Considering the health effects of fluoride, the present study was undertaken to assess the concentration of fluoride in ground - water, and urine of school children in Bass region of Haryana state. Fluoride in groundwater was observed to vary from 0.5 to 2.4 mg/l with an average concentration of 0.46 mg/l. On the other hand, F in urine ranged from below the detection limit to 1.8 mg/l among girls and 0.17–1.2 mg/l among the boys. Higher average concentration of fluoride in urine (0.65 mg/l for boys and 0.34 mg/l for girls) may be ascribed to exposure to bioavailable fluoride through food, milk, tea, toothpaste, etc., in addition to intake through groundwater. Relatively more intake of water and food by the boys might be the reason for more cases of severe dental fluorosis (44%) among boys compared to girls (29% cases of moderate to severe dental fluorosis). The groundwater quality for drinking was compromised with respect to dissolved solids, hardness, magnesium ions, and dissolved iron. Hydro-geochemical investigation revealed that rock–water interaction, in terms of direct cation exchange, dominantly regulates groundwater chemistry, and groundwater is of Ca-Na-HCO type. Keywords Fluoride · Urine · Fluorosis · Groundwater · School children Introduction 2007), fluoridated salt (García-Pérez et al. 2013), etc. United States Environmental Protection Agency (USEPA) recom- Fluorine is 13th most common element in the earth’s crust mended range on fluoride in drinking water is 0.7–1.2 mg/l, and is widely distributed as fluorspar (CaF ), fluorapatite effectively setting the maximum level at the lower end (Ca (PO ) ), and cryolite (N a AlF ). These minerals are (0.7 mg/l) to maximize dental caries protection benefits 5 4 3 3 6 easily soluble in water and, therefore, higher fluoride levels and to prevent excessive fluoride exposure in the popula - are observed in groundwater which interacts with fluoride tion which receives fluoridated salt. Absorption of ingested containing rocks during percolation. Consumption of fluo - fluoride is observed to be 100% on empty/fasting stomach; ride (0.5–1.0 mg/l) through drinking water is beneficial in and around 60% when taken with a calcium-rich diet (WHO terms of dental health preventing dental caries. But, higher 2002). Hector et al. (2009) reported that retention of fluo - levels of fluoride (> 1.5 mg/l) may result in dental or skeletal ride in young children may be higher (≈ 70%) on account of fluorosis depending on the intensity and duration of expo - higher ingestion through food and dentifrice. Young chil- sure. Apart from drinking water, exposure may also occur dren swallow a part of dentifrice voluntarily or involuntar- through bioavailable fluoride present in milk, food, meat ily during brushing which may result in enhanced exposure (IPCS 2002), toothpaste/dentifrice, tea, tobacco (Yadav et al. to systemic fluoride. Once ingested, fluoride reaches the blood stream within 30 min to 02 h depending upon ease in digestion of food and absorption of fluoride. Blood/plasma * A. K. Haritash fluoride level is a contemporary biomarker of exposure to email@example.com fluoride. Apart from blood, bone surface area, saliva, milk is also contemporary biomarkers; and whereas nails and hair Department of Environmental Engineering, Delhi Technological University, Bawana Road, Shahbad Daulatpur, are biomarkers of recent exposure, bone and teeth are the Delhi 110042, India biomarkers for historical exposure (WHO 2014). But, till Department of Basic and Applied Science, Bhagat Phool date urine is considered as the most useful biomarker for Singh Mahila Vishwavidyalaya, Khanpur Kalan, Sonepat, Haryana 131305, India Vol.:(0123456789) 1 3 52 Page 2 of 8 Applied Water Science (2018) 8:52 Table 1 Concentration of fluoride in ground water and urine, and fluoride exposure since it is widely used, relatively simple, prevalence of fluorosis among school children in Bass village and non-invasive (Szymaczek and Lewicka 2005). Prevalence of dental fluorosis in early age (15–20 years) Parameter Groundwater Urinary Urinary (n = 25) fluoride (girls) fluoride (boys) is an expression of higher exposure to fluoride, and it is fairly (n = 25) (n = 25) important since it affects permanent teeth leading to mild, moderate, or severe level of dental fluorosis. Some stud- Range ies (García-Pérez et al. 2013; Del Carmen et al. 2016) have Min. 0.10 BDL 0.17 reported prevalence of dental fluorosis in school children of Max. 2.40 1.80 1.20 younger age groups of 8–12 years and 12–15 years as well. Mean ± SD 0.46 ± 0.47 0.34 ± 0.44 0.65 ± 0.29 Therefore, monitoring of urinary fluoride concentration is Prevalence Nil 23 32 of fluorosis a useful tool to assess the exposure particularly among the Mild 48 24 (%) children at places with problem of endemic fluoride. Con- Moderate 21 36 tinued exposure to high level of fluoride may lead to osteo/ Severe 8 8 skeletal fluorosis after the age of 30 years, but it shall be preceded with dental fluorosis. Skeletal fluorosis is accom- panied by neurological, excessive tiredness, sleepiness, samples were collected from various locations within the vil- headache, and loss of sensation, altered reflexes, impotence, lage and from the fields around the village. The schoolchil- and loss of sphincter control. Some studies have reported dren aged between 15 and 18 years were chosen as subjects (Jolly et al. 1974) that skeletal fluorosis is also associated (n = 50) with equal number of both the genders to assess with nervous system damage. Studies in USA had no clear the exposure through urinary fluoride levels. The younger evidence that consumption of water with fluoride level up to age-groups were excluded since it is difficult for the young 8 mg/l had any association with dental and skeletal fluoro- children to hold urine for about 4 h after first meal of the day. sis, but the reports from India and China clearly present an The urine samples were collected during 1:00–2:00 PM in evidence of dental fluorosis, osteosclerosis, and bone frac- the afternoon to let the excretory concentration of ingested ture at concentration of 6 mg/l (IPCS 2002). Investigations by different authors in China have reported an association between higher level of fluoride in drinking water and lower IQ of children (Zhao et al. 1996; Xiang et al. 2003). There- fore, it becomes important to study the exposure of children, particularly school children, towards higher level of fluoride in drinking water in areas with endemic fluoride problem. Apart from fluoride, it is important to classify the water in respect of suitability for drinking for rest of the chemical constituents (Haritash et al. 2016); and to determine the major geochemical processes responsible for regulating groundwater chemistry (Haritash et al. 2017). Materials and methods Haryana is a major agricultural state of India with an area of 44,212 Km , and it has regional pockets of high concentra- tion of fluoride in groundwater throughout its stretch (Har - itash et al. 2008). Bass village of Hisar district in Haryana was selected as the study area since it has been identified as a water-challenged site by Department of Science and Technology owing to the problem of fluoride in ground- water. The village is classified as exclusive rural area with a total population of about 15,000 people. The sources of groundwater (hand-pump, tube-well, and submersible pump) were identified to collect representative groundwater sam- ples to determine fluoride, since groundwater is the primary Fig. 1 Prevalence of fluorosis (%) among girls (a) and boys (b) in the source for drinking and irrigation. A total of 25 groundwater present study (n = 25 in each) 1 3 22++ 22-- 22++ C Caa ++ M Mgg SSO O ++ ++ N Naa ++ K K Applied Water Science (2018) 8:52 Page 3 of 8 52 Table 2 Suitability of groundwater for drinking in the present study S. No. Parameter Value/concentration Desirable limit Suitable samples (%) Range Mean ± SD BIS (2012) WHO (2006) (n = 25) 1 pH 6.8–8.2 7.5 ± 0.33 6.5–8.5 NM 100 2 Total dissolved solids (TDS) (mg/l) 58–5350 1144 ± 1192 500 NM 24 3 Total hardness (as CaCO ) 56–2740 526 ± 522 200 NM 20 (mg/l) + b 4Sodium (Na ) 9–727 186 ± 208 NM 200 64 (mg/l) 2+ a 5Calcium (Ca ) 8–331 96 ± 98 75 NM 68 (mg/l) 2+ a 6Magnesium (Mg ) 0–463 69 ± 91 30 NM 32 (mg/l) 7 Iron (Fe) 0.83–1.46 0.91 ± 0.12 0.3 0.3 0 (mg/l) − a 8Chloride (Cl ) 14–701 171 ± 226 250 250 88 (mg/l) 2− a 9Sulphate (SO ) 21–315 173 ± 81 200 500 56 (mg/l) − a 10Nitrate (NO ) 0.3–10.1 4.9 ± 3.1 45 50 100 (mg/l) 11 Fluoride (Fˉ) 0.05–2.4 0.46 ± 0.47 1.0 1.5 96 (mg/l) SD Standard deviation, NM not mentioned As per BIS As per WHO Fig. 2 Piper-trilinear diagram 1 1 -C -CaH aHCO CO Ty Type pe 3 3 for geochemical classification of 2 2 -N -NaC aClT lTyp ype e groundwater 3 3 -M -Mix ixed ed Ca CaNa NaHC HCO O Ty Type pe 3 3 4 4 -M -Mix ixed ed Ca CaMg MgCl Cl Ty Type pe 5 5 5 5 -C -CaC aClT lTyp ype e 6 6 -N -NaH aHCO CO Ty Type pe 3 3 4 4 2 2 1 1 3 3 6 6 -- 2+ 2+ C Cll C Caa C CA AT TIIO ON NSS A AN NIIO ON NSS 1 3 22++ 22-- -- M Mgg SSO O ++ ll C C 22-- -- C CO O ++ H HC CO O 33 52 Page 4 of 8 Applied Water Science (2018) 8:52 is not of much concern in the study area. However, spatial 1 1 1000 000 0000 0 0 variations and observed value of 2.40 mg/l at one location Evaporation dominance Evaporation dominance indicates that the health of exposed population may be com- 1 1 1000 000 000 promised at few places, particularly if the source is used for drinking water. Moreover, intake of more volume of water Ro Rock dominance ck do minance 100 100 100 during early growing stage may result in fluorosis among children since most of the ingested minerals are absorbed by 10 10 10 the body during growing stage (Whitford 1999). Absorption of fluoride is regulated by the diet as well. The population Precipitation dominance Precipitation dominance 1 1 1 having more of vegetables in food is expected to excrete 00 00 00.2 .2 .2 0. 0. 0.40 40 40.6 .6 .6 0. 0. 0.81 81 81 more of fluoride in urine compared to those who consume Na/(Na + Ca) more of meat (WHO 2014). In the present study, urinary fluoride concentration varied from below the detection limit Fig. 3 Gibb’s diagram for the factors regulating groundwater chem- (BDL) to 1.8 mg/l for girls and 0.17–1.20 mg/l for boys, istry with a mean value of 0.34 and 0.65 mg/l, respectively. Low concentration of urinary fluoride in girls may be attributed fluoride reach urine. Spot samples of urine were collected to relatively less consumption of drinking water and food in pre-cleaned polypropylene (PP) bottles of 50 ml capac- compared to boys. The average level of fluoride in urine of ity. The collection of urine samples was done with prior boys was higher than in drinking water which may be an intimation and consent of the parents; and approval from outcome of additional ingestion of fluoride via intake of tea, the institutional committee for ethics and research. Fluo- milk, vegetables, etc. Similar observations of higher F in ride concentration in groundwater and urine samples was urine have been made in other studies too (Paez and Dapas determined using a F ion specific electrode (Orion 96-09 1983; Szymaczek and Lewicka 2005; Rango et al. 2014; BNWP) fitted with an Orion Star A329 ISE Meter, MA, Del Carmen et al. 2016) ascribing the reason to additional USA. A cross-sectional survey was also carried out (for 50 intake of bioavailable fluoride through food. Based on the students) to assess the prevalence of dental fluorosis. Based survey for dental fluorosis, it was observed that majority of on the prevalence, dental fluorosis was classified as nil, mild, the subjects suffered from dental fluorosis with the degree moderate, and severe as per the Dean’s Index (Dean 1942). of expression varying from nil to severe through mild and Physicochemical characterization of groundwater was also moderate as per Dean’s Index. Prevalence of fluorosis was performed using standard methods of APHA (Eaton et al. observed to be 77% among the girls, and 68% among the 1995) to get the information about possible soil–water chem- boys (Table 1). But based on the grading of intensity, most istry governing the water quality. The statistical analysis of of the girls had mild fluorosis (48%) followed by moderate the results obtained was done on SPSS ver. 20. Analysis of (21%) and severe (8%). On the other hand, most of the boys correlation, cluster analysis, and principal component anal- suffered from moderate fluorosis (36%) and relatively less ysis were performed to understand the factors controlling from mild (24%) and severe (8%) (Fig. 1). More prevalence groundwater chemistry. of moderate and severe dental fluorosis (44%) among boys (As against 29% of girls) further strengthens the premise that boys had more ingestion of fluoride through food and water, Results and discussion and hence higher urinary fluoride concentration. Statistical evaluation for correlation between urinary fluoride concen- Based on the analysis of groundwater, it was observed that tration and prevalence of fluorosis, too, revealed relatively fluoride was within the permissible limit for most of the stronger correlation for boys (0.64) than the girls (0.44) (p samples. It varied from 0.10–2.40 mg/l with an average value > 0.01). Calculations of correlation coefficients among value of 0.46 mg/l in groundwater (Table 1). Only one sam- different physico-chemical parameters revealed that fluoride ple exceeded the standard prescribed limit of 1.0 mg/l (BIS is significantly and positively correlated with Na and Ca 2012). Based on the recorded mean concentration, it may indicating the possible presence of fluorspar, fluoraptite, be inferred that exposure to fluoride from drinking water cryolite in sub surface soil/rocks. While determining the 1 3 TDS (m g/l) Applied Water Science (2018) 8:52 Page 5 of 8 52 Table 3 Concentration of fluoride in groundwater and urine, and prevalence of dental fluorosis in different regions of the world − − S. No. Country Region Age group F in drinking F in urine Prevalence of Criteria for Reference (years) water (mg/l) (mg/l) dental fluoro- classifica- (Remarks) sis (%) tion of dental fluorosis 1. India Bass Village, 15–18 0.1–2.4 0.17–1.80 72.0 DI Present Study Haryana 2. Mexico (a) Morelos 8–12 0.7–1.5 NA 39.4–60.5 TFI García-Pérez (b) Guanajuato 11–20 4.4 0.50–6.65 91.90 TFI et al. 2013 Del Carmen et al. 2016 3. Ethiopia Ethiopian Rift 10–15 1.1–18.0 1.1–39.8 91.00 TFI Rango et al. Valley 2014 4. China (a) Xinhuai 8–13 0.18–0.76 0.37–2.50 NA – Xiang et al. (b) Wamiao 0.57–4.50 0.90–12.50 2003 (Lower IQ level related to higher fluoride in drinking water) 5. Poland Poznan 22–34 0.40–0.80 0.84–2.22 NA – Szymaczek and Lewicka 2005 6. Venezuela Maracay, 1.25–6 0.07–0.09 0.79–0.92 NA – Hector et al. Aragua (*average (average 2009 total intake- values) mg/kg/day) 7. Rajasthan (a) Banswara 17–22 1.5–4.0 NA 77.11 DI Choubisa 2001 (b) Dungarpur (c) Udaipur 8. India (a) Jhajjar City 8–15 1.90–2.60 0.05–2.64 51.90 TSIF Kumar et al. (Haryana (b) Dadanpur 2.53–3.14 0.69–2.80 94.63 2017 State) Village 1.63–3.33 0.31–2.50 36.84 (c) Dariyapur Village 9. India (Haryana (a) Beri Block 7–15 1.56–3.05 NA 59.76 TSIF Yadav et al. State) (b) Bahadur- 1.53–3.52 66.32 2009 garh 1.52–4.00 44.99 (c) Jhajjar 1.53–3.14 58.02 Block 1.52–3.16 62.10 (d) Sahlawas Block (e) Matanhail Block DI Dean’s Index, TFI Thylstrup and Fejerskov Index, TSIF Tooth Surface Index of Fluorosis (Horowitz et al. 1984), NA not analysed 2− − suitability of groundwater, the only source for drinking, it weak acids ( CO and H CO ) exceeded strong acids 3 3 − 2− was observed that the quality was compromised with respect (Cl and SO ) (Fig. 2). Based on the values of base- to total dissolved solids (TDS), total hardness (TH), Mg, Fe exchange (Matthess 1982) all the samples were found to 2− and SO chiefly (Table 2), apart from the effect of fluo- be sodium sulfate typed (value < 1) except one sample. ride. A comparative analysis of concentration of fluoride in Negative values of chlor-alkaline index (Schoeller 1977) drinking water, urine, and prevalence of fluorosis in school- suggest that most of the sample had direct base-exchange children around the world has been made in Table 3. reaction resulting in exchange of Ca and Mg of rocks/ Hydro-geochemical classification of the ground water soil with Na and K of water. Gibbs classification (Gibbs revealed that most of the samples were CaHC O type or 1970) to determine the major regulating factor revealed mixed CaNaHCO type. Piper tri-linear classification that the quality of ground water is predominately governed + + (Piper 1953) indicated that the alkaline (N a and K ) spe- by rock–water interaction (Fig. 3). The average values of 2+ 2+ cies exceeded the alkaline earth (Ca and Mg ); and ratio of Ca/Na (0.72), Mg/Na (1.15), and HCO /Na (3.84) 1 3 52 Page 6 of 8 Applied Water Science (2018) 8:52 Table 4 Principal component analysis of observed parameters in the fluoride from the underlying strata. Among the other ions, present study significant positive correlation of Na was observed with Ca, 2− − − 2− Li, CO, HCO, Cl, SO etc. and these ions signifi - Variables Component 3 3 4 cantly contributed to total alkalinity and total hardness of 1 2 3 4 water. Principal component analysis (PCA) (Table 4) also pH − 0.50 0.32 0.66 0.14 revealed that total alkalinity, total hardness, sodium, potas- EC 0.33 0.85 − 0.21 − 0.05 sium, lithium, calcium, magnesium, carbonate, bicarbo- TDS 0.33 0.85 − 0.20 − 0.05 nate, chloride, and sulphate regulated the water quality; and TH 0.85 − 0.45 0.03 − 0.18 indicates that the source is primarily natural. A hierarchical TA 0.95 − 0.13 0.21 0.01 cluster analysis using Centroid Linkage was performed to Na 0.86 0.35 0.27 0.12 highlight the inter-relationships among various sites along K 0.37 − 0.45 − 0.42 − 0.07 with the selected water parameters. The dendrogram clas- Ca 0.90 0.28 0.01 − 0.04 sified the data into three cluster membership. First cluster Mg 0.77 − 0.56 0.13 − 0.07 includes all the sites except site 21 (second cluster), and site Li 0.95 − 0.06 0.06 0.04 23 (third cluster) (Fig. 4). Cluster analysis indicated that the Fe 0.15 0.09 − 0.07 0.89 water quality is almost the same with the only variation at 2− CO 0.73 − 0.38 0.51 0.08 two sites (Site 21 and 23). HCO 0.93 0.07 − 0.06 − 0.05 Cl 0.80 0.12 − 0.18 − 0.31 2− SO 0.83 0.16 − 0.23 0.08 Conclusion NO 0.51 − 0.31 − 0.21 0.45 3− PO 0.72 0.04 0.33 0.02 4 The study concludes that the concentration of fluoride in F 0.35 0.70 0.41 − 0.06 groundwater in Bass village is within the prescribed limits Eigen values 9.054 3.301 2.122 1.195 except a few locations. Although intake through drinking CV (%) 47.66 65.03 76.20 82.49 water is limited, ingestion of fluoride through food, tea, milk, toothpaste, etc., may be alternate route for exposure. Statistically significant p values are in bold (p < 0.05) Depending upon the total daily ingestion, boys are more exposed to fluoride as observed in higher average urinary indicated that silicate weathering primarily governs water fluoride level. It has lead to more severe cases of dental chemistry (Negrel et al. 1993) followed by carbonate fluorosis among the boys than the girls. Significant num- weathering as represented by high average value (5.82) of ber of cases of dental fluorosis (72%) despite a relatively (Ca + Mg)/(Na + K) ratio. lower concentration of fluoride in drinking, as compared to other studies around the world, is a cause of concern. Statistical analysis The study recommends extensive screening of groundwater sources for fluoride levels, and a regular monitoring of 24-h The statistical analysis of the results obtained revealed that urine samples for a bigger sample size to better understand a significant positive correlation of fluoride existed with sodium, TDS, and EC indicating to natural dissolution of 1 3 Applied Water Science (2018) 8:52 Page 7 of 8 52 Fig. 4 Cluster analysis of the locations with respect to analysed parameters the exposure to fluoride, and its control. 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