Abstract

Fluoride contamination in groundwater is a major problem throughout the world as well as in India. High-fluoride content was reported in the hot springs of Atri and Tarbalo sites in Odisha, India, and residents of nearby villages showed the manifestations of fluorosis. Around 39% of the groundwater samples showed fluoride concentration > 1 mg/l, higher than the desirable limit specified by the WHO. The dominant chemical facies of groundwaters were ions of Ca-Mg-HCO3 and Ca-Na-Cl, which infers the lithological control over the hydrochemistry of this area. A strong correlation between fluoride and other major ions could not be found, suggesting that multiple processes are responsible for the enriched fluoride concentration observed in the study area. The major geochemical processes include dissolution of fluoride-bearing minerals from the rocks, evapotranspiration, agricultural input and mixing of cold groundwater with hot spring water containing high fluoride. The maximum fluoride exposure doses through drinking water from fluoride-contaminated tube wells were estimated to be 0.07 mg/kg/d for infants, 0.125 mg/kg/d for children and 0.06 mg/kg/d for adults, which are higher than the minimum risk level (0.05 mg/kg/d). Exposure doses of fluoride indicate that exposure risk is doubled for children in comparison to infants and adults, which might cause severe dental fluorosis and other ailments. Considering the environmental and hydrological set up of the study area, membrane defluoridation process can be suggested as the best remediation method. Nalgonda technique, dilution of fluoride-rich groundwater and better nutrition containing calcium and vitamin C are other possible options that can be included for early mitigation of fluoride contamination.

References

Adimalla N, Li P, Qian H (2019) Evaluation of groundwater contamination for fluoride and nitrate in semi-arid region of Nirmal Province, South India: a special emphasis on human health risk assessment (HHRA). Hum Ecol Risk Assess 25(5):1107–1124. https://doi.org/10.1080/10807039.2018.1460579

CAS  Article  Google Scholar

Alabaster G (2010) Urbanization and water management–trends, challenges and perspectives. Presentation at World Water Week Stockholm (online http://www. worldwaterweek. org/documents/WWW_PDF/2010/tuesday/T5/Graham_Ala baster. pdf-accessed 1/4/2015)

Ali S, Thakur SK, Sarkar A, Shekhar S (2016) Worldwide contamination of water by fluoride. Environ Chem Lett 14(3):291–315

CAS  Article  Google Scholar

APHA (1992) Standard methods for the examination of water and wastewater, 19th edn. APHA, Washington, DC

Google Scholar

ATSDR (2003) Toxicological profile for fluorides, hydrogen fluoride, and fluorine; US Department of Health and Human Services, Public Health Service, Agency for Toxic Substances and Disease Registry, Atlanta, 404p

Batra J, Vispute J, Deshmukh A, Vali S (1995) Contribution from rock, soil and ground water to fluoride content of food stuffs grown in some selected villages of Bhadravati Tehsil, Chadrapur District, Maharashtra Fluoride in environment Nagpur, India: Gondwana Geological Society:81-90

Bhattacharta P, Samal AC (2018) Fluoride contamination in groundwater, soil and cultivated foodstuffs of India and its associated health risks: a review. Res J Recent Sci (ISSN: 2277-2502) 7(4):3647

Google Scholar

Bhattacharya P (2016) Analysis of fluoride distribution and community health risk in Purulia district of West Bengal, India. Proceedings of 9th National Level Science Symposium (ISBN: 9788192952123), Christ College, Rajkot, vol 3, pp 88 ? 92

Bhattacharya P, Samal AC, Banerjee S, Pyne J, Santra SC (2017) Assessment of potential health risk of fluoride consumption through rice, pulses, and vegetables in addition to comsumption of fluoride-contaminated drinking water of West Bengal, India. Environ Sci Pollut Res 24:20300–20314. https://doi.org/10.1007/s11356-017-9649-2

CAS  Article  Google Scholar

Bhattacharya P, Adhikari S, Samal AC, Das R, Dey D, Deb A, Ahmed S, Hussein J, de A, Das A, Joardar M, Panigrahi AK, Roychowdhury T, Santra SC (2020) Health risk assessment of co-occurrence of toxic fluoride and arsenic in groundwater of Dharmanagar region, North Tripura (India). Groundw Sustain Dev:100430. https://doi.org/10.1016/j.gsd.2020.100430

BIS (2012) Bureau of Indian Standards, drinking water specification (2nd revision) ICS 13.060.20, IS 10500:2012

Böttcher J, Strebel O, Voerkelius S, Schmidt HL (1990) Using isotope fractionation of nitrate-nitrogen and nitrate oxygen for evaluation of microbial denitrification in a sandy aquifer. J Hydrol 114(3-4):413–424

Article  Google Scholar

Brindha K, Elango L (2013) Geochemistry of fluoride rich groundwater in a weathered granitic rock region, Southern India. Water Qual Expo Health 5:127–138. https://doi.org/10.1007/s12403-013-0096-0

CAS  Article  Google Scholar

Brindha K, Jagadeshan G, Kalpana L, Elango L (2016) Fluoride in weathered rock aquifers of southern India: managed aquifer recharge for mitigation. Environ Sci Pollut Res 23:8302–8316. https://doi.org/10.1007/s11356-016-6069-7

CAS  Article  Google Scholar

CGWB (2018) Ground water quality in shallow aquifers of India; Central Ground Water Board, Ministry of Water Resources, Government of India, Faridabad http://cgwb.gov.in/WQ/Ground%20Water%20Book-F.pdf. Accessed 2 Mar 2020

Chatterjee S, Sinha UK, Biswal BP, Jaryal A, Jain PK, Patbhaje S, Dash A (2019) An integrated isotope-geochemical approach to characterize a medium enthalpy geothermal system in India. Aquat Geochem 25:63–89. https://doi.org/10.1007/s10498-019-09352-z

CAS  Article  Google Scholar

Edmunds W, Smedley P (2005) In: Alloway BJ, Selinus O (eds) Fluoride in natural waters Essentials of Medical Geology. Elsevier, London

Google Scholar

Evans SW, Jones NL, Williams GP, Ames DP, Nelson EJ (2020) Groundwater Level Mapping Tool: An open source web application for assessing groundwater sustainability. Environ Model Softw 131:104782

Article  Google Scholar

Farooq SH, Prusty P, Singh RK, Sen S, Chandrasekharam D (2018) Fluoride contamination of groundwater and its seasonal variability in parts of Purulia district, West Bengal, India. Arab J Geosci 11(22):709. https://doi.org/10.1007/s12517-018-4062-9

CAS  Article  Google Scholar

Gizaw B (1996) The origin of high bicarbonate and fluoride concentrations in waters of the Main Ethiopian Rift Valley, East African Rift system. J Afr Earth Sci 22:391–402

CAS  Article  Google Scholar

Gleick PH (1993a) Water and conflict: Fresh water resources and international security. Int Secur 18:79–112

Article  Google Scholar

Gleick PH (1993b) Water in crisis Pacific Institute for Studies in Dev, Environment & Security Stockholm Env Institute, Oxford Univ Press 473p 9

Grimaldo M, Borjaaburto VH, Ramirez AL, Ponce M, Rosas M, Diazbarriga F (1995) Endemic fluorosis in San-Luis-Potosi, Mexico. 1. Identification of risk-factors associated with human exposure to fluoride. Environ Res 68:25–30

CAS  Article  Google Scholar

Gupta S (2004) The Eastern Ghats Belt, India-a new look at an old orogen. Geol Surv India Spec Publ 84:75–100

Google Scholar

Gupta S (2012) Strain localization, granulite formation and geodynamic setting of ‘hot orogens’: a case study from the Eastern Ghats Province, India. Geol J 47:334–351. https://doi.org/10.1002/gj.132

CAS  Article  Google Scholar

Handa B (1975) Geochemistry and genesis of fluoride-containing ground waters in india. Groundwater 13:275–281

CAS  Article  Google Scholar

He S, Li P (2019) A MATLAB based graphical user interface (GUI) for quickly producing widely used hydrogeochemical diagrams. Geochemistry:125550. https://doi.org/10.1016/j.chemer.2019.125550

He S, Wu J (2019) Hydrogeochemical characteristics, groundwater quality and health risks from hexavalent chromium and nitrate in groundwater of Huanhe Formation in Wuqi County, northwest China. Expo Health 11(2):125–137. https://doi.org/10.1007/s12403-018-0289-7

CAS  Article  Google Scholar

He X, Wu J, He S (2019) Hydrochemical characteristics and quality evaluation of groundwater in terms of health risks in Luohe aquifer in Wuqi County of the Chinese Loess Plateau, northwest China. Hum Ecol Risk Assess 25(1-2):32–51. https://doi.org/10.1080/10807039.2018.1531693

CAS  Article  Google Scholar

He X, Li P, Ji Y, Wang Y, Su Z, Elumalai V (2020) Groundwater arsenic and fluoride and associated arsenicosis and fluorosis in China: occurrence, distribution and management. Expo Health 12(3):355–368. https://doi.org/10.1007/s12403-020-00347-8

CAS  Article  Google Scholar Hounslow A (1995) Water quality data: analysis and interpretation. CRC press

ICMR (1975) Manual of standards of quality for drinking water supplies, special report series number 44, 2nd edn. Indian Council of Medical Research, New Delhi

Google Scholar

Jacks G, Bhattacharya P, Chaudhary V, Singh K (2005) Controls on the genesis of some high-fluoride groundwaters in India. Appl Geochem 20:221–228

CAS  Article  Google Scholar

Jackson P, Harvey P, Young W (2002) Chemistry and bioavailability aspects of fluoride in drinking water Marlow, Buckinghamshire: WRc-NSF

Jagadeshan G, Kalpana L, Elango L (2015) Major ion signatures for identification of geochemical reactions responsible for release of fluoride from geogenic sources to groundwater and associated risk in Vaniyar River basin, Dharmapuri district, Tamil Nadu, India. Environ Earth Sci 74:2439–2450

CAS  Article  Google Scholar

Jha S, Nayak A, Sharma Y (2009) Fluoride occurrence and assessment of exposure dose of fluoride in shallow aquifers of Makur, Unnao district Uttar Pradesh, India. Environ Monit Assess 156:561–566

CAS  Article  Google Scholar

Keesari T, Shivanna K, Jalihal AA (2007) Isotope hydrochemical approach to understand fluoride release into groundwaters of Ilkal area, Bagalkot District, Karnataka, India. Hydrogeol J 15:589–598

Article  Google Scholar

Keesari T, Sinha UK, Deodhar A, Krishna S, Ansari A, Mohokar H, Dash A (2016) High fluoride in groundwater of an industrialized area of Eastern India (Odisha): inferences from geochemical and isotopic investigation. Environ Earth Sci 75:1090

Article  Google Scholar

Keesari T, Chatterjee S, Pant D, Kumar M, Sakhare V, Sinha UK, Mohokar H, Jaryal A, Roy A, Maitra A (2019a) Dating of hot springs at Attri, Tarabalo and Athmalik sites in Odisha, India using radiocarbon technique. J Radioanal Nucl Chem 323:1227–1235. https://doi.org/10.1007/s10967-019-06867-1

CAS  Article  Google Scholar

Keesari T, Sinha UK, Kamaraj P, Sharma DA (2019b) Groundwater quality in a semi-arid region of India: Suitability for drinking, agriculture and fluoride exposure risk. J Earth Syst Sci 128:24

Article  Google Scholar

Kundu N, Panigrahi M, Tripathy S, Munshi S, Powell M, Hart B (2001) Geochemical appraisal of fluoride contamination of groundwater in the Nayagarh District of Orissa, India. Environ Geol 41:451–460

CAS  Article  Google Scholar

Kundu N, Panigrahi M, Sharma S, Tripathy S (2002) Delineation of fluoride contaminated groundwater around a hot spring in Nayagarh, Orissa, India using geochemical and resistivity studies. Environ Geol 43:228–235

CAS  Article  Google Scholar

Levy SM (1994) Review of fluoride exposures and ingestion. Community Dent Oral Epidemiol 22:173–180

CAS  Article  Google Scholar

Li P, Qian H, Wu J, Chen J, Zhang Y, Zhang H (2014) Occurrence and hydrogeochemistry of fluoride in shallow alluvial aquifer of Weihe River, China. Environ Earth Sci 71(7):3133–3145. https://doi.org/10.1007/s12665-013-2691-6

CAS  Article  Google Scholar

Li P, Wu J, Qian H, Zhang Y, Yang N, Jing L, Yu P (2016) Hydrogeochemical characterization of groundwater in and around a wastewater irrigated forest in the southeastern edge of the Tengger Desert, northwest China. Expo Health 8(3):331–348. https://doi.org/10.1007/s12403-016-0193-y

CAS  Article  Google Scholar

Li P, Tian R, Xue C, Wu J (2017) Progress, opportunities and key fields for groundwater quality research under the impacts of human activities in China with a special focus on western China. Environ Sci Pollut Res 24(15):13224–13234. https://doi.org/10.1007/s11356-017-8753-7

Article  Google Scholar

Li P, He S, He X, Tian R (2018) Seasonal hydrochemical characterization and groundwater quality delineation based on matter element extension analysis in a paper wastewater irrigation area, northwest China. Expo Health 10(4):241–258. https://doi.org/10.1007/s12403-17-0258-6

CAS  Article  Google Scholar

Li P, He X, Li Y, Xiang G (2019) Occurrence and health implication of fluoride in groundwater of Loess aquifer in the Chinese Loess Plateau: a case study of Tongchuan, Northwest China. Expo Health 11(2):95–107. https://doi.org/10.1007/s12403-018-0278-x

CAS  Article  Google Scholar

Maitra A, Chatterjee A, Keesari T, Gupta S (2020a) Forming topography in granulite terrains: evaluating the role of chemical weathering. J Earth Syst Sci 129:1–13. https://doi.org/10.1007/s12040-019-1293-4

CAS  Article  Google Scholar

Maitra A, Singh A, Keesari T, Sharma S, Gupta S (2020b) Elevated equilibrium geotherm in stable continental shield: evidence from integrated structural, hydrological, and electromagnetic studies on nonvolcanic hot springs in the Eastern Ghats Belt, India. J Geophys Res Solid Earth 125:e2019JB017747. https://doi.org/10.1029/2019JB017747

CAS  Article  Google Scholar

Malde MK, Scheidegger R, Julshamn K, Bader H-P (2011) Substance flow analysis: a case study of fluoride exposure through food and beverages in young children living in Ethiopia. Environ Health Perspect 119:579–584

CAS  Article  Google Scholar

Mukherjee A, Scanlon BR, Fryar AE, Saha D, Ghosh A, Chowdhuri S, Mishra R (2012) Solute chemistry and arsenic fate in aquifers between the Himalayan foothills and Indian craton (including central Gangetic plain): influence of geology and geomorphology. Geochim Cosmochim Acta 90:283–302

CAS  Article  Google Scholar

NRC (1993) Health effects of ingested fluoride; National Research Council. National Academy Press, Washington DC

Google Scholar

Podgorski JE, Labhasetwar P, Saha D, Berg M (2018) Prediction modeling and mapping of groundwater fluoride contamination throughout India. Environ Sci Technol 52:9889–9898

CAS  Article  Google Scholar

Praharaj T, Tripathy S, Powell M, Hart B (2003) Geochemical studies to delineate topsoil contamination around an ash pond of a coal-based thermal power plant in India. Environ Geol 45:86–97

CAS  Article  Google Scholar

Samal AC, Bhattacharya P, Mallick A, Ali MM, Pyne J, Santra SC (2015) A study to investigate fluoride contamination and fluoride exposure dose assessment in lateritic zones of West Bengal, India. Environ Sci Pollut Res 22:6220–6229. https://doi.org/10.1007/s11356-014-3817-4

CAS  Article  Google Scholar

Shah S, Bandekar K (1998) IS 10500: 91 Drinking Water compared to WHO Guidelines (1993). J Indian Waterworks Assoc 30:179–184

Google Scholar

Shah M, Sircar A, Shaikh N, Patel K, Sharma D, Vaidya D (2019) Comprehensive geochemical/hydrochemical and geo-thermometry analysis of Unai geothermal field, Gujarat, India. Acta Geochim 38(1):145–158

CAS  Article  Google Scholar

Subba Rao N, Ravindra B, Wu J (2020) Geochemical and health risk evaluation of fluoride rich groundwater in Sattenapalle Region, Guntur district, Andhra Pradesh, India. Hum Ecol Risk Assess:1–33. https://doi.org/10.1080/10807039.2020.1741338

Teotia S, Teotia M (1988) Endemic skeletal fluorosis: clinical and radiological variants. Fluoride 21:39–44

Google Scholar

Tiwary R, Dhakate R, Sinha A, Singh V (2009) Evaluation of impact of mining on groundwater resources in Talcher Coalfield, India. Int J Earth Sci Eng 2:238–252

Google Scholar

USPHS (United States Public Health Service): Report on fluoride benefits and risks: review of fluoride benefits and risks. Report of the Ad Hoc Subcommittee on Fluoride. 1991

Verma S, Mukherjee A, Choudhury R, Mahanta C (2015) Brahmaputra river basin groundwater: solute distribution, chemical evolution and arsenic occurrences in different geomorphic settings. J Hydrol 4:131–153

Google Scholar

Viswanathan G, Jaswanth A, Gopalakrishnan S (2009) Mapping of fluoride endemic areas and assessment of fluoride exposure. Sci Total Environ 407:1579–1587

CAS  Article  Google Scholar

Wang D, Wu J, Wang Y, Ji Y (2020) Finding high-quality groundwater resources to reduce the hydatidosis incidence in the Shiqu County of Sichuan Province, China: analysis, assessment, and management. Expo Health 12(2):307–322. https://doi.org/10.1007/s12403-019-00314-y

CAS  Article  Google Scholar

WHO (2002) Fluorides, environmental health criteria 227; International Programme on Chemical Safety, Geneva

WHO (2010) Exposure to arsenic: a major public health concern. Public Health and Environment, WHO, Geneva. https://www.who.int/ipcs/features/arsenic.pdf. Accessed 30 Mar 2020

WHO (2011) Guidelines for drinking water quality; 4th edn, WHO Press, 20 Avenue Appia, Geneva

Wood JM (1974) Biological cycles for toxic elements in the environment. Science 183:1049–1052

CAS  Article  Google Scholar

Wu J, Li P, Qian H (2015) Hydrochemical characterization of drinking groundwater with special reference to fluoride in an arid area of China and the control of aquifer leakage on its concentrations. Environ Earth Sci 73(12):8575–8588. https://doi.org/10.1007/s12665-015-4018-2

CAS  Article  Google Scholar

Wu J, Wang L, Wang S, Tian R, Xue C, Feng W, Li Y (2017) Spatiotemporal variation of groundwater quality in an arid area experiencing long-term paper wastewater irrigation, northwest China. Environ Earth Sci 76(13):460. https://doi.org/10.1007/s12665-017-6787-2

Article  Google Scholar

Wu J, Zhou H, He S, Zhang Y (2019) Comprehensive understanding of groundwater quality for domestic and agricultural purposes in terms of health risks in a coal mine area of the Ordos basin, north of the Chinese Loess Plateau. Environ Earth Sci 78(15):446. https://doi.org/10.1007/s12665-019-8471-1

CAS  Article  Google Scholar

Zimik HV, Farooq S, Prusty P (2017) Geochemical evaluation of thermal springs in Odisha, India. Environ Earth Sci 76:593

Article  Google Scholar

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Acknowledgements

The authors duly acknowledge the support by the RTAC-BRNS, Department of Atomic Energy, India (Project sanction No. 35/14/12/2016-BRNS/35049). The first author (Asmita Maitra) would like to thank the Ministry of Human Resource Development (MHRD), Department of Higher Education, New Delhi, India, for providing student fellowship. We sincerely thank Mr. Ajay Jaryal and Mr. S.N. Kamble of the Isotope Hydrology Section, Bhabha Atomic Research Centre for helping in the field work. Dr. U.K. Sinha (Head, Isotope Hydrology Section), Dr. H. J Pant (Head, Isotope and Radiation Application Division) and Dr. Pradeep Kumar Pujari (Group Director, Radiochemistry and Isotope Group) of the Bhabha Atomic Research Centre are duly acknowledged for their constant support and encouragement during the course of this project. The study has improved substantially from the comments of the handling editor and three anonymous referees.

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Contributions

Asmita Maitra: conceptualization, data-curation, formal analysis, investigation, methodology, validation, visualization, writing- original draft; Tirumalesh Keesari: supervision, conceptualization, formal analysis, investigation, writing- review and editing; Annadasankar Roy: investigation, data-curation, visualization; Saibal Gupta: supervision, conceptualization, investigation, writing- review and editing.

Corresponding author

Correspondence to Tirumalesh Keesari.

*Original abstract online at https://link.springer.com/article/10.1007/s11356-020-10948-0