0.53 1.60 2.40 0.01 0.03 0.05
Heptachlor 0.02 0.5 0.56 1.68 2.52 0.00 0.00 0.01
HI 0.14 0.42 0.63
a-HCH 0.014 6 0.47 1.40 2.10 0.000 0.000 0.000 18 Turkey Bulut et al. (2010)
b-HCH 0.159 6 5.30 15.90 23.85 0.001 0.003 0.004
g-HCH 0.014 0.3 0.47 1.40 2.10 0.002 0.005 0.007
d-HCH 0.034 6 1.13 3.40 5.10 0.000 0.001 0.001
Heptachlor 0.031 0.5 1.03 3.10 4.65 0.002 0.006 0.009
Aldrin 0.02 0.3 0.67 2.00 3.00 0.002 0.007 0.010
Heptachlor epoxide 0.007 0.5 0.23 0.70 1.05 0.000 0.001 0.002
a-Endosulfan 0.01 6 0.33 1.00 1.50 0.000 0.000 0.000
4,4′ -DDE 0.013 0.5 0.43 1.30 1.95 0.001 0.003 0.004
Dieldrin 0.011 0.05 0.37 1.10 1.65 0.007 0.022 0.033
Endrin 0.01 0.3 0.33 1.00 1.50 0.001 0.003 0.005
B-Endosulfan 0.009 6 0.30 0.90 1.35 0.000 0.000 0.000
4,4′ -DDD 0.025 0.5 0.83 2.50 3.75 0.002 0.005 0.008
Endrin aldehyde 0.027 0.3 0.90 2.70 4.05 0.003 0.009 0.014
Endosulfan sulfate 0.022 6 0.73 2.20 3.30 0.000 0.000 0.001
4,4′ -DDT 0.085 0.5 2.83 8.50 12.75 0.006 0.017 0.026
Endrin Ketone 0.02 0.3 0.67 2.00 3.00 0.002 0.007 0.010
Methoxychlor 0.032 5 1.07 3.20 4.80 0.000 0.001 0.001
0.030 0.089 0.134
δ-HCH 0.02 6 0.67 2.00 3.00 0.00 0.00 0.00 15 22 Lebanon Chaza et al. (2018)
2,4′ -DDD 12.82 0.5 427.33 1282.00 1923.00 0.85 2.56 3.85
4,4′ -DDE 0.03 0.5 1.00 3.00 4.50 0.00 0.01 0.01
4,4′ -DDT 0.3 0.5 10.00 30.00 45.00 0.02 0.06 0.09
2,4′ -DDT 0.39 0.5 13.00 39.00 58.50 0.03 0.08 0.12
4,4′ -DDD 0.15 0.5 5.00 15.00 22.50 0.01 0.03 0.05
Aldrin 2.3 0.03 76.67 230.00 345.00 2.56 7.67 11.50
Heptachlor epoxide 9.01 0.5 300.33 901.00 1351.50 0.60 1.80 2.70
Dieldrin 2.72 0.05 90.67 272.00 408.00 1.81 5.44 8.16
Endosulfan 0.05 6 1.67 5.00 7.50 0.00 0.00 0.00
Endrin 0.28 0.3 9.33 28.00 42.00 0.03 0.09 0.14
Endrin aldehyde 0.06 0.3 2.00 6.00 9.00 0.01 0.02 0.03
Endosulfan sulfate 0.63 6 21.00 63.00 94.50 0.00 0.01 0.02
Metoxychlor 0.13 5 4.33 13.00 19.50 0.00 0.00 0.00
Heptachlor 4.22 0.5 140.67 422.00 633.00 0.28 0.84 1.27
O,O,O-Triethylphosphate 0.33 100 11.00 33.00 49.50 0.00 0.00 0.00
Thionazin 2.13 100 71.00 213.00 319.50 0.00 0.00 0.00
Dimethoate 3.78 10 126.00 378.00 567.00 0.01 0.04 0.06
Disulfoton 2.34 100 78.00 234.00 351.00 0.00 0.00 0.00
Methyl-parathion 27.72 6 924.00 2772.00 4158.00 0.15 0.46 0.69
Parathion 2.08 6 69.33 208.00 312.00 0.01 0.03 0.05
Famphur 5.34 100 178.00 534.00 801.00 0.00 0.01 0.01
HI 6.39 19.16 28.74
3
RN CF ARfD μg/L Average daily intake ng/g *10− HQ AS DR Cn Au
μg/L
Ad Ch In Ad Ch In

α-HCH 0.03 6 0.88 2.63 3.94 0.00 0.00 0.00 16 15 South Africa Fatoki and Awofolu (2004)
HCB 0.03 6 1.01 3.04 4.56 0.00 0.00 0.00
β-HCH 0.02 6 0.56 1.69 2.53 0.00 0.00 0.00
δ-HCH 0.02 6 0.64 1.91 2.86 0.00 0.00 0.00
Heptachlor 0.01 0.5 0.40 1.20 1.80 0.00 0.00 0.00
Aldrin 0.01 0.03 0.25 0.75 1.13 0.01 0.03 0.04
g-Chlordane 0.02 0.5 0.69 2.06 3.09 0.00 0.00 0.01
2,4-DDE 0.01 0.5 0.26 0.77 1.16 0.00 0.00 0.00
Endosulfan 0.02 6 0.62 1.85 2.78 0.00 0.00 0.00
Dieldrin 0.01 0.05 0.19 0.57 0.86 0.00 0.01 0.02
2,4-DDD 0.01 0.5 0.18 0.55 0.83 0.00 0.00 0.00
Endrin 0.01 0.3 0.49 1.47 2.21 0.00 0.00 0.01
4,4-DDD 0.01 0.5 0.45 1.34 2.01 0.00 0.00 0.00
2,4-DDT 0.01 0.5 0.20 0.60 0.90 0.00 0.00 0.00
4,4-DDT 0.02 0.5 0.63 1.89 2.84 0.00 0.00 0.01
HI 0.02 0.06 0.09
a-HCH 0.06 6 2.00 6.00 9.00 0.00 0.00 0.00 36 14 Mexico Díaz et al., 2009
b-HCH 0.09 6 3.00 9.00 13.50 0.00 0.00 0.00
c-HCH 0.026 0.3 0.87 2.60 3.90 0.00 0.01 0.01
d-HCH 0.028 6 0.93 2.80 4.20 0.00 0.00 0.00
Heptachlor 0.039 0.5 1.30 3.90 5.85 0.00 0.01 0.01
Aldrin 0.021 0.3 0.70 2.10 3.15 0.00 0.01 0.01
(continued on next page)

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I. El-Nahhal and Y. El-Nahhal Journal of Environmental Management 299 (2021) 113611

Table 1 (continued )
3
RN CF ARfD μg/L Average daily intake ng/g *10− HQ AS DR Cn Au
μg/L
Ad Ch In Ad Ch In

Heptachlor epoxide 0.005 6 0.17 0.50 0.75 0.00 0.00 0.00

Endosulfan 0.003 6 0.10 0.30 0.45 0.00 0.00 0.00
p,p’-DDE 0.049 0.5 1.63 4.90 7.35 0.00 0.01 0.01
Endrin 0.005 0.3 0.17 0.50 0.75 0.00 0.00 0.00
p,p’-DDD 0.002 0.5 0.07 0.20 0.30 0.00 0.00 0.00
Endrin aldehyde 0.004 0.3 0.13 0.40 0.60 0.00 0.00 0.00
Endosulfan sulfate 0.024 6 0.80 2.40 3.60 0.00 0.00 0.00
p,p’-DDT 0.004 0.5 0.13 0.40 0.60 0.00 0.00 0.00
00 0.03 0.04
α-HCH 0.294 6 9.80 29.40 44.10 0.00 0.00 0.01 8 16 West Bengal Mondal et al. (2018)
β-HCH 0.563 6 18.77 56.30 84.45 0.00 0.01 0.01
γ-HCH 0.026 0.3 0.87 2.60 3.90 0.00 0.01 0.01
δ-HCH 1.106 6 36.87 110.60 165.90 0.01 0.02 0.03
2,4 ́ -DDE 0.101 0.5 3.37 10.10 15.15 0.01 0.02 0.03
4,4 ́ -DDE 0.049 0.5 1.63 4.90 7.35 0.00 0.01 0.01
2,4 ́ -DDD 0.014 0.5 0.47 1.40 2.10 0.00 0.00 0.00
4,4 ́ -DDD 0.059 0.5 1.97 5.90 8.85 0.00 0.01 0.02
2,4 ́ -DDT 0.091 0.5 3.03 9.10 13.65 0.01 0.02 0.03
4,4 ́ -DDT 0.526 0.5 17.53 52.60 78.90 0.04 0.11 0.16
α-endosulfan 0.068 6 2.27 6.80 10.20 0.00 0.00 0.00
β-endosulfan 0.055 6 1.83 5.50 8.25 0.00 0.00 0.00
Chlorpyrifos 0.092 5 3.07 9.20 13.80 0.00 0.00 0.00
Methyl parathion 0.095 6 3.17 9.50 14.25 0.00 0.00 0.00
Monocrotophos 0.009 0.3 0.30 0.90 1.35 0.00 0.00 0.00
Phorate 0.027 25 0.90 2.70 4.05 0.00 0.00 0.00
HI 0.073 0.218 0.327
γ-HCH 0.04 0.3 1.33 4.00 6.00 0.00 0.01 0.02 64 6 Ghana Fosu-Mensah et al. (2016)
α-Endosulfan 0.03 6 1.00 3.00 4.50 0.00 0.00 0.00
Dieldrin 0.03 0.05 1.00 3.00 4.50 0.02 0.06 0.09
DDT 0.04 0.5 1.33 4.00 6.00 0.00 0.01 0.01
Endosulfanulfate 0.04 6 1.33 4.00 6.00 0.00 0.00 0.00
Heptachlor 0.027 0.5 0.90 2.70 4.05 0.00 0.01 0.01
HI 0.03 0.09 0.13
β-HCH 0.01 6.00 0.33 1.00 1.50 0.00 0.00 0.00 44 13 Ghana Affum et al. (2018)
p,p′ -DDT 0.04 0.50 1.17 3.50 5.25 0.00 0.01 0.01
Endrin 0.01 0.30 0.33 1.00 1.50 0.00 0.00 0.01
Methoxychlor 0.01 5.00 0.33 1.00 1.50 0.00 0.00 0.00
Methamidophos 0.01 3.00 0.43 1.30 1.95 0.00 0.00 0.00
Fenpropathrin 0.04 30.00 1.27 3.80 5.70 0.00 0.00 0.00
L-cyhalothrin 0.01 5 0.33 1.00 1.50 0.00 0.00 0.00
Permethrin 0.03 250.00 1.03 3.10 4.65 0.00 0.00 0.00
Cyfluthrin 0.01 25 0.47 1.40 2.10 0.00 0.00 0.00
Cypermethrin 0.04 100 1.27 3.80 5.70 0.00 0.00 0.00
Deltamethrin 0.05 10.00 1.50 4.50 6.75 0.00 0.00 0.00
Chlorpyrifos 0.41 5 13.73 41.20 61.80 0.00 0.01 0.01
Ethoprophos 0.02 50.00 0.73 2.20 3.30 0.00 0.00 0.00
HI 0.007 0.020 0.030
3
RN CF ARfD μg/L Average daily intake ng/g *10− HQ AS DR Cn Au
μg/L
Ad Ch In Ad Ch In

Dieldrin 0.028 0.05 0.93 2.80 4.20 0.02 0.06 0.08 4 10 Philippines Navarrete et al. (2018)
Endrin aldehyde 0.74 0.3 24.67 74.00 111.00 0.08 0.25 0.37
α-HCH 0.039 6 1.30 3.90 5.85 0.00 0.00 0.00
β-HCH 0.036 6 1.20 3.60 5.40 0.00 0.00 0.00
δ-HCH 0.288 0.03 9.60 28.80 43.20 0.32 0.96 1.44
γ-Chlordane 0.02 0.5 0.67 2.00 3.00 0.00 0.00 0.01
Endosulfan 0.056 6 1.87 5.60 8.40 0.00 0.00 0.00
Heptachlor 0.029 0.5 0.97 2.90 4.35 0.00 0.01 0.01
Heptachlor epoxide 0.022 0.5 0.73 2.20 3.30 0.00 0.00 0.01
Methoxychlor 0.026 5 0.87 2.60 3.90 0.00 0.00 0.00
0.427 1.280 1.919
γ-HCH 0.3 0.3 10.00 30.00 45.00 0.03 0.10 0.15 7 9 Egypt Derbalah et al. (2014)
Heptachlor 0.18 0.5 6.00 18.00 27.00 0.01 0.04 0.05
Aldrin 6.00 0.03 200.00 600.00 900.00 6.67 20.00 30.00
Heptachlor epo. 0.23 0.5 7.67 23.00 34.50 0.02 0.05 0.07
Endosulfan 0.1 6 3.33 10.00 15.00 0.00 0.00 0.00
Dieldrin 0.14 0.05 4.67 14.00 21.00 0.09 0.28 0.42
Endrin 0.26 0.3 8.67 26.00 39.00 0.03 0.09 0.13
DDD 0.32 0.5 10.67 32.00 48.00 0.02 0.06 0.10
p,p′ -DDT 0.16 0.5 5.33 16.00 24.00 0.01 0.03 0.05
HI 6.88 20.65 30.97
(continued on next page)

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I. El-Nahhal and Y. El-Nahhal Journal of Environmental Management 299 (2021) 113611

Table 1 (continued )
3
RN CF ARfD μg/L Average daily intake ng/g *10− HQ AS DR Cn Au
μg/L
Ad Ch In Ad Ch In

p,p -DDE
′
0.06 0.5 2.00 6.00 9.00 0.00 0.01 0.02 3 14 Nicaragua McConnell et al. (1999)
p,p′ -DDD 0.1 0.5 3.33 10.00 15.00 0.01 0.02 0.03
o,p′ -DDT 0.2 0.5 6.67 20.00 30.00 0.01 0.04 0.06
p,p′ -DDT 1.2 0.5 40.00 120.00 180.00 0.08 0.24 0.36
β-HCH 0.7 6 23.33 70.00 105.00 0.00 0.01 0.02
γ-HCH 0.02 0.3 0.67 2.00 3.00 0.00 0.01 0.01
Toxaphene 10.07 100 335.67 1007.00 1510.50 0.00 0.01 0.02
Chlordimeform 2.6 100 86.67 260.00 390.00 0.00 0.00 0.00
Chlorpyrifos 0.3 5 10.00 30.00 45.00 0.00 0.00 0.00
Diazinon 0.07 30 2.33 7.00 10.50 0.00 0.00 0.00
Fenthion 4.5 7 150.00 450.00 675.00 0.02 0.06 0.10
Fenthion sulf. 1.4 7 46.67 140.00 210.00 0.01 0.02 0.03
Mephosfolan 0.7 500 23.33 70.00 105.00 0.00 0.00 0.00
Methyl parathion 0.85 6 28.33 85.00 127.50 0.00 0.01 0.02
HI 0.15 0.44 0.67
,4-DDE 0.02 0.5 0.67 2.00 3.00 0.00 0.00 0.01 9 7 Togo -Africa Mawussi et al. (2009)
4,4-DDT 0.03 0.5 1.00 3.00 4.50 0.00 0.01 0.01
Dieldrin 0.02 0.05 0.67 2.00 3.00 0.01 0.04 0.06
Heptaclor 0.33 0.5 11.00 33.00 49.50 0.02 0.07 0.10
Hepta epoxide 0.09 0.5 3.00 9.00 13.50 0.01 0.02 0.03
α-Endosulfan 0.05 6 1.67 5.00 7.50 0.00 0.00 0.00
β-Endosulfan 0.02 6 0.67 2.00 3.00 0.00 0.00 0.00
HI 0.05 0.14 0.20
Aldrin 0.37 0.03 12.33 37.00 55.50 0.41 1.23 1.85 9 5 Co^te d’Ivoire Wandan and Zabik (1996)
p,p’-DDT 0.47 0.5 15.67 47.00 70.50 0.03 0.09 0.14
Dieldrin 0.38 0.05 12.67 38.00 57.00 0.25 0.76 1.14
Endosulfan 1.73 6 57.67 173.00 259.50 0.01 0.03 0.04
γ-HCH 2.61 0.3 87.00 261.00 391.50 0.29 0.87 1.31
HI 1.00 2.99 4.48
γ-HCH 0.0004 0.3 0.01 0.04 0.07 0.000 0.000 0.000 40 2 Canada Woudneh et al. (2009)
Heptachlor 0.0000 0.5 0.00 0.00 0.00 0.000 0.000 0.000
Chlorpyriphos 0.0001 5 0.00 0.01 0.01 0.000 0.000 0.000
Phosmet 0.0000 45 0.00 0.00 0.00 0.000 0.000 0.000
Pirimiphos 0.0000 100 0.00 0.00 0.00 0.000 0.000 0.000
HI 0.000 0.000 0.000
heptachlor 0.039 0.5 1.30 3.90 5.85 0.00 0.01 0.01 3 2 Ireland McManus et al. (2013)
Lindane 0.042 0.3 1.40 4.20 6.30 0.00 0.01 0.02
HI 00 0.02 0.03
Chlordane 0.22 0.5 7.33 22.00 33.00 0.01 0.04 0.07 15 4 USA Eitzer and Chevalier (1999)
Lindane 0.06 0.3 2.00 6.00 9.00 0.01 0.02 0.03
Chlorpyrifos 0.06 5 2.00 6.00 9.00 0.00 0.00 0.00
Diazinon 0.02 30 0.67 2.00 3.00 0.00 0.00 0.00
HI 0.02 0.07 0.10
3
RN CF ARfD μg/L Average daily intake ng/g *10− HQ AS DR Cn Au
μg/L
Ad Ch In Ad Ch In

Azadirachtin 0.20 750.00 6.80 20.41 30.62 0.00 0.00 0.00 106 9 Burkina Faso Lehmann et al. (2017)
Carbofuran 0.06 5 2.01 6.02 9.03 0.00 0.00 0.00
Chlorpyrifos 0.06 5 1.84 5.51 8.27 0.00 0.00 0.00
λ-Cyhalothrin 0.03 5 0.98 2.94 4.41 0.00 0.00 0.00
Cypermethrin 0.22 100.00 7.32 21.97 32.96 0.00 0.00 0.00
Dieldrin 0.11 0.05 3.56 10.69 16.04 0.07 0.21 0.32
Imidacloprid 0.01 57 0.23 0.68 1.02 0.00 0.00 0.00
Profenofos 0.05 1000.00 1.63 4.90 7.35 0.00 0.00 0.00
Triazophos 0.001 1.00 0.04 0.13 0.20 0.00 0.00 0.00
0.07 0.22 0.33
carbaryl 0.170 10 5.65 16.95 25.43 0.001 0.002 0.003 4 16 Japan Tanabe et al. (2001)
chlorfenvinphos 0.012 5 0.40 1.20 1.80 0.000 0.000 0.000
chlorpyrifos 0.009 5 0.28 0.85 1.28 0.000 0.000 0.000
cyanophos 0.016 100 0.54 1.63 2.45 0.000 0.000 0.000
diazinon 0.040 25 1.33 4.00 6.00 0.000 0.000 0.000
dichlofenthion 0.010 100 0.33 1.00 1.50 0.000 0.000 0.000
dichlorvos 0.051 2 1.68 5.05 7.58 0.001 0.003 0.004
dimethoate 0.087 10 2.89 8.67 13.00 0.000 0.001 0.001
etofenprox 0.041 1000 1.37 4.10 6.15 0.000 0.000 0.000
fenitrothion 0.089 13 2.96 8.88 13.31 0.000 0.001 0.001
fenobucarb 0.074 100 2.45 7.35 11.03 0.000 0.000 0.000
malathion 0.026 300 0.85 2.55 3.83 0.000 0.000 0.000
propoxur 0.032 20 1.06 3.17 4.75 0.000 0.000 0.000
pyridaphenthion 0.040 100 1.34 4.03 6.04 0.000 0.000 0.000
isofenphos oxon 0.044 1 1.47 4.40 6.60 0.001 0.004 0.007
(continued on next page)

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I. El-Nahhal and Y. El-Nahhal Journal of Environmental Management 299 (2021) 113611

Table 1 (continued )
3
RN CF ARfD μg/L Average daily intake ng/g *10− HQ AS DR Cn Au
μg/L
Ad Ch In Ad Ch In

HI 0.004 0.011 0.017

3-Hydroxycarbofuran, 2.95 100 98.33 295.00 442.50 0.00 0.00 0.00 15 Spain Ccanccapa et al. (2016)
Methiocarb, 1.35 5 45.11 135.33 203.00 0.01 0.03 0.04
Imidacloprid 3.99 57 132.94 398.83 598.25 0.00 0.01 0.01
Azinphos Methyl 1.57 75 52.44 157.33 236.00 0.00 0.00 0.00
Chlorfenvinphos 10.83 20 360.89 1082.67 1624.00 0.02 0.05 0.08
Chlorpyrifos, 4.87 5 162.22 486.67 730.00 0.03 0.10 0.15
Diazinon, 6.94 30 231.22 693.67 1040.50 0.01 0.02 0.03
Diclofenthion, 16.40 500 546.78 1640.33 2460.50 0.00 0.00 0.00
Dimethoate, 21.95 10 731.56 2194.67 3292.00 0.07 0.22 0.33
Fenitrothion, 11.61 13 387.10 1161.29 1741.93 0.03 0.09 0.13
Fenthion, 1.01 100 33.67 101.00 151.50 0.00 0.00 0.00
Fenthion Sulfone, 1.80 100 59.89 179.67 269.50 0.00 0.00 0.00
Malathion 5.40 300 179.89 539.67 809.50 0.00 0.00 0.00
Omethoate 2.36 2 78.67 236.00 354.00 0.04 0.12 0.18
Parathion-Ethyl, 9.88 6 329.44 988.33 1482.50 0.07 0.20 0.30
HI 0.29 0.85 1.26
Dichlorvos 0.257 40 8.57 25.70 38.55 0.00 0.00 0.00 64 7 Iran Heidar et al. (2017)
Diazinon 0.21 30 7.10 21.30 31.95 0.00 0.00 0.00
Methyl parathion 0.57 6 19.10 57.30 85.95 0.00 0.01 0.01
Fenitrothion 0.28 40 9.47 28.40 42.60 0.00 0.00 0.00
Malathion 0.37 300 12.23 36.70 55.05 0.00 0.00 0.00
Profenofos 0.32 1000 10.50 31.50 47.25 0.00 0.00 0.00
Ethion 0.35 0.5 11.60 34.80 52.20 0.02 0.07 0.10
HI 0.03 0.08 0.12
Diazinon 57.53 30 1917.67 5753.00 8629.50 0.06 0.19 0.29 24 2 Iran Shayeghi et al. (2007)
malathion 38.69 300 1289.67 3869.00 5803.50 0.00 0.01 0.02
HI 0.07 0.20 0.31
Carbofuran 0.39 5 13.08 39.25 58.88 0.00 0.01 0.01 23 8 Brazil Albuquerque et al., 2016,
Imidacloprid 1.28 57 42.67 128.00 192.00 0.00 0.00 0.00
Chlorpyrifos 0.26 5 8.50 25.50 38.25 0.00 0.01 0.01
Dimethoate 2.56 10 85.17 255.50 383.25 0.01 0.03 0.04
Ethion 0.12 15 4.00 12.00 18.00 0.00 0.00 0.00
Malathion 0.22 300 7.48 22.43 33.64 0.00 0.00 0.00
Profenofos 0.01 1000 0.20 0.60 0.90 0.00 0.00 0.00
Permethrin 0.82 1500 27.17 81.50 122.25 0.00 0.00 0.00
HI 0.01 0.04 0.06
Diazinon 2.95 30 98.25 294.76 442.14 0.00 0.01 0.01 45 2 Ethiopia Mekonen et al. (2016)
Malathion 9.75 300 324.90 974.70 1462.05 0.01 0.03 0.05
HI 0.014 0.042 0.064
Fenobucarb 0.04 100 1.33 4.00 6.00 0.00 0.00 0.00 54 4 Vietnam Toan et al. (2013)
Fipronil 0.16 3 5.33 16.00 24.00 0.00 0.01 0.01
Buprofezin 0.12 500 4.00 12.00 18.00 0.00 0.00 0.00
Profenofos 0.04 1000 1.33 4.00 6.00 0.00 0.00 0.00
HI 0.002 0.005 0.008

Dimethoate 0.001 10 0.03 0.08 0.12 0.00 0.00 0.00 81 3 Portugal Palma et al. (2009)

Malathion 0.002 300 0.07 0.21 0.32 0.00 0.00 0.00

Diazinon 0.003 30 0.08 0.25 0.38 0.00 0.00 0.00
0.000 0.000 0.000
Diazinon 0.002 30 0.07 0.22 0.33 0.00 0.00 0.00 2 Portugal Palma et al. (2014)
Dimethoate 0.004 10 0.12 0.35 0.53 0.00 0.00 0.00
0.000 0.000 0.000
Diazinon 0.083 30 2.77 8.30 12.45 0.000 0.000 0.000 2 Nigeria Sosan et al., (2008)
Propoxur 0.029 20 0.97 2.90 4.35 0.000 0.001 0.001
HI 0.000 0.001 0.002
Chlorpyrifos 0.11 5 3.67 11.00 16.50 0.00 0.00 0.00 100 3 Thailand Jaipieam et al., (2009)
Dicrotophos 0.145 40 4.83 14.50 21.75 0.00 0.00 0.00
Profenofos 0.258 1000 8.60 25.80 38.70 0.00 0.00 0.00
HI 0.001 0.003 0.004
Diazinon 3.46 30 115.45 346.35 519.53 0.004 0.01 0.02 2 Germany Stehlea et al. 2019
Chlorpyrifos 0.18 5 5.85 17.55 26.33 0.001 0.00 0.01
HI 0.005 0.01 0.03

water samples from 31 countries around the world were analyzed for OC insecticides (14 compounds), organophosphorus (OP) insecticides
pesticide residues. Approximately 58 insecticide residues in addition to (27 compounds), carbamate (CT) insecticides (five compounds), pyre­
some metabolites were detected in the water samples at different fre­ throid (PY) insecticides (eight compounds), neonicotinoids (N) (one
quencies. These insecticides belong to different chemical groups, such as compound) and other chemical groups denoted as others (O) (three

9
I. El-Nahhal and Y. El-Nahhal
compounds).
Fig. 1a shows insecticide residues that were detected two times or
more. DDT and its analogs were detected 53 times among all residues,
whereas disulfoton was detected only one time. The OC residues
detected in water samples included fourteen parent compounds, aldrin,
chlordane, DDT, dieldrin, endrin, α-endosulfan, β-endosulfan, HCH,
heptachlor, lindane, methoxychlor, toxaphene, γ-chlordane, and γ-HCH
(α-HCH, β-HCH, γ-HCH, δ-HCH), and four metabolites, 1,1-dichloro-2,2-
bis(p-chlorophenyl)ethylene (DDE), 1,1-dichloro-2,2-bis(p-chloro­
phenyl)ethane (DDD), heptachlor-epo, and endrin aldehyde.
Approximately 42 OC residues with a concentration range of
0.001–2.65 μg/L were detected in the water samples from China (Wu
et al., 2014; Liu et al., 2016; Li et al., 2012; Zhou et al., 2008), and the
concentration of one residue exceeded the ARfD value. Twenty-three OC
residues with a concentration range of 0.01–0.34 μg/L were detected in
the water samples from India (Kaushik et al., 2012; Mohapatra et al.,
1995). Eighteen OC residues with a concentration range of 0.007–0.159
were identified in the water samples from Turkey (Bulut et al., 2010).
Fifteen OC residues were detected in the water samples from Lebanon,
with a concentration range of 0.02–12.82 μg/L, and concentrations of
five residues exceeded the ARfD value (Chaza et al., 2018). The water
samples from South Africa had a concentration range of 0.01–0.03 μg/L
(Fatoki and Awofolu, 2004). Fourteen OC residues were detected in the
water samples from Mexico, with a concentration range of 0.003–0.09
μg/L (Díaz et al., 2009). Twelve OC residues were detected in the water
samples from West Bengal, with a concentration range of 0.014–1.106
μg/L (Mondal et al., 2018). Ten OC residues were detected in the water
samples from Ghana, with a concentration range of 0.01–0.04 μg/L
(Fosu-Mensah et al., 2016; Affum et al., 2018), and from the Philippines,
with a concentration range of 0.02–0.74 μg/L (Navarrete et al., 2018).
Nine OC residues were detected in the water samples from Egypt, with a
concentration range of 0.10–6.00 μg/L (Derbalah et al., 2014). Seven OC
residues with a concentration range of 0.02–10.07 μg/L were detected in
the water samples from Nicaragua (McConnell et al., 1999) and from
Togo-Africa, with a concentration range of 0.02–0.33 μg/L (Mawussi
et al., 2009). Five OC residues with a concentration range of 0.37–2.61
μg/L were detected in the water samples from Co^te d’Ivoire (Wandan,
and Zabik, 1996). Two OC residues were detected in the water samples
from Canada (Woudneh et al., 2009), Ireland (McManus et al., 2013)
and the USA (Eitzer and Chevalier, 1999) with a concentration range of
0.0004–0.22 μg/L. One OC residue was detected in the water samples
from Burkina Faso at a concentration of 0.11 μg/L (Lehmann et al.,
2017). The occurrence of OC residues in water samples may be due to
direct application of OC insecticides in agricultural sections using
OC-contaminated pesticides, such as in China, where application of
Dicofol in cotton fields was a source of DDT contamination in northern
Jiangsu Province (Yang et al., 2008). In addition, flooding practices in
rice fields may enhance the distribution of OC from contaminated soil to
non-contaminated soil. Yao et al. (2007) emphasized this phenomenon.
However, historical application and illegal use of technical DDT or
dicofol may still occur in some urban areas. A similar explanation was
given for the distribution of DDT in Italian soil (Thiombane et al., 2018).
Bhadouria et al. (2012) indicated that concentrations of α-HCH, β-HCH,
γ-HCH, δ-HCH, aldrin, dieldrin, heptachlor, hept.epoxide, endosulfan-I,
endosulfan-II, endo.sulfate, endrin, 4,4′ -DDE, 4,4′ -DDD, and DDT were
high in the sediments in and out of Keoladeo National Park, an impor­
tant wintering ground in India. Additionally, contamination of surface
soil with OC insecticides from agricultural application became a major
source of water pollution in India (Khuman et al., 2020). Additionally,
OC insecticides may still be in use in India and be a major source of
water contamination. This finding is in accordance with a previous
report that indicated that OC insecticides are still being applied in India
(Bakore et al., 2004; Agarwal et al., 2015).
The occurrence of OC residues in water samples from Turkey may
emerge from using dicofol formulations contaminated with DDT or
other OC insecticide residues. This is in accordance with a report by
10
Journal of Environmental Management 299 (2021) 113611
Turgut et al. (2009), who found a high concentration (14.3%) of DDT in
dicofol formulations. Additionally, Pazi et al. (2011) found high con­
centrations of DDT and other OC residues in sediments from Izmir Bay
and from the Gediz River estuary, indicating OC insecticide usage,
probably linked to public health emergencies. Similarly, the distribution
of OC residues in Lebanon may have emerged from agricultural prac­
tices, high rainfall and movement of OC-contaminated sediment (Kou­
zayha et al., 2013). However, the occurrence of OC residues in water
samples in South Africa may have emerged from the use of OC in­
secticides in public health sectors. This is in agreement with a report by
Buah-Kwofie and Humphries (2017), who found high concentrations of
OC residues (e.g., DDT, HCH, Aldrin, endrin endosulfan and heptachlor)
in sediments collected from the lakes and wetlands of iSimangaliso.
Buah-Kwofie and Humphries attributed these high levels of OC residues
to the application of DDT and other insecticides for malaria control.
Furthermore, the occurrence of OC residues in water samples from
the USA may emerge from the direct application of OC insecticide on
cotton farms and contaminated air. This is in accordance with Hoh and
Hites (2004), who identified cotton farms and the Gulf of Mexico as
potential sources of toxaphene or DDEs. Similarly, Alegria et al. (2006)
found elevated levels of some OC pesticides (DDTs, chlordane, toxa­
phene) in the ambient air of Chiapas, Mexico, during 2000–2001, sug­
gesting a potential source of water contamination through air exchange
processes. The occurrence of OC residues in water samples from
Nicaragua may emerge from erosion of contaminated soil with OC res­
idues to water resources (Lacayo-Romero et al., 2006), whereas in the
Philippines, DDT and DDE sediment residues were slowly released into
sterile and nonsterile brackish water systems. DDT residues are easily
adsorbed in sediments (95.0%) and slowly released in hard water (8.4%)
and seawater (0.1%) (Bajet and Navarro, 2002). Studies from Ghana
revealed high levels of DDT and its isomers in mosquito breeding sites
(Kudom et al., 2018) and contaminated sediments in the harbor (Botwe
et al., 2017), suggesting that a history of OC insecticide application for
mosquito control could be the main source of contamination. In Canada,
Poole et al. (1998) indicated that the occurrence of OC residues in water
samples could be from long-range atmospheric transport, whereas
Bidleman et al. (2002) found that volatilization of OC residues from seas
and large lakes can be a source of water contamination based on the
appearance of nonracemic alpha-HCH in the air boundary layer above
the water. However, Marvin et al. (2004) showed that historical
contamination of sediments and large lakes could be a source of water
contamination with OC residues. However, Rawn et al. (2001) noted
that glacial runoff could be a significant source of OC residues for water
contamination. More recently, Jantunen et al. (2015) highlighted the
rule of air-water gas exchange as a source of OC residues in drinking
water. Studies from Egypt (Wahaab, and Badawy, 2004) indicated that
polluted lakes (Maryut and Manzala) and the Nile River could be the
source of OC residue transfer to drinking water.
The names of the OC residues, their concentrations, and the ARfD
values in each country are shown in Table 1. The highest concentrations
of OC residues (2,4′ -DDD, 12.82 μg/L; heptachlor epoxide, heptachlor
9.01; 4.22 μg/L; aldrin 6.0) were detected in water from Lebanon and
Egypt, and the lowest concentration was in water from Canada (hepta­
chlor, 0.000525 μg/L). The highest values of OC residues occurred in
water samples from Lebanon, and the lowest number occurred in water
samples from Burkina Faso.
The detection of OC residues in the water samples from the countries
mentioned above may be attributed to historical agricultural application
of these compounds. Moreover, OC residues continue to cycle through
various routes, such as atmospheric transport and runoff (Kim et al.,
2020), and to resist degradation and, thus, remain in the environment
for longer periods (Yadav et al., 2015). Consequently, OC residues are
transported via environmental components and can be detected again in
water (Table 1) and/or accumulate in fruit and vegetables (Mohammed
et al., 2019), honey (El-Nahhal, 2020) and plants (Panseri et al., 2014).
Additionally, DDT and/or its analogs have been used in the public health
I. El-Nahhal and Y. El-Nahhal Journal of Environmental Management 299 (2021) 113611

Fig. 1. a. Frequency of pesticide residues detection. Pesticide detection range is 2–50. The highest frequency detected pesticide is DDT (53 Times) and the lowest one
is tolchlofos methyl oxon. Pesticide residues detected only one time is not presented here. Fig. 1b. Number of pesticide residues detected in water samples from
different countries. Blue, orange and gray colors represent Insecticide, herbicide and fungicide residue detected respectively. (For interpretation of the references to
color in this figure legend, the reader is referred to the Web version of this article.)

11
I. El-Nahhal and Y. El-Nahhal
sector, such as for head lice control (El-Nahhal and Hammad et al.,
2019), and in the agriculture and public health sectors (Olisah et al.,
2019b).
Due to the high KOW values of OC residues, they remain in soil
components for a long time and can be adsorbed in clay minerals or soil
organic matter due to their high hydrophobicity and then slowly
released in water systems (Umulisa et al., 2020; Ukalska-Jaruga et al.
(2020a, 2020b); Bhandari et al., 2020). OC residues may evaporate from
the soil to the atmosphere and diffuse throughout water systems, as
noted in several published studies (Hearon et al., 2020; Kim et al., 2020;
Jeon et al., 2019; Snow et al., 2020; Karlsson et al., 2000).
3.1.2. Organophosphate (OP) insecticide residues
The average concentrations of organophosphate (OP) residues in
the water samples are presented in Table 1. Approximately 27 OP
residues were detected in the water samples from many countries. OP
residues include azinphos-methyl, chlorfenvinphos, chlorpyrifos,
cyanophos, diazinon, dichlofenthion, dichlorvos, dicrotophos, dimeth­
oate, ethion, ethoprophos, fenitrothion, fenthion, isofenphos-oxon,
malathion, mephosfolan, methamidophos, monocrotophos, omethoate,
parathion-ethyl, parathion-methyl, phosphate, photoset, profenofos,
pyridafenthion, thionazin, and triazophos.
For instance, fourteen OP residues were detected in water samples
from Japan (Tanabe et al., 2001). Twelve OP residues with a concen­
tration range of 1.01–21.95 μg/L were identified in the water samples
from Spain (Ccanccapa et al., 2016). Nine OP residues with a concen­
tration range of 0.21–0.57 μg/L were identified in the water samples
from Iran (Heidar et al., 2017; Shayeghi et al., 2007), and seven OP
residues with a concentration range of 0.33–27.72 μg/L were found in
the water samples from Lebanon (Chaza et al., 2018). Six OP residues
with a concentration range of 0.07–4.5 μg/L were detected in the water
samples from Nicaragua (McConnell et al., 1999), and five OP residues
with a concentration range of 0.01–2.56 μg/L were detected in the water
samples from Brazil (Albuquerque et al., 2016).
Four OP residues with a concentration range of 0.01–0.41 μg/L were
detected in the water samples from Ghana (Affum et al., 2018), OP
residues with a concentration range of 0.009–0.095 μg/L were found in
the water samples from West Bengal (Mondal et al., 2018), and OP
residues with a similar concentration range were detected in the water
samples from Vietnam (Toan et al., 2013).
Three OP residues with a concentration range of 0.001–0.06 μg/L
were detected in the water samples from Burkina Faso (Lehmann et al.,
2017), Portugal (Palma et al. 2009, 2014), and Canada (Woudneh et al.,
2009). Two OP residues with a concentration range of 0.06–0.22 μg/L
were detected in the water samples from the USA (Eitzer and Chevalier,
1999), two with a concentration range of 2.95–9.75 μg/L were detected
in the water samples from Ethiopia (Mekonen et al., 2016), and 2 with a
concentration range of 0.18–3.46 μg/L were detected in the water
samples from Germany (Stehle et al., 2019). Compared with OC resi­
dues, OP residues were less frequently detected in water samples. For
instance, diazinon, chlorpyrifos, malathion, dimethoate and fenthion
were detected 15, 10, 7, 6 and 4 times, respectively, in the water samples
from Ghana, West Bengal, USA, Ethiopia, Iran, Brazil, Vietnam, Spain
Portugal and Ethiopia.
The occurrence of OP residues in drinking water may emerge from
the intensive application of OP pesticides in agricultural systems, such as
in China, where they use 1.5–4-fold higher concentrations than the
world average concentration (Zhang et al., 2015). Additionally, the
application of high concentrations of pesticides to soil may result in the
adsorption of pesticides on soil particles, and soil-adsorbed pesticides
may enter the aquatic ecosystem via soil leaching (El-Nahhal and
Hamdona, 2017), erosion, surface runoff, and sewer overflow (Xu et al.,
2020). Moreover, the degradation of OP residues in ecosystems could be
an additional source of drinking water contamination (Y. Zhang et al.,
2020). Furthermore, pesticide application methods, such as aerial
application, can tremendously be a serious source of contamination
12
Journal of Environmental Management 299 (2021) 113611
(Suarez-Lopez et al., 2020). Similarly, ultralow-volume aerosols of in­
secticides (Britch et al., 2018) could be an additional source of water
contamination. Moreover, atmospheric dust can carry OP residues
(chlorpyrifos and diazinon) through adsorption to water systems (Deziel
et al., 2015). Photodegradation, volatilization and hydrolysis enable the
mobility of OP residues to contaminate water systems (Kromer et al.,
2004; Kiss and Virág, 2009).
The lower frequency of OP residue detection compared with that of
OC residue can be explained by several factors, such as sensitivity to
water hydrolysis at alkaline pH, as shown for chlorpyrifos and other
organophosphorus esters in drinking water (pubmed.ncbi.nlm.nih.gov/
?sort=pubdate&size=20&term=Lockridge+O&cauthor_id=31401088
Lockridge et al., 2019). Moreover, OP residues may undergo photo­
chemical degradation, as shown for methyl parathion (Weber et al.,
2009; Bouhala et al., 2020), malathion (Ramos-Delgado et al., 2013),
chlorpyrifos (pubmed.ncbi.nlm.nih.gov/?sort=pubdate&size=20&term
=Femia+J&cauthor_id=24292479Femia et al., 2013), and biodegra­
dation in water systems (Alvarenga et al., 2014).
In general, the detected concentrations of OP residues were higher
than those of OC residues because OC residues are highly hydrophobic
and have low solubility in water (1–10,000 μg/L) and very high lipid
solubility (log P of 4–7) (PPDB, 2007).
3.1.3. Carbamate (CT) insecticide residues
The means of the CT residues in the water samples are presented in
Table 1. Five CT residues, carbofuran, carbaryl, methiocarb, fenobucarb
and propoxur, were detected in the water samples from Burkina Faso,
Brazil, Spain, and Vietnam. Carbofuran was detected three times with a
concentration range of 0.06–2.95 μg/L. Carbaryl and methiocarb were
detected once in the water samples from Spain at concentrations of 0.17
and 1.35 μg/L, respectively. Fenobucarb was detected twice at concen­
trations of 0.04 and 0.074 μg/L in Vietnam and Japan, respectively.
Propoxur residues were detected in Nigeria and Japan with a concen­
tration range of 0.029–0.023 μg/L. However, some metabolites from
group 3, such as hydroxyl-carbofuran, were detected three times at
moderate to low concentrations (<5 μg/L), such as 0.06, 0.39, and 2.95
μg/L in Burkina Faso, Brazil, and Spain, respectively. The occurrence of
CT residues in water may be attributed to intensive use in agricultural
systems (Kunstadter et al., 2001; Ruggieri et al., 2008), erosion of
contaminated soil (Ukalska-Jaruga et al. (2020a, 2020b)), dust fall
adsorbing OC residues (Deziel et al., 2015), wastewater (Karpuzcu et al.,
2014; Wu et al., 2019a, 2019b), leaching in the soil profile (Hulbert
et al., 2020), wash-off from plants by rainfall (Willis et al., 1996) and
contaminated rainfall (Vogel et al., 2008).
The low frequency of carbamate detection in the water samples was
due to its sensitivity to water hydrolysis (Katagi, 2010), photo­
degradation (Derbalah et al., 2020) and biodegradation (Birolli et al.,
2016).
3.1.4. Pyrethroid (PY) neonicotinoid family (N) and other (O) insecticide
residues
Eight PY residues were detected in the water samples (Table 1). Six
PY residues were detected at a concentration range of 0.01–0.41 μg/L in
the water samples from Ghana (Affum et al., 2018). Two PY residues
were detected in the water samples from Burkina Faso with a concen­
tration range of 0.001–0.22 μg/L (Lehmann et al., 2017). One PY residue
(etofenprox) with a concentration of 0.041 μg/L was detected in the
water samples from Japan (Tanabe et al., 2001).
The low frequency of PY detection was because it is sensitive to
photochemical degradation (Rafique and Tariq, 2015). The occurrence
of PY residues in water may emerge from using large amounts of them in
both agricultural and urban settings (Taylor et al., 2019), the movement
of PY-contaminated sediments to aquatic systems (Li et al., 2017), sus­
pended sediment in surface water such as rivers and/or lakes (Hladik
and Kuivila, 2009; Cheng et al., 2017), and wastewater and associated
sediments (Li et al., 2011).
I. El-Nahhal and Y. El-Nahhal
Moreover, the detection of PY residues in the water samples from
Ghana and Brazil may have occurred because these two countries
extensively used pyrethroids to control mosquitos because of their high
activity as insecticides and their low mammalian toxicity (Varloud et al.,
2015; Willemin et al., 2015).
Five N residues (acetamiprid, clothianidin, imidacloprid, thiame­
thoxam, and thiacloprid) at a concentration lower than 0.01 μg/L were
detected in water samples from China (Mahai et al., 2021; Wan et al.,
2019; Wang et al., 2020), Vietnam (Wan et al., 2021), Canada (Sultana
et al., 2018) and the USA (Klarich et al., 2017; Craddock et al., 2019).
However, only imidacloprid concentrations of 0.01, 1.28, 3.99 and 8.33
μg/L were detected in drinking water samples from Burkina Faso (Leh­
mann et al., 2017), Brazil (Albuquerque et al., 2016), Spain (Ccanccapa
et al., 2016) and China (Mahai et al., 2021).
The occurrence of N residues in drinking water may be due to the
presence of N residues in many environmental samples, such as fruits
and vegetables (Lu et al., 2018), indoor dust (Salis et al., 2017), outdoor
dust (Forero et al., 2017), urine (Tao et al., 2019) and runoff loss from
contaminated watersheds (Lamers et al., 2011).
Three insecticide residues belonging to the different chemical groups
(others) were detected in the water samples from Vietnam, Spain, and
Nicaragua. These insecticides were buprofezin, chlordimeform, and
fipronil (Table 1).
The concentrations of the insecticides listed in Table 1 were divided
into three groups as described in section 2.7.1. Group 1 included those
that had residue concentrations above the ARfD values, such as aldrin,
γ-HCH (China); aldrin (India); 2,4′ -DDD, aldrin, heptachlor-epoxide,
dieldrin, heptachlor, and parathion-methyl (Lebanon); 4,4́ –DDT (West
Bengal); endrin-aldehyde and δ-HCH (Philippines); γ-HCH, aldrin, and
dieldrin (Egypt); p,p′ -DDT (Nicaragua); aldrin, dieldrin, and γ-HCH
(Co^te d’Ivoire); dieldrin (Burkina Faso); dimethoate, omethoate, and
parathion-ethyl (Spain); and Diazinon (Iran). Almost 11 countries have
elevated levels of pesticide residues.
Groups 2 and 3 included residues with concentrations below the
ARfD values. The insecticide residues listed in Table 1 and not
mentioned in this section were determined to be at either medium or low
concentrations. Thus, the concentrations of residues in groups 1 and 2
contributed to high HI values in some countries.
3.1.5. Herbicide residues
Table 2 shows the concentrations of herbicide residues in water
worldwide. Approximately 31 parent herbicide residues belonging to
different chemical groups were detected in more than 768 water samples
from 18 countries (Brazil, Burkina Faso, Canada, China, Ethiopia,
France, Germany, Iran, Lebanon, Luxembourg, Portugal, Slovenia,
Spain, USA, Vietnam, and West Bengal). These residues were 2,4-D,
acetochlor, alachlor, ametryn, atrazine, bentazone, butachlor, cloma­
zone, cyanazine diuron, hexazinone, imazethapyr, isoproturon, glyph­
osate, linuron, mecoprop, metoalachlor, metribuzin, molinate,
pendimethalin, prometon, propanil, propazine, simazine, tebuthiuron,
terbumeton, trifluralin, terbuthylazine, terbutryn, and pretilachlor.
Additionally, seven herbicide metabolites (deethylatrazine, deisopro­
pylatrazine, deisopropylatrazine, desethylatrazine, desethyl terbuthy­
lazine, terbumeton-deethyl, terbuthylazine deethyl, and − 2 hydroxy-
terbutylene) were detected in the water samples.
For instance, twenty-eight herbicide residues were detected in the
water samples from Portugal with a concentration range of 0.002–0.27
μg/L (Palma et al., 2009, 2014). Twenty-two herbicide residues were
detected in the water samples from Brazil with a concentration range of
0.01–4.90 μg/L (Albuquerque et al., 2016; Dores et al., 2008). Fourteen
herbicide residues were detected in the water samples from Spain with a
concentration range of 1.16–32.32 μg/L (Ccanccapa et al., 2016). Eight
herbicide residues were detected in the water samples from Slovenia
with a concentration range of 0.0001–0.051 μg/L (Koroša et al., 2016).
Eight herbicide residues were detected in the water samples from
Vietnam with a concentration range of 0.0001–0.47 μg/L (Toan et al.,
13
Journal of Environmental Management 299 (2021) 113611
2013; Wan et al., 2021).
Seven herbicide residues were detected in the water samples from
Lebanon with a concentration range of 0.26–1.73 μg/L (Chaza et al.,
2018) and from Germany with a concentration range of 1.22–79.02 μg/L
(Stehle et al., 2019). Five herbicide residues were detected in the water
samples from the USA with a concentration range of 0.03–1.8 μg/L
(Postle et al., 2004; Eitzer and Chevalier, 1999) and from Luxembourg
with a concentration range of 0.001–0.03 μg/L (Bohn et al., 2011).
Four herbicide residues were detected with a concentration range of
0.0001–0.051 μg/L in water samples from Canada (Woudneh et al.,
2009), and three herbicide residues were detected with a concentration
range of 0.001–0.021 μg/L in water samples from China (Shi et al., 2020;
Wang et al., 2020).
Two residues were detected in the water samples from Vietnam and
France, whereas one residue was detected in the water samples from
Burkina Faso, West Bengal, Ethiopia and Iran. However, glyphosate is a
widely used herbicide, and it is considered a nontoxic pesticide to
humans due to its high LD50 value (>2000 mg/kg) and class III toxicity.
It is highly soluble in water (10.5 g/L) and has a high dissociation
constant (pKa = 2.32) and a low partitioning coefficient (Log P = − 3.2)
(PPDB, 2007). For these reasons, less attention may have been given to
glyphosate. Nevertheless, there is growing concern for potential toxicity
to aquatic organisms due to high solubility in water and high dissocia­
tion constant (see above). To date, glyphosate has been detected in many
water bodies, including drinking water, due to possible spillage, runoff,
and leaching. Moreover, it has been detected in groundwater with a
maximum concentration of 1.42 μg/L (Rendon-von Osten and
Dzul-Caamal 2017).
The occurrence of herbicide residues in the water samples was due to
direct application to soil followed by water irrigation/rainfall resulting
in herbicide leaching into the groundwater (El-Nahhal et al., 1998,
2000; Nir et al., 2000; El-Nahhal and Hamdona, 2017) or transport as
colloidal particles in the soil (Terzaghi et al., 2020). Moreover, it has
been shown that soil erosion (Rheinheimer Dos Santos et al., 2020), dust
fall (Deziel et al., 2015), rainfall runoff (Imfeld et al., 2020) and dry-wet
conditions have critical impacts on drinking water contamination.
3.1.6. Fungicide residues
The concentrations of the fungicide residues determined in the water
samples are listed below. Approximately 23 residues were detected in 32
water samples from three countries. These residues were azoxystrobin,
carbendazim, chlorothalonil, difenoconazole, edifenphos, epox­
iconazole, etridiazole, flutolanil, flutriafol, imazalil, iprobenfos, iso­
prothiolane, mepronil, pencycuron, picoxystrobin, probenazole,
prochloraz, quintozene, tebuconazole, thiabendazole, and tricyclazole.
To date, eleven residues with a concentration range of 0.013–0.473 μg/L
have been detected in Japan (Tanabe et al., 2001). Eight residues with a
concentration range of 0.001–0.39 μg/L were detected in Brazil (Albu­
querque et al., 2016). Five fungicide residues with a concentration range
of 4.82–101.03 μg/L were detected in the water samples from Spain
(Ccanccapa et al., 2016), and only one residue exceeded the ARfD value.
Additionally, the fungicide residues carbendazim, difenoconazole,
epoxiconazole, flutolanil, picoxystrobin, prochloraz, tebuconazole,
thiabendazole, and tricyclazole were detected in water samples from
China with a concentration range of 0.0011–0.077 μg/L, and the fre­
quency of detection reached 43.4% (n = 166 water samples) in some
cases (Li et al., 2020). Similar fungicide residues were also detected in
water samples from Malaysia (Elfikrie et al., 2020).
The occurrence of fungicide residues in the drinking water samples
was due to the widespread use of these chemicals in soil to control soil-
borne diseases, often as seed dressings and other times as foliar sprays to
control fungi during the growing seasons (Tosi et al., 2018). Further­
more, eroded sediments (Rheinheimer Dos Santos et al., 2020), indus­
trial wastewater (Kapsi et al., 2019), contaminated estuaries (Kapsi
et al., 2019), and animal manure (Kreuzig et al., 2010) could be an
additional source of water contamination with fungicide residues.
I. El-Nahhal and Y. El-Nahhal Journal of Environmental Management 299 (2021) 113611

Table 2
Average concentration of herbicide residues in drinking water.
3
RN CFμg/L ARfD μg/L Average daily intake ng/g *10− HQ AS DR Cn Au

Ad Ch In Ad Ch In

Simazine 0.033 5 1.11 3.33 5.00 0.00 0.00 0.00 81 12 Portugal Palma et al. (2009)
Isoproturon 0.003 15 0.11 0.33 0.50 0.00 0.00 0.00
Chlortoluron 0.008 40 0.26 0.78 1.17 0.00 0.00 0.00
Atrazine 0.270 100 9.01 27.02 40.54 0.00 0.00 0.00
Diuron 0.049 3 1.65 4.95 7.42 0.00 0.00 0.00
Cyanazine 0.000 100 0.01 0.04 0.06 0.00 0.00 0.00
Molinate 0.002 100 0.06 0.17 0.25 0.00 0.00 0.00
Linuron 0.001 30 0.04 0.11 0.16 0.00 0.00 0.00
Alachlor 0.009 10 0.31 0.94 1.41 0.00 0.00 0.00
Metolachlor 0.010 97 0.34 1.02 1.53 0.00 0.00 0.00
HI 0.001 0.003 0.004
Atrazine 0.005 100 0.18 0.54 0.81 0.00 0.00 0.00 NR 16 Portugal Palma et al. (2014)
Cyanazine 0.001 100 0.02 0.06 0.10 0.00 0.00 0.00
Simazine 0.008 5 0.28 0.84 1.26 0.00 0.00 0.00
Terbuthylazine 0.155 8 5.18 15.53 23.29 0.00 0.00 0.00
Chlortoluron 0.015 40 0.49 1.48 2.22 0.00 0.00 0.00
Diuron 0.004 3 0.14 0.42 0.63 0.00 0.00 0.00
Isoproturon 0.002 15 0.08 0.23 0.34 0.00 0.00 0.00
Linuron 0.001 30 0.04 0.13 0.20 0.00 0.00 0.00
Alachlor 0.001 10 0.04 0.13 0.20 0.00 0.00 0.00
Metolachlor 0.037 97 1.23 3.69 5.54 0.00 0.00 0.00
Propanil 0.001 70 0.03 0.10 0.15 0.00 0.00 0.00
Molinate 0.012 100 0.38 1.15 1.73 0.00 0.00 0.00
2,4-D 0.036 750 1.20 3.59 5.39 0.00 0.00 0.00
Bentazone 0.195 250 6.49 19.46 29.19 0.00 0.00 0.00
MCPA 0.025 150 0.83 2.48 3.72 0.00 0.00 0.00
Mecoprop 0.005 10 0.17 0.50 0.74 0.00 0.00 0.00
HI 0.001 0.003 0.004
2,4-D 1.85 750 61.67 185.00 277.50 0.00 0.00 0.00 23 16 Brazil Albuquerque et al., 2016,
Propanil 4.90 70 163.17 489.50 734.25 0.00 0.01 0.01
Bentazone 1.43 250 47.64 142.93 214.40 0.00 0.00 0.00
Acetochlor 0.01 20 0.25 0.75 1.13 0.00 0.00 0.00
Metolachlor 0.42 97 14.00 42.00 63.00 0.00 0.00 0.00
Alachlor 0.01 10 0.37 1.10 1.65 0.00 0.00 0.00
Pendimethalin 0.01 300 0.37 1.10 1.65 0.00 0.00 0.00
Trifuralin 1.16 15 38.67 116.00 174.00 0.00 0.01 0.01
Imazethapyr 0.65 440 21.67 65.00 97.50 0.00 0.00 0.00
Diuron 0.12 3 4.13 12.40 18.60 0.00 0.00 0.01
Clomazone 4.48 2500 149.24 447.73 671.60 0.00 0.00 0.00
Hexazinone 0.40 50 13.33 40.00 60.00 0.00 0.00 0.00
Metribuzin 0.07 20 2.39 7.18 10.76 0.00 0.00 0.00
Ametryn 0.75 15 24.89 74.68 112.02 0.00 0.00 0.01
Atrazine 1.06 100 35.26 105.79 158.69 0.00 0.00 0.00
Simazine 0.17 5 5.66 16.99 25.48 0.00 0.00 0.01
atrazine 0.063 100 2.10 6.30 9.45 0.000 0.000 0.000 23 6 Brazil Dores et al. (2008)
DEA 0.158 100 5.27 15.80 23.70 0.000 0.000 0.000
simazine 0.064 5 2.13 6.40 9.60 0.000 0.001 0.002
metribuzin 0.151 5 5.03 15.10 22.65 0.001 0.003 0.005
trifluralin 0.142 7.5 4.73 14.20 21.30 0.001 0.002 0.003
metolachlor 0.253 97 8.43 25.30 37.95 0.000 0.000 0.000
HI 0.012 0.037 0.060
Metoalachlor 2.17 97 72.33 217.00 325.50 0.00 0.00 00 NR 14 Spain Ccanccapa et al. (2016)
Atrazine, 7.45 100 248.22 744.67 1117.00 0.00 0.01 0.01
Deisopropylatrazine 7.94 100 264.67 794.00 1191.00 0.00 0.01 0.01
Deethylatrazine 13.88 100 462.50 1387.50 2081.25 0.00 0.01 0.02
Simazine, 27.31 5 910.44 2731.33 4097.00 0.18 0.55 0.82
Terbumeton, 3.55 75 118.44 355.33 533.00 0.00 0.00 0.01
Terbumeton-Deethyl, 3.68 75 122.56 367.67 551.50 0.00 0.00 0.01
Terbuthylazine 4.14 8 138.00 414.00 621.00 0.02 0.05 0.08
Terbuthylazine Deethyl, 1.16 8 38.56 115.67 173.50 0.00 0.01 0.02
Terbuthylazine-2 Hydroxy 4.41 8 147.00 441.00 661.50 0.02 0.06 0.08
Terbutryn 11.58 27 385.94 1157.83 1736.75 0.01 0.04 0.06
Diuron, 32.32 3 1077.44 3232.33 4848.50 0.36 1.08 1.62
Isoproturon 5.76 15 192.11 576.33 864.50 0.01 0.04 0.06
HI 0.62 1.87 2.80
Atrazine 0.0508 100 1.69 5.08 7.62 0.00 0.00 0.00 NR 8 Slovenia Koroša et al. (2016)
Desethylatrazine 0.051 100 1.70 5.10 7.65 0.00 0.00 0.00
Deisopropylatrazine 0.005 100 0.17 0.50 0.75 0.00 0.00 0.00
Simazine 0.0052 5 0.17 0.52 0.78 0.00 0.00 0.00
Terbuthylazine 0.0011 8 0.04 0.11 0.17 0.00 0.00 0.00
Desethylterbuthylazine 0.0026 8 0.09 0.26 0.39 0.00 0.00 0.00
Metolachlor 0.001 97 0.03 0.10 0.15 0.00 0.00 0.00
Propazine 0.001 100 0.03 0.10 0.15 0.00 0.00 0.00
HI 0.000 0.000 0.000

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I. El-Nahhal and Y. El-Nahhal Journal of Environmental Management 299 (2021) 113611

3
RN CF ARfD Average daily intake ng/g *10− HQ AS DR Cn Au
μg/L μg/L
Ad Ch In Ad Ch In

Isoprothiolane 0.17 100 5.67 17.00 25.50 0.000 0.000 0.000 54 2 Vietnam Toan et al. (2013)
Butachlor 0.47 100 15.67 47.00 70.50 0.000 0.000 0.001
Atrazine 0.02 100 0.66 1.99 2.99 0.000 0.000 0.000 39 6 Wan et al. (2021)
Simazine 0.00 5 0.00 0.01 0.01 0.000 0.000 0.000
Terbuthylazine 0.00 8 0.00 0.00 0.00 0.000 0.000 0.000
MCPA 0.00 150 0.01 0.04 0.06 0.000 0.000 0.000
2,4-D 0.00 750 0.01 0.03 0.05 0.000 0.000 0.000
Bentazone 0.00 250 0.00 0.01 0.01 0.000 0.000 0.000
HI 0.000 0.001 0.001
Molinate 1.08 100 36.00 108.00 162.00 0.00 0.00 0.00 15 7 Lebanon Chaza et al. (2018)
Atrazine 1.24 100 41.33 124.00 186.00 0.00 0.00 0.00
Acetochlor 1.53 20 51.00 153.00 229.50 0.00 0.01 0.01
Alachlor 1.73 10 57.67 173.00 259.50 0.01 0.02 0.03
Metolachlor 0.26 97 8.67 26.00 39.00 0.00 0.00 0.00
Butachlor 1.08 100 36.00 108.00 162.00 0.00 0.00 0.00
HI 0.01 0.03 0.04
Atrazine 7.01 100 233.63 700.90 1051.35 0.00 0.01 0.01 NR 7 Germany Stehlea et al., 2009
Simazine 79.02 5 2633.93 7901.80 11852.70 0.53 1.58 2.37
Prometon 2.12 100 70.57 211.70 317.55 0.00 0.00 0.00
Metolachlor 1.22 97 40.58 121.75 182.63 0.00 0.00 0.00
Tebuthiuron 1.43 70 47.53 142.60 213.90 0.00 0.00 0.00
2,4-D 17.96 750 598.70 1796.10 2694.15 0.00 0.00 0.00
Diuron 5.54 3 184.67 554.00 831.00 0.06 0.18 0.28
HI 0.59 1.78 2.67
alachlor 1.8 10 60.00 180.00 270.00 0.01 0.02 0.03 237 3 USA Postle et al. (2004)
acetochlor 0.15 20 5.00 15.00 22.50 0.00 0.00 0.00
metolachlor 0.79 97 26.33 79.00 118.50 0.00 0.00 0.00
Dacthal (DCPA) 0.03 100 1.00 3.00 4.50 0.00 0.00 0.00 15 2 USA Eitzer and Chevalier
(1999)
Trifluralin 0.04 7.5 1.33 4.00 6.00 0.00 0.00 0.00
HI 0.01 0.02 0.03
Atrazine 0.009 100 0.30 0.90 1.35 0.00 0.00 0.00 69 5 Luxembourg Bohn et al. (2011)
Desethylatrazine 0.019 100 0.63 1.90 2.85 0.00 0.00 0.00
Deisopropylatrazine 0.003 100 0.10 0.30 0.45 0.00 0.00 0.00
Simazine 0.001 5 0.03 0.10 0.15 0.00 0.00 0.00
2 P,6-Dichlorobenzamide 0.03 100 1.00 3.00 4.50 0.00 0.00 0.00
HI 0.000 0.000 0.000
Ametryn 0.0001 15 0.00 0.01 0.01 0.000 0.000 0.000 NR 4 Canada Woudneh et al. (2009)
Desethylatrazine 0.0001 100 0.00 0.01 0.01 0.000 0.000 0.000
Metribuzin 0.0000 20 0.00 0.00 0.01 0.000 0.000 0.000
Alachlor 0.0003 10 0.01 0.03 0.04 0.000 0.000 0.000
000 000 000
2, 4-D 0.00 750 0.04 0.12 0.17 0.000 0.000 0.000 789 2 China Shi et al., 2020
MCPA 0.00 150 0.04 0.12 0.18 0.000 0.000 0.000
Atrazine 0.02 100 0.70 2.11 3.17 0.000 0.000 0.000 884 1 Wang et al. (2020)
HI 0.000 0.000 0.000
Glyphosate 0.145 100 4.83 14.50 21.75 0.00 0.00 0.00 2 France Botta et al., (2009)
AMPA (Metabolite of 0.464 100 15.47 46.40 69.60 0.00 0.00 0.00
glyphosate)
HI 0.000 0.001 0.001
Atrazine 0.01 100 0.45 1.35 2.03 0.00 0.00 0.00 106 1 Burkina Faso Lehmann et al. (2017)
HI 0.00 0.00 0.00
Butachlor 0.005 100 0.17 0.50 0.75 0.00 0.00 0.00 1 West Bengal Mondal et al. (2018)
0.00 0.00 0.00
2,4-D 2.58 759 86.00 258.00 387.00 0.00 0.00 0.00 45 1 Ethiopia Mekonen et al. (2016)
0.00 0.00 0.001
Trifluralin 0.21 7.5 6.90 20.70 31.05 0.001 0.003 0.004 64 1 Iran Heidar et al. (2017)
0.001 0.003 0.004

Fig. 1b shows the total number of pesticide residues distributed by
country. It appears that the highest number of insecticides was found in
Lebanon, followed by Spain and West Bengal, whereas the lowest
number was found in Ireland. The highest amount of herbicide residues
was found in Brazil, and the lowest amount was found in Iran. The
highest amount of fungicide residue was found in Japan, and the lowest
amount was found in Spain. The differences in the detected number of
pesticide residues among counties may be attributed to different regu­
lations and restrictions.
3.1.7. Concentrations of pesticide residues at the country level
Fig. 2 shows the Rel Aver of pesticide residues in water. Fig. 2a shows
the Rel Aver of insecticides. This figure consists of four sections. Section
A includes countries with Rel Aver values of insecticide residues below
0.01 and includes water samples from five countries (Canada, Portugal,
China, South Africa, and Mexico). Section B includes countries with Rel
Aver values in the range of 0.01–0.1 and includes water samples from
thirteen countries (Ireland, Japan, Ghana, Nigeria, India, Togo-Africa,
Burkina Faso, Vietnam, the USA, the Philippines, Thailand, West Ben­
gal, and Iran). Section C includes countries with Rel Aver values of
insecticide residues in the range of 0.11–0.5 and includes water samples
from seven countries (Ghana, China, Brazil, Egypt, Co^te d’Ivoire, and
Nicaragua), and Section D includes countries with Rel Aver values of
insecticide residues >0.5 and includes water samples from six countries
(Germany, Lebanon, Ethiopia, Spain, Iran, and India).
Similarly, Fig. 2b shows the Rel Aver of herbicide residues. This

15
I. El-Nahhal and Y. El-Nahhal Journal of Environmental Management 299 (2021) 113611

a b

Fig. 2. a. Rel Aver of insecticide residues in water from different countries. Rel Aver ranges are <0.01; 0.011–0.099; 0.1–0.5; >0.5 represented by A, B, C, and D
respectively. Countries have the same letter on Rel Aver in a box are not significantly different at p-value >0.05. Error bars represent relative standard error of a
country. Fig. 2b. Relative average (Rel Aver) of herbicide residues in water from different countries. Rel Aver ranges are <0.01; 0.011–0.099; 0.1–0.5; >0.5 rep­
resented by A, B, C, and D respectively. Countries have the same letter on Rel Aver in a box are not significantly different at p-value ≤ 0.05. Error bars represent
relative standard error of a country. Fig. 2c. Relative average (Rel Aver) of fungicide residues in water from different countries. Countries have the same letter on Rel
Aver in a box are not significantly different at p-value ≤ 0.05. Error bars represent relative standard error of a country.

16
I. El-Nahhal and Y. El-Nahhal Journal of Environmental Management 299 (2021) 113611

figure consists of four sections. Section A includes countries with Rel
Aver values < 0.01 and includes water samples from five countries
(Canada, West Bengal, Luxembourg, Burkina Faso, and Slovenia). Sec­
tion B includes countries with Rel Aver values in the range of 0.01–0.1.
This section includes water samples from three countries (Portugal
2014, Portugal 2009; Brazil, and Iran). Section C includes countries with
Rel Aver values in the range of 0.11–0.5 and includes water samples
from five countries (France, Vietnam, USA, Japan, and Brazil), and
Section D includes countries with Rel Aver values for herbicide residues
of >0.5 and includes water samples from four countries (Lebanon,
Ethiopia, Spain, and Germany).
Additionally, Fig. 2c shows the Rel Aver of fungicide residues and
consists of two sections only. Section A includes countries with Rel Aver
values < 0.01 and includes water samples from Brazil and Japan. Sec­
tions B and C do not include any country, whereas section D includes
countries with Rel Aver values for fungicide residues of >0.5 and in­
cludes water samples from Spain.
Statistically significant differences among the Rel Aver values in
different countries are illustrated by letters a, b and c in the vicinity of
the error bars.
3.1.8. Classification of pesticide residues
Pesticide residues in this review were summarized and classified into
four toxicity classes as follows: toxicity class Ia (extremely toxic com­
pounds, with LD50 values < 5 μg/g.b.w.); toxicity class Ib (highly toxic
compounds, with LD50 values in the range of 5-<50 μg/g.b.w.); toxicity
class II (moderately toxic compounds, with LD50 values in the range of
50-<500 μg/g.b.w.); toxicity class III (slightly toxic compounds, with
LD50 values in the range of 500-<2000 μg/g.b.w.); and toxicity class IV
(less toxic compounds, with LD50 values > 2000 μg/g.b.w.). A summary
of pesticide toxicity classes is presented in Table 3a, b, c.
Table 3 shows the name, toxicity class and chemical groups of the
pesticides considered in this study. Table 3a shows the insecticides,
which included six chemical groups (OC, OP, CT, PY, N, and/or O) and
four toxicity classes.
Four and thirteen insecticide residues belonged to toxicity classes Ia
and Ib, respectively, and belonged to four chemical classes, OP, CT, OC
and PY. Additionally, thirty-one, four and six insecticide residues
belonged to toxicity classes II, III and IV, respectively (Table 3a).
Furthermore, 16, 10 and 5 herbicide residues belonged to toxicity
classes II, III and IV, respectively (Table 3b). However, 1, 8, 3 and 11
fungicide residues belonged to classes Ib, II, III and IV, respectively
(Table 3c).
3.2. Potential health risks associated with drinking water
Applying equations 1–4 to pesticide residues (Tables 1 and 2) pro­
vided the average daily intake HQs and HIs for adults, children, and
infants for insecticide, herbicide, and fungicide residues.
HIs for adults, children and infants had values ranging from <1 to
30.97 for infants in Egypt. The HI values for infants were the highest
among all age groups, indicating a high risk. The HI values for infants
were classified into four groups: group 1 included countries with HI
values less than 0.01, such as Portugal, Canada, Nigeria, Thailand,
China, and Vietnam; group 2 included countries with HI values ranging
from 0.01 to 0.1, such as Japan, Germany, Ghana, Ireland, China,
Mexico, Brazil, Ethiopia, South Africa and the USA; group 3 included
countries with HI values ranging from 0.1 to 1.0, such as Iran, Turkey,
Togo-Africa, China, Iran, Burkina Faso, West Bengal, Nicaragua, India,
and Ghana; and group 4 included countries with HI values > 1.0, such as
China, Spain, the Philippines, Cote d’lvoire, Lebanon, Egypt, and India.
Fig. 3 demonstrates the differences between all groups.

Table 3a
Name, toxicity class and chemical group of insecticide residues found in water samples from several countries.
Na ToxC ChemG Na ToxC ChemG Na ToxC ChemG Na ToxC ChemG

Parathion-methyl Ia OP Azinphos Methyl Ib OP Chlorpyrifos II OP Malathion III OP

Parathion-Ethyl Ia OP Isofenphosoxon Ib OP cyanophos II OP Buprofezin III Others
Phorate Ia OP Dicrotophos Ib OP Fenitrothion II OP Methoxychlor III OC
Ethoprophos Ia OP Monocrotophos Ib OP Pyridafenthion II OP etofenprox III PY
Dichlorvos Ib OP Profenofos II OP Thionazin IV OP
Methamidophos Ib OP Dimethoate II OP Chlordimeform IV Others
Omethoate Ib OP Ethion II OP Aldrin IV OC
Triazophos Ib OP Diazinon II OP Endrin IV OC
Chlorfenvinphos Ib OP Phosmet II OP dichlofenthion IV OP
Methiocarb Ib CT Fenthion II OP Mephosfolan IV OP
Carbofuran Ib CT Toxaphene II OC thiamethoxam IV N
Dieldrin Ib OC γ-Chlordane II OC Clothianidin IV N
Cyfluthrin Ib PY γ-HCH II OC
Chlordane II OC
py = 8 DDT II OC
CT = 5 heptachlor II OC
N=4 α-Endosulfan II OC
OP = 27 β-Endosulfan II OC
OC = 14 HCH II OC
OTHERS = 3 Lindane II OC
Total = 61 Fenpropathrin II PY
Deltamethrin II PY
Cypermethrin II PY
L-cyhalothrin II PY
Permethrin II PY
λ-Cyhalothrin II PY
carbaryl II CT
Fenobucarb II CT
Propoxur II CT
Thiacloprid II N
Imidacloprid II N
Fipronil II Others
Total 4 13 32 12

Abbreviations: CT, OP, N, PY, OC, are carbamate, organophosphorus, neonicotinoid, pyrethroids, organochlorine compounds respectively. O= (Obsolete substance).
Na = name, ToxC = toxicity class, ChemG = chemical group.

17
I. El-Nahhal and Y. El-Nahhal Journal of Environmental Management 299 (2021) 113611

Table 3b
Name, toxicity class and chemical group of herbicide residues found in water samples from several countries.
Na ToxC ChemG Na ToxC ChemG Na ToxC ChemG

Alachlor II chloroacetanilide Acetochlor III chloroacetanilide Imazethapyr IV Imidazolinone

Ametryn II triazine Atrazine III triazine Pretilachlor IV Chloroacetamide
2,4-D II Alkylchlorophenoxy Butachlor III Chloroacetamide Propazine IV Triazine
Bentazone II diazinone Diuron III Phenylamide Simazine IV Triazine
Clomazone II Isoxazolidinone Glyphosate III Phosphonoglycine Trifluralin IV Dinitroaniline
Cyanazine II Triazine Linuron III Urea
Hexazinone II Triazinone Metoalachlor III Chloroacetamide
Isoproturon II Urea Prometon III Methoxytriazine
Mecoprop II Aryloxyalkanoic acid Terbutryn III Triazine
Metribuzin II Triazinone Terbuthylazine III Triazine
Molinate II Thiocarbamate
Pendimethalin II Dinitroaniline
Propanil II Anilide
Tebuthiuron II Urea
Terbumeton II Triazine
MCPA II Aryloxyalkanoic acid
Total 16 10 5

The high HI values in group 4 may be explained by the fact that many
OC insecticide residues were detected in the water samples from those
countries with concentration values exceeding the ARfD.
The HI index of insecticides increased in the water samples from
different countries in the following order: Portugal < Canada < Nigeria
< Thailand < China < Vietnam < Japan < Germany < Ghana < Ireland
< China < Mexico < Brazil < Mexico < Ethiopia < South Africa < USA
< Iran < Turkey < Togo-Africa < China < Iran < Burkina Faso < West
Bengal < Nicaragua < India < Ghana < China < Spain < Philippines <
Cote d’Ivoire < Lebanon < Egypt.
The HIs associated with herbicide residues (Table 2) had values in
the range of 0.0001–2.81. According to the classification mentioned
above, group 1 included countries with HI values less than 0.01 (Burkina
Faso, West Bengal, Luxembourg, Ethiopia, Vietnam, France, and Iran),
group 2 included countries with HI values between 0.01 and 0.1 (Brazil,
the USA and Lebanon), group 3 included countries with HI values be­
tween 0.11 and 1.0 (no countries), and group 4 included countries with
HI values > 1.0 (Germany and Spain).
The high HI values in group 4 may be attributed to the fact that the
water samples contained high concentrations of herbicides that were
close to or exceeded the value of the ARfD.
The HIs associated with fungicide residues in the water samples
ranged from 0.001 to 0.23, suggesting that these were low-risk groups
(data not shown). According to these data, group 1 included Brazil and
Japan, with HIs below 0.01; no water samples were in group 2 (HI values
between 0.01 and 0.1); group 3 included Spain (HI between 0.11 and
1.0); and no water samples were in group 4 due to the low fungicide
residues found.
3.2.1. Reproductive toxicity
It has been shown that exposure to pesticide residues may cause
reproductive toxicity in both men and women (El-Nahhal, 2020). For
instance, exposure to OP insecticides caused semen quality deterioration
among Chinese OP pesticide factory workers (Padungtod et al. 2000;
Recio-Vega et al., 2008). Similar effects were observed among farm
workers occupationally exposed to OP and carbamate pesticides (Mir­
anda-Contreras et al., 2013). Similarly, deterioration in semen quality
has been found among workers exposed to different organochlorine
insecticides (e.g., DDT, β-HCH, γ-HCH) (Jamal et al., 2016). Similarly,
exposure to herbicides (e.g., glyphosate) decreased the semen quality
parameters of exposed farmers (Sutyarso and Kanedi, 2014).
3.2.2. Potential endocrine disruptors
Furthermore, exposure to pesticide residues may create disruption in
the endocrine system. For instance, Miranda-Contreras et al. (2013)
found alterations in testosterone levels due to occupational exposure to
OP and carbamate pesticides. Arbuckle et al. (2001) also found an as­
sociation between spontaneous abortion in Canadian women and
exposure to 2,4-D. Moreover, acetamiprid (Kong et al., 2017), chlor­
pyrifos (Brandt et al., 2015), cypermethrin (Saillenfait et al., 2017),
diazinon, permethrin (Wang et al., 2012), dimethoate (Jallouli et al.,
2016), endosulfan (Yan et al., 2019), esfenvalerate, (Saillenfait et al.,
2018), and glyphosate (Romano et al., 2010) interfered with testos­
terone biosynthesis.
3.2.3. Potential carcinogenic agents
It has been suggested that exposure to pesticide residues may
enhance carcinogenicity among populations. For instance, Yang et al.
(2020) indicated that exposure to malathion, terbufos, and chlorpyrifos
was positively associated with human breast cancer risk. Additionally,
Pardo et al. (2020) showed an increased aggressive prostate cancer risk
among ever users of the organodithioate insecticide dimethoate (n = 54
exposed cases, health risk = 1.37, 95% CI = 1.04, 1.80) compared with
never users. However, they observed an inverse association between
aggressive prostate cancer and the herbicide triclopyr (n = 35 exposed
cases, health risk = 0.68, 95% CI = 0.48, 0.95), with the strongest in­
verse association for those reporting durations of use above the median
(≥4 years; n = 13 exposed cases, health risk = 0.44, 95% CI = 0.26,
0.77). In contrast, Brasil et al. (2018) indicated that the literature review
does not provide clear evidence for an association between pesticide
exposure and the occurrence of head and neck cancer. Furthermore,
Hyland et al. (2018) observed that self-reported maternal insecticide use
inside the home in the year before pregnancy, during pregnancy, and
while breastfeeding was associated with increased odds of acute
lymphoblastic leukemia among boys [adjusted odds ratio (aOR) = 1.63
(95% confidence interval [95% CI]: 1.05–2.53), 1.75 (1.13–2.73), and
1.75 (1.12–2.73), respectively]. Additionally, Liang et al. (2016) indi­
cated that pesticide exposure was associated with an increased risk of
bladder cancer. Similarly, Alavanja and Bonner (2012) found that in­
secticides, herbicides, fungicides, and fumigants have significant asso­
ciations with an array of cancer sites. Furthermore, Roberts et al. (2012)
demonstrated the associations between parental use of insecticides and
acute lymphocytic leukemia and brain tumors. Van Maele-Fabry et al.
(2006) pointed out that occupational exposure to pesticides is a possible
risk factor for prostate cancer, but the question of causality remains
unanswered.
Additionally, Pouchieu et al. (2018) suggested that the risk of Par­
kinson’s disease is increased in farmers exposed to pesticides used on
several French crops and livestock, and their research provides addi­
tional evidence of an association of Parkinson’s disease with dithiocar­
bamate fungicides, rotenone and the herbicides diquat and paraquat.

18
I. El-Nahhal and Y. El-Nahhal Journal of Environmental Management 299 (2021) 113611

3.2.4. Potential cardiovascular toxicity

It has been shown that exposure to organochlorine insecticides may
cause cardiotoxicity in populations. For instance, DDT and its isomers
cause cardiotoxicity in humans (Lamichhane et al., 2019), the devel­

Strobilurin type
Benzisothiazole
Benzimidazole

Chlorophenyl
Chlorophenyl
Chloronitrile
opment of arteriosclerosis and arterial hypertension (Morgan et al.,

Benzanilide
Phenylurea
strobilurin
1980; Donat-Vargas et al. 2018; La Merrill et al. 2013; La Merrill et al.

Oxathiin

Triazole
ChemG 2018; Vafeiadi et al. 2015; Teixeira et al. 2015).
Additionally, organophosphorus insecticide residues may cause
cardiac complications due to direct or indirect exposure. For instance,
occupational exposure to chlorpyrifos increased the risk factor to a value
ToxC

above 1 for acute infarction, whereas exposure to fenitrothion and

11
IV
IV
IV
IV
IV
IV
IV
IV
IV
IV
IV
malathion residues increased blood pressure, leading to cardiovascular
complications among male farmworkers (Zago et al., 2020) and female
tolchlofos methyl oxon farmworkers (Dayton et al., 2010).
Moreover, exposure to herbicides such as alachlor and butachlor
Chlorothalonil

Epoxiconazole

caused hypotension and coma among humans (Lo et al., 2008), whereas
Picoxystrobin
Carbendazim
Azoxystrobin

probenazole
pencycuron
quintozene

atrazine caused heart and lung complications at low concentrations in

flutolanil
mepronil

drinking water (EC 1998; Meghdad. 2013).

Na

3.3. Health hazards of repeated doses

Aromatic hydrocarbon

The influence of repeated consumption of contaminated water on

adults, children and infants is calculated and discussed below.
Benzimidazole

It appears that the HI value increased as the amount of time drinking

Morpholine

water was consumed increased from 0 to 1; 10, 25, 50 and 75 positive

ChemG

associations were obtained in all cases with a regression coefficient

equal to 1. These data indicated that repeated drinking of contaminated
water may result in health risks to populations. However, exposure of
infants and children was worse than that of adults because adults receive
ToxC

less residue with respect to their body weight. These data are provided in
III
III
III

Tables 1 and 2 Furthermore, the highest HI value was found in Germany,

and the lowest HI value was found in Vietnam.
Fenpropimorph

Vietnam and Brazil had HI values < 0.4, and Ghana and Ethiopia had
Thiabendazole
Name, toxicity class and chemical group of fungicide residues found in water samples from several countries.

HI values > 1 and < 3. India, Burkina Faso, and China 2 had HI values >
Etridiazole

5 and < 10, whereas the USA had an HI value of 11.67. West Bengal,
India 2, and China had HI values > 20 and < 50, and Germany had an HI
Na

of 89.57.
These HI values are expected to be two-to threefold higher for chil­
dren and infants. This result suggests that the potential HI for infants is
Triazolobenzothiazole

higher than the HI for children and adults.

Phosphorothiolate
Organophosphate

In conclusion, repeatedly drinking water containing pesticide resi­

dues at concentrations greater than, equal to or a few times lower than
Imidazole

Imidazole
Triazole
Triazole

Triazole

the ARfD may expose the population to potential health risks.

ChemG

Keeping in mind the high values of HI, it is necessary to propose ways

to remove pesticide residues from drinking water to make it suitable for
human consumption.
ToxC

II
II
II
II
II
II
II
II

3.4. Proposed pesticide residue removal options

Selection or design of a suitable method for pesticide removal from

Difenoconazole

Isoprothiolane
Tebuconazole

drinking water requires a full understanding of the physicochemical

tricyclazole
Prochloraz
Iprobenfos
Flutriafol

properties of pesticides, such as their water solubility, chemical struc­

Imazalil

ture, ionic status of molecules, and KOW. The pesticides listed in this
Na

manuscript can be subdivided into seven groups (Table 4) based on their

water solubility. Group 1 included pesticides with a solubility limit
below 1 mg/L and denoted as practically insoluble. This group included
ChemG

23 insecticides, 3 herbicides and 4 fungicides. Group 2 included pesti­

OP

cides with a solubility range of 1–9.99 mg/L and was denoted as poorly
soluble. This group included 6 insecticides, 7 herbicides, and 6 fungicide
residues. Group 3 included pesticides with a solubility range of
ToxC

Ib

10–29.99 mg/L and was denoted as mildly soluble. This group included
1

9 insecticide residues, 7 herbicide residues and 3 fungicides. Group 4

included pesticides with a solubility range of 30–99.99 mg/L and was
Edifenphos

denoted as slightly soluble. This group included 6 insecticide residues, 8

Table 3c

Total

herbicide residues and 6 fungicide residues. Group 5 included pesticides

Na

with a solubility range of 100–999.99 mg/L and was denoted as

19
I. El-Nahhal and Y. El-Nahhal
Fig. 3. Hazards index (HI) of insecticide calculated for infant from different countries. There are four groups of HI among counties. HI range is shown in each graph.
Values above 1 suggest potential cardiotoxicity among infant. Country marked by * has value 4.5 times higher than presented.
moderately soluble. This group included 6 insecticide residues, 8 her­
bicide residues and 4 fungicides. Group 6 included pesticides with a
solubility range of 1000–9999.99 mg/L and was denoted soluble. This
group included 3 insecticide residues, 4 herbicide residues and 0 fungi­
cide residues. Group 7 included pesticides with a solubility range of
>10000 mg/L and was denoted as highly soluble. This group included 6
insecticide residues, 6 herbicide residues and 0 fungicide residues.
Furthermore, these pesticides are organic molecules classified into
different chemical groups.
3.4.1. Removal by physical processes using adsorption
Adsorption is denoted here as the adhesion of pesticide ions or
molecules from water to the surfaces of solid materials. This may create
an accumulation of pesticide molecules, forming a monolayer or bi­
layers, depending on the physicochemical properties of pesticides and
solid materials (El-Nahhal et al., 1998).
The removal of pesticide residues is affected by physicochemical
properties such as hydrophobicity, water solubility, molecular weight,
evaporation and sensitivity to photodegradation (Rodriguez et al., 2016;
Gonzalez et al., 2013).
Accordingly, we propose an adsorption method to remove highly
hydrophobic residues (groups 1–3, Table 4) and use organic adsorbing
materials such as activated carbon, activated charcoal, nanoorganic
materials, organoclays, and bioadsorbents such as plant residues. For
instance, highly hydrophobic pesticide residues (groups 1–3, Table 4)
were removed using modified clay (Boyd et al., 1988; Boyd and Jaynes,
20
Journal of Environmental Management 299 (2021) 113611
1992; Nir et al., 2000; El-Nahhal and Safi, 2010), activated carbon
(Alves et al., 2019; Gamboa-Carballo et al., 2016; Grassi et al., 2012;
Gupta et al., 2011), carbon nanoparticles (Brooks et al., 2012), and plant
materials (El-Bakouri et al., 2007).
Organoclays remove several chloroacetamide herbicides (El-Nahhal
et al., 1998; Nir et al., 2000). Porous materials removed simazine from
water (Esposito et al., 2016); activated carbon removed carbaryl,
methomyl and carbofuran (Alves et al., 2019); granular activated carbon
and carbon nanotubes removed atrazine, simazine and diuron (Alves
et al., 2020); carbon slurry removed endosulfan and methoxychlor
(Gupta and Ali, 2008); and activated carbon removed methoxychlor,
methyl parathion and atrazine (Gupta et al., 2011). The authors
emphasized the importance of adsorptive materials used, specific su­
perficial area, and size and distribution of specific pore volume. Bio­
adsorbents removed atrazine, alachlor, endosulfan sulfate and trifluralin
from water (Rojas et al., 2014). Plant materials removed 4 herbicide
residues, alachlor, atrazine, simazine and trifluralin (Sharma et al.,
2008), and 8 insecticide residues, aldrin, chlorpyrifos, chlorfenvinphos,
dieldrin, α-endosulfan, endrin, hexachlorobenzene, β-HCH, γ-HCH,
(El-Bakouri et al., 2007), carbaryl and fenuron (Loffredo and Taskin,
2017).
In contrast, atrazine (Yang et al., 2018) and λ-cyhalothrin (An et al.,
2020) were removed using colloidal biochar. Similarly, carbendazim
and linuron were removed from aqueous solutions with activated carbon
produced from spent coffee grounds (Hgeig et al., 2019).
In summary, adsorption is a suitable, easily applicable, cost effective
I. El-Nahhal and Y. El-Nahhal
and efficient method for removing OC insecticides (Gamboa-Carballo
et al., 2016), herbicides (Brooks et al., 2012) and fungicides (El-Nahhal
and Safi, 2008).
3.4.2. Removal by physical processes using membrane filtration
The membrane filtration process is a physical separation method
used to separate molecules of different sizes and characteristics. Con­
centration differences between the two sides of a special membrane may
control the separation. Separation by membranes may depend on the
sieving power and the physiochemical properties of the membrane. To
date, membrane filtration processes (e.g., nanofiltration and ultrafil­
tration) have been used for natural organic matter and pesticide
removal. The general separation trend of these membranes is based on
hydrophobic adsorption as a function of the octanol–water partition
coefficient between the hydrophobic compounds and porous hydro­
phobic membrane during membrane filtration (Yoon et al., 2007).
Therefore, this method may be suitable for pesticide residues in groups
1–3 (Table 4). However, a single method usually does not achieve 100%
removal of pesticides. Accordingly, it is suggested to use membrane
filtration in tandem with adsorption using activated carbon to further
enhance the removal efficiency of pesticide residues. A combination of
methods (activated carbon + and membrane filtration) has successfully
removed pharmaceuticals and pesticide residues from water (Acero
et al., 2012; Margot et al., 2013; Rodriguez et al., 2016; Snyder et al.,
2007). However, Alves et al. (2020) used a microfiltration technique
combined with granular activated carbon fixed bed adsorption tech­
nology to remove large amounts (100%) of carbaryl and carbofuran
from public water supplies.
3.4.3. Removal by advanced oxidation processes
Advanced oxidation processes (AOPs) are based on initiating chem­
ical reactions that produce hydroxyl radicals (⋅OH) to partially or
completely degrade pesticide residues to nontoxic fragments. The for­
mation of hydroxide radicals was previously reported (Fenton, 1894).
Recent works emphasized the importance of peroxide reactions in the
removal of organic and inorganic pollutants from water (Buxton et al.,
1988). Later, several attempts were made to enhance the production of
hydroxyl radicals (⋅OH), including chemical and photochemical at­
tempts (Munter, 2001; Stefan, 2017). AOPs may be suitable for
removing pesticide residues with different chemical groups in their
chemical structure with different electronegativities, such as chlorinated
hydrocarbon (OC insecticides and chloroacetamide herbicide), organo­
phosphates, carbamates, pyrethroids, and dinitroaniline derivatives.
Hydroxyl radicals are highly reactive and nonselective oxidizing
agents for decomposing organic pollutants in water systems (Glaze et al.,
1987). Accordingly, pesticide residues such as 2,4-D, 2,4,5-T, chlor­
ophenols, paraquat, diquat, glyphosate, parathion, malathion, pyrethrin
and carbaryl may be degraded or mineralized. This is in accordance with
the findings reported by Munter (2001), who revealed fast decomposi­
tion of organic molecules (e.g., acids, alcohols, aldehydes, aromatics,
amines, ethers, ketones). Advanced oxidation treatment resulted in
detoxification of many chlorinated hydrocarbons and pesticides
(Andreozzi et al., 1999).
The following reactions are used to produce *OH radicals:
1. Chemical reactions
1.1 Ozonation at alkaline pH (>8.5)
1.2 O3 + H2O2
1.3 O3 + catalyst
1.4 Fenton system (H2O2/Fe2+)
2. Photochemical reactions
2.1 O3/UV
2.2 H2O2/UV
2.3 O3/H2O2/UV
2.4 Photo-Fenton/Fenton-like systems
2.5 Photocatalytic oxidation (UV/TiO2)
21
Journal of Environmental Management 299 (2021) 113611
The mechanism of generating hydroxyl radicals in each step has
previously been described in detail (Munter, 2001).
AOPs have successfully removed OC residues (e.g., DDT, DDE, DDD),
OP residues (e.g., chlorpyrifos), chloroacetamide herbicides (e.g., ala­
chlor, metolachlor), triazines (e.g., atrazine) and dinitroaniline (e.g.,
pendimethalin) from water (Sayles et al., 1997; Pirnie et al., 2006;
Thomas et al., 2008; Zhu et al., 2016; Marican and Durán-Lara, 2018).
Similarly, they increased the degradation of triazine (e.g., atrazine) and
chloroacetamide (e.g., metolachlor) herbicides due to the addition of
zerovalent iron to soil containing residues (Marican and Durán-Lara,
2018). Moreover, AOPs removed 100% of ametryn (Sangami and Manu,
2017), 98% of malathion and parathion-methyl (Roe and Lemley, 1997),
and caused rapid degradation of alachlor, chlorpyrifos, and pendime­
thalin due to the addition of aluminum sulfate and acetic acid with
zerovalent iron (Shea et al., 2004). Nurul Amin et al. (2008) completely
removed thiobencarb from water using a powdered zero valent iron and
batch experimental system. Yu (2002) revealed efficient and fast
removal of OP residues from water (fenitrothion, chlorpyrifos, diazinon,
methamidophos, edifenphos, mevinphos, fenthion, and acephate) by
supercritical carbon dioxide extraction followed by Fenton’s solution
treatment. da Costa et al. (2019) showed the ability of the photo-Fenton
reaction to degrade the fungicide carbendazim within 15 min with 96%
removal, indicating that both solar photo-Fenton and artificially irra­
diated systems are promising routes for carbendazim degradation. Erol
et al. (2019) removed DDT and its analogs very quickly from water by
magnetic diatomite. However, Kamel et al. (2009) showed the efficiency
of chlorine as a strong oxidizing reagent in completely oxidizing ten OP
insecticides (phorate, disulfoton, terbufos, methidathion, bensulide,
chlorethoxyfos, phosmet, parathion-methyl, phostebupirim, and teme­
phos) in water samples within 72 h under laboratory conditions.
3.4.4. Removal of pesticide residues via combined processes
It has been shown that using a combination of two advanced
oxidation systems (ZnO(normal)/H2O2/artificial sunlight and ZnO
(nano)/H2O2/artificial sunlight) successfully removed imidacloprid
from water (pubmed.ncbi.nlm.nih.gov/?term=Derbalah+A&cauthor
_id=30942775Derbalah et al., 2019).
Including electro-oxidation-ozone treatment removed all imidaclo­
prid within 120 min and increased mineralization to 50% TOC (Segura
et al., 2008; Malato et al., 2002; González et al., 2020). Using
electro-Fenton processes further improved the degradation rate of imi­
dacloprid (Iglesias et al., 2014) and carbofuran (Abdessalem et al., 2010;
Ma et al., 2009). Similarly, 94% of imidacloprid (pubmed.ncbi.nlm.nih.
gov/?term=Turabik+M&cauthor_id=24671401Turabik et al., 2014),
100% of λ-cyhalothrin (pubmed.ncbi.nlm.nih.gov/?term=Colombo
+R&cauthor_id=23380363Colombo et al., 2013) and 99% of atrazine
were removed from water within 2 h by electrochemical advanced
oxidation processes and electro-Fenton processes with a boron-doped
diamond anode (pubmed.ncbi.nlm.nih.gov/?term=Komtchou+S&
cauthor_id=28837868Komtchou et al., 2017).
Barbosa et al. (2016) showed the possibility of removing imidaclo­
prid, methiocarb, and oxadiazon using a UV filter (2-ethyl­
hexyl-4-methoxycinnamate) and an antioxidant (2,6-di-tert-butyl
-4-methylphenol).
Deltamethrin (Lafi and Al-Qodah, 2006) and chlorothalonil (Kiefer
et al., 2020) were completely removed within 210 min using O3 and
O3/UV oxidation systems followed by biological treatments.
Moreover, using a combination of oxidation methods (UV/H2O2,
UV/S2O82− , and UV/H2O2/S2O82− ) further completed the photo­
degradation of carbofuran (Chu et al., 2006), diazinon (Rasoulifard
et al., 2015), metolachlor (Wu et al., 2007), and endosulfan (Shah et al.,
2013) in water systems.
Simazine was removed from water by various techniques, with a
removal rate following this order: ozone < ozone/hydrogen peroxide <
UV radiation < ozone/UV radiation and UV radiation/hydrogen
peroxide (Beltrán et al., 2000).
I. El-Nahhal and Y. El-Nahhal
Moreover, 99% of atrazine was removed from water within 15–45
min using Fenton reactions (photoelectro-Fenton, electro-Fenton and
anodic oxidation with simultaneous H2O2 formation (AO - H2O2)).
Approximately 98% of chlorothalonil, parathion-methyl and meth­
amidophos were removed from water using the Fenton reaction within
40 min (Gutiérrez et al., 2007), whereas 75% of alachlor and diuron
were removed within 30 min after treatment using a falling film
dielectric barrier discharge plasma reactor combined with adsorption on
activated carbon (Vanraes et al., 2018).
Inclusion of an aerobic reactor along with the Photo-Fenton tech­
nique yielded acceptable degradation rates of chlorothalonil, chlorpyr­
ifos, and cypermethrin, improving water quality up to local standards
(Affam et al., 2014).
High percentages of 2,4-D, glyphosate, trifluralin, and butachlor
were removed using chemical oxidation (graphene oxide/TiO) followed
by adsorption (Hosseini and Toosi, 2019). Similarly, 83.4% of trifluralin
was removed by ozonation after 20 min (Milhome et al., 2018), and 2,
4-D residues were removed using bioadsorbents (Brito et al., 2020).
Chlorothalonil residue was removed from different materials after 5
min of ozonation (Kusvuran et al., 2012) and from water by catalytic
degradation using bimetallic iron (Ghauch and Tuqan, 2008). Similarly,
> 92% of both dieldrin and DDT were removed by ozonation followed
by microfiltration (Kenny et al., 2018). Approximately 95% of fenpro­
pathrin and λ-cyhalothrin were removed by UV light and simulated
sunlight (Liu et al., 2014), whereas 90% of λ-cyhalothrin and cyper­
methrin were removed by photodegradation and chemical oxidation
using copper (Xie et al., 2011). However, Yabalak and Gizir (2020)
demonstrated the ability of oxidation methods to remove pesticide res­
idues with different chemical structures (e.g., chlorpyrifos, penconazole,
brassilexin, buprofezin, etoxazole, and pyriproxyfen). Wardenier et al.
(2019) removed atrazine, alachlor, diuron, dichlorvos and pentachlo­
rophenol using an innovative AOP based on electrical discharges in a
continuous-flow pulsed dielectric barrier discharge reactor. Addition­
ally, Yang and Zhang (2019) revealed rapid degradation and elimination
of dimethoate, atrazine and propoxur due to exposure to vacuum
ultraviolet/ultraviolet/chlorine. Westlund et al. (2018) eliminated
50–70% of the biological activity of atrazine, 2,4-D, terbutryn, diuron,
and tebuconazole by ozonation. Furthermore, Aliste et al. (2020)
removed seven fungicide residues, including difenoconazole, from
leaching water using different homogeneous (photo-Fenton and
photo-Fenton-like) and heterogeneous (ZnO and TiO2) photocatalytic
systems. They indicated that mineralization of initial dissolved organic
carbon was not complete, but the conversion rate under ZnO/Na2S2O8
treatment was approximately 1.3 times higher than that using
TiO2/Na2S2O8.
Furthermore, advanced chemical method application (chlorination,
ozonation, chemical precipitation) followed by adsorption using acti­
vated carbon successfully removed 44 pesticide residues from water,
with removal percentages that reached 90%. The tested pesticides are
herbicides from different groups, and insecticides from OC and OP-
residues are listed in Table 1 (Ormad et al., 2008). In contrast, Khedr
et al. (2019) showed the ability of gamma irradiation to completely
eliminate chlorfenvinphos, diazinon, dimethoate, and profenofos from
deionized and ionized water at low pesticide concentrations. It can be
concluded that AOPs are suitable and effective methods to remove
pesticide residues in groups 1–7 (Table 4).
3.4.5. Removal of pesticide residues via phytoremediation
The use of living plants to remove pesticide residues from water is
denoted as phytoremediation, although the phytoremediation definition
includes using living plants to clean up soil, air and water contaminated
with hazardous contaminants (Reichenauer and Germida, 2008). Phy­
toremediation has been successfully used to remove clomazone residues
in water (Escoto et al., 2019), 56% for acetochlor and 51% for alachlor,
whereas metolachlor was resistant to removal with an efficiency of 23%
(Elsayed et al., 2014), and similarly for imazalil and tebuconazole (Lv
22
Journal of Environmental Management 299 (2021) 113611
et al., 2016). In contrast, Garcinuño et al. (2006) removed 57% of
carbaryl, 53% of linuron and 55% of permethrin using aquatic plants
(Upinus angustifolius), indicating that some plants (e.g., L. angustifolius)
could be a useful biotechnology for pesticide removal from water.
Similarly, Su et al. (2019) showed the ability of genetically modified
plants to remove acetochlor from water, with a percentage removal that
reached 51.7–57.4%. However, Hwang et al. (2020) completely
removed atrazine residues in 12 weeks from water by floating treatment
in wetlands planted with Canna flaccida.
However, organochlorine, strobilurin/strobin, organosphosphate
and pyrethroid residues were removed from agricultural wastewater
using constructed wetlands (Vymazal and Březinová, 2015). To date,
pesticide removal generally increases in direct proportion with KOC;
however, the relationship is not strong. Similarly, many pesticides of
different chemical structures (e.g., fluoranthene, trifluralin, alachlor,
isoproturon, diuron, tributyltin compounds, simazine, atrazine, chlor­
pyrifos, chlorfenvinphos, hexachlorobenzene, pentachlorophenol,
endosulfan, DDT and dieldrin) were removed at high weekly removal
efficiencies (>87%) (Gorito et al., 2017, 2018). Moreover, a high
removal rate (87.22 ± 16.61%) of OP residues was found using con­
structed wetlands (Liu et al., 2019). Similarly, Sherrard et al. (2004)
showed the efficiency of constructed wetland in removing chlorothalonil
and chlorpyrifos from water. Similar observations were obtained with
simazine and wetlands (Wilson et al., 2011). However, Xia and Ma
(2006) emphasized the phytoremediation potential of water hyacinth
(Eichhornia crassest) to remove ethion from water. In summary, this
method is suitable for pesticide residues in groups 1–4 (Table 4) because
their water solubility enables them to stay in the root zone, hence
exposing them to potential microbial degradation associated with plant
roots.
3.4.6. Removal of pesticide residues via biodegradation
Pesticide biodegradation is a partial or total destruction of pesticide
molecules by bacteria or fungi throughout three stages. This includes
biodeterioration (partial metabolism that may introduce minor changes
to the chemical structure of pesticide molecules), biofragmentation (a
complete conversion of pesticide molecules to carbon dioxide, water
and/or other gases), and assimilation (the conversion of carbon dioxide
and water by plants to glucose). A similar definition was given for other
cases (Lucas et al., 2008). Several pesticides have been removed from
water by biodegradation. For instance, chlorpyrifos and diazinon (OP
residues) were removed from liquid medium, soil and a biobed bio­
mixture using a Streptomyces mixed culture with removal rates of 0.036
and 0.015/h and half-lives of 19 and 46/h, respectively (Briceño et al.,
2018). Similarly, phorate (OP residue) was removed from water using a
biodegradation method consisting of three microorganisms (Brevibacte­
rium frigoritolerans, Bacillus aerophilus and Pseudomonas fulva), and the
biodegradation efficiency ranged from 97.65 to 98.31% (Jariyal et al.,
2018).
In contrast, carbaryl was completely (100%) removed from water
using Rhodopseudomonas sphaeroides (Wu et al., 2019a, 2019b), DDT was
removed using Stenotrophomonas sp (Pan et al., 2016), and lindane was
removed using Gram-negative bacteria (Zhang et al., 2020). Alvar­
ado-Gutiérrez et al. (2020) showed the ability of three bacteria (Klebsi­
ella oxytoca, Flavobacterium johnsoniae, and Stenotrophomonas
maltophilia) to biodegrade carbendazim. Additionally, Wu et al. (2018)
showed the ability of Sphingomonas sp. to remove highly toxic and
recalcitrant tricyclazole from wastewater.
3.5. Comparison between this study and studies in the literature
A comparison of the present study with previously published studies
on this subject matter is shown in Table 5. The unique aspect of the
present review is that it collected concentrations of pesticide residues
from many countries and then classified these pesticide residues into
different functional and toxicity groups. It also estimated the ODI values
I. El-Nahhal and Y. El-Nahhal Journal of Environmental Management 299 (2021) 113611

Table 4
Classes of some pesticide according to solubility limit in water.
Solubility class Solubility range Insecticides Herbicides Fungicides
(mg/L)

Practically <1 PY (L-Cyhalothrin, λ-Cyhalothrin, Cyfluthrin, Dinitroaniline (Trifluralin, Phenylurea (pencycuron)

insoluble Cypermethrin, Deltamethrin, Etofenprox, Permethrin, Pendimethalin) Chlorophenyl (quintozene,
Fenpropathrin) Oxidiazole (oxadiazon) Chloronitrile
OC (Aldrin, heptachlor, α-/β-/γ-Chlordane, Methoxychlor, (Chlorothalonil)
Dieldrin, Endrin, α-/β-Endosulfan)
O (Buprofezin, Pyriproxyphen,
OP (dichlofenthion)
Poorly soluble 1–9.99 OC (Lindane) Amide (bromobutide) Methoxyacrylate
OP (Chlorpyrifos, Ethion, Fenthion) Oxyacetamide (mefenacet) (Picoxystrobin)
CT (carbaryl) Thiocarbamate (esprocarb) Morpholine (Fenpropimorph)
O (Fipronil) OP (butamifos) Strobilurin (Azoxystrobin)
Triazine (Simazine, Terbuthylazine, Triazole (Epoxiconazole)
Propazine) Benzimidazole
(Carbendazim)
Oxathiin (flutolanil)
Low soluble 10–29.99 OP (Azinphos-Methyl, Disulfoton, Fenitrothion, isofenphos Chloroacetamide (alachlor, Butachlor) Benzanilide (mepronil)
oxon, Parathion-Ethyl, Phosmet, Profenofos) Thiocarbamate (thiobencarb, Triazole (Difenoconazole)
CT (Methiocarb) dimepiperate) Imidazole (Prochloraz)
Benzonitrile (dichlobenil)
OP (piperophos)
Triazine (Terbutryn)
Slightly soluble 30–99.99 OP (Triazophos, cyanophos, Phorate, Parathion-methyl, Triazine (prometryn, Atrazine) Benzimidazole
Mephosfolan, Diazinon) Phenylamide (Diuron) (Thiabendazole)
Methylthiotriazine (dimethametryn) Triazole (Tebuconazole,
Urea (Linuron, Isoproturon, Flutriafol)
Chlorotoluron) OP(edifenphos)
Anilide (Propanil) O (Etridiazole)
Moderately 100–999.99 OP (pyridaphenthion, Chlorfenvinphos, malathion) Triazine (Terbumeton, Cyanazine, Benzisothiazole
soluble CT (Carbofuran, Fenobucarb) Ametryn, simetryn, Prometon) (probenazole)
N (Imidacloprid) Chloroacetanilide (Acetochlor, Alachlor, Imidazole (Imazalil)
Pretilachlor, Metoalachlor) OP (iprobenfos)
Triazolobenzothiazole
(tricyclazole)
soluble 1000–9999.99 OP (Thionazin, Ethoprophos) Thiocarbamate (Molinate)
CT (Propoxur) Isoxazolidinone (Clomazone)
Imidazolinone (Imazethapyr)
Urea (Tebuthiuron)
highly soluble >10000 OP (Dichlorvos, Dimethoate, Methamidophos, Omethoate, Phosphonoglycine (Glyphosate)
Monocrotophos, Dicrotophos) Triazinone (Metribuzin, Hexazinone)
Alkylchlorophenoxy (2,4-D, MCPA,
Mecoprop)

of pesticide residues and compared them with ARfD values; calculated
HQ and HI for adults, children and infants in each country; predicted
future toxicity; classified countries into four groups; and discussed
human health risk. The present review provides removal options.
In contrast, previously published studies neither classified pesticide
residues into toxic classes nor provided removal options for these resi­
dues. Additionally, the published articles did not review the potential
health risk among populations.
In conclusion, the present review highlights the current status of
pesticide residues in countries and provides suitable options for their
removal. Thus, it fills the research gap in the field of pesticide residues in
drinking water and their purification options that can reduce the po­
tential health risk and provide valuable information that can serve as a
baseline for further developments in the field.

Table 5
Comparison between this review and those published previously.
Reviewed parameter Morrissey et al. Mohammed et al. Elibariki and Bruce-Vanderpuije et al. Li and Jennings Olisah et al. Present
(2015) (2019) Maguta (2017) (2019) (2017) (2020) review

Countries
Insecticide residues
Acaricide residues
Fungicide residues
Herbicide residues
Classification of residues
Estimation of ADI
Estimation of MDI
Predicted toxics scenario
HI for adult,
HI for child
HI for infant
Removal options
guidelines for a safe water
protection
Many countries Ghana Tanzania Ghana Few countries Few countries, Many
countries
✓ ✓ ✓ ✓ ✓ X ✓
X X X X X X ✓
X X X X ✓ X ✓
X X ✓ X ✓ X ✓
X X X X X X ✓
X X X X X X ✓
X X X X X X ✓
X X X X X ✓
X X X X X X ✓
X X X X X X ✓
X X X X X X ✓
X X X X X X ✓
X X X X X X ✓

23
I. El-Nahhal and Y. El-Nahhal
4. Conclusion
This review highlighted the levels of pesticide residues in drinking
water samples in several countries and demonstrated the presence of
hazardous residues of pesticides with class Ia, Ib and II toxicity. More­
over, pesticides with class Ia or Ib toxicity are extremely toxic pesticides,
and most of them are cholinesterase inhibitors.
This review also estimated the average ODI of pesticides in many
countries, calculated the corresponding HI and demonstrated high
values in many countries (4.48, 28.74, 30.97), suggesting potential risk
among consumers. Moreover, this review demonstrated health risks
among water consumers. The review highlights the value of the Rel Std
Error as a statistical tool with which to compare the concentration of
pesticide residues between countries. Furthermore, this review presents
pesticide removal options.
Nevertheless, the limitation of this study is that there is a lack of
published data regarding pesticide residues, and only old literature can
be found in some cases.
Nonetheless, the main point of the study is that the number of
countries included is a representative sample of all countries, as well as
the fact that many pesticide residues were similarly found in some
countries. Furthermore, this review also provides a systematic reference
with which to estimate the daily intake of pesticide residues, allowing
researchers to determine HIs that are best suited for the study. In
conclusion, this review updates the state of the art in the field of pesti­
cide residues in drinking water and their potential health risks. This
manuscript may help young scholars in the field of pesticide residues in
water.
Declaration of competing interest
No competing interest to declare.
Acknowledgment
Prof Dr Yasser El-Nahhal thanks the AvH Foundation for funding the
research stay in Berlin, Germany.
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