Ecotoxicology and Environmental Safety 182 (2019) 109362

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Ecotoxicology and Environmental Safety

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

Review

Fluoride contamination, health problems and remediation methods in Asian T

groundwater: A comprehensive review
Krishna Kumar Yadavb, Sandeep Kumarc, Quoc Bao Phamh, Neha Guptab, Shahabaldin Rezaniad,
Hesam Kamyabe, Shalini Yadavf, Jan Vymazalg, Vinit Kumarb, Doan Quang Tria,∗,
Amirreza Talaiekhozanii, Shiv Prasadc, Lisa M. Reecej, Neeraja Singhk, Pradip Kumar Mauryal,
Jinwoo Chod
a
Sustainable Management of Natural Resources and Environment Research Group, Faculty of Environment and Labour Safety, Ton Duc Thang University, Ho Chi Minh
City, Viet Nam
b
Institute of Environment and Development Studies, Bundelkhand University, Kanpur Road, Jhansi, 284128, India
c
Centre for Environment Science and Climate Resilient Agriculture, Indian Agricultural Research Institute, New Delhi, 110012, India
d
Department of Environment and Energy, Sejong University, Seoul, 05006, South Korea
e
UTM Razak School of Engineering and Advanced Technology, Universiti Teknologi Malaysia, Malaysia
f
Department of Civil Engineering Rabindranath Tagore University Raisen, Madhya Prades, India
g
Czech University of Life Sciences Prague, Faculty of Environmental Sciences, Kamýcká 129, 165 21 Praha 6, Czech Republic
h
Department of Hydraulic and Ocean Engineering, National Cheng-Kung University, Tainan 701, Taiwan
i
Department of Civil Engineering, Jami Institute of Technology, Isfahan, Iran
j
Sealy Institute for Vaccine Sciences, University of Texas Medical Branch, Galveston, TX, 77555, USA
k
Department of Botany, University of Delhi, New Delhi, 110007, India
l
Department of Zoology and Environmental Science, Gurukula Kangari Vishwavidyalaya, Haridwar, Uttarakhand, India

A R T I C LE I N FO A B S T R A C T

Keywords: In low concentration, fluoride is considered a necessary compound for human health. Exposure to high con-
Asia centrations of fluoride is the reason for a serious disease called fluorosis. Fluorosis is categorized as Skeletal and
Contamination Dental fluorosis. Several Asian countries, such as India, face contamination of water resources with fluoride. In
Defluoridation this study, a comprehensive overview on fluoride contamination in Asian water resources has been presented.
Groundwater
Since water contamination with fluoride in India is higher than other Asian countries, a separate section was
Health effects
dedicated to review published articles on fluoride contamination in this country. The status of health effects in
Removal
Asian countries was another topic that was reviewed in this study. The effects of fluoride on human organs/
systems such as urinary, renal, endocrine, gastrointestinal, cardiovascular, brain, and reproductive systems were
another topic that was reviewed in this study. Different methods to remove fluoride from water such as reverse
osmosis, electrocoagulation, nanofiltration, adsorption, ion-exchange and precipitation/coagulation were in-
troduced in this study. Although several studies have been carried out on contamination of water resources with
fluoride, the situation of water contamination with fluoride and newly developed technology to remove fluoride
from water in Asian countries has not been reviewed. Therefore, this review is focused on these issues: 1) The
status of fluoride contamination in Asian countries, 2) health effects of fluoride contamination in drinking water
in Asia, and 3) the existing current technologies for defluoridation in Asia.

1. Introduction
Groundwater is the main source of drinking water in most of the
Asian countries (Al-Hatim et al., 2015; Raj and Shaji, 2017). The esti-
mated population of Asia is 4.5 billion, which is about 60% of the
world's total population (WPR, 2018). Consequently, the demand of
groundwater for drinking and irrigation purposes in this continent in-
creases steadily due to population growth, while the supply of
groundwater decreases due to over-exploitation (Gleeson et al., 2012;
Gupta et al., 2013; Alhababy and Al-Rajab, 2015). Five Asian countries
including India, Nepal, Bangladesh, Pakistan and China use over
300 Km3 of groundwater annually, nearly half of the world's total

∗
Corresponding author.
E-mail address: doanquangtri@tdtu.edu.vn (D.Q. Tri).

https://doi.org/10.1016/j.ecoenv.2019.06.045
Received 19 January 2019; Received in revised form 10 June 2019; Accepted 14 June 2019
0147-6513/ © 2019 Elsevier Inc. All rights reserved.
K.K. Yadav, et al.
annual use (Shah et al., 2003). About 85% of groundwater used in ir-
rigation is considered the primary contributor to groundwater depletion
in Asia (FAO, 2013).
The presence of fluoride (F−) in drinking water has some health
benefits for consumers such as reducing dental cavities, but an ex-
cessive intake of this anion or its presence at high concentration
(> 1.5 mg/L) can lead to dental and Skeletal Fluorosis (Guissouma
et al., 2017; Raj and Shaji, 2017; Yadav et al., 2015). Fluoride is found
naturally in groundwater and soil, but some anthropogenic activities
increase the concentration of F− with fluorinated industrial waste (iron,
steel, glass, aluminum), or agricultural activities by using the phosphate
fertilizers and certain pesticides (Gupta et al., 2015, 2019; Srivastav
et al., 2018; Maurya et al., 2019). The level of daily F− exposure varies
by region. The fish and tea consuming population is more prone to
fluoride exposure as it contains high concentration of fluoride (Kanduti
et al., 2016).
Fluoride contamination in groundwater is becoming a worldwide
problem because it is natural and uncontrollable. Based on available
literature, geogenic sources are the main cause of fluoride exposure due
to the consumption of F− contaminated groundwater (Sharma et al.,
2015a, 2015b; Mukherjee and Singh, 2018). Dangerous levels of F− are
increasingly found in groundwater in South and Southeastern Asia
along with infectious or other toxic substances (WHO, 2000). South
Asia represents the southern region of the Asian continent, which
comprises Afghanistan, Bangladesh, Bhutan, Maldives, Nepal, India,
Pakistan and Sri Lanka with 39.5% of the total Asian population being
present in these countries and comprising 24% of the total world's
population (Sikdar, 2019). Hence, a high rate of F− in India, Pakistan
and China groundwater is reported to have considerable impact on
human health. For instance, the consumption of water with a higher F−
rate (3 mg/L) causes Skeletal Fluorosis effect in adults and children.
Fluorosis is endemic in atleast 25 countries in all the continents
including Asia, Africa, Europe, North and South America (Fawell et al.,
2006). In addition, excess of F− causes several other health problems
such as severe gastroenteritis, salivation, anorexia, muscle weakness,
stiffness, restlessness, sweating, dyspnea, ventricular abnormalities and
tachycardia (Sahu et al., 2017). Factors of chemical reactions such as
precipitation, weathering, dissolution, ion exchange, and various bio-
logical processes commonly occur below the surface, influencing F−
concentrations in groundwater. Due to the detrimental F− effects on
human health and the fact that very few studies have been conducted
on the factors affecting low F− amounts, these issues were investigated
in Sistan and Baluchestan Province (Iran).
There are several issues which should be considered when assessing
the effects of F− exposure and contamination: (1) high F− concentra-
tion in groundwater is mainly confined to arid and semiarid regions of
Asia and North Africa; (2) geogenic sources of F− in water are fluorine-
bearing minerals in rocks and sediments, whereas anthropogenic
sources of F− in water are mainly pesticides and industrial waste; (3)
F− mobilization from geogenic sources is mainly controlled by alkali-
nity and temperature; and (4) F− occurrence in water is associated with
ions such as sodium, arsenic, chloride and bicarbonate (Kanchan et al.,
2015; Ali et al., 2016). Although, many investigations have been car-
ried out on defluoridation, there is no sustainable solution to this salient
crisis. Therefore, there is still a need to find a suitable and effective
technology for defluoridation of drinking water.
It is evident from the literature survey that Asian and African
countries are more prone to fluoride exposure due to the consumption
of fluoride contaminated groundwater. The major source of fluoride in
groundwater is geogenic and includes many rock-forming minerals. The
status of fluoride contamination in African grounwater has been al-
ready reviewed (Kut et al., 2016). Hence, the present review aimed to
describe the contamination of fluoride in Asian groundwater, its pos-
sible health effects and remediation techniques.
2
Ecotoxicology and Environmental Safety 182 (2019) 109362
2. Fluoride contamination in groundwater
Fluorine is the 13th most abundant element, containing within
600–700 ppm (0.06–0.09%) of the crust by mass in the Earth's crust
(Armienta and Segovia, 2008). The chief source of F− in water are
fluorine-bearing minerals such as fluorspar, cryolite, fluorapatite, and
hydroxyapatite found in local rocks, sediments (Farooqi et al., 2007;
Yadav et al., 2018a) and clay minerals (Katsanou et al., 2013). It is
found around 330 mg/kg in soil (Dey and Giri, 2016), seawater
(1.2–1.4 mg/L), groundwater (67 mg/L) and surface water bodies
(< 0.1 mg/L) (IPCS, 2002). The F− occurrence in groundwater basi-
cally takes place due to weathering, leaching processes and subsequent
percolating through soil and sediments. The various factors that govern
the release of F− in the groundwater are temperature, pH and solubility
of F− bearing minerals, as well as anion exchange capacity of aquifer
materials (Jha and Mishra, 2016). Interestingly, F− contamination of
the groundwater is related to the installed tube wells at shallow depth
that results in enrichment of shallow ground water by evaporation
(Patel et al., 2017). For decades, groundwater has been a major source
of water supply in the Yuncheng Basin. In this region, endemic fluorosis
was first confirmed in 1980s, and 22% of the villages in Linyi County
had severe fluorosis due to the F− contamination in drinking water (Li
et al., 2015).
Data indicate that the hydrological condition of groundwater is also
an important factor controlling the amount of F− in groundwater. A
recent report (Biglari et al., 2016) details numerous factors affecting the
occurrence of F− in groundwater where groundwater is stored. For
instance, in the Qiji area (China), F−-bearing mineral dissolution, ca-
tion exchange, and alkaline conditions are the driving factors for F−
enrichment in groundwater (Li et al., 2018).
In the Huaibei Plain, a high fluorine area in the Northern China,
high F− concentrations are associated with weakly alkaline conditions,
moderate total dissolved solids, with calcium and sodium ions being the
dominant ions (Hu et al., 2017). In mid-1960s in the Northern Thailand,
studies by the United States Inter-Departmental Committee on Nutrition
for National Defense (US IDCNND) were implemented on F−-related
fluorosis cases (Leatherwood et al., 1965). It was determined that the
complex nature of F− genesis and its transport across wide geographic
areas creates many challenges/problems on water resource manage-
ment for safe human consumption. It was determined that variable
water depths resulted in unpredictable F− concentrations, and there-
fore, the simplistic idea that deep water (e.g. well water) is safer to
drink than water found at more shallow levels, is unconvincing (Chuah
et al., 2016).
2.1. Asian scenario
As stated previously, contamination of F− in groundwater of the
Asian countries varies from region to region based on climate, rainfall,
composition of rocks, and topography. The F− concentration exceeded
1.5 mg/L in groundwater in most regions of the Asian countries. Several
investigations have reported the highest level of F− at Province of
Afghanistan (up to 79.2 mg/L). The F− content varied from 20 to
79.2 mg/L in different regions of South Korea (Chae et al., 2007), Ka-
lalanwala, Pakistan (Farooqi et al., 2007), Ninh Hoa, Vietnam (Tu,
2008), Jenderam Hilir, Malaysia (Shamsuddin et al., 2015) and Pro-
vince of Afghanistan, Afghanistan (Hayat and Baba, 2017). These high
F− contents were mainly due to geological processes, F− containing
rocks, and the presence of apatite minerals in groundwater (Msonda
et al., 2007).
The F− concentration in groundwater ranged between 0.02 and
9.2 mg/L have been reported in the Muteh region, Iran (Keshavarzi
et al., 2010), While the Yuncheng Basin in China reported up to
14.10 mg/L F− contamination in groundwater (Li et al., 2015). The F−
content in groundwater was ranged from 10 to 20 mg/L in many re-
gions such as Birbhum at West Bengal; Balod and Brahmaputra flood
K.K. Yadav, et al.
plain region in India (Batabyal and Gupta, 2017; Yadav et al., 2016; Das
et al., 2016a); Anuradhapura at Sri Lanka (Chandrajith et al., 2012);
East Java at Indonesia (Heikens et al., 2005) and parts of Anatolia at
Turkey (Oruc, 2008). In the Gaza Strip, F− concentration was observed
to ranged from 0.30 to 6.45 mg/L (Jabal et al., 2014). Similarly, in the
Negev Desert (Israel), F− content up to 5.5 mg/L has been reported
(Kafri et al., 1989).
Groundwater contamination in Iran (Posht-e-Kooh-e-Dashtestan
Southern Iran), Japan (Mizunami region), China (Shanxi and Inner
Mongolia, Taiyuan basin, Datong basin and Northern China) Mongolia
(Hetao Basin, Oyu Tolgoi and Tavan Tolgoi), Saudi Arabia, and Yemen
(NW Taiz city) was recorded between 5 and 10 mg/L (Looie and Moore,
2010; Abdelgawad et al., 2008; Hu et al., 2013; Guo et al., 2007, 2008;
Li et al., 2012; Nakazawa et al., 2016; Alabdulaaly et al., 2013; Al-
Amry, 2009). Similarly, F− concentrations between > 1.5 and 5 mg/L
have been reported in Bangladesh and Myingyan Township of Myanmar
(Hoque et al., 2003; Bacquart et al., 2015). In North Jordan, the Su-
laimani province of Iraq, Bahrain (semi-arid tracts of Bahrain) and
Thailand (remote areas), the groundwater F− contamination was re-
corded below 1.5 mg/L (Rukah and Alsokhny, 2004; Khursheed et al.,
2015; Akhter, 1998; Chuckpaiwong et al., 2000).
Pakistan is also suffering from F− contamination problem (Farooqi,
2015). A study carried out by Rasool et al. (2017) at 29 large cities of
Pakistan reported that 34% of the cities exhibited F− levels more than
1.5 mg/L while Lahore, Quetta and Tehsil Mailsi were observed having
maximum values of 23.6, 24.4, 5.5 mg/L, respectively. Another study
(Tahir and Rasheed, 2012) was carried out at 16 main cities to explore
the F− levels using 747 groundwater water samples. The results showed
that about 16% of observed sources having F− value above the per-
missible limit (1.5 mg/L), Punjab had high levels (0.05–19.70 mg/L)
and Baluchistan (0.1–24.48 mg/L) exceeded permissible F- levels (Tahir
and Rasheed, 2012). Table 1 and Fig. 1 illustrates the F− status in many
regions of the Asian countries.
2.2. Indian scenario
India is one of the most affected countries by F− contamination in
groundwater. The presence of F− in groundwater is higher than the
permissible limit, and is a serious health problem. Nearly 12 million of
the 85 million tons of F− deposits on the earth's crust are found in India
which might be the reason of high F− occurrence in groundwater. In
terms of the number of people affected and distribution area, arsenic
and F− are considered as the two main contaminants (Sahu, 2019). For
instance, the occurrence of F− and NO32− (nitrate) above desirable
limits showed the possibility of anthropogenic enrichment of F− in
groundwater of Siwani Block, Western Haryana, India (Ali et al., 2018).
Meanwhile, the groundwater of the Dongargaon area in India was
found to be unsuitable for drinking purposes due to F− contamination.
However, this water can be used for irrigation (Sahu et al., 2017).
F− contamination has been recognized as one of the most sig-
nificant natural groundwater-quality problems affecting arid and semi-
arid regions of India. For example, high levels of F− have been found in
the Nalgonda region of Andra Pradesh. Thereafter, many parts of the
country were identified with high F− concentrations among which the
severely-affected states were Andra-Pradesh, Rajasthan, Haryana,
Punjab, Gujarat and Assam (Kumar et al., 2016).
The groundwater flow rate is higher in areas by a nearby river
where residence time is lower, and there is less time of contact between
water and F− bearing rocks. This has led to lower concentrations of F−
in the groundwater. Groundwater in semiarid areas surrounding
Gujarat is known to have F− concentrations that go above the guideline
for drinking water (1.5 mg/L) set by the World Health Organization
(WHO, 2005; Raza et al., 2016). Groundwater F− concentrations below
5 mg/L have been reported in Bihar, Chhattisgarh, Jammu and
Kashmir, Jharkhand, Karnataka, Maharashtra, Tamil Nadu, and Uttar
Pradesh states of India. In Andra Pradesh, Delhi, Gujarat, Kerala, Orissa,
3
Ecotoxicology and Environmental Safety 182 (2019) 109362
and West Bengal F− concentrations have been reported between 5 and
10 mg/L. Fluoride concentrations ≥10–20 mg/L were recorded in areas
of Madhya Pradesh, Punjab, Assam and Haryana. It has been reported
that in many parts of Rajasthan, the maximum F− concentration has
exceeded beyond 20 mg/L (CGWB, 2014). The maximum F− affected
regions have been reported to be Rajasthan and Gujarat (80–100%),
followed by Andhra Pradesh and Punjab (60–80%) as shown in
Fig. 2(b). In Madhya Pradesh, Maharashtra, Kerala, Tamil Nadu,
Jharkhand, West Bengal, and Sikkim, about 21–40% areas are affected
by F− contamination. In some regions of India, the F− enrichment is
restricted and found in very few areas of Haryana, Jammu and Kashmir,
Karnataka, Uttar Pradesh, and Assam (10–20%). In Andhra Pradesh,
nearly 70% of the districts are affected by groundwater F− con-
tamination. In Delhi, mainly the Northwest and West Regions are af-
fected by F− contamination. Almost 92% of the districts in Gujarat are
affected by F− contamination and have reported up to 7.5 mg/L. In
Rajasthan, 97% of the districts (mainly arid regions) are severely af-
fected and have recorded up to 38 mg/L F− content. In West Bengal,
37% of the districts are under F− contamination zone. In Punjab, F−
concentrations were observed up to 11.30 mg/L in Sangrur and Ghor-
enab regions, whereas nearly 77% of the other districts are under high
F− contamination risk. In Orissa, 60% of the districts are under high F−
content zone (CGWB, 2010). Table 2 and Fig. 2(a) and (b) (affected
districts) show the status of F− concentration in different parts of India.
3. Mode of action of fluoride toxicity in humans from
contaminated water
Fluoride ion transportation through biological cell membranes oc-
curs mainly by the non-ionic diffusion process of hydrogen fluoride
(HF) (Barbier et al., 2010). After toxic exposure of F−, the toxic effects
may not medically manifest during the initial stages and may be mis-
diagnosed as rheumatoid arthritis (NRC, 2006). The systematic ex-
posure of F− and biological consequences of human cells are illustrated
in Fig. 3. Around 45% of ingested F− is absorbed in the intestinal layer,
and this absorbed F− is less sensitive to pH in the intestine and may
occur via facilitated diffusion processes (He et al., 1998). The ingested
F− forms insoluble complex compounds with cations (Ca2+, Mg2+, K+,
Na+, Al3+) that can considerably decrease gastrointestinal absorption
of F− thereby causing hypocalcemia and hindering the Mg and Mn-
dependent enzymes (Whitford et al., 1997). Fluoride binds with Ca2+
ions to form Ca ionospheres that can readily permeabilize the cell
membrane (Sireli and Bulbul, 2004). However, the alliance of calcium-
channel blocking agents can prevent the F− movement across the cell
membrane. Once absorbed into the blood vessels, F− quickly diffuses
throughout the body and localizes in calcium-rich areas such as bone
and teeth. According to the ATSDR (2003), around 80–90% of the ab-
sorbed F− is retained in infants, while 60% of F− is retained in adults.
The primary toxic influence of F− in cells occurs when F− interacts
with enzymes (Adamek et al., 2005). Absorbed F− at the micromolar
level is regarded as an effective anabolic agent because it favours cel-
lular generation, whereas at the millimolar level the contaminant may
inhibit numerous cellular enzymes like phosphatases which are im-
portant for maintenance of cellular homeostasis (Mendoza-Schulz et al.,
2009).
These F− modify the activity of several mitochondria-rich cells like
human kidney cells (Dabrowska et al., 2004). The high concentration of
F− exposure is associated with the generation of reactive oxygen spe-
cies (ROS) within cellular mitochondria by aiding in the production of
nitric oxide (NO) and reduction of cellular antioxidant defenses against
oxidative damage (García-Montalvo et al., 2009). Fluoride can combine
with the functional groups of amino acids by surrounding all the active
sites of an enzyme like the enzymes of the glycolytic pathway and the
Krebs cycle. This reaction causes an inhibitory effect on Na+/K+-AT-
Pases of the glycolytic pathway and the Krebs cycle, whereby F− pre-
vents cellular respiration and ATP production (Adamek et al., 2005) as
 Table 1
Reported concentration of F− in the selected Asian groundwater with possible affecting factor.
Country Source of water Possible cause Climatology Number of Region, province or F− concentration References
samples village (mg/L)
K.K. Yadav, et al.

Climatic conditions Rainfall (mm/ Temp. (oC)

annum)

Afghanistan Groundwater Granite rocks, igneous rocks, Arid to semi-arid 300 −20 to 50 1808 Province of Afghanistan 0.010 - 79.20 Hayat and Baba (2017)
sedimentary, volcanic rocks
Groundwater Calcite, dolomite, biotite Arid to semi-arid 312 −7.1–32.1 – Kabul Basin Up to 1.32 Broshears et al. (2005)
Bahrain Groundwater F− bearing minerals Desert climate 72 Up to 47 31 Semi-arid tract of 0.50 - 1.46 Akhter (1998)
Bahrain
Bangladesh Groundwater F− bearing minerals – – – 163 Bangladesh 0.02–2.32 Hoque et al. (2003)
China Groundwater F−bearing minerals, fluorite and Semi-arid climate 428 – 105 Xiji County 0.2–3.01 Wei et al. (2016)
calcite
Shallow F− bearing minerals in the aquifer Arid climate 130–220 7 49 and 62 Shanxi and Inner 0.3–5.60 Hu et al. (2013)
groundwater Mongolia
Shallow Fluorite and fluorapatite Semi-arid climate 550 – 100 Yuncheng Basin 0.5–14.10 Li et al. (2015)
groundwater
Shallow F− in F− rich minerals, fluorite Semi-arid Region 446.6 5.6–7.8 59 Taiyuan basin Up to 6.20 Guo et al. (2007)
groundwater
−
Groundwater F bearing minerals Arid climate 637 14.3–26.4 304 Yuanmou county Up to 4.0 Chen et al. (2012)
Groundwater Coal mining activities, carbonate Subtropical humid 1436 14.1 20 Central Guizhou 0.05–0.38 Li et al. (2016)
rocks, climatic factor
Deep groundwater Calcite, fluorite, Fe-hydroxides Semi-arid 225–400 14.9–22.8 94 Datong basin, Northern Up to 8.30 Li et al. (2012)
China
Groundwater Fluorine-rich sediment, fluorite and Semi-arid climate 400–1200 – 133 North China Plain 0.18 - 5.59 Li et al. (2017)
calcite
Gaza strip, Groundwater mineral–water interaction, Calcite Semi-arid, Mediterranean 300 9.0–29.0 200 Gaza strip 0.3–6.45 Jabal et al. (2014)

4
Palestine and fluorite climate
Indonesia Groundwater Infiltration, irrigation practices Tropical climate 700 29 54 East Java 0.1–4.20 Heikens et al. (2005)
(continued on next page)
Ecotoxicology and Environmental Safety 182 (2019) 109362
 Table 1 (continued)

Country Source of water Possible cause Climatology Number of Region, province or F− concentration References
samples village (mg/L)
o
Climatic conditions Rainfall (mm/ Temp. ( C)
K.K. Yadav, et al.

annum)

India Groundwater Fluorapatite – – – 16 Alleppey 0.68–2.88 Raj and Shaji (2017)

Groundwater Archaean, Gondwanas rocks Semi-arid climatic 1200–1400 10–45 147 Birbhum, West Bengal 0.01–19 Batabyal and Gupta
(2017)
Groundwater Barberiite, bararite, hieratite, – – 50 Balod 1.5–14 Yadav et al. (2016)
ferruccite, sellatite, cryolite –
Groundwater Biotite, hornblende, muscovite, and Semiarid and subtropical 875 14–41 419 Prakasam 0. 50–9.84 Reddy et al. (2016)
pyroxene continental climate
Groundwater Biotite and hornblende – 875 20–40 650 Dharmapuri, Tamil 0.14–6.48 Jagadeshan and Elango
Nadu (2015)
Groundwater Amphibole, biotite, fluorite, mica Semi-arid zone 994 8–38 49 Mulugu-Venkatapur 0.28–5.48 Satyanarayana et al.,
and apatite Mandals 2017
Groundwater Fluorite, Granite, calcite Warm, sub-humid and sub- 765 5–48 62 Patan, Gujarat 0.4–4.80 Kumar et al. (2017)
tropical
Groundwater Sandstone and limestone Semi-arid climate Average 25–46 150 Fatehpur Sikri 1.1–3.80 Mishra (2013)
Shallow F− bearing minerals, florahalite, Semi-arid to subtropical 584 4.2–45 28 Agra city 0.9–4.12 Yadav et al. (2018b)
groundwater fluorite climate
Groundwater Gneisses, schists, pegmatites – – – 40 Nalbari 0.02–1.56 Sharma et al., 2012
Groundwater Chemical fertilizers and industrial Semi-arid climate 1250 – 228 Kalpakkam 0.0–0.7 Samantara et al. (2017)
wastes
Groundwater Hard rock aquifer, Charnockite, Semi-arid climate 902 – 54 Madurai 0.29–1.8 Thivya et al. (2017)
mafic appearance
Groundwater Weathering of rock, phosphorus Moderate Climate – – 44 Ranchi city 0 .0–2.19 Tirkey et al. (2017)
fertilizer

5
Groundwater Geogenic, phosphatic fertilizers Semi-arid to arid climate 1000 – 55 Pratapgarh 0.41–3.99 Tiwari et al. (2017)
Groundwater Fracture hard rock terrain Semi-arid to arid climate – 18–44 98 Nalgonda 3.0–7.60 Reddy et al. (2010)
Groundwater Granite, pegmatites schists, gneissic Semiarid climate 1000–1200 – 39 Central India 1.3–3.80 Naaz and Anshumali
rocks (2015)
Groundwater Rock-water interaction Rain shadow zones – 40 40 Brahmaputra 0.0–14.40 Das et al. (2016a)
Floodplains
Groundwater Fluorite, mica, apatite, amphiboles, Semi-arid climatic region, 618 13–40 36 Bhavani Basin 0.18–1.56 Kumar (2016)
illuminates
Groundwater Fluorite and fluorapatite Tropical climate 570–740 – 100 Thoothukudi Up to 3.30 Singaraja et al. (2014)
Groundwater Sewage water, manures Subtropical monsoon climate 923 – – Ramganga 0.01–85 Rajmohan and
Sub-Basin Amarasinghe (2016)
Groundwater Apatite, hornblende, and biotite – 1400 – 50 Simlapal block 0.0–4.90 Das et al. (2016b)
Groundwater F− bearing minerals Semi-arid climate 745 30 104 Siddipet area 0.4–2.20 Narsimha and Sudarsha
(2016)
(continued on next page)
Ecotoxicology and Environmental Safety 182 (2019) 109362
 Table 1 (continued)

Country Source of water Possible cause Climatology Number of Region, province or F− concentration References
samples village (mg/L)
o
Climatic conditions Rainfall (mm/ Temp. ( C)
K.K. Yadav, et al.

annum)

Iran Groundwater Limestone Arid climate 151.8 32.6 – Larestan and Gerash 1.6–3.80 Amini et al. (2016)
regions
Groundwater F− bearing minerals in rocks Arid climate 270 Bushehr Province 0.5–3.0 Battaleb-Looie et al.
(limestone dolomite, gypsiferrous, 31 - 47.5 28 (2013)
conglomeratic
Groundwater Water-rock interaction, basaltic Cold and arid climate 300 35.1–16.2 72 Maku 0.3–5.96 Moghaddam and Fijani
rocks, limestones (2008)
Groundwater Dolomite and limestone along with Acid climate 270 8.29–47.5 28 Posht-e-Kooh-e- 0.7–6.60 Looie and Moore (2010)
gypsum Dashtestan, Southern
Iran
Groundwater Amphibole and mica group minerals Arid to semi-arid climate 180–300 −5 to 32 47 Muteh area, Isfahan 0.2–9.20 Keshavarzi et al., 2010
in metamorphic and granitic rocks
Groundwater Volcanic rocks – 32.5 – Urban areas of Iran 0.02–5.00 Mesdaghinia et al.
(2010)
Groundwater Limestone – – – – Zarand, Kerman 0.33–3.51 Derakhshani et al.
province (2014)
Groundwater Food, dental products, and – – – 384 Hamadan province 0.0–1.78 Rafati et al. (2013)
pesticides
Groundwater F− in F− rich minerals Semi-arid climate 775 16.72 43 Babol City 0.4–34.0 Amouei et al. (2016)
Iraq Groundwater Volcanic, granitic and gneissic rocks Some areas were hot and – – 22 Sulaimani province 0.0–0.15 Khursheed et al. (2015)
others cold
Israel Groundwater Leaching of rock formations, Acid, mediterranean climate – 20–57 100 Different part of the 0.0–5.50 Kafri et al. (1989)
intensive confinement, vertical country

6
movement of water
Japan Groundwater F− rich minerals fluorite, and mica – – – – Mizunami area 2.0–7.0 Abdelgawad et al.
minerals, granite (2008)
Jordan Groundwater Fluorite and calcite solubility Mediterranean climate 200–500 – 22 North Jordan 0.009–0.05 Rukah and Alsokhny
(2004)
Malaysia Shallow Quaternary sediments with granitic Tropical rainforest weather – – 29 Parts of Kelantan state 0.20–0.39 Mathialagan et al.
groundwater bedrock (2017)
Groundwater Fluorite, apatite, amphiboles, and Tropical climate – 25–35 28 Jenderam Hilir 0.0–24 Shamsuddin et al.
micas (2015)
Mongolia Shallow Hypo-metamorphic rocks, water- Arid and temperate climate – – 20 Hetao Plain Up to 2.79 Xu et al. (2013)
groundwater rock interaction processes
Groundwater Fluorite and calcite Arid and temperate climate – – 29 Shahai town 0.30–2.58 Guo et al. (2012)
Groundwater Calcite, dolomite, Siderite and pyrite Arid temperate climate 130–220 5.6–7.8 63 Hetao basin Up to 7.87 Guo et al. (2008)
Groundwater F− in F− containing minerals Semiarid to arid 180 5.6–7.8 90 Hangjinhouqi, Hetao 0.30–6.01 Deng et al. (2009)
plain
Groundwater Coal mine, copper and gold mine Desert climate 50–250 – 39 Oyu Tolgoi and Tavan 0.37–5.46 Nakazawa et al. (2016)
area Tolgoi
Myanmar Groundwater Bedrock Dry climate 900 – 18 Myingyan Township 0.3–3.60 Bacquart et al. (2015)
Nepal Shallow Geological origin Warm temperate climate zone 1900 0–30 56 Kathmandu Valley 0.06–1.92 Pant (2011)
groundwater
Groundwater Quartzite, basalt, granite Sub-tropical, temperate 1362.2 −2 to 32 85 Bhaktapur Municipality 0.037–1.89 Thakur et al. (2015)
climate
(continued on next page)
Ecotoxicology and Environmental Safety 182 (2019) 109362
 Table 1 (continued)

Country Source of water Possible cause Climatology Number of Region, province or F− concentration References
samples village (mg/L)
o
Climatic conditions Rainfall (mm/ Temp. ( C)
K.K. Yadav, et al.

annum)

Pakistan Shallow Pleistocene/Quaternary sediments Semiarid and subtropical 510 4–41 24 Kalalanwala area 2.47–21.10 Farooqi et al. (2007)
groundwater continental climate
Groundwater Granitic rocks Tropical to subtropical – – 32 Southeastern Pakistan 1.13–7.85 Rafique et al. (2009)
climatic
Shallow Industrial and urban wastes, Climate is hot and humid 950 4–40 22 Sialkot 0.41–0.99 Ullah et al. (2009)
groundwater chemical substances during summer and cold
during winters
Groundwater Granitic rocks – – 32 Nagar Parkar Town, 1.13–7.85 Naseem et al. (2010)
Groundwater Industrial and anthropogenic – – 106 Karachi 0.60–3.64 Siddique et al. (2006)
effluent
Shallow and deep Fluorspar, fluorspatite, and – 650 – 60 Lahore area 0.0–8.46 Naeem et al. (2007)
groundwater amphiboles
Groundwater – – – – 4 Quetta 0.70–0.98 Jabeen et al. (2016)
Groundwater F− containing rocks – – – 40 Faisalabad 0.38–1.15 Kausar et al. (2003)
Saudi Arabia Groundwater – Desert climate – – 21 Kingdom of Saudi 0.10–5.4 Alabdulaaly et al.
Arabia (2013)
Groundwater Climatic conditions Hot and dry conditions, desert 185.6 28.8 – Hail region 0.5–2.8 Akpata et al. (1997)
climate
Groundwater Fluorite, apatite, and micas Desert climate – – 6 Al-Makhwah region 0.66–1.51 Al-Ghamdi et al. (2014)
Groundwater – – – – 40 Hael region 0.20–1.90 Al-Turki (2009)
Sri Lanka Shallow Granitic gneiss and biotite Intermediate, and dry zones 1000 – North-central and 0.01–4.34 Young et al. (2011)
groundwater gneiss dominate 294 Northwestern Sri Lanka
Groundwater Biotite, hornblende, garnet, and Tropical climate 1000 33 74 North Central 0.02–8.0 Jayawardana et al.

7
pyroxenes (2012)
Groundwater Climatic feature, fracture Dry zone, semi-arid 1500 25–30 14,500 Anuradhapura 0.02–13.70 Chandrajith et al.
intensity of rocks (2012)
South Korea Deep thermal Metamorphic rocks, granitoids, and – – – 377 South Korea Up to 40.8 Chae et al. (2007)
groundwater complex rocks, biotite
Groundwater Pegmatite Temperate climate 1286 – 40 Gimcheon 0.04–2.15 Kim et al. (2011)
Groundwater F− rich granitic rocks Temperate climate 1122 – 477 Southeastern part of the 0.20–5.0 Kim and Jeong (2005)
Korean
Groundwater Granite and biotite – – – 51 Jungwon area 6.0–10.0 Chae et al. (2006)
Groundwater – – – – 14,009 Rural areas of South 0.06–16.20 Lee et al. (2017)
Korea
Thailand Groundwater F− bearing minerals Tropical climate – – – Remote areas of 0.04–0.65 Chuckpaiwong et al.
Thailand (2000)
Turkey Groundwater Apatite, F− bearing micas, Semi closed area Southwestern Anatolia 0.39–5.62 Davraz (2015)
amphiboles, Miocene clastics, – – –
Gölcük pyroclastics, volcanic rocks
Groundwater – Continental climate – – 23 Different parts of 1.50–13.70 Oruc (2008)
Anatolia
Groundwater Water–rock interaction and regional Continental climate – – – Isparta (SW-Turkey) 1.40–4.60 Davraz et al. (2008)
thermal water mixing, calcite,
fluorite
Vietnam Groundwater Biotites and amphiboles Tropical climate 1228 26.8 1178 Ninh Hoa Up to 28.1 Tu (2008)
Yemen Groundwater Calcite and fluorite Humid subtropical climate 400 16.66–28.96 31 NW Taiz city 1.08–10.0 Al-Amry (2009)
Groundwater Sewage and anthropogenic source, Subtropical dry, hot desert 500 – 93 Governorate of Taizin 0.85–2.83 Naser et al. (2016)
water-rock interaction climate
Ecotoxicology and Environmental Safety 182 (2019) 109362
K.K. Yadav, et al.
Fig. 1. Reported F− concentration scenario in groundwater (average maximum concentration observed in the particular region or country) of Asian countries.
well as cyt C activity. Furthermore, there is an increase in the pro-
duction of ADP, AMP, GDP and Pi (Hassan and Yousef, 2009). It has
also been reported that F− can activate cellular stress response thereby
signaling regulation and affecting MAP kinases (Karube et al., 2009).
The extracellular signal-regulated protein kinase (ERK) mechanism is
initiated by the Ras/MEKK/MEK-mediated pathway in cellular mi-
tochondria (Paul et al., 1997). In mitochondria, the PKC-dependent
pathway and modifications in tyrosine phosphorylation are associated
with NaF induced MAPK activation (Refsnes et al., 2003). Many in-
vestigations found that intracellular calcium in F− induced apoptosis
causes a direct target of toxicity or an indirect result of altered cellular
mechanism (Kubota et al., 2005; Murao et al., 2000). Results have
shown that exposure to high F− concentration can alter the appearance
of apoptotic genes in peripheral blood mononuclear cells (PBMC) in the
human populations of Mexico (Salgado-Bustamante et al., 2010). F−
exposure also affects the vesicular traffic in Golgi bodies and en-
doplasmic reticulum (ER) in biological systems, through the interven-
tion with protein synthesis and secretion (Mellman and Warren, 2000).
Neurotransmitter secretion is also influenced by F− exposure (Flora
et al., 2009; Borasio et al., 2004). Fluoride have both inhibitory and
stimulatory effects on calcium pump in the cardiac sarcoplasmic re-
ticulum. These cellular responses were due to differential sensitivity of
the conformational state of the Ca pump (Narayanan et al., 1991).
Cellular exposure to F− also increases the Na+/K+-ATPase activity in
osteoblasts (Anderson et al., 1984). One study found that mRNA levels
can be decreased in neural cell adhesion molecules (NCAM) when ex-
posed to F− in a concentration-dependent manner in primary rat hip-
pocampal neurons (Zhang et al., 2007). Fluoride also has adverse ef-
fects on cell migration in embryonic neurons (Barbier et al., 2010). Still,
more research is required to investigate mechanisms of F− exposure in
biological systems, even though several studies provided no clear evi-
dence on the potential adverse effects of F− ingestion at permissible
8
Ecotoxicology and Environmental Safety 182 (2019) 109362
limits and/or overdoses on cellular processes.
4. Fluoride concentration in different foodstuffs
Fluorine comes under the halogen group of the periodic table and is
a chemically reactive element present in minute quantity in air, water,
plants and animals (Yadav et al., 2012; Rafique et al., 2015). As stated
previously, F− mainly enters the body through drinking water intake
(Li et al., 2014) and the occurrence of F− contamination is high in
groundwater of arid and semiarid areas where the aquifer is surrounded
by calcareous unconsolidated sediments to bedrock (Rasool et al., 2017;
Kim et al., 2012; Pauwels and Ahmed, 2007). Almost 96% of total F− is
present in bones, skeleton and teeth of the human body. It has an in-
dispensable role in the normal mineralization of bones and formation of
dental enamel (Park and Premnagar, 2011). The primary sources of F−
are dental products (toothpaste), tea, coffee, fish, shellfish, meat,
chicken, grapes (raisins, wine, grape juice), artificial sweeteners, sodas,
potatoes, baby foods and tap water (Passmore et al., 1974; USDA,
2015). Table 3 shows the concentration of F− in different foods.
The concentration of F− in drinking water vary according to dif-
ferent agencies or organizations all over the world. For example, Bureau
of Indian Standards (BIS, 2012), European council (EU (European
Union) Council, 1998) and World Health Organization (WHO, 2011) set
the maximum permissible limits of F− is 1.5 mg/L but the United States
Environmental Protection Agency (USEPA, 2009) set this limit as
4.0 mg/L in drinking water. The adequate intake (AI) and upper limit
(UL) of F− for infants, children and adults may vary according to their
age and life style as described in Table S1.
 Table 2
Scenario of F− in India.
Sl. Statea Number of % of districts F−affected Districts (in parts)a F− concentration range (mg/L)c
No. Districta affecteda habitationsb
K.K. Yadav, et al.

Minimum Maximum

Districts Location Districts Location

1 Andhra Pradesh 19 70 442 Viziangaram, Medak, Nellore, Krishna, West Godawari, Mahbubnagar R.G.Tanda and Bonkur Prakasham Podili
Adilabad, Guntur, Kurnool, Vishakhapatanam, 1.50 8.24
Mehaboobnagar, Hyderabad, Prakasham, Khammam,
Rangareddy, Chitoor, Karimnagar, Anantpur, Nalgonda,
Warangal
2 Assam 4 7 155 Anglong, Goalpara, Karbi, Kamrup Naugoan, Karbi Anglong Howraghat Karbi Anglong Ramsapathar
1.52 20.60
3 Bihar 9 16 1013 Aurangabad, Supaul, Nawada, Jamui, Kaimur, Munger, Nawada and Rohtas Roh and Dawath Jamui Navinagar
Rohtas, Buxar, Banka 1.70 2.85
4 Chhattisgarh 12 11 75 Kanker, Suguja, Bastar, Rajnandgoan, Korba, Rajnandgaon Khairagarh Bilaspur Dhanpur
Mahasamund, Koriya, Janjgir-Champa, Bilaspur, Raipur, 1.50 2.30
Dantewara, Jashpur
5 Delhi 6 78 – South Delhi, West Delhi, New Delhi, Northwest Delhi, West Delhi West Delhi North West Puthkalan
Southwest Delhi, East Delhi, Delhi
1.57 6.10
6 Gujarat 18 92 – Kachchh, Rajkot, Surat, Vadodara, Ahmedabad, Narmada and Vadodara Tilakwada and Nasvadi Kachchh Gagodar
Sabarkantha, Panchmahals, Anand, Dahod, Patan, 1.50 7.50
Junagarh, Narmada, Banaskantha, Bhavnagar, Amreli,
Mahesana, Bharuch, Surendranagar
7 Haryana 14 52 195 Jhajjar, Kaithal, Rewari, Sonepat, Bhiwani, Hissar, Jind, Sonepat Rai Gurgaon Akbarpur
Mahendragarh, Gurgaon, Kurkshetra, Panipat, Rohtak, 1.51 17.0

9
Sirsa, Faridabad
8 Jammu & 2 5 – Rajauri, Udhampur Udhampur Ramnagar Rajauri Jhangar
Kashmir 2.00 2.06
9 Jharkhand 6 21 992 Godda, Palamau, Bokaro, Ranchi, Giridih, Gumla, Giridih Khijri Ranchi Chutupalu
1.60 2.60
10 Karnataka 20 53 853 Chitradurga, Bellary, Gadag, Haveri, Mysore, Tumkur, Gulbarga Shorapur Bijapur Nidugundi
Bangalore, Chamarajnagar, Devangere, Bagalkot, 1.55 4.90
Gulbarga, Chikmagalur, Mandya, Belgaum, Kolar,
Raichur, Bijapur, Koppala, Dharwar, Bidar
11 Kerala 1 21 73 Palakkad Palakkad Chittor Palakkad Kopanur
2.50 5.70
12 Madhya Pradesh 19 28 109 Bhind, Sidhi, Jhabua, Chhindwara, Satna, Guna, Sheopur Karahal Seoni Gharghatia
Chhatarpur, Harda, Dhar, Khargone, Sheopur, Dewas, 1.50 12.00
Rajgarh, Gwalior, Datia, Shajapur, Jabalpur, Mandsaur,
Seoni.
13 Maharashtra 9 29 91 Nagpur, Dhule, Gondia, Amrawati, Chandrapur, Nanded, Gadchiroli Sironcha Chandrapur Bhimni
Gadchiroli, Jalna 1.50 4.01
14 Orissa 11 60 62 Boudh, Jajpur, Dhenkanal, Cuttack, Bargarh, Keonjhar, Deogarh Riamal Jajpur Rampei
Suvarnapur, Bhadrak, Angul, Deogarh, Balasore 1.52 5.20
15 Punjab 11 77 281 Mansa, Fatehgarh Saheb, Gurdaspur, Muktsar, Bhatinda, Fatehgarh Sahib Fatehgarh Sahib Sangrur Ghorenab (S)
Moga, Faridkot, Patiala, Amritsar, Sangrur, Firozpur 1.54 11.30
16 Rajasthan 30 97 6538 Jaisalmer, Alwar, Udaipur, Ganaganagar, Barmer, Sikar, Banswara, Barmer, Bhilwara, Anandpuri, Dhorimanna, Bikaner, Arjansar
Jhunjhunu, Hanumangarh, Kota, Chhittorgarh, Bhilwara, Bikaner, Chittaurgarh, Churu Shahpura, Lunkaransar,
Bikaner, Churu, Dausa, Banswara, Jalore, Dungarpur, and Jaisalmer Chhatargarh, Choti Sadri, Rajgarh
Bundi, Nagaur, Pali, Bharatpur, Rajasamand, Sawai and Sam
Modhopur, Karauli, Jaipur, Sirohi, Tonk, Dholpur, 1.50 38.00
Ajmer, Jodhpur,
(continued on next page)
Ecotoxicology and Environmental Safety 182 (2019) 109362
K.K. Yadav, et al. Ecotoxicology and Environmental Safety 182 (2019) 109362

5. Health effects due to the consumption of fluoride contaminated

groundwater in Asian countries

Khyrasol
Location

Harur1

Locha
The consumption of F− higher than allowable level causes several
health problems in infants, children, adult males and females, i.e.
Dharmapuri dental fluorosis, osteoporosis, injury to kidney, deformation of bones,
Maximum

inactivation of reproductive organs, nerve and muscle degeneration,

Birbhum
Districts

Skeletal Fluorosis and more (Yadav et al., 2019). It has both acute and
Etah
3.80

3.11

9.10
chronic effects on the body as summarized in Table S2. Several other
effects on different human body systems are given in Table 4. Major

Navadwip, Hura and Hemtabad

effects and number of affected people for different Asian countries have
been figure-out in Table S3 and Table S4 represent the status of fluoride
affected people in India. Dental fluorosis and skeletal fluorosis have
Nalhati-I, Gangarampur,

been described in detail as these two are the major diseases occurred
due to the consumption of contaminated groundwater in Asian coun-
tries.
Andhiyur
Location

Jalalpur

5.1. Dental fluorosis

Dental fluorosis in humans occur due to intake of excess levels of

Nadia Purulia, and Uttardinajpur
F− concentration range (mg/L)c

F−-contaminated drinking water during the tooth development stage,

Birbhum, Dakshindinajpur,

generally from birth to 6–8 years of age. Dental fluorosis, also termed as
hypoplasia or hypomineralization of dental enamel, is related to the
lavish inclusion of F− into these structures.
During tooth formation or calcification stage, teeth are more sen-
sitive to fluorosis, especially in the initial 7 years of life. The tooth
Minimum

Jaunpur
Districts

enamel is made up of nearly 87% crystalline calcium phosphate (hy-

Erode

droxyapatite) (Arlappa et al., 2013). The high intake of F− with

1.51

1.50

1.50

drinking water displaces the hydroxide ions (OH−) from the oxidation
of hydroxyapatite that finally forms fluoroapatite. This is the beginning
Mahamayanagar, Aligarh, Maunathbhanjan, Firozabad
Virudunagar, Namakkal, Puddukotai, Salem, Dindigul,

of dental fluorosis, though prolonged intake of F−-contaminated water

Shivaganga, Perambalur, Dharmapuri, Karur, Theni,

Krishnagiri, Thiruvannamalai, Vellore, Coimbatore,

Jaunpur, Mainpuri, Etah, Mathura, Agra, Kannauj,

Bankura, Purulia, Dakhin, Birbhum, Malda, Uttar

leads to hard and brittle teeth. The mottling, discoloration (yellow to

brown to black) and pit formation in the enamel also take place. Dis-
coloration can be in the form of spots or appear as horizontal streaks.
Dinajpur, Bardhhman, Nadia, Dinajpur

Generally, discoloration of teeth becomes an essential part of the tooth

matrix, that results in loss in lustureh/shine of teeth (Susheela, 2003).
The types of dental fluorosis depend on the amount of F− intake and
the severity of contamination in drinking water, i.e., normal, mild,
Central Ground Water Board, Ministry of Water Resources, Government of India (2010)

moderate mild, moderate and severe (Table S5). As mentioned pre-

Ramnathpuram, Erode

Ministry of Drinking Water and Sanitation, Government of India, Annexure-I, 2017.

viously, white horizontal striations occur during mild forms of dental

Districts (in parts)a

fluorosis on the tooth surface or opaque patches of chalky white dis-

colorations may appear as well (Susheela, 2003; Pini et al., 2015). In
moderate to severe forms (advanced forms) of dental fluorosis, the
opaque spots can become yellow to brown or even black, and even-
tually the increased tooth porosity may lead to structural damages, such
as pitting or chipping (Pini et al., 2015).
habitationsb
F−affected

5.2. Skeletal fluorosis

1041

1019
200

Skeletal Fluorosis is identified by increased bone mass and density,

followed by a range in skeletal and joint symptoms such as joint pain,
% of districts

calcification and hardening of joints. In India, the problem is extremely

affecteda

State of Environment Report India-2009.

severe in North Rajasthan, Gujarat and Andhra Pradesh. States such as

Punjab, Haryana, Madhya Pradesh and Maharashtra, are slightly af-
28

10

37

fected, while Tamil Nadu, West Bengal, Uttar Pradesh, Bihar and
Number of

Assam, are lightly affected (Arlappa et al., 2013). Prolonged exposure

Districta

by either inhalation or ingestion to high concentrations (> 4 mg/L) of

F− results in skeleton fluorosis (may be acute and/or chronic). Pro-
16

10

longed exposure to high concentrations of F− (> 10 mg/L) for more

than 10 years can lead to crippling fluorosis (Arlappa et al., 2013; NRC,
Uttar Pradesh
Table 2 (continued)

West Bengal

1993). During the initial stage of skeletal fluorosis, several mild

Tamil Nadu

symptoms may occur such as muscle weakness, pain in joints, stiffness

Statea

of joints and bones, sporadic pain and chronic fatigue. In the inter-
mediate stage of fluorosis, calcification of bone and finally tightening or
Sources.

hardening of joints takes place. During the first and second clinical
No.

17

18

19
Sl.

b
a

phases of skeletal fluorosis, stiffness of the joints, sporadic pain, severe

10
K.K. Yadav, et al. Ecotoxicology and Environmental Safety 182 (2019) 109362

Fig. 2. State wise F− distribution in Indian groundwater (CGWB, 2010). b. Fluoride affected districts in India (in percentage).

11
K.K. Yadav, et al.
Fig. 3. Exposure of F− and biological consequences of human cells (Modified from Barbier et al., 2010).
joint pain, osteosclerosis and calcification of ligaments are significant
problems. In severe cases of skeletal fluorosis, the stiffness of bones
increases continuously until the whole spine becomes one fixed column
of bone, a situation known as ‘‘poker back’‘. Finally, the onset of the
third clinical phase (crippling skeletal fluorosis) presents with limited
movement of the joints, skeletal bone deformities, acute calcification of
ligaments, muscle wasting and neurological deficits (Itai et al., 2010). A
investigation at Faridabad district, India was carried out in four villages
to observe the cases of skeletal fluorosis due to the consumption of F−
contaminated groundwater. The authors reported the 57%, 43%, 18%
and 17% population was affected with skeletal fluorosis due to con-
sumption of groundwater with 3.2, 3.7, 2.5 and 1.0 mg/L of F− con-
centration, respectively (Susheela et al., 1993).
6. Fluoride removal from groundwater in Asian countries
Reduction of drinking water F− to permissible levels recommended
by international or local responsible organizations is important to avoid
or lessen negative health effects due to toxic F− exposure. In Asian
countries contamination of groundwater with F− is very prevalent;
therefore, having a comprehensive source providing different strategies
and methods to reduce health risks of F− is very important. In this
section such a comprehensive source has been provided. Different
strategies can be used to reduce the risk of dental fluorosis specifically
(a) using alternative water sources, (b) better nutrition and (c)
12
Ecotoxicology and Environmental Safety 182 (2019) 109362
defluoridation of water. These approaches are discussed in the below
sections.
One of the strategies to avoid adverse effects of consumption of
water contaminated with F− is using alternate water sources such as
surface water, rainwater and low F− groundwater. Consumption of
surface water without treatment and disinfection is not usually possible
due to its inherent biological and chemical contamination.
Furthermore, treatment of surface water may be too expensive and
complex for poor countries. Rainwater can provide a cleaner water
source in comparison with surface water which is a low-cost simple
solution. Sometimes using rainwater has problems such as the uneven
distribution of rainwater and the limitation of rainwater storage capa-
city in communities or households (Kim et al., 2016). Distribution of F−
in groundwater is uneven and concentration can be changed over time
both vertically and horizontally. Therefore, the concentration of F− in
each well should be monitored individually which is not always pos-
sible in Asian remote or rural areas (Meenakshi and Maheshwari,
2006). Thus, the option of using alternate water sources has its own
limitations.
Defluoridation is an effective and applicable method to reduce the
concentration of F− in drinking water when alternate water sources are
not available. Several studies have been carried out on F− removal from
drinking water when it was discovered that excessive concentrations of
F− cause fluorosis. Defluoridation methods can be categorized as ad-
sorption (Jorfi et al., 2011; Asgari et al., 2012; Yadav et al., 2013, 2017;
K.K. Yadav, et al. Ecotoxicology and Environmental Safety 182 (2019) 109362

Table 3
Fluoride concentration in different foodstuffs.
Category Foodstuff F− concentration (in ppm) Reference

Animal products Milk and its products 0.01–0.8 Fewtrell et al. (2006)
Milk (cow) 1.73–6.87 Bhargava and Bhardwaj (2009)
Milk (buffalo) 3.32–6.85 Bhargava and Bhardwaj (2009)
Fermented milk products 1.76–93.68 Lodi et al. (2011)
Meat and chicken 0.01–1.7 Fewtrell et al. (2006)
Fish 0.06–4.6 Fewtrell et al. (2006)
Meat, fish, poultry 0.22 Taves (1983)
Dairy products 0.25 Taves (1983)
Cereals General 0.04–1.9 Fewtrell et al. (2006)
Rice 0.012–0.031 Casarin et al. (2007)
Breakfast cereals 0.08–1.86 Da Silva Cardoso et al., 2003
Grain and cereal products 0.42 Taves (1983)
Wheat 0.51–14.03 Sengupta and Pal, 1971;
Lakdawala and Punekar (1973)
Rice 0.51–5.52 Lakdawala and Punekar (1973)
Maize 5.6 Sengupta and Pal (1971)
Barley 0.45–3.65 Bhargava and Bhardwaj (2009)
Bajra 2.76–3.84 Gautam et al. (2010)
Legumes/Pulses Beans 0.042–0.086 Casarin et al. (2007)
Soybean 4.0 Sengupta and Pal (1971)
Peas 10.77 Gautam et al. (2010)
Red gram 2.34–4.84 Lakdawala and Punekar (1973)
Bengal gram 3.84–4.84 Lakdawala and Punekar (1973)
Fruits General 0.06 Taves (1983)
Apple 0.009 Casarin et al. (2007)
Pear 0.017 Casarin et al. (2007)
Banana 0.067 Casarin et al. (2007)
Grape 0.84–1.74 Lakdawala and Punekar (1973)
Mango 0.8–1.8 Lakdawala and Punekar (1973)
Apple 1.05–2.20 Lakdawala and Punekar (1973)
Bakery products Baked goods 0.04–1.9 Fewtrell et al. (2006)
Snacks 0.22–0.40 Da Silva Cardoso et al. (2003)
Vegetables General 0.01–1.3 Fewtrell et al. (2006)
Leafy vegetables 0.27 Taves (1983)
Root vegetables 0.38 Taves (1983)
Legume vegetables 0.53 Taves (1983)
Potatoes 0.49 Taves (1983)
Spinach 9.87–29.15 Gautam et al. (2010)
Cabbage 4.25–11.30 Bhargava and Bhardwaj (2009)
Lettuce 5.7 Sengupta and Pal (1971)
Beverages General 0.003–1.3 Fewtrell et al. (2006)
General 0.76 Taves (1983)
Brewed tea 0.05–5 Fewtrell et al. (2006)
Green tea leaf 72.62–89.02 Ericsson and Forsman (1969)
Aerated drinks 0.77–1.44 Lakdawala and Punekar (1973)
Coconut water 0.43–0.60 Lakdawala and Punekar (1973)
Chocolate Bar and cookies 0.04–7.06 Buzalaf et al. (2003)
Others Oils and fats 0.25 Taves (1983)
Sugar and adjunct substances 0.28 Taves (1983)
Non-classifiable products 0.59 Taves (1983)

Tomar et al., 2014), participation/coagulation (Rahmani et al., 2010),
electrocoagulation (Khatibikamal et al., 2010; Malakootian et al., 2011;
Behbahani et al., 2011; Emamjomeh and Sivakumar, 2006; Bazrafshan
et al., 2012), nanofiltration (Poursaberi et al., 2012; Hosseini et al.,
2019) and ion-exchange (Samatya et al., 2007).
Each of these methods has its own advantages and disadvantages.
Jadhav et al. (2015) reported that the precipitation/coagulation
method is able to remove high amounts of F− from water. However,
since the precipitation/coagulation method cannot reduce concentra-
tions of F− within WHO permissible limits, this method should be used
in conjunction with other methods as a primary treatment technique
(Islam and Patel, 2007). This methodology offers advantage of better
life expectancy with secondary or tertiary treatments due to decreased
treatment loads. Methods to remove F− from water are discussed in the
following sections.
6.1. Precipitation/coagulation
The initial trials for developing a technology to remove F− from
water date back to the early 1930's. At that time, scientists had been
widely studying ways to find a sustainable cost-effective technology to
decrease concentrations of F− in water. Precipitation/coagulation is
one of the most common processes to remove contaminants/particles
from water thereby decreasing turbidity. Coagulation is a chemical
process that involves using special chemicals called coagulants to de-
stabilize small particles in water. Three valence ions such as iron and
aluminium are the most widely used coagulants. This process is not
only used for small particle removal but also can be used for removal of
F− from water. Several materials may be used for the removal of F−
from water such as alum, sodium silicate, zeolites, sodium aluminate,
lime, silica gel, bauxite and ferric chloride (Nawlakhe and
Paramasivam, 1993). Except for lime and alum, none of the above-
mentioned materials has been found to be very practical. Lime and
alum can be simultaneously used to remove F− from water. In the
precipitation method, F− is precipitated out of water in the form of
calcium F− (CaF2) (Nawlakhe and Paramasivam, 1993). The other
process, coagulation, can be utilized with alum as an effective method
to remove F− from water. However, the presence of organic ligands

13
K.K. Yadav, et al.
Table 4
Effects of F− on human health.
Effects
Effects on reproductive system:
Reduction in fertility rate in females
Reduction in quantity of testosterone, follicle stimulating hormones (FSH), and inhibin-B
Affects the structure and mobility of sperms in males
Neurobehavioural effects:
Reduction in intelligent quotient (IQ) and ability of thinking
Affects the mental ability of children
Neurotoxicity to the developing brain in children
Interfere with the glycolysis cycle which ultimately affects the energy requirement of Central Nervous System (CNS)
Interference with enzymatic function, protein structure, functions of brain and impaired cognition and memory
Cognitive Effects, Mental and Physiological Changes, Dementia
Affects the bio-chemical activities and visuospatial abilities
Effects on cardiovascular system:
Oxidative stress that promotes inflammatory mechanisms, atherosclerosis, vascular stiffness and myocardial cell damage, Bradycardia,
abnormal heart rhythms, reduced myocardial function, Hypothyroidism, diabetes mellitus and obesity
Causes hypocalcemia and hypercalcemia
Gastrointestinal effects:
Loss of the mucus layer, hyperaemia, oedema, haemorrhage, and rupture of the stomach lining
Nausea, vomiting, and gastric pain
Effects on endocrine system:
Structural changes and dysfunctions in the thyroid gland
Increased parathyroid and calcitonin activity, secondary hyperparathyroidism, and impaired glucose tolerance
Effects on urinary/renal system:
Enhances the risk of kidney stones
Metabolic, histopathological, and pathological changes in the glomeruli
during precipitation/coagulation has a negative effect on F− removal.
There are two ways to remove F− from water by alum, specifically (a)
adsorption of F− on an aluminum precipitate surface and, (b) in-
corporation of F− into an aluminum precipitate structure (Lawler et al.,
2016). This defluoridation method is known as the Nalgonda technique
which was developed in 1975 by the National Environmental En-
gineering Research Institute (NEERI), India (Venkobachar et al., 1997).
Defluoridation of water by the Nalgonda technique is a household
process usually used in areas of endemic fluorosis in villages around
Nalgonda (Andhra Pradesh, India). Although the Nalgonda technique
was first developed in India, it is now widely used throughout Asia. The
Nalgonda technique includes six consecutive stages: rapid mixing,
coagulation/flocculation, sedimentation, filtration, disinfection and
sludge concentration (Nawlakhe and Paramasivam, 1993).
Hydrated aluminum sulfate known as alum [Al2(SO4)3·H2O] is the
most important coagulant used to remove F− from water. Lime is added
to provide an alkaline condition for better F− removal. The impact of
F− on the precipitation structure of aluminum hydroxide can be ob-
served by scanning electron microscope (SEM) images (Lawler et al.,
2016). As seen in Fig. 4 smaller particles can be formed when F− is
presented in water (Fig. 4b).
Although removal of F− from water using the Nalgonda technique is
not fully understood yet, some pathways are suggested (Malik et al.,
2010). The following reactions take place during Nalgonda techniques:
Al2 (SO4 )3. 18H2 O→ 2Al3 + + 3SO24− + 18H2 O
2Al3 + + 6H2 O→ 2Al(OH)3 + 6H+
F− + Al(OH)3 → Al − F complex + undefined product
6Ca(OH)2 + 12H+ → 6Ca2 + + 12H2 O
−
Ca(OH)2 can react with F to form CaF2 that is insoluble in water as
shown in Eq. (5).
Ca(OH)2 + 2F− → CaF2 + 2OH−
−
A manual for removal of F from drinking wat'er using the
Nalgonda technique was published by Nawlakhe and Paramasivam
(1993). The optimum amount of alum for removal of F− from drinking
water has a recommended range from 700 to 1200 mg/L. The exact
Ecotoxicology and Environmental Safety 182 (2019) 109362
References
Naseem et al. (2016)
Ortiz-Pérez et al., 2003
Chinoy and Narayana (1994)
Trivedi et al. (2007)
Choi et al. (2012)
Grandjean and Landrigan (2006)
Valdez-Jiménez et al. (2011)
Spittle (1994)
USEPA, 2009
Calderon et al. (2000)
Xu et al. (1997)
Nureddin (2018)
Pratusha et al. (2011)
Nabavi et al. (2013)
Kheradpisheh et al. (2018)
Doull et al. (2006)
Doull et al. (2006)
Bouaziz et al., 2006
amount of alum for F− removal is determined by paying attention to
water pH and F− concentration. Since the accuracy of the Nalgonda
technique for F− removal is nearly 70%, it cannot be used for treatment
of water contaminated with high concentrations of F−. The application
of the Nalgonda process is expensive due to the cost of alum (Nawlakhe
and Paramasivam, 1993).
Besides F− removal, coagulation is also utilized to remove colloidal
particles from drinking water. The adverse effects of F− on particle
removal using alum and lime were reported by Liu et al. (2013). If the
ratio of F− to aluminum (FTAR) is as much as 10:10, F− induces ne-
gative effects on colloidal particle removal. On the other hand, F−
concentrations can produce negligible effects on coagulation at a FTAR
below 2:10 at a pH less than 8. Also, at a pH more than 8, little effect
was observed on particle removal over FTAR ranges between 1:10 and
30:30 (Liu et al., 2013).
It was reported that the adverse effects of F− removal is associated
with a decreasing zeta potential, smaller flocculant particles (flocs), and
elevated levels of residual aluminum in the presence of F−. At pH 6, the
F− at a FTAR of 10:10 contributes to the decrease of zeta potential from
−1.7 to −6.7 mV, where there is a corresponding decrease of floc size
from 119.7 to 29.0 μm, and an increase of residual aluminum of
0.22 mg/L. For high concentrations of aluminum (20 mg/L), the pre-
sence of F− decreases as the residual turbidity is reduced from 22.7 to
20.6 NTU (Liu et al., 2013).
(1)
6.2. Adsorption and ion-exchange
(2)
It is not surprising that the removal of F− is controlled by several
(3)
parameters, possibly one of the most important being the heterogenous
(4) nature of the ground water itself and how effective adsorption is when
utilized in F− removal. Adsorption is defined as “the adhesion of atoms,
ions or molecules from a gas, dissolved solid, or liquid onto a surface.
This process creates a film of the adsorbate on the surface of the ad-
sorbent” (USEPA, 2018). Adsorption can therefore be explained in three
(5)
stages: (1) external mass transfer of F− from the bulk heterogenous
solution across the boundary layers of adsorbent particles; (2) adsorp-
tion of F− ions onto the particle surfaces; and (3) intra-particle diffu-
sion where adsorbed fluoride ions are conveyed to the internal surfaces
of the porous adsorbent materials (Mohapatra et al., 2009; Habuda-
14
K.K. Yadav, et al.
Fig. 4. Comparison of (a) aluminum precipitates and (b) aluminum precipitates with F− (Adopted from Lawler et al., 2016).
Stanić et al., 2014). In other words, water purification from F− con-
tamination is the amount of F− adsorbed per unit mass of adsorbent
(Talaiekhozani et al., 2018). Since F− depletion from water is a pro-
blematic and multifaceted process, an adsorbent with maximum ad-
sorption capacity may not possess maximum F− removal efficiency
(Mohapatra et al., 2009). Removal efficiency, also known as removal
performance, is another important parameter in designing an adsorp-
tion reactor. This parameter reflects the maximum percentage of F−
removal at optimal conditions (Habuda-Stanić et al., 2014). A summary
of adsorption capacities of different materials used for drinking water
defluoridation in Asia is shown in Table S6.
Several natural and artificial materials have been investigated to
find a suitable and cheap adsorbent to remove F− from drinking water
(George et al., 2010; Jagtap et al., 2012). Active alumina is an ad-
sorbent that has been widely applied to remove F− from drinking water
that can be used at both community and domestic levels. It was re-
ported that removal of F− from drinking water using active alumina
was the result of both ion exchange and adsorption processes (Ghorai
and Pant, 2004). The investigations showed that the surface of alu-
minum hydroxide is protonated by hydroxyl groups (Goldberg et al.,
1996). Presence of hydroxyl groups renders a positive surface charge of
compounds that they are bound to since the hydrogen side of hydroxyl
groups is positive. At a pH below 6, the surface charge of active alumina
is positive that confers an increased affinity for F− thus facilitating the
removal of F− from drinking water. At a neutral pH value around 7, the
capacity of active alumina for F− removal is much lower than acidic
conditions. Several factors such as characteristics of raw water, the size
of active alumina particles, water flow rate, active alumina grade and
adsorbent depth control the F− removal using active alumina (Kut
et al., 2016). If the depth of active alumina decreases and the other
factors are constant, the concentration of F− may dramatically decrease
from the time the effluent is first discharged from the absorber (i.e.
alumina surface) (Goldberg et al., 1996). Active alumina is a proven
and efficient process to remove F− however, it can be a threat to human
health. Aluminum and its F− complex can be leached out of drinking
water during the treatment process at a pH < 6 when active alumina is
used. Aluminum and its F− complexes have been considered the un-
derlying cause of Alzheimer's disease and other health complications
15
Ecotoxicology and Environmental Safety 182 (2019) 109362
(Todorović and Milonjić, 2004; George et al., 2009).
Several groups have reported that adsorption materials consisting of
active alumina (AA) may increase F−-adsorption capacities.
Manganese/manganese oxide-amended AA, and iron hydroxide-
amended AA have shown increased efficacies for F− purification
(Biswas et al., 2007; Tripathy and Raichur, 2008; Maliyekkal et al.,
2008; Teng et al., 2009; Alemu et al., 2014). Furthermore, cost reduc-
tion of F− removal is aided by the use of AA-based materials. In ad-
dition, Schoeman's group found that the determination of AA's optimum
F−-uptake capacity was not offset by the alumina dissolution me-
chanism on the alumina surface in presence of high F− levels
(Schoeman, 2009). Alternatively in another investigation, Kut et al.
(2016) found that employing both AA and HAP to remove F− from
water exhibited drawbacks including the need for frequent adsorbent
recharging. Furthermore, the adsorption flow rate in F− removal is
controlled by the obligate longer minimum hydraulic retention time
resulting in low volumetric treatment capacity thereby limiting this
application for exploitation in larger communities (Kut et al., 2016).
It has been reported that magnesium–hydroxyapatite (Mg-HAP) has
a high potential for the removal of F− from drinking water with a ca-
pacity of 1.4 mg/g. Mg-HAP (dosage of 10 g/L) has been shown to re-
move 92% of F− from drinking water with a hydraulic retention time of
180 min. It was found that increasing both the concentration of Mg-
HAP and the hydraulic retention time can increase the performance of
F− removal initially; however, the reaction attains equilibrium over
time and becomes constant (Mondal and George, 2015). Interestingly,
pH is not an effective parameter on the removal of F− by the Mg-HAP
process. Although the presence of anions, including nitrate and chloride
has not been considered effective parameters for F− removal by Mg-
HAP, the presence of bicarbonate, sulfate and phosphate ions decreases
the defluoridation performance (Dubey et al., 2018). The adsorption
pattern of Mg-HAP can be described by the Langmuir isotherm. Studies
revealed that the rate of reaction followed pseudo-second-order kinetics
(Mondal and George, 2015). Also, the sorption of F− ion onto Mg-HAP
was illustrated to occur through intraparticle diffusion patterns.
Ferric hydroxide [Fe(OH)3] in the form of granules, is a combina-
tion of poorly crystallized iron oxide (FeOOH) and has been used to
remove F− from drinking water (Shams et al., 2010). The results of this
K.K. Yadav, et al.
study showed that longer hydraulic retention times, higher initial F−
concentrations and a lower pH could increase the performance of F−
removal. In the absence of SO42− and Cl− under pH 6, the hydraulic
retention time of 30 min and the initial F− concentration of 7 mg/L
yielded maximum F− removal as much as 88%. Considering economic
and feasibility aspects, adsorption of F− with granular ferric hydroxide
is recommended as a successful method of F− removal from drinking
water and wastewater treatment plants.
Another investigation showed that chitosan/Al(OH)3·(CS/Al(OH)3)
was used as a low-cost absorbent to remove F− from water. The effect
of temperature on F− removal by chitosan/Al(OH)3·(CS/Al(OH)3)
showed that the adsorption was spontaneous and endothermic. The F−
removal capacity of chitosan/Al(OH)3·(CS/Al(OH)3) was determined to
be 23.06 mg/g under a temperature of 19.85 °C and pH 4 (Hu et al.,
2018).
6.3. Nanofiltration
Another F− purification technique is nanofiltration. Nanofiltration
reduces water hardness by employing membranes with high retention
capacities for charged particles such as bivalent ions. Due to this in-
herent property, nanofiltration may be considered the most optimum
membrane process for F− removal because of highly specific membrane
selectivity (Tahaikt et al., 2007). Several studies have been conducted
on removal of F− from water using nanofiltration. One such analysis
compared nanofiltration to another membrane technology, low pres-
sure reverse osmosis (LPRO) in the elimination of F− and reduction of
salinity from brackish drinking water (Diawara et al., 2011). It was
reported that nanofiltration membranes were much more successful in
F− removal from contaminated drinking water as compared to LPRO
membranes. Another investigation involved two commercial nanofil-
tration membranes: NF-90 and NF-270 (Hoinkis et al., 2011). NF-270
decreased the F− concentration from 10 to 1.5 mg/L while NF-90 re-
duced the fluoride concentration from 20 mg/L to 0.5 mg/L. Existing
anions such as bicarbonate (HCO3−) were found to confer no negative
significant effects on water purification of F−, however, F− removal
was diminished under acidic conditions (Hoinkis et al., 2011). Bejaoui
et al. (2014) assessed the removal of F− from water using reverse os-
mosis (RO) evaluated against NF-90 on various parameters such as feed
pressure, pH, F− concentration, ionic strength and the nature of cations
associated with F−. Their results showed that F− removal was opti-
mized at higher pH concentrations due to an increase in overall nega-
tive charges of the membranes tested (Bejaoui et al., 2014).
Emamjomeh et al. (2018) conducted a laboratory scale study by a
pilot plant using a nanofiltration membrane (FILMTEC-NF90-4040). In
this study, F− was removed from raw water where the F− concentra-
tion was between 1.50 and 2.17 mg/L. The effective parameters, spe-
cifically pressures (between 4 and 12 bars) and temperatures (between
10 and 30 °C) were investigated. The results showed that the lowest and
highest performances of F− removal were 30% and 70%, respectively.
It was also reported that an increase in pressure and temperature in-
creased the performance of F− removal and membrane permeate flow
rate.
Van der Bruggen et al. (2008) reported that chemical resistance,
membrane fouling, limited lifetimes of membranes, insufficient se-
paration and rejection are some of the disadvantages of nanofiltration
technique. One of the disadvantages of using nanofiltration membranes
is production of fouling which should be collected and disposed. In one
study, the ability of two commercial nanofiltration membranes known
as NF5 and NF9 were compared to remove F− from groundwater (Nasr
et al., 2013). The concentration of F− in treated water using NF5 and
NF9 membranes were 1.45 and 0.38 mg/L, respectively. Although NF5
and NF9 membranes could remove high amounts of divalent anions
from water, the smaller ions were removed more efficiently than the
others. It was suggested that the solvation energy of these ions causes
this behavior. The results showed that chlorine could penetrate into the
16
Ecotoxicology and Environmental Safety 182 (2019) 109362
NF5 and NF9 membranes faster than F−. It was reported that BW30 and
NF90 membranes were able to reduce F− concentration from
417.9 mg/L to less than 1.5 mg/L (Shen and Schäfer, 2014).
It was reported that the main fouling component on the nanofil-
tration membranes was calcium carbonate. Citric acid and ammonia
cleaning method can be used to recover the nanofiltration membranes
(Wei-fang et al., 2009). A summary of advances in F− removal using the
nanofiltration process in Asian countries are shown in Table S7.
6.4. Electrocoagulation
Electrocoagulation (EC) is a filtration process that eliminates sus-
pended solids (e.g. F−) to sub-μm levels from water (Noling, 2004).
Electrocoagulation is an electrolytic method where the synthesis of
metallic cations occurs at sacrificial anodes when an electrical charge is
applied through an external power source (Kobya and Ulu, 2016).
During the past decade, use of electrocoagulation has increased. Elec-
trocoagulation has been recently introduced as a suitable method to
remove F− from drinking water (Malakootian et al., 2011; Hu et al.,
2005). Electrocoagulation can be effectively used for removal of a wide
range of pollutants including oil, dye, heavy metals and F− (Hu et al.,
2005). Electrocoagulation does not produce secondary pollutants and
useful substances existing in raw water can be retained during de-
fluoridation using this method. Sinha et al. (2012) reported that elec-
trocoagulation was quite successful in removing both F− and aluminum
simultaneously under 230 V DC with aluminum electrodes. Longer re-
tention time also yielded better F− removal from drinking water.
Charge loading in EC (total charge passed through a solution by an
electrical current) is the most important parameter for controlling EC
reaction rates which in turn, determine coagulation rates (Kobya and
Ulu, 2016). They found that the charge loading and F− depletion per-
formances do not have a linear relationship. Though charge loading is
the most important parameter for EC itself, it is not considered a critical
parameter in the removal of F− from drinking water. The increase in
charge loading initially reduces the concentration of F− in treated
water, however, after a critical point the decrease in F− concentration
is not significant (Sinha et al., 2012). Lesser amounts of aluminum can
be released from water by the electrocoagulation method compared to
the Nalgonda technique and active alumina process. Data showed that
the concentration of aluminum in treated water increased when input
energy is raised. It is also reported that using bentonite clay as a coa-
gulant in the flocculation tank could reduce the aluminum concentra-
tion of treated water below the WHO guideline (0.7 mg/L) (Sinha et al.,
2012).
Khatibikamal et al. (2010) showed that electrocoagulation processes
are able to remove F− from steel industry wastewater. They studied the
effects of various F− removal conditions including hydraulic retention
time, voltage, temperature, pH, and number of aluminum plates be-
tween the anode and cathode plates on performance of. Results showed
that increasing hydraulic retention time up to 5 min, yielded an in-
crease in performance of F− removal. It means that the total required
hydraulic retention time was only 5 min. It was reported that the pH
value reduced from 6.91 to 4.6 within the first 10 min but it rose to 9.5
when the hydraulic retention time was extended up to 50 min. Elec-
trocoagulation can reduce the concentration of F− from initial
4.0–6.0 mg/L to lower than 0.5 mg/L. Emamjomeh and Sivakumar
(2006) reported that the highest treatment efficiency was achieved at a
current density of 50 A/m2 (Emamjomeh et al., 2011). They found that
the performance of F− removal depends on different parameters such as
the initial F− concentration, the current density and the wastewater
flow rate when the final pH ranged between 6 and 8. The composition
of the sludge produced during electrocoagulation technique using the
X-ray diffraction spectrum was analyzed. The removal of F− from water
is related to the formation of aluminum F− hydroxide complex
[AlnFm(OH)3n−m] during the electrocoagulation technique
(Emamjomeh et al., 2011). A summary of advances in F− removal using
K.K. Yadav, et al.
electrocoagulation processes in Asian countries are shown in Table S8.
6.5. Reverse osmosis
Reverse osmosis is composed of a tank that has been divided into
two parts using a semi-permeable membrane. Water contaminated with
F− is passed through the semi-permeable membrane by exerting hy-
draulic pressure on one side of tank. Although water and some im-
purities can be passed through the semi permeable membrane, salts and
several other impurities are unable to do so (Dubey et al., 2018). It has
been found that the successful filtration of different sizes of impurities
passing through semi-permeable membranes depends on the pressure
exerted onto the membranes. Reverse osmosis (RO) takes advantage of
man-induced pressure on the mineral content side of a membrane (i.e.
“dirty side”) to overcome the natural osmotic pressure attempting to
flow in the opposite direction. Further, more osmotic pressure is added
to the reaction to increase the speed of the process to force water across
the semi-permeable membrane to the opposite side (i.e. “clean side”)
(Demeuse, 2009; WaterProfessionals®, 2018). It was reported that RO
could provide drinking water of suitable quality with a salinity < 0.1 g
salts/L (Mazighi et al., 2015).
In electrodialysis, ions within water can be carried through mem-
branes by the application of an electric current. The pH and tempera-
ture are two really important effective parameters on the performance
of membranes. The performance of F− removal by RO varies from 45 to
90% when pH increases from 5.5 to 7. Reverse osmosis possess inherent
problems such as fouling by particulate matter, chemical attacks,
plugging of the membrane pores by large quantities of waste. The vo-
lume of waste produced by RO is even larger than the ion exchange
process. If the quality of raw water is not optimal, it must be pre-treated
before introduction into the produced unit. A major disadvantage of RO
is that this process can remove all the ions present in water. Since
humans need minerals for normal growth and other metabolic pro-
cesses, re-mineralization of reverse osmosis-treated water is required
thereby rendering this process more expensive in comparison to other
options. The methodology is more expensive than other options as the
water becomes more acidic during the purification process thereby
requiring multiple pH corrections, and there is an abundant loss of
water to brine waste (Kumar and Gopal, 2000). The most important
factors for RO membrane selection include purified water recovery,
rejection properties, cost, pre-treatment steps and raw water composi-
tion (Jagtap et al., 2012; Yadav et al., 2017, 2018c).
6.6. Comparison of different techniques for F− removal
A summary of different techniques of fluoride removal has been
presented in Table 5. On the basis of literature reviewed, the following
remarks were concluded about fluoride removal methodologies:
• A perusal of Table 5 reveals that adsorption has been found pro-
mising in terms of cost, efficiency and technology but the disposal of
sludge produced from this process is a huge problem.
• Ion-exchange method is very efficient for fluoride removal but it is
expensive and the treated water has high chloride content.
• Coagulation/precipation technology is limited to 33% of F− re-
moval and also generates a huge amout of residue with high content
of residual alumium.
• Reverse osmosis and nanofiltration methods are efficient to remove
the fluoride to a greater extent but these technologies are very ex-
pensive and removes some essential ions from the water.
• Electrocoagulation technique is appropriate for fluoride removal if
considers above-mentioned problems but this technique need con-
tinuous power supply.
• It is worthwhile to note that adsorption technology has attracted
considerable attention in the recent years for removal of fluoride
and the adsorbents have shown higher fluoride adsorption capacity.
17
Ecotoxicology and Environmental Safety 182 (2019) 109362
However, a particular adsorbent which showed higher adsorption in
laboratory, may fail in the field. Thus, it is very difficult to select an
appropriate adsorbent.
• Last but not least, it would be worthwhile to note that a single
technique cannot be adapt by all Asian countries as every country
and region has different level of fluoride and other competitive ions
in groundwater and each techniques has some limitations.
7. Conclusions
Presently, F− contamination in water has dramatically increased
due to urbanization and world population growth. The presence of F−
in higher amounts than permissible limits in groundwater has created
serious health problems. Nearly 12 million of the 85 million tons of F−
deposits on the earth's crust are found in India which might be the
reason of high F− occurrence in groundwater. In South and
Southeastern Asia, the countries such as India, Pakistan, Bangladesh
and China, dangerous levels of F− in groundwater have been reported.
In addition, high F− concentrations in groundwater are obviously
detrimental to human health. Approximately 96% of total F− is present
in bones, skeleton and teeth of the human body, resulting in possible
excessive F− levels that can cause several health ailments such as se-
vere gastroenteritis, salivation, anorexia, muscle weakness, stiffness,
restlessness, sweating, dyspnea and tachycardia. Defluoridation can be
categorized into three different strategies, specifically (a) using alter-
native water sources; (b) better nutrition and (c) defluoridation of
water. Based on the review of literature, several methods for removal of
F− from water have been utilized such as precipitation/coagulation,
RO, electrocoagulation, nanofiltration adsorption and ion-exchange
processes. Lack of alternative water sources and better nutrition for
people living in Asia are not always possible, so the defluoridation of
water may be the best strategy. Precipitation/coagulation, reverse os-
mosis, electrocoagulation, nanofiltration adsorption and ion-exchange
processes are the most important methods for removal of F− from
water. Although several compounds during the precipitation/coagula-
tion process can efficiently remove F−, alum appears to be the most
commonly used compound. Additionally, the amount of waste sludge
production by electrocoagulation is much less than that produced by
conventional precipitation/coagulation process. Nanofiltration needs
lower pressure compared to RO which reduces energy costs. However,
nanofiltration membranes are more expensive than RO membranes.
8. Challenges and future prospects
Groundwater is the primary source of drinking water in Asian
countries. The increasing population of Asian countries puts huge
pressures on groundwater resources by exploiting them in an un-
sustainable manner. Generally, the appearance of F−-bearing minerals
in deep rocks and their interaction with water are recognized to be the
leading causes of F− enrichment in groundwater. High F− concentra-
tions were observed in many regions of Asian countries, but several
areas cannot analyze F− levels in drinking water. This lack of in-
formation is required to understand the behavior of F− in natural water
and how that impacts local hydrogeological settings, climatic condi-
tions, industrial and agricultural practices. Groundwater F− con-
tamination is difficult to remediate once it occurs. In Asian countries,
large numbers of the population living below the poverty line are
unaware of the F− health risks in drinking water. However, despite
knowing the health risks F− contamination carries, local regulating
agencies are not focusing on remediation. On a large scale, F− treat-
ment is a costly affair such that local governments and communities
should focus on community-based treatment processes. Local popula-
tions should be made aware and educated to aid in providing suitable
and cheap remedial technology. Several F− remediation issues and
challenges that exist in Asia include:
K.K. Yadav, et al.
Table 5
Comparison of various methods for F− removal.
Techniques Advantages
Adsorption • High performance (up to 90%)
• Cost-effective process
Ion-exchange • High performance (up to 95%)
• Water color and test will be not changed
Coagulation–precipitation • The Nalgonda technique is considered as the
−
most effective technique for F removal.
• It is a tested technique in actual condition
Reverse osmosis and • ItMicroorganisms,
is very effective for deflouridation.
nanofiltration • pollutants as wellorganic and inorganic
as suspended solids can be
efficiently removed with fluoride
simultaneously.
• The quality of treated water is constant during
the time.
• Very limited mantanance is needed.
• No chemical are used.
• Membrane life-time is too long.
• The operation of system is not depending on
pH.
• Other ions do not have interference by
membrane process.
• The process is almost automatic and reliable.
• Minimum man-power is required.
Electrocoagulation • It is an efficient technique.
• A wide range of pollutants can be removed
using this technique.
• Electrocoagulation does not produce
secondary pollutants.
• Useful ions are not removed when this
technique is used.
• High F− removal efficiency is achieved when
this technique is employed (more than 80%).
• Microorganisns can be partially removed by
this technique
• Lack of awareness and knowledge of F contamination;
−
• Poor understanding about the ill-effects of F on health;
−
• Lack of groundwater F monitoring and regulation systems;
−
• Lack of clear policies and guidelines on groundwater F manage- −
ment;
• Lack of clear enforcement of laws and regulations of F
Ecotoxicology and Environmental Safety 182 (2019) 109362
Disadvantages References
• The best performance is in pH between 5 and 6. Bhatnagar et al. (2011);
• High amount of sludge is produced. Mukherjee and Halder
• Carbonate,
−
phosphate or sulfate are competitive for
F adsorption.
(2018)
• There is no high adsorption capacity; then,
pretreatment is required.
• The adsorbents should be regenerated after 4 or 5
months. The adsorption capacity of adsorbents will be
reduced after regeneration.
• The −
F sludge disposal is a big problem.
• Carbonate, phosphate or sulfate are competitive for Mohapatra et al. (2009);
−
F adsorption Kimambo et al. (2019)
• Resin regeneration is considered as a problem because
−
it produces F rich waste.
• Ion-exchange is an expensive technique.
• Treated
low pH.
water has a high level of chloride and very
• The Nalgonda technique is able to remove only
−
18–33% of F in the form of precipitates. This
Mumtaz et al. (2015); Dubey
et al. (2018)
technique is also able to convert 67–82% of F−into
soluble aluminium F− complex ion. That is why this
technique is erroneous.
• The sulfate ion in treated water is very higher than
row water.
• The residual aluminium in treated water is more than
maximum limitation level (0.2 mg/L).
• The test of water is changed during the process.
• Since the water quality can be changed during the
time, the row water should be regularly analyzed to
determine the correct dose of chemicals
• The cost of maintenance is very high (around US$43
per month for a plant of 10,000 L/day.
• Automation of coagulation-percipitation is not easy.
• A big space is needed to dry sludge.
• Existence of silicates in water has negative effects on
defluoridation.
• Defluridation capacity can be changed by temperature
variation.
• Some essential ions in water are removed. Shen and Schäfer (2014);
• The process is expensive in comparison to other
techniques
Samrat et al. (2018); Moran
Ayala et al., 2018; Owusu-
• The pH of treated water is reduced; therefore, pH
should be corrected after treatment.
Agyeman et al. (2019)
• A large amount of water is wasted as brine when this
technique is used.
• The disposal of brine is not easy.
• Aluminum can be released into water during using Emamjomeh and
electrocoagulation. SivaKumar, 2009; Moussa
• High amount of electrical power is needed. et al. (2017)
contaminated groundwater;
• Undefined water rights in developing countries;
• Costly treatment of remedial technologies on a large scale;
• Lack of coordination between groundwater management agencies
and local populations;
−
• Shortage of cheap and region-based F remedial methods;
−
18
K.K. Yadav, et al.
• People being unaware about future climate change that can impact
−
F contamination in groundwater;
• Inadequate medical facilities in the affected areas and no regular
check-ups provided by local medical authorities;
• No guidelines and demarcation of F affected risk zones.
− Al-Ghamdi, A.Y., Saraya, M.E.S.I., Al-Ghamdi, A.O., Zabin, S.A., 2014. Study of physico-
In future, better groundwater resource utilization coupled with
economical, sustainable and adoptable measures should be employed.
These solutions are summarized as follows:
• Formulating or re-designing policy options to manage groundwater
−
F concentrations;
• Building new institutions responsible for monitoring groundwater
−
F concentrations in an integrated manner;
• Obtaining data on groundwater resources by strengthening database
management, adopting alternative techniques for recharge assess-
ment, and mapping aquifers effectively;
• Forceful implementation of policies and regulations to manage F−
concentrations in groundwater;
• Government needs to recommend guidelines for F− concentration in
drinking water;
• Strict penalties need to be levied for violations of rules concerning
pollution and contamination of groundwater resources;
• Community-based awareness campaigns to educate the population
in affected areas;
•
Adoption of community-level regulatory options;
• Establishment of medical facilities and regular health check-ups;
• Formation of regular F−-monitoring facilities in affected areas;
• Provision of basic facilities for pooper to overcome health issues;
and
• Government should develop specific criteria for labeling risk zones
having F− contaminated water (e.g. low risk, medium risk, high
risk, and severe risk).
9. Final remarks
It is evident that some parts of Afghanistan, China, India, Iraq,
Pakistan, Sri Lanka, South Korea, Turkey, Vietnam, and Yemen are
severely affected with more than 10 mg/L fluoride concentration. These
countries need more attention for fluoride remediation and an ad-
sorption technique is more suitable for this purpose from the view point
of cost and technology after considering its limitations.
Conflicts of interest
The authors declare no conflict of interest.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://
doi.org/10.1016/j.ecoenv.2019.06.045.
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