J Radioanal Nucl Chem (2013) 295:357–367 DOI 10.1007/s10967-012-2090-6

Occurrence of uranium in groundwater of a shallow granitic aquifer and its suitability for domestic use in southern India K. Brindha • L. Elango

Received: 19 March 2012 / Published online: 28 September 2012 Ó Akade´miai Kiado´, Budapest, Hungary 2012

Abstract Groundwater used for domestic purpose without proper treatment should be free from chemical and biological contaminants. This study was carried out to assess the groundwater quality with respect to uranium in a part of Nalgonda district, Andhra Pradesh, India. Groundwater was regularly monitored for uranium concentration by collection of samples once every two months from March 2008 to November 2009 from 44 wells. The concentration of uranium in groundwater ranged from 0.2 to 118.4 ppb. Groundwater is unsuitable for domestic use in 2 % of this area based on the limit of 60 ppb prescribed by the Atomic Energy Regulatory Board of India. However, due the wide variation in limit suggested by different organizations and countries, the no-observed-adverseeffect level and lowest-observed-adverse-effect level (in mg/kg day) was used to understand the dosage of uranium that reaches the people through drinking water pathway. This level varied from 0 to 0.02 mg/kg day and 0 to 0.08 mg/kg day based on an uncertainty factor of 10 and 50 respectively for the mean uranium concentration in groundwater in each well. With an uncertainty factor of 50, 5 groundwater samples had uranium above 0.06 mg/kg day which is the lowest-observed-adverse-effect level. This study showed that with the presence of present level of uranium concentration in groundwater of this area there is no major threat to humans through the drinking water pathway.

K. Brindha  L. Elango (&) Department of Geology, Anna University, Chennai 600 025, India e-mail: [email protected]; [email protected] K. Brindha e-mail: [email protected]

Keywords Geology  Granitic rock  Drinking water  Uranium standard  NOAEL  LOAEL  Nalgonda  India

Introduction Naturally groundwater consists of major ions, minor ions, trace metals, heavy metals, radionuclides, organic matter etc. It is often used for drinking and domestic purposes apart from agricultural and industrial purposes due to its wide distribution and as it is comparatively less polluted than surface water. The groundwater quality needs to be monitored regularly so as to check that its composition do not exceed the limits of drinking water quality standards. Assessment of groundwater quality for different uses based on these standards has been carried out in several parts of the world [1–5]. India is one among several developing countries where treated piped water supply is not available throughout the day and hence the people depend on using groundwater for their basic needs without treatment from private wells. It is therefore important to monitor the groundwater quality in such areas regularly to advice the community to exercise proper caution while using the groundwater for different domestic purposes. The groundwater quality in these areas may be controlled by several factors. Geochemical processes and geology of an area control the groundwater quality [6–8]. The geology in an area play a significant role especially in an ore mineralised region. The present study was carried out in a part of Nalgonda district, Andhra Pradesh, southern India (Fig. 1) where unconformity related uranium deposits have been reported [9]. Uranium is a radionuclide present in minute quantity in groundwater naturally which has been studied by several researchers [10–12]. In this area uranium is abundant in the

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granitic rocks as reported by Shrivastava et al. [13]. Singh et al. [14] reported the range of uranium concentration from 0.5 to 410 ppb in groundwater in Palnadu sub-basin which is located adjacent to the present study area having a similar geological setup. Previous studies have been carried out in this area on groundwater quality based on EC (electrical conductivity), fluoride, bromide and nitrate [15–18]. The impact on the groundwater environment due to the transport of uranium and other radionuclides from the proposed tailings pond in this area was studied by Elango et al. [19]. Brindha et al. [20] reported that the concentration of uranium was relatively higher than the USEPA drinking water limit of 30 ppb [21] in three areas based on the sampling carried out in this area for six times during March 2008 to January 2009. The present study was a continuation of this work carried out by the collection and analysis of groundwater samples until the end of the year 2009. As the uranium concentration in groundwater varies dynamically with respect to space and time, it is important to consider this variation over a longer period of time for classifying this region with suitable or unsuitable groundwater quality. This aspect is essential when management measures are to be planned and implemented. Thus this study was carried out with an aim of assessing the groundwater quality with respect to uranium based on two year regular monitoring in a part of Nalgonda district, Andhra Pradesh.

Fig. 1 Location of study area

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Description of study site The study area is located in Nalgonda district at a distance of about 80 km from Hyderabad in the state of Andhra Pradesh in India (Fig. 1). Arid to semi-arid climate prevails in this area, with hot climate during April-June with a temperature ranging from 30 °C to 46.5 °C and in November–January the temperature is varying between 16 °C and 29 °C. Average annual rainfall in this area is about 600 mm which occurs usually during the southwest monsoon (June–September). The study area was demarcated as far as possible with well-defined hydrological boundary covering an area of about 724 km2 (Fig. 2a). Gudipalli Vagu and Pedda Vagu are two rivers that form the northern and southern boundaries of the study area respectively. These two rivers are seasonal and they flow for a few days during the southwest monsoon period of June–September. Nagarjuna Sagar reservoir is located at the southeastern side of the study area. The forest cover in this area is thin to moderate. Most of the study area comprises of agricultural land (Fig. 2b). Paddy is the principle crop grown in this area while other crops include sweet lime, castor, cotton, grams and groundnut. Drip irrigation is practiced in this area especially for growing sweet lime. Most of this study area has an undulating topography with a minimum elevation of 150 m msl (Fig. 2c). In general, the ground surface slopes towards southeast direction with intermittent hillocks with height ranging

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Fig. 2 a Drainage with monitoring wells, b land use, c topography, and d geology of the study area

from 250 to 300 m. The rainfall, topography and nature of formation have lead to dentritic to subdentritic drainage pattern in this area (Fig. 2a). Trellis type drainage pattern is also seen. Numerous small reservoirs are present in the depressed parts of the undulating topography of the study area. There are also wide lined canal networks catering for irrigation purposes. Geologically this region is largely comprised of granite/ granitic gneisss, pink biotite granite, grey hornblende biotite gneiss, migmatite granite and metabasalt belonging to late Archean (Fig. 2d). These rocks are generally medium to coarse grained. Most part of the investigated area has exposures of granitic rocks belonging to late Archaen. The granitic rocks are characterised by criss crossing joints and they are the most commonly observed structural feature in the area. The Srisailam formation, the youngest member of the Cuddapah supergroup overlies the basement granite with a distinct unconformity. This Srisailam formation is exposed in the southeastern part of the study area. The Srisailam formation are mainly arenaceous and include pebbly–gritty quartzite shale with dolomitic limestone, intercalated sequence of shale–quartzite and massive quartzite. The litho units of this formation are dipping at an angle ranging from

38 to 58 towards SE. In the early 1990s uranium mineralisation was located in the unconformity of this area between Srisailam formation of Cuddapah supergroup and the basement granites [22].

Materials and methods Data collection To prepare the base map and drainage map of the study area, toposheet nos. 56 L/13 SE, 56 L/13/SW, 56 P/1/SW, 56 P/1/SE, 56 L/14/NW, 56 L/14/NE, 56 P/2/NW, 56 P/2/ NE, 56 P/6/NW, 56 P/2/SW, 56 P/2/SE, 56 P/5/SW and 56 P/6/SW (scale-1:25,000) covering the study area was obtained from Survey of India, Hyderabad, Andhra Pradesh, India. The Shuttle Radar Topography Mission (SRTM) data was used to prepare the topographic map of the study area. The geological map (scale-1:50,000) was acquired from Geological Survey of India (GSI) [23], Hyderabad, and this was modified based on field investigations.

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Fig. 3 Uranium concentration (ppb) in groundwater of different locations

Groundwater sampling and analysis An intensive field survey was carried out and nearly 240 wells were studied for choosing appropriate sampling wells for periodical monitoring of uranium concentration. Based on the EC a representative well approximately at a distance of 5 km each was chosen. Forty-four wells were thus selected for periodical monitoring which is shown in Fig. 2a. Groundwater samples were collected from these wells from March 2008 to November 2009, once every 2 months. The sampling bottles of 500 ml capacity were cleaned prior to sampling by soaking them in 1:1 diluted HNO3 for 24 h and they were washed thoroughly with distilled water. Further, these bottles were washed again before each sampling at least two times with the filtrates of the sample. The uranium concentration in these

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groundwater samples was determined using laser fluorimeter which has a detection limit of 0.1 ppb [24, 25]. All the analytical reagents used were procured from Merck. Blanks and standards were run intermittently during the measurement for ensuring accuracy of the result. For every ten samples, three samples were run in triplicates by varying the concentration of the standard and a calibration curve was obtained to cross check the accuracy of the instrument and to avoid handling errors.

Software used Groundwater quality maps based on uranium were plotted out using Arc GIS 9.3. This software was also used for the preparation of topography, drainage, geology and land use maps.

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Fig. 4 Variation in uranium concentration (ppb) from March 2008 to November 2009 along with the maximum permissible limits

Fig. 5 Temporal variation in uranium concentration (ppb) in groundwater of few wells

Results and discussion It is essential to study the groundwater quality of areas where ores of any mineral occur as there are chances that the groundwater may be enriched by that mineral due to natural processes. Taking account of this the uranium concentration in groundwater of this uranium mineralised area is studied. No other studies carried out from this area have reported adverse-effect of major ions on groundwater quality except for the spatial and temporal variation in the concentration of EC, fluoride, bromide and nitrate [15–18].

Several studies have also reported uranium occurrence in groundwater and surface water around the world based on one time sampling and hence they did not take into account the temporal variation. A total of 446 groundwater samples were collected and analysed in this study based on which the interpretation has been made. Variation in uranium concentration Uranium concentration in groundwater of the study area varies significantly with respect to space and time. The

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Table 1 Uranium content in granite rocks Rock type

Location

Uranium concentration (ppm)

Reference

Quartz monzonite and granite

South California

5.2–5.3

[26]

Idaho

2.2–6.3

Sierra Nevada

2.3–7.2

Granite

Alaska

5.6–35.4

[27]

Mica granite

Egypt

20.3 average

[28]

Hornblende biotite granite Granite Granite

4.9 average Shingbhum, India

4.75 average

[29]

Shingbhum, India

7 average

[30]

concentration of uranium in groundwater samples collected from various wells for September 2008 and September 2009 are shown in Fig. 3. Uranium concentration in groundwater ranged from 0.2 to 118.4 ppb with an average of 18.5 ppb in the study area and the range varied with time (Fig. 4). The temporal variation in uranium concentration is in the order of magnitude of 2 to 10. As an example the temporal variation in a few wells are shown in Fig. 5. The concentration of uranium in groundwater greatly depends on the composition of the rocks in the aquifer. The concentration of uranium in granitic rocks has been studied widely by several researchers (Table 1) which is up to 35.4 ppm [26–30]. The granitic rocks which occur in most of the study area contain uranium in the range of 10.2–116 ppm with an average of 35 ppm and thorium between 25.5 and 60.7 ppm with an average of 50 ppm [13]. Interaction between the uranium rich weathered granitic rocks or top soil and groundwater has resulted in increase Fig. 6 Uranium concentration in groundwater under different rock types

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in uranium concentration in groundwater of this study area. Based on the rock type the sampling wells were divided to understand its relationship with uranium (Fig. 6). Uranium concentration was higher in wells located in granitic gneiss, followed by migmatite granite and pink biotite granite respectively. This shows that granitic rocks contribute significantly to uranium concentration in groundwater of this area. Water quality based on uranium Continuous monitoring of uranium concentration in groundwater over a period of two years was used to assess the groundwater quality in this area. WHO [31] had recommended 15 ppb of uranium in drinking water as safe limit. USEPA [21] has put forth 30 ppb of uranium as the permissible limit. Though the Indian standards specification for drinking water [32] does not specify any maximum permissible limit for uranium, a maximum limit of 60 ppb as recommended by the Atomic Energy Regulatory Board (AERB), India [33]. Of the total 446 groundwater samples collected and analyzed, 2 % of the groundwater samples were above the AERB limit (Fig. 7). The number of groundwater samples exceeding this limit is also shown in Fig. 4. Based on USEPA limit, 22.5 % of the groundwater samples had uranium above the maximum permissible limit of 30 ppb (Fig. 7). The mean uranium concentration in different wells based on AERB limit and its suitability for drinking is shown in Fig. 8. Groundwater of these locations are suitable for domestic use such as cooking and drinking as it contains average uranium concentration below 60 ppb. Number of groundwater samples with various ranges of uranium concentration is shown in Fig. 9. Nearly 40 % of the groundwater samples had uranium concentration within 10 ppb. Even though the mean uranium concentration based on eleven bimonthly measurements is within the AERB limit of 60 ppb (Fig. 8) during certain times the

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uranium in the human body rather than assessing the suitability based on its absolute concentration.

NOAEL/LOAEL

Fig. 7 Percentage of groundwater samples with uranium concentration above various standards

concentration of uranium in groundwater exceeded the maximum limit of 60 ppb (Fig. 4). Hence it is important to assess its possible impact on humans who may consume this water. The maximum permissible limit of uranium in drinking water recommended by different countries and organisations are very different. As mentioned in the earlier section, the maximum permissible limit for uranium in drinking water as per WHO is 15 ppb [31], USEPA is 30 ppb [21] and AERB is 60 ppb [33]. Hence delineation of wells into suitable and unsuitable based on these standards is not meaningful. Further, uranium is occurring in relatively high concentration in the rocks in India and hence the background level of concentration in groundwater is expected to be more. Hence, it will be better to compare the groundwater quality based on the toxicity caused by intake of groundwater containing

The toxicological effects of uranium on animals have been studied by various researchers. The no-observed-adverseeffect level (NOAEL) is the highest dose in a toxicity study that does not result in any observed adverse-effect (an adverse-effect significantly alters the health of the target animal for a sustained period of time or reduces survival) [34]. The lowest-observed-adverse-effect level (LOAEL) is the lowest dose in a toxicity study that results in an observed adverse-effect (usually one dosage level above the NOAEL) [34]. So classifying the groundwater of the study area on the basis of NOAEL or LOAEL will give us an insight into the level of contamination of groundwater by the natural geogenic sources. NOAEL/LOAEL is given as [35], C ¼

NOAEL=LOAEL  BW  RSC UF  DW

ð1Þ

where, C = a public health-protective concentration (C) for uranium in drinking water (mg/l); NOAEL/LOAEL = no-observed-adverse-effect-level/lowest-observedadverse-effect level (mg/kg day); BW = body weight of an adult human (kg); RSC = relative source contribution; UF = uncertainty factor; and DW = daily water consumption default for an adult (l/day). With the variations in drinking water standards of various countries and organisations like WHO, USEPA and AERB it

Fig. 8 Mean uranium concentration (ppb) in groundwater based on eleven times of sampling once in 2 months

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Fig. 9 Groundwater samples with uranium concentration in different ranges

Fig. 10 Range and mean LOAEL of uranium at different sampling locations

is not reasonable to estimate the suitability of water for drinking purposes. It is more meaningful to estimate the intake of natural uranium through drinking water and then comparing it with the NOAEL/LOAEL. The measured uranium concentration in groundwater of each sampling location was used and the NOAEL/LOAEL were calculated to determine its suitability for drinking purpose. This method

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will help in assessing the groundwater quality with respect to the chemical toxicity of uranium. So, NOAEL/LOAEL is calculated by, NOAEL=LOAEL ¼ ðDW  UF  CÞ=ðBW  RSCÞ

ð2Þ

The daily water consumption for an adult is 2 l/day and the average adult body weight is considered 70 kg for this

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Fig. 11 Variation in LOAEL with UF = 50 and 100 at sampling locations

purpose. Instead of C which helps to arrive at a public health-protective concentration (C) for uranium in drinking water, in this equation, C was substituted with the concentration of uranium in groundwater. For conservative estimates of the intakes, a UF of 10, 50 and 100 was used in the derivation. The NOAEL for natural uranium is estimated as 0.2 mg/ kg day for adult by California Environmental Protection Agency in 1997 [36]. But studies by Gilman in 1998 [37] has estimated the LOAEL based on toxicity in rats evidenced by a variety of kidney and liver histological lesions to be 0.06 mg/kg day [35]. Hence it is reasonable to

consider the LOAEL for comparison of uranium concentration in groundwater obtained from this study. The LOAEL with UF = 10 calculated for mean uranium concentration of each sampling location varied from 0 to 0.02 mg/kg day. As the LOAEL did not exceed the limit of 0.06 mg/kg day [35] with an UF of 10 at any of the sampling wells, the spatial variation based on this is not shown. The range and mean LOAEL of uranium at different sampling locations for UF = 50 and 100 is given in Fig. 10. Figure 11 shows the variation in LOAEL with UF = 50 and 100 at different sampling locations. The suitability of groundwater based on the LOAEL of 0.6 mg/

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Fig. 12 LOAEL calculated with mean uranium in groundwater and UF = 50 in sample locations

kg day and UF of 50 calculated for mean uranium concentration in each sampling location is given in Fig. 12. Of the 44 sampling wells, 5 wells had LOAEL above 0.06 mg/ kg day. Thus 11 % of the groundwater samples exceeded the LOAEL of uranium in groundwater of this study area with an uncertainty factor of 50. The LOAEL was also calculated for the overall mean uranium concentration in this study area of 18.5 ppb (based on 446 groundwater samples) with UF = 10, 50 and 100. The level varied from 0.005 (UF = 10); 0.03 (UF = 50) and 0.05 (UF = 100). Hence, in general considering the average uranium concentration in groundwater even with an UF of 100, there is no major threat due to consumption to the people of this area.

With an UF of 50, 11 % of the groundwater samples were above the LOAEL of 0.06 mg/kg day. Thus this study helped to understand the groundwater suitability based on uranium in a region where groundwater is used for drinking and domestic purposes. Acknowledgments The authors would like to acknowledge the Board of Research in Nuclear Sciences, Department of Atomic Energy, Government of India for funding this work (Grant no. 2007/36/35). Authors also like to thank the Department of Science and Technology’s Funds for Improvement in Science and Technology scheme (Grant No. SR/FST/ESI-106/2010) and University Grants Commission’s Special Assistance Programme (Grant No. UGC DRS II F.550/10/DRS/2007(SAP-1)) for their support in creating laboratory facilities, which helped in carrying out part of this work. The authors also thank the anonymous reviewer for the critical and valuable comments that helped in significantly improving the manuscript.

Conclusion References Periodical monitoring of uranium concentration in groundwater was carried out from March 2008 to November 2009 once every 2 months from 44 wells in a part of Nalgonda district, Andhra Pradesh, India. The uranium concentration varied from 0.2 to 118.4 ppb with a mean of 18.5 ppb. The uranium concentration in groundwater of 446 groundwater samples analysed was compared with the maximum permissible limit of 60 ppb as put forth by AERB of India and was found that 2 % of groundwater samples were above this limit. The groundwater suitability was also determined based on the LOAEL using the mean concentration of uranium in each sampling well. Groundwater was suitable based on LOEAL with an UF of 10.

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