Abstract

Highlights

  • Alluvium and Gneissic aquifers were found prone to groundwater contamination.
  • Groundwater pollution index confirms Fluoride and Nitrate as contaminants.
  • Aquifer composition primarily controls Uranium occurrence in groundwater.
  • Uranium mobility depends on carbonate-complex formation in alkaline conditions.
  • Exposure to contaminated groundwater causes higher carcinogenic risk in Jaipur.

Groundwater contamination threat has been evaluated to ascertain its impact on public health. An integrated approach of experiments, modeling and field survey was employed to examine the occurrence, hydrogeochemistry, and synergistic health risks associated with geogenic and anthropogenic contaminants, specifically Fluoride (F), Uranium (U), and Nitrate (NO3). The Groundwater Pollution Index unveiled F and NO3 as potential contaminants, while higher U concentrations were primarily detected in prevailing Alluvium aquifers. Principal component analysis and scatter plot have pointed out natural and anthropogenic sources’ contributions to elevating concentrations, while analysis of variance (ANOVA) indicated significant differences in quality parameters. Hydrogeochemical modeling identified evaporation, crystallization, ion exchange, silicate and carbonate-weathering as controlling processes along with ionic speciation and determined Nasingle bondCl and Na-HCO3 principal groundwater facies representing saline aquifer systems. Evaluation of potential health risks from oral and dermal exposure across infants, children, teenagers, and adult age-groups was ascertained using deterministic and probabilistic approaches through Monte Carlo simulation (MCS) with a 95 % confidence level. The assessment of carcinogenic and non-carcinogenic health risks indicates that infants and children are most vulnerable, especially in the Jaipur region (Mean oral hazard quotient: 2.0804, dermal: 0.0027). MCS results endorsed the health risk trend with a probability of 95.01 % for oral and 90.95 % for dermal pathways, with contaminant concentration being the leading factor for health risks. The integrated methodological framework delineates spatial hotspots and elucidates the underlying hydrogeochemical mechanisms that regulate groundwater quality. This approach systematically characterizes associated human health risks, facilitating the implementation of timely mitigation strategies.

Introduction

Groundwater resources are crucial for maintaining a healthy ecosystem and ensuring environmental stability in geographically diverse areas (Li et al., 2018). However, the challenges related to water scarcity and continuous water quality deterioration caused by geogenic and anthropogenic contaminants are diminishing the clean and potable water supply. These challenges are exacerbated by a changing climate, unplanned development, population growth, extensive use of chemical fertilizers, and expanding anthropogenic activities (He and Wu, 2019). The excessive reliance on groundwater for irrigation, industrial, and domestic purposes is placing alarming pressure on this vital resource, especially in developing countries (Rao et al., 2024).

In recent decades, regions like the northwest of the Indian subcontinent have experienced a consistent decline in groundwater level and quality (Joshi et al., 2021). Contaminants’ accumulation in prevailing aquifers across northwest India, driven by irrigation practices, evaporation, groundwater abstraction, mineralization, and leachates, is regarded as a more significant threat to groundwater quality than groundwater depletion, resulting in health risks. Earlier, Lapworth et al. (2017) revealed that Alluvium aquifers in some parts of Northwest India are severely impacted by excessive Fluoride (F), Uranium (U), and Nitrate (NO3) contents. However, health risks from the consumption of F, U, and NO3 contaminated groundwater through multiple pathways have been rarely studied in the region, which significantly affects the life span of an individual.

F is released in groundwater from the dissolution of minerals such as Fluorite, Fluorapatite, Villiaumite, Hornblende, Muscovite, and Biotite (Reddy et al., 2010). F concentrations ranging from 0.5 to 1.5 mg/l are crucial for promoting teeth and bone development. However, exceeding the concentration of more than >1.5 mg/l (WHO, 2017) can lead to pitting and mottling of teeth, skeletal and dental fluorosis, as well as chronic kidney diseases (Li et al., 2019). Moreover, F is capable of replacing the hydroxide ion present in hydroxyapatite in bones, which causes bone damage (Montazeri et al., 2011).

Similarly, U enters the groundwater through the dissolution of minerals like Uraninite, Pitchblende, Rutherfordine, Gummite, Schoepite, Coffinite, and Uranophane (Devaraj et al., 2021). U can also contaminate groundwater through anthropogenic sources, including phosphate fertilizers, mining activities, and radioactive waste disposal. The intake of high concentrations of U via oral and dermal routes with >30 ug/l is considered unsafe for health (Ramadan et al., 2022), and its impacts are often found to be connected with bone-health-related issues and chronic nephrotoxicity (Kumar et al., 2020). Depleted U can enter the human body as uranyl oxides. The primary uranyl oxides (U3O8, UO2, and UO3) exhibit varying solubility in body fluids, with UO3 dissolving within weeks, while U3O8 and UO2 take years to dissolve. Uranium-hexafluoride (UF6) is a readily soluble U compound than uranyl oxides [UO3, U3O8 and UO2]. In body fluids, U dissolves as the uranyl ion (UO22+), which can interact with biological molecules. Once absorbed into the bloodstream, U is transported and retained in body tissues and organs, forming soluble complexes with bicarbonate, citrate, or proteins (Bleise et al., 2003). U is also capable of binding with Ca2+, which ultimately modifies the crystal structure of minerals present in bone (Kurttio et al., 2005).

The excessive concentrations of NO3 (>50 mg/L) in shallow aquifers act as an indicator of anthropogenic contamination, as it primarily enters the aquifer through leaching from nitrogenous fertilizers, herbicides, pesticides, agricultural activities, untreated industrial waste products, and leachate from landfills, septic systems, and farms (Reddy et al., 2009). These anthropogenic sources could add NO3 to the aquifer system, resulting from nitrification. The consumption of NO3 contaminated groundwater can cause hypertension and reduce blood cells’ oxygen-carrying capacity, ultimately leading to methemoglobinemia (blue baby syndrome) in newborn babies (Zhang et al., 2018). However, NO3 is not carcinogenic; it becomes so after binding with secondary and tertiary amines in the gastrointestinal tract (Dan-Hassan et al., 2012).

Regarding arid and semi-arid climatic regions such as Rajasthan, Coyte et al. (2019) highlighted elevated concentrations of these contaminants amid prevailing adverse climatic conditions and water scarcity resulting from over-extraction. This study mainly focused on the occurrence, hydrogeochemistry, geogenic and anthropogenic contaminants and associated health risks. However, studies published by Mittal et al. (2017), Pandit et al. (2022), Rani et al. (2023), and Menaria et al. (2023) have emphasized health risks associated with U in various parts of Rajasthan. Still, the status of the synergistic health impact of tri-contaminants on the different age-groups persists as a gap and remains unclear. The lack of such studies encourages further research on groundwater contamination and its carcinogenic and non-carcinogenic effects, as well as radio-sensitive threats to various age-groups in groundwater-vulnerable regions. The current study focuses on F, U, and NO3 as key contaminants due to their co-occurrence in similar hydrogeological conditions, such as alkaline and oxidizing groundwater, through processes like rock-water interaction, leaching, and evaporation (Post et al., 2017). Moreover, drinking water guidelines overlook their combined risks, focusing on individual contaminants despite evidence of increased toxicity from co-occurring contaminants.

Therefore, the current study uses an integrated approach to investigate F, U, and NO3 status in groundwater, controlling processes, and associated health risks in different age-groups using the Monte Carlo simulation. An extensive health survey was also conducted to understand health impacts. Hence, this study provides valuable insights into the occurrence of contaminants, their geochemical controls, and potential health impacts. The current study stands out for its distinctive focus on a diverse population residing in both underdeveloped rural areas and well-developed urban regions, encompassing various economic backgrounds. The population’s active involvement in groundwater-dependent activities, such as extensive irrigation and industrial work, adds a unique dimension to the research. Moreover, the Central Ground Water Board in India (CGWB, 2023) classifies this region as critical for groundwater extraction, highlighting an urgent need for innovative studies. By employing a novel approach, this research aims to assess the contamination and potential impacts on the population within the context of their prevailing environmental conditions, offering fresh insights into risk assessment.

Section snippets

Materials and methods

The methodology framework for groundwater contamination and health risk assessment is illustrated in Fig. S1. This section further elaborates on areas of interest, groundwater quality evaluation, accuracy assessment of analytical data, groundwater contamination, and age-dependent health risk calculations, including uncertainty analysis and health survey.

Chemical characteristics of groundwater

To comprehend the changes in groundwater quality, it is essential to elucidate the chemical composition of groundwater. Table 2 illustrates the statistics of groundwater physico-chemical parameters. The pH ranged between 6.68 and 8.50, averaging 7.40, indicating slightly alkaline groundwater. The mean TDS and total hardness were 1965.38 ppm and 417.87 ppm, respectively, indicating poor groundwater quality. Moreover, Cl, Br, Na+, K+, Ca2+, Mg2+, and salinity parameters statistics describe the

Conclusion

The current study presented a combined approach for a comprehensive understanding of groundwater quality and health risks associated with geogenic (F and U) and anthropogenic (NO3) contaminants. This study revealed F prevalence in the groundwater of the central part, whereas NO3 and U were prominent in the western part of the Jaipur district, extending into the western and central parts of the prevailing Alluvium aquifer. GPI scores confirmed F and NO3 as potential contaminants, and

CRediT authorship contribution statement

Vipin Garg: Writing – original draft, Visualization, Software, Investigation, Formal analysis. Rajesh Kumar: Writing – review & editing, Supervision, Resources. Chander Kumar Singh: Writing – review & editing, Validation, Resources. Alok Kumar: Writing – review & editing, Validation, Supervision, Methodology, Funding acquisition, Conceptualization.

Declaration of competing interest

The authors declare the following financial interests/personal relationships which may be considered as potential competing interests: Alok Kumar reports financial support was provided by Institution of Eminence, University of Delhi. If there are other authors, they declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgements

The authors would like to thank the Department of Environmental Science, School of Earth Sciences, Central University of Rajasthan (CURaj), Kishangarh, India, for providing the necessary facilities for groundwater sample collection, storage and analysis. The author would also like to thank the Department of Natural and Applied Sciences, TERI School of Advanced Studies, New Delhi, India, for providing laboratory facilities for radioactive element Uranium analysis. The corresponding author would

References (141)

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