Environmental Chemistry and Ecotoxicology 2 (2020) 150–161

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Environmental Chemistry and Ecotoxicology

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Geochemical and health risk assessment of fluoride and nitrate toxicity in

semi-arid region of Anantapur District, South India
Muralidhara Reddy B. a, , Sunitha V. b
⁎
a
Department of Earth Sciences, Yogi Vemana University, Kadapa 516005, Andhra Pradesh, India
b
Department of Geology, Yogi Vemana University, Kadapa 516005, Andhra Pradesh, India

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

Article history: This paper reports to the fluoride and nitrate concentration in groundwater resources of the semi-arid region of
Received 14 July 2020 Anantapur district, South India, and its related potential health risk assessment issues with the resident peoples. For
Received in revised form 28 August 2020 this purpose, 50 groundwater samples were analyzed for hydrochemical parameters including major ions, fluoride
Accepted 7 September 2020
and nitrate. The results revealed that most of the groundwater samples are alkaline in nature. Hydrochemical type
Available online 11 September 2020
of groundwater in the study area mainly Na+-K+-Cl−-SO2− + + −
4 and few samples belong to Na -K -HCO3 . Non carcino-

Keywords:
genic health risks due to fluoride and nitrate exposure through consumption of groundwater were assessed using the
Fluoride USEPA method. In the study area groundwater samples, fluoride and nitrate concentration ranges from 1.2 to 5.9 mg/L
Nitrate and 36 to 92 mg/L. Based on these results, 86% of fluoride (>1.5 mg/L) and 94% of the nitrate (>45 mg/L) in ground-
Groundwater water samples exceed the permissible limit. The Total Hazard Index (THI) quotients for adults, children and infants had
Health risk assessment health hazards (THI > 1) in 98%, 88%, and 80% of samples, respectively. Hence, proper precautionary measures have
Anantapur district to be taken to control health risk in this area.
South India

1. Introduction
Groundwater is used for drinking and irrigation purposes in arid and
semi-arid regions are increasing considerably over around the world [22].
It evaluated that around 1.5 billion people rely on groundwater for irriga-
tion and drinking purpose all over the world. In India groundwater consti-
tutes nearly 80% for domestic purposes, around 45% of all agricultural
water irrigating 39 million hectares [21,36,67]. Urban and rural areas
rely on groundwater for drinking and around 90% of the rural people de-
pend on groundwater for domestic purposes [57]. Due to overuse, fresh
water is getting contaminated has become a scanty commodity and contin-
ued irrigation practices may also lead to groundwater pollution [41].
Groundwater pollution is associated with many sources like geogenic or
anthropogenic source, nitrogen pollutants, agricultural pesticides, dissolu-
tion or weathering of the rocks and soil [4,5,14,18,42,64,65]. The quality
of groundwater is of major concern in choosing the applicability of ground-
water for a particular purpose and water for drinking purpose must be de-
void of harmful elements, excessive minerals, living and non living
organisms which may impact human health [27]. Contamination due to
toxic metals and metalloids is of huge health problem noticed in semi-
arid area of Anantapur district, Andhra Pradesh [30,58–60]. Owing to nat-
ural and anthropogenic activities like agricultural and industrial activities,
groundwater quality is slowly deteriorating, leading to water shortage crisis
and numerous environmental health implications [24,47,70,71]. As public
health directly linked with the quality of drinking water, its systematic
monitoring is very essential.
Globally, since two decades, groundwater pollution by fluoride and ni-
trate is of major public health concern. In view of its importance, these stud-
ies have been carried out in arid and semi-arid areas around the world
[12,17,19,25,37–39,63]. Fluoride concentration rely on various factors
such as availability of circulating water to fluoride containing minerals,
rock-water interaction mechanism, evaporation and evapotranspiration,
complexion of fluoride ion with aluminum, beryllium, ferric iron and a se-
ries of mixed fluoride hydroxide complex with Boron [15]. Fluorides occur
in three forms, namely fluorspar or calcium fluoride (CaF2), apatite or rock
phosphate [Ca3F(PO4)3] and cryolite (Na3AlF6) [57]. Though fluoride is re-
quired for normal mineralization of bones and formation of dental enamel
in little quantities, when consumed in higher dosages (>1.5 mg/L), it causes

⁎ Corresponding author.
E-mail address: bandiphd@gmail.com. (M.R. B.).

http://dx.doi.org/10.1016/j.enceco.2020.09.002
2590-1826/© 2020 The Authors. Production and hosting by Elsevier B.V. on behalf of KeAi Communications Co., Ltd. This is an open access article under the CC BY-NC-ND
license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
M.R. B., S. V. /
dental fluorosis or mottled enamel and higher concentration (>3.0 mg/L)
of fluoride may causes skeletal fluorosis [56]. The highest concentration
of fluoride is of major health implication in many countries. Higher fluoride
concentrations are noted in more than 23 countries in the world, particu-
larly in parts of India, China, Central Africa, South America [49,50]. Several
groundwater quality studies concerning to fluoride have been taken up in
arid and semi-arid areas in the world [28,29,36–38,54,55,62,66].
Nitrate is regarded as major chemical contaminants in groundwater
across the globe. The content of nitrates in groundwater is increasing in
India. The nitrate concentration in groundwater has shown rising trends
in many countries in the last 30 years [13]. In view of the prominent nitrate
concentrations in drinking water to create health impact on the human
body like methemoglobinemia in infants and stomach cancer in adults
[7]. As such, the United States Environmental Protection Agency (USEPA)
has demarcated a maximum contaminant level (MCL) of 10 mg/L NO3-N
(50 mg/L NO3) [68], and also some of the research studies show that agri-
culture activities are the major cause for increasing nitrates in groundwater
[16,26]. Many parts of states in India like Andhra Pradesh, Bihar, Delhi, Ha-
ryana, Himachal Pradesh, Karnataka, Kerala, Madhya Pradesh, Maharash-
tra, Orissa, Punjab, Tamil Nadu, Rajasthan, West Bengal and Uttar
Pradesh contain higher nitrate concentration in groundwater (more than
45 ppm) have been found [9,58].
Toxic elements like fluoride and nitrate are released in to groundwa-
ter, and can be accumulated in crops and may cause significant on
human health [10]. Decline of groundwater quality is of major concern
not only in developed countries like India and China and also important
Fig. 1. Study area located at the southeastern part of Anantapur district in south India.
151
Environmental Chemistry and Ecotoxicology 2 (2020) 150–161
worldwide [40]. Groundwater quality is continuously deteriorating in
recent decades due to the presence of chemicals and fertilizers and
due to this there is increased awareness of health risk to humans [17].
Considering this factor the important objective of the present study is
to assess the health risk of fluoride and nitrate toxicity in groundwater,
which further aids in taking proper suitable measures in preventing
health risk in and around parts of Anantapur District, A.P.
2. Materials and methods
2.1. Description of the study area
The study area of Mudigubba, Nallamada, Kadiri mandals covering an
area of 1136.3 km2 falls in the southeastern part of Anantapur district,
South India and lies between latitudes 140 0′0″-140 35′0″ N and longitudes
770 15′0″-780 50′0″ E and falls in the Survey of India (SOI) toposheet Nos:
57 F/14, F/15, F/16, 57 J/3 and J/4 (Fig. 1). Important geological forma-
tions observed in this area are peninsular gneisses of Archean age compris-
ing of pink granites, schists, composite gneisses of Dharwar age, intruded
by a few pegmatite dykes (Fig. 2). Denudational Hills, Dissected pediments,
Pediplain, Alluvium are few geomorphic features noted in this region [57].
The study area is drained by Chitravathi River and its tributaries. Temper-
ature differs from 17 °C in January to 42 °C in May. Black and red soils are
observed in this area. The average yearly rainfall is 560 mm. The depth of
open wells ranges from 6.0 to 25.0 m below ground level (bgl) and depth
to water level varies from 1.5 to 23 m bgl [9].
M.R. B., S. V. / Environmental Chemistry and Ecotoxicology 2 (2020) 150–161

Fig. 2. Geology map of the study area.

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M.R. B., S. V. / Environmental Chemistry and Ecotoxicology 2 (2020) 150–161

2.2. Determination of major ions, fluoride and nitrate concentrations in drinking
water
Fifty groundwater samples were collected from 50 villages in the
study area during April 2019. Depth of bore wells varied between
20 m and 60 m below the ground level. Samples were collected in poly-
ethylene bottles. The groundwater samples are analyzed as followed by
American Public Health Association (APHA), 2012 [1] procedure and
suggested precautions are taken to avoid contamination [15,44]. The
various parameters such as pH, electrical conductivity (EC) and total
dissolved solids were analyzed during field work using water analyzer
371 field kit. Total Hardness, and major cations such as Ca2+, Mg2+
were determined by titrimetry, though Na+ and K + are determined
by flame photometry (Systronic Model No.128). Major anions like
HCO− 3 and Cl
−
are determined by titrimetry, SO2−
4 and NO− 3 are mea-
ˉ
sured by spectrophotometric method. F is determined by using ion se-
lective electrode (Orion 4 star ion meter with pH/ISE Model).
Standard fluoride solutions (0.1 to 10 mg/L) were set up from a stock so-
lution (100 mg/L) of sodium fluoride. According to test prerequisite,
2 mL of total ionic strength adjusting buffer (TISAB III) was added to
20 mL of testing sample. Spatial distribution maps were prepared by
using the interpolation technique in Arc GIS tool Inverse distance
weight (IDW) to understand groundwater quality. The spatial distribu-
tion of fluoride and nitrate ions in groundwater was highlighted in the
maps. The chemical data of the groundwater samples were additionally
represented by using Gibbs and bivariate diagrams for identifying the
mechanisms governing the groundwater chemistry.
2.3. Health risk assessment
Health risk assessment consists of four stages like Identification of
risk; Assessment of Dosage; Exposure valuation and Hazard characteri-
zation are recommended by the United States environmental protection
agency [23,35]. In this work F− and NO− 3 concentration in groundwater
were selected as the parameter for evolution of human health risk as-
sessment [68]. Average daily dosage (ADD) of F− and NO− 3 ingested
from drinking of groundwater in the study area was calculated by the
Eq. (1) [67]:
CPW  IR  ED  EF
ADD ¼
ABW  AET
where ADD indicates F− and NO− 3 intake (mg/kg/day); CPW indicate
specific groundwater pollutant (mg/L); IR denotes rate of ingestion
2.5 L/day for adults, 0.78 L/day for children, 0.3 L/day for infants
[35]; ED indicates duration of exposure (64 years for adults, 12 years
for children and < 1 for infants respectively [2]; EF indicates frequency
of exposure (365 days/year for adults, children and infants); Average
body weight (ABW) denotes average body weight of human body in
57.5 kg for adults, 18.7 kg for children, 16.9 kg for infants; Average
time (AET) denotes average exposure time 23,360 days for adults,
4380 days for children's and 365 days for infants.
Hazard quotient (HQ) appears if the pollutant exposure dose exceeds
the reference dose toxicity effects may appear. RfD referred as exposure
dosage of F− and NO−3 is 0.06 and 1.6 mg/kg/day respectively. HQ is deter-
mined by the following Eq. (2).
ADD
HQ ¼ ð2Þ
RfD
As per the health risk assessment standard suggested by the USEPA, the
acceptable level of non carcinogenic THI is 1, while THI values exceed 1, it
is treated as exceeds the permissible limit of non carcinogenic risk [68]. The
non carcinogenic risk of total hazard index (THI) is determined by applying
the Eq. (3)
THI ¼ ∑ni¼1 HQi ð3Þ
3. Results and discussion
3.1. General chemical composition of groundwater
The statistical data of physico-chemical parameters like minimum,
maximum, mean and standard deviation values denoted in Table 1. In
the study area, the pH of groundwater ranges from 7.4–9.0 indicating
alkaline nature. EC ranges from 480 to 740 μS/cm. Based on EC ground-
water can classify into three categories as (i) low salt concentration: EC
< 1500 μS/cm, (ii) average salt concentration: EC: 1500–3000 μS/cm,
(iii) high salt concentration: EC > 3000 μS/cm [52,53]. According to
this classification of the EC, 100% of the samples belong to low salt con-
centration. Total dissolved solids (TDS) vary between 380 and
450 mg/L with a mean of 519 mg/L. All the samples are below the per-
missible limit of TDS. Total Hardness (TH) varies from 390 to 730 mg/L.
permissible limit of TH for drinking purpose is 500 mg/L [69], and 28%
of the samples were exceeding the permissible limit. However, accord-
ing to Sawyer and McCarthy [48], TH is <75 belong to soft category;
75–150 (moderately hard); 150–300 (hard); >300 (very hard catego-
ries). As per the classification 100% of TH are very hard category.
ð1Þ
Na+ and K + concentration ranges from 80 to 200 mg/L and
20–36 mg/L. Ca 2+ and Mg 2+ in concentration ranges from 42 to
80 mg/L and 45–92 mg/L. HCO − 3 concentration ranges from 74 to
130 mg/L. SO2− 4 and Cl− concentration ranges from 82 to 240 mg/L
and 110–300 mg/L, respectively. All of the samples are within the per-
missible limit of Na+, K+, Ca2+, Mg2+, HCO− 2−
3 , SO4 and Cl−. Nitrate
concentration ranges from 36 to 92 mg/L. 94% of the samples are ex-
ceeding the permissible limit of nitrate. Fluoride Concentration ranges
from 1.2–5.9 mg/L. 86% of the samples are exceeding the permissible
limit of fluoride (Table 2).

Table 1
Descriptive statistics of groundwater hydrochemistry and guideline values of WHO (2011) in the study area.
Water Quality Parameters Minimum Maximum Mean Standard Deviation W.H·O accept limit BIS accept limit % of samples exceed the Permissible limit

pH 7.4 9.0 7.94 0.445 6.5–8.5 6.5–8.5 10

EC (μS/cm) 480 740 534.6 67.77 500–1500 500–1500 Nil
TDS (mg/L) 380 450 343.5 41.883 500–1500 500–1500 Nil
TH (mg/L) 390 730 519 91.152 100–500 300–600 28
Na+ (mg/L) 80 200 114.8 31.49 50–200 – Nil
K+ (mg/L) 20 36 15.76 6.30 200 – Nil
Ca2+ (mg/L) 42 80 53.86 9.46 75–200 75–200 Nil
Mg2+ (mg/L) 45 92 63.94 14.94 50–150 30–100 Nil
HCO− 3 (mg/L) 74 130 96.84 17.210 30–150 – Nil
SO2−
4 (mg/L) 82 240 132.64 42.580 200–400 150–400 Nil
Cl− (mg/L) 110 300 200.6 62.58 200–600 250–1000 Nil
F− (mg/L) 1.2 5.9 3.234 1.295 0.6–1.5 0.6–1.5 86
NO−3 (mg/L) 36 92 67.9 13.56 45 45 94

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M.R. B., S. V. / Environmental Chemistry and Ecotoxicology 2 (2020) 150–161

Table 2
Health risk related to fluoride ingestion in individuals.
Classes F− mg/L Effects on Human Health (WHO, 1996; Dissanayake, 1991) Samples % of Samples

Class - I <0.5 Conductive to Dental Caries Nil Nil

Class - II 0.5–1.5 Enhances Strengthening of Bones and Teeth 7 14
Class - III 1.5–4.0 Dental Fluorosis (Mottling of Teeth) 27 54
Class - IV 4.0–10 Dental and Skeletal Fluorosis 16 32
(Pain in neck and Back bones)
Class - V >10 Crippling Fluorosis Nil Nil

3.2. Groundwater types 3.3. Governing factors of groundwater chemistry

The Piper trilinear diagram [43] is one of the most valuable graph- Gibb's diagram is plotted to determine the mechanism controlling
ical representation in groundwater quality investigations to compre- groundwater chemistry of the Semi-arid region of Anantapur district.
hend the hydro-geochemical facies as far as analogies, dissimilarities Na+ +K +/Na ++K + +Ca 2+ & Cl − /Cl− + HCO − 3 as a function of
and water types in the study area. The results of the chemical analysis TDS are plotted to denote precipitation dominance (PD), rock domi-
of the groundwater samples were plotted in the Fig. 3, which clearly nance (RD) and evaporate dominance (ED). All groundwater samples
clarifies the variations of cation and anion concentration in the were plotted as shown in Fig. 4 a & b. From the figures it is clear that
study area. The diamond shaped field of piper chart is additionally all of the groundwater samples belong to rock dominance (RD) zone re-
separated into four classes, in particular Ca 2+ -Mg 2+-Cl− -SO 2− 4 ; vealing rock weathering and dissolution of fluoride bearing minerals
Na+-K+-Cl−-SO2− + + −
4 ; Na -K -HCO3 ; Ca
2+
-Mg2+-HCO− 3 . The piper di- from the source rock are chief contributing factors for release of fluoride
agram reveals that 92% of the samples belong to the Na+-K+-Cl−-SO24 to groundwater [34,57].
−
and 8% of the samples are of Na+-K+-HCO− 3 type rock water inter- A Numerous lithological processes, including weathering and dissolu-
action and the nature of aquifer influencing the groundwater quality tion control the groundwater chemistry. It is evident by observing the
in the study area. plots of Ca2+/Na+ vs HCO− 3 /Na
+
and Ca2+/Na+ vs Mg2+/Na+ (Fig. 5

Fig. 3. Piper trilinear diagram for the chemical composition of groundwater samples in the study area.

154
M.R. B., S. V. /
Fig. 4. Mechanism controlling groundwater chemistry for study area (a) TDS vs. (Cl−)/(Cl− + HCO−
Fig. 5. Bivariate plots (a) Ca2+/Na+ vs. Mg2+/Na+ (b) Ca2+/Na+ vs. HCO−
a & b) groundwater chemistry depends on silicate weathering and partially
by carbonate dissolution. Therefore, sodium, calcium and magnesium are
greatly contributing through silicate weathering. Similar findings were no-
ticed in silica rich lithogenic areas [6,45].
3.4. Fluoride occurrence in the groundwater
Fluoride concentration in the study area ranges from 1.2–5.9 mg/L with
a mean of 3.23 mg/L (Tables 1 & 3). Based on the results, 86% of the
groundwater samples exceeded the permissible limits [69]. Groundwater
is the only source of drinking in the study area. The study area was majorly
occupied by peninsular gneisses of archean age rocks, which have an abun-
dant source of fluoride rich minerals. A Fractured hard rock zone with peg-
matite veins are major sources of fluoride in groundwater [46]. High
sodium, potassium, bicarbonate and an alkaline pH increase the ion ex-
change of fluoride by hydroxyl ions (OH−). The Na+ gained by groundwa-
ter from the chemical weathering of rock forming minerals is used as an
index of the weathering of minerals interchange wet and dry conditions
of the semi-arid climate. This is answerable for leaching fluoride from the
minerals present in the soils and rocks [51]. In this way, geogenic (fluoride
bearing minerals: fluorite, apatite, biotite, hornblende, cryolite, villiaumite,
155
Environmental Chemistry and Ecotoxicology 2 (2020) 150–161
+ + + +
3 ); (b) TDS vs. (Na +K )/(Na +K +Ca
2+
).
+
3 /Na .
topaz, amphibole and micas) sources are the principle key factors for fluo-
ride content under the alkaline condition in the groundwater of the study
area [3]. Moreover, other than the geogenic sources, a significant quantity
of fluorine could be contributed by intensive application of phosphate fer-
tilizers, which also contain fluorine as an impurity and are leached down
to the saturated zone by irrigation return flows [35,55,61]. Therefore,
groundwater could be enriched with higher fluoride content in the study
area.
3.5. Nitrate occurrence in the groundwater
Nitrate concentrations in the study area ranges from 36 to 92 mg/L
in groundwater samples with a mean of 61.5 mg/L (Tables 1 & 3). Based
on the results, 94% of the groundwater samples exceed the permissible
limit of nitrate (45 mg/L). Nitrate contamination is primarily due to exten-
sive use of N-fertilizer and manures, which was the principle cause for
higher nitrate concentration in the study area groundwater. Also, this con-
tamination can potentially originate from agricultural fertilizer leaching,
septic tank leakage, inappropriate removal of domestic wastes and effluent
of organic matter [20,27]. Consequently, nitrate has the highest penetra-
tion depth into soil horizons and finally into the groundwater resources
M.R. B., S. V. / Environmental Chemistry and Ecotoxicology 2 (2020) 150–161

Table 3
Fluoride, nitrate concentration and computation of hazard quotient for adults, children and infants.
S·No Latitude Longitude Fluoride Nitrate Adults Children Infants Total Hazard Index
mg/L mg/L
HQF HQN HQF HQN HQF HQN Adults Childrens Infants
0 0
1 14 45′47.79″N 77 94′17.23″E 5.0 65 3.21 1.56 3.25 1.58 2.48 1.21 4.77 4.83 3.69
2 14039′61.40″N 78007′94.57″E 4.3 55 2.76 1.34 2.79 1.34 2.13 1.02 4.1 4.13 3.15
3 14040′59.74″N 77099′09.67″E 3.4 56 2.18 1.39 2.21 1.37 1.68 1.04 3.57 3.58 2.72
4 14026′99.00″N 78005′35.80″E 3.6 58 2.31 1.4 2.34 1.34 1.78 1.08 3.71 3.68 2.86
5 14049′33.03″N 77096′70.51″E 5.2 60 3.33 2.04 3.38 1.41 2.58 1.11 5.37 4.79 3.69
6 14034′12.74″N 78012′48.40″E 2.4 85 1.54 2.07 1.56 1.46 1.19 1.58 3.61 3.02 2.77
7 14043′50.12″N 77061′70.45″E 4.9 86 3.14 2.12 3.18 1.99 2.43 1.59 5.26 5.17 4.02
8 14047′11.05″N 77096′24.89″E 4.8 88 3.08 2.02 3.12 2.07 2.38 1.63 5.1 5.19 4.01
9 14023′59.95″N 78007′14.51″E 4.2 84 2.69 1.82 2.73 2.10 2.08 1.56 4.51 4.83 3.64
10 14043′14.07″N 77096′22.32″E 1.2 76 0.77 1.97 0.78 2.15 0.59 1.41 2.74 2.93 2
11 14033′04.59″N 78008′31.83″E 2.9 82 1.86 1.63 1.89 1.83 1.44 1.52 3.49 3.72 2.96
12 14045′46.90″N 77097′51.49″E 5.9 68 3.78 1.68 3.84 2.05 2.92 1.27 5.46 5.89 4.19
13 14044′68.36″N 77099′84.95″E 2.6 70 1.67 1.39 1.69 1.58 1.29 1.29 3.06 3.27 2.58
14 14038′91.91″N 78000′45.72″E 4.9 58 3.14 1.49 3.19 1.86 2.43 1.08 4.63 5.05 3.51
15 14035′21.72″N 78000′23.88″E 2.2 62 1.41 1.25 1.43 1.39 1.09 1.15 2.66 2.82 2.24
16 14033′73.56″N 78014′87.60″E 1.4 52 0.89 1.39 0.91 1.99 0.69 0.97 2.28 2.9 1.66
17 14035′17.31″N 77096′03.19″E 1.4 58 0.89 1.51 1.69 1.66 0.69 1.08 2.4 3.35 1.77
18 14033′46.50″N 77096′98.66″E 2.6 59 1.67 1.73 1.43 1.71 1.29 1.09 3.4 3.14 2.38
19 14035′04.23″N 77091′24.44″E 2.2 58 1.41 1.88 3.12 1.32 1.09 1.08 3.29 4.44 2.17
20 14031′09.08″N 77097′82.55″E 4.8 63 3.08 1.88 0.91 1.41 2.38 1.17 4.96 2.32 3.55
21 14030′43.59″N 78008′30.09″E 1.4 72 2.69 1.88 3.12 1.51 0.69 1.21 4.57 4.63 1.9
22 14034′95.13″N 77092′81.93″E 4.8 78 3.08 1.92 2.73 1.27 2.38 1.34 5 4 3.72
23 14035′39.76″N 77091′87.77″E 4.2 78 1.54 1.97 1.56 1.41 2.07 1.37 3.51 2.97 3.44
24 14036′99.55″N 78011′09.87″E 2.4 78 2.24 2.02 1.28 1.44 1.19 1.45 4.26 2.72 2.64
25 14052′75.01″N 77095′56.62″E 3.5 80 1.54 2.21 1.56 1.41 1.73 1.49 3.75 2.97 3.22
26 14034′95.71″N 77096′31.51″E 2.4 82 1.67 1.88 1.69 1.54 0.19 1.52 3.55 3.23 1.71
27 14027′91.01″N 77096′46.59″E 2.6 84 2.44 2.02 2.47 1.76 1.29 1.56 4.46 4.23 2.85
28 14007′84.19″N 78007′40.44″E 3.8 88 0.89 1.88 0.91 1.90 1.88 1.63 2.77 2.81 3.51
29 14010′91.31″N 78000′52.20″E 1.4 92 3.14 1.73 3.19 1.90 0.69 1.71 4.87 5.09 2.4
30 14017′67.08″N 78003′61.06″E 4.9 84 1.54 2.21 1.56 1.90 2.43 1.56 3.75 3.46 3.99
31 14014′17.63″N 77098′18.60″E 2.4 78 2.18 1.88 2.21 1.95 1.19 1.45 4.06 4.16 2.64
32 14009′54.02″N 78001′29.56″E 3.4 72 3.58 1.75 3.64 1.99 1.68 1.34 5.33 5.63 3.02
33 14010′90.15″N 78005′87.48″E 5.6 78 2.18 1.97 2.21 2.04 2.77 1.45 4.15 4.25 4.22
34 14023′38.34″N 78003′60.28″E 3.4 73 2.31 1.75 2.34 2.15 1.78 1.36 4.06 4.49 3.14
35 14013′10.58″N 78003′65.19″E 3.6 82 0.89 1.51 0.91 2.24 1.69 1.52 2.4 3.15 3.21
36 14016′80.19″N 78009′45.15″E 1.4 73 0.77 1.75 1.69 2.04 0.29 1.36 2.52 3.73 1.65
37 14018′61.12″N 77099′14.74″E 2.6 63 1.67 1.54 1.56 1.90 1.19 1.17 3.21 3.46 2.36
38 14031′42.84″N 78004′73.51″E 2.4 64 1.54 1.35 1.43 1.78 1.09 1.19 2.89 3.21 2.28
39 14011′27.60″N 77099′02.37″E 2.2 56 1.41 1.35 1.56 1.99 1.19 1.04 2.76 3.55 2.23
40 14011′31.30″N 78016′03.87″E 2.4 56 1.53 1.08 0.09 1.78 0.01 1.04 2.61 1.87 1.05
41 14023′38.40″N 78009′31.18″E 2.6 45 0.09 1.35 0.05 1.54 0.04 0.51 1.44 1.59 0.55
42 14006′72.88″N 78013′93.17″E 2.8 48 0.05 1.15 0.06 1.56 0.05 0.39 1.2 1.62 0.44
43 14016′95.46″N 78017′93.36″E 5.0 46 0.06 1.11 0.04 1.37 0.03 0.29 1.17 1.41 0.32
44 14018′71.39″N 78018′62.25″E 4.6 42 0.04 1.01 0.01 1.37 0.01 0.22 1.05 1.38 0.23
45 14019′12.98″N 78010′35.99″E 1.8 36 0.01 0.87 0.03 0.68 0.02 0.16 0.88 0.71 0.18
46 14017′32.73″N 78016′35.39″E 4.9 52 0.03 1.25 0.01 0.52 0.01 0.18 1.28 0.53 0.19
47 14010′28.14″N 78008′49.38″E 1.5 58 0.01 1.39 0.01 0.39 0.01 0.17 1.4 0.4 0.18
48 4020′51.71″N 78011′03.74″E 2.6 68 0.01 1.63 0.01 0.29 0.01 0.19 1.64 0.3 0.2
49 14007′73.81″N 78010′46.17″E 2.8 73 0.01 1.75 0.01 0.21 0.01 0.18 1.76 0.22 0.19
50 14007′27.42″N 78017′24.91″E 2.4 75 0.01 1.80 0.01 0.27 0.01 0.23 1.81 0.28 0.24

[11,32,33,55]. In this way, increased nitrate concentration in ground- District. From the results revealed that hazard quotient (HQ) of fluoride
water supplies can potentially cause human health problems, for example, in the study area ranges between 0.01 and 3.78 (adults), 0.01 to 3.84 (chil-
low oxygen levels in the blood of infants, and it is well known as methemo- dren), 0.01 to 2.92 (infants) and nitrate ranges from 0.87 to 2.21 (adults),
globinemia [8]. 0.21 to 2.24 (children), 0.16 to 1.71 (infants) (Table 3). According to

3.6. Human health risk assessment of fluoride and nitrate in groundwater results
Table 4
In the study, we used the human health risk assessment methodology Assessment of Non Carcinogenic risk for adults, children and infants based on total
proposed by USEPA (United States Environment Protection Agency) to as- hazard index.
sess the non carcinogenic health risk of fluoride and nitrate to adults, chil- HQ Fluoride HQ Nitrate Total hazard index
dren and infants. The evolution of Non carcinogenic risks due to fluoride Safe Risk Safe Risk Safe Risk
and nitrate in groundwater is of greater concern in many countries
NCA NS <1 NS >1 NS <1 NS >1 NS <1 NS >1
[31,38]. Continuous consumption of contaminated drinking water affects (PS) (PS) (PS) (PS) (PS) (PS)
the human health. Adults 16 (32%) 35 (68%) 1 (2%) 49 (98%) 1 (2%) 49 (98%)
In order to estimate the non carcinogenic health risk to human health Childrens 16 (32%) 35 (68%) 6 (12%) 44 (88%) 6 (12%) 44 (88%)
due to the intake of fluoride and nitrate in the groundwater, a total hazard Infants 18 (36%) 32 (64%) 11 (22%) 39 (78%) 10 (20%) 40 (80%)

index quotient (THI) as represented in (Table 4). The higher concentration *NCA-Non Carcinogenic Risk; HQ-Hazard Quotient; THI-Total Hazard Index; NS-
of fluoride and nitrate ions is observed in semi-arid region of Anantapur Number of Samples; PS-Percentage of Samples.

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USEPA guidelines, HQ values of fluoride concentration were 68% (adults), values in this region range from 0.88 to 5.46 (adults), 0.22 to 5.89 (chil-
68% (children), 64% (infants) and nitrate concentration were 98% (adults), dren), 0.18 to 4.22 (infants). According to USEPA guidelines, THI quotients
88% (children), 78% (infants) of the groundwater samples are exceeding for adults, children and infants in 98%, 88%, and 80% of samples have
the permissible limit (>1). From the results, Total Hazard Index (THI) exceeded the permissible limit (>1) and may cause adverse health risks.

Fig. 6. Spatial distribution map of total hazard index quotient for Adults in the study area.

157
M.R. B., S. V. / Environmental Chemistry and Ecotoxicology 2 (2020) 150–161

Spatial distribution map of THI group of adults, children and infants in- value in each of the three groups was >1, which has to be taken care
dicated in Fig. 6, Fig. 7 & Fig. 8 and comparison of THI in the studied of and proper precautionary measures to have to be measure have to
different age groups is represented in Table 4 and Fig. 9. The THI be taken care.

Fig. 7. Spatial distribution map of total hazard index quotient for Childrens in the study area.

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M.R. B., S. V. / Environmental Chemistry and Ecotoxicology 2 (2020) 150–161

Fig. 8. Spatial distribution map of total hazard index quotient for Infants in the study area.

4. Conclusions in groundwater is the weathering and leaching of fluoride bearing min-

erals from the basement granitic rocks of this region under alkaline en-
Groundwater is alkaline and hard in nature. Fluoride concentration vironment. Around 86% of the groundwater samples exceed the
in this region varies from 1.2–5.9 mg/L. A Possible source of fluoride permissible limit (1.5 mg/L) of fluoride indicating a high health risk

159
M.R. B., S. V. /
Fig. 9. Rose diagram of Total Hazard Index quotients for different age groups in the
study region.
to residents and appropriate defluoridation methods is important to pu-
rify this water. The study area nitrate concentration in groundwater
varies from 36 to 92 mg/L. 94% of the samples are exceeding the per-
missible limit (>45 mg/L). Anthropogenic activity is the main reason
for the increase of groundwater nitrate concentration, and continuous
intake of the higher nitrate water may cause health problems. The
high nitrate concentration in the groundwater could be a result of exces-
sive utilization of chemical fertilizers and manure that could be released
into groundwater by weathering host rock fractures. Dominant
hydrochemical types of water observed in the study area is of Na+ -
K+-Cl−-SO2− 4 . The Groundwater of the study area is mainly controlled
by rock weathering/rock water interaction dominance, which shows
that continuous and extended this rock water interaction has led to
the enrichment of fluoride concentration in the groundwater of the
study area. Groundwater chemistry depends on silicate weathering
and partially by carbonate dissolution.
The non carcinogenic risks of fluoride and nitrate are computed for
the study area. Hazard Quotient values of fluoride in this region range
from 0.01 to 3.78 (adults), 0.01 to 3.84 (children), 0.01 to 2.92 (in-
fants). HQ values of nitrates range from 0.87 to 2.21 (adults), 0.21 to
2.24 (children), 0.16 to 1.71 (infants). Total Hazard Index values vary
from 0.88 to 5.46 (adults), 0.22 to 5.89 (children), 0.18 to 4.22 (in-
fants). According to USEPA guidelines, the recommended THI value
must be <1. 98% of samples exceeding the standard limit of THI for
adults, 88% of groundwater are above the recommended standards of
THI for children and 80% of groundwater is a higher than the recom-
mended limit of THI for infants. Adults are more prone to risk of fluoride
and nitrate concentrations in the groundwater. The study results to give
valuable data to further work arranging and imperative to survey the
potential health outcomes from fluoride and nitrate exposure and rec-
ommend the security and the executive measures for maintainable im-
provement of groundwater resources to decrease the health disorders
in the study area.
Acknowledgements
The authors are appreciative of the Department of Science and Technol-
ogy, Government of India, New Delhi for research grant under the fast track
scheme is gratefully acknowledged. One of the authors Dr.V.Sunitha is
grateful to the DST for providing financial assistance in the form of Fast
Track Young Scientist Scheme. The authors are grateful to the editor and
anonymous reviewers for suggestions and comments which improved the
manuscript significantly.
160
Environmental Chemistry and Ecotoxicology 2 (2020) 150–161
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