uranium estimation in drinking water samples from ...

Radiation Protection Dosimetry Advance Access published April 25, 2013 Radiation Protection Dosimetry (2013), pp. 1–6

doi:10.1093/rpd/nct112

NOTE

URANIUM ESTIMATION IN DRINKING WATER SAMPLES FROM SOME AREAS OF PUNJAB AND HIMACHAL PRADESH, INDIA USING ICP-MS Asha Rani1,*, Surinder Singh2, Vikas Duggal3 and V. Balaram4 1 Department of Applied Sciences, Ferozpur College of Engineering and Technology, Ferozshah, Ferozpur, Punjab 142052, India 2 Department of Physics, Guru Nanak Dev University, Amritsar, Punjab 143005, India 3 Department of Applied Sciences, Punjab Technical University, Jalandhar, Punjab 144001, India 4 Geochemistry Division, National Geophysical Research Institute (Council of Scientific and Industrial Research), Uppal Road, Hyderabad 500 007, India *Corresponding author: [email protected]

The uranium concentration in drinking water samples collected from areas of Punjab and Himachal Pradesh has been measured using inductively coupled plasma mass spectrometry. The sources of water comprise hand pumps and tube wells. The uranium concentration lies in the range of 1.24–45.42 mg l21 with a mean value of 14.91 mg l21 in drinking water samples from Punjab and 0.56– 10.11 mg l21 with a mean value of 2.17 mg l21 in Himachal Pradesh. The measured uranium content in 4 % water samples from Punjab has been found to be higher than the limit of 30 mg l21 recommended by the World Health Organization (WHO) and US Environmental Protection Agency. However, the uranium concentration in all the water samples from Himachal Pradesh is well below the recommended limit. The annual effective dose associated with drinking water due to uranium concentration is estimated from its annual intake using dosimetric information based on International Commission on Radiological Protection 72. The resulting value of the annual effective dose from drinking water sources is in the range of 0.33– 37.78 mSv, which is well within the limit of 100 mSv recommended by the WHO.

INTRODUCTION Uranium occurs in a dispersed state in the Earth’s crust. Uranium salt is the most soluble of the longlived radionuclides and forms ions with oxidation states of þ4 (UO2 and U4þ) and þ6 (UO3 and (1) UO2þ 2 ) . Uranium present in the Earth is transferred to water, plants, food supplements and then to human beings. Uranium nuclides emit alpha rays of high ionisation power and therefore it may be hazardous if inhaled or ingested in higher quantity. According to an estimate food contributes 15 % of ingested uranium, while drinking water contributes 85 %(2). Adverse health effects from natural uranium can be due to its radioactive and chemical properties. Radioactive effects are very small from natural uranium; chemically it can be harmful to the kidneys from large exposure(3). The need of estimation of uranium concentration in water is multifold: it is an important fuel for nuclear power reactors, the hydrogeochemical prospecting for uranium is essential and the assessment of risk of health hazards due to high concentration of uranium in water is most important. Water sources having uranium concentration above few micrograms per litre are not safe for drinking purposes. Uranium prospecting through the analysis of soil, rocks, plants and water has been reported by

many workers(4, 5). Many surveys have been carried out in India for determining uranium content in water(6 – 12). In the present investigations, uranium concentration in drinking water collected from some areas of Punjab and Himachal Pradesh has been measured using inductively coupled plasma mass spectrometry (ICP-MS). The resident of these areas use these water sources for drinking and other domestic purposes. The main purpose of the study is to measure the level of uranium in drinking water samples from the health hazard point of view. GEOLOGY OF STUDY AREA Figure 1 shows the geographical location of the states of the Punjab and Himachal Pradesh on the map of India, as well as the location of the sampling sites. The geographical location of the study area in Punjab (Amritsar to Pathankot) is between latitude 31.37 and 32.17N and between longitude 74.55 and 75.42E. Punjab sediments are derived from Shivalik Himalayas and occur in the form of alluvium. The study area in Himachal Pradesh lies between 32.05 and 32.18 N latitude and between 75.56 and 76.18 longitudes. The area is characterised by the occurrence

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Received February 1 2013, revised April 2 2013, accepted April 4 2013

A. RANI ET AL. Table 1. Instrumental and data acquisition parameters of ICP mass spectrometer.

1100 W 0.86 l min21 1.20 l min21 15 l min21 5.00 0.80 ml min21 Quantitative mode

Measuring mode Point per peak Number of sweeps Dwell time (ms) Integration time (ms) Replicates Internal standard

Peak hopping 1 50 50 2500 3 103 Rha

a

Figure 1. Map of Punjab and Himachal Pradesh showing sample locations.

of follows: Dhauladhar granites, Chil formation, Dharamshala traps, Dharamkot limestone, Sabathus, Dharamshala Group and Shivalik Group. The individual formation and groups are separated from one another by longitudinal thrust systems; significant among them are the Main Boundary Thrust, Chail Thrust and the Drini Thrust, apart from these tectonic planes, the rock units are crosscut by transverse faults/lineaments trending NE–SW. In the southern extremity and parallel to the lesser Himalayas is the Shivalik Group of rocks, which are succeeded by vast stretch of Quaternary alluvium of the state of Punjab. The aim of present investigations is to see the trend in variation of uranium concentration in drinking water as one moves from Punjab to Himachal Pradesh and also to see the uranium concentration near the MBF areas in Himachal Pradesh. EXPERIMENTALTECHNIQUES Uranium concentration in drinking water samples was determined using ICP-MS. The water samples were collected from the hand pumps and tube wells. The residents of these areas use these water sources for drinking and other domestic purposes. The hand pumps from where the sample collection was done were in proper working condition. The system was pumped for at least 10 min before the sample was taken. New polyethylene sample bottles were washed out with filtered water to be sampled. The sampled water was acidified immediately with nitric acid, and uranium analyses were carried out in the Geochemistry Division ICP-MS Laboratory, National

Semiquantitative mode Peak hopping 1 6 50 300 3 —

At an overall concentration of 20 ng ml21.

Geophysical Research Institute (NGRI), Hyderabad, India. Calibration was performed using NIST 1640 (National Institute of Standards and Technology, USA), which is a reference material for trace elements in a natural water, to minimise matrix and other associated interference effects and to check the precision and accuracy of the analysis. The analytical procedure utilised is described in detail by Balaram et al.(13). The precisions achieved were ,5 % relative standard deviation with comparable levels of accuracy; in most cases suggesting that the data obtained by ICP-MS are best suited for high-precision geochemical studies. Instrumental and data acquisition parameters of ICPMS are summarised in Table 1.

RESULTS AND DISCUSSION A total of 45 drinking water samples collected from areas of Punjab and Himachal Pradesh have been analysed for uranium concentration using ICP-MS. The data for uranium concentration (mg l21), corresponding activity concentration (Bq l21), annual effective dose (mSv y21), cumulative dose (mSv) and lifetime stochastic cancer risk to the exposed populations of these areas are summarised in Table 2. The values in samples from Amritsar district of Punjab ranges from 6.87 mg l21 (Ram Tirath) to 45.42 mg l21 (Bauli) with an average value of 26.09 mg l21, for Gurdaspur district these values ranges from 1.24 mg l21 (Pathankot) to 24.30 mg l21 (Batala) with an average value of 7.46 mg l21. The values in samples from Kangra district of Himachal Pradesh ranges from 0.98 mg l21 (Nagri) to 6.14 mg l21 (Nurpur) with an average value of 2.29 mg l21, for Mandi

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Instrumental parameters RF power Nebuliser Auxiliary Plasma Lens voltage Sample uptake rate Data acquisition parameters

URANIUM ESTIMATION IN PUNJAB AND HIMACHAL PRADESH Table 2. Uranium concentration in drinking water samples from some areas of Punjab and Himachal Pradesh using ICP-MS Sample no.

Sample location

Uranium activity concentration (Bq l21)

Annual effective dose (mSv y21)

Cumulative dose (mSv)

Lifetime stochastic health effect 1026

45.31 20.41 45.42 19.86 6.87 18.69 26.09

1.14 0.52 1.15 0.50 0.17 0.47 0.66

37.45 17.08 37.78 16.42 5.58 15.44 21.62

2621.5 1195.6 2644.6 1149.4 390.6 1080.8 1513.7

2.73 1.25 2.76 1.20 0.41 1.13 1.58

24.30 1.52

0.61 0.04

20.04 1.31

1402.8 91.7

1.46 0.10

1.93 12.39 13.55 1.31 8.42 2.46 1.24 7.46

0.05 0.31 0.34 0.03 0.21 0.06 0.03 0.19

1.64 10.18 11.17 0.99 6.90 1.97 0.99 6.13

114.8 712.6 781.9 69.3 483 137.9 69.3 429.3

0.12 0.74 0.81 0.07 0.50 0.14 0.07 0.45

6.14 1.34 1.34 5.65 1.25 0.98 1.21 1.44 1.23 2.29

0.15 0.03 0.03 0.14 0.03 0.02 0.03 0.04 0.03 0.06

4.93 0.99 0.99 4.60 0.99 0.66 0.99 1.31 0.99 1.83

345.1 69.3 69.3 322 69.3 46.2 69.3 91.7 69.3 127.9

0.36 0.07 0.07 0.34 0.07 0.05 0.07 0.10 0.07 0.13

1.47 1.29 1.79 5.65 0.64 2.17

0.04 0.03 0.04 0.14 0.02 0.05

1.31 0.99 1.31 4.60 0.66 1.77

91.7 69.3 91.7 322 46.2 124.2

0.10 0.07 0.10 0.34 0.05 0.13

2.15 2.36 1.01 2.63 2.08 1.33 0.56 0.97 1.34 1.60

0.05 0.06 0.02 0.07 0.05 0.03 0.01 0.02 0.03 0.04

1.64 1.97 0.66 2.30 1.64 0.99 0.33 0.66 0.99 1.24

114.8 137.9 46.2 161 114.8 69.3 23.1 46.2 69.3 87

0.12 0.14 0.05 0.17 0.12 0.07 0.02 0.05 0.07 0.09

1.69 0.71 0.61 1.51

0.04 0.01 0.01 0.04

1.31 0.33 0.33 1.31

91.7 23.1 23.1 91.7

0.10 0.02 0.02 0.10 Continued

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Punjab District Amritsar 1 Chogawan 2 Wadala 3 Bauli 4 Sewa Nagar 5 Ram Tirath 6 G.N.D.U Average District Gurdaspur 7 Batala 8 Adda Dalam Nangal 9 Shikar Machiyan 10 Kalanaur 11 Bhikhariwal 12 Dhariwal 13 Gurdaspur 14 Dinanagar 15 Pathankot Average Himachal Pradesh District Kangra 16 Nurpur 17 Kotla 18 Shahpur 19 Gaggal 20 Dharamkot 21 Nagri 22 Nagrota 23 Kangra 24 Bandla mata Average District Mandi 25 Darg 26 Joginder Nagar 27 Pandoh 28 Hanogi Mata 29 Aut Average District Kullu 30 Bhuntar 31 Sarsarhi 32 Manikaran 33 Tattapani 34 Namhol 35 Jari 36 Durgaghaat 37 Vasisht 38 Shaat Average District Shimla 39 Shimla 40 Varmanha 41 Bhararhi Ghaat 42 Dadla Ghat

Uranium concentration (mg l21)

A. RANI ET AL. Table 2. Continued Sample no.

Sample location

43 Panahatti 44 Ghanahatti 45 Kethlighaat Average

Uranium concentration (mg l21)

Uranium activity concentration (Bq l21)

Annual effective dose (mSv y21)

Cumulative dose (mSv)

Lifetime stochastic health effect 1026

10.11 3.58 0.95 2.74

0.26 0.09 0.02 0.07

8.54 2.96 0.66 2.21

597.8 207.2 46.2 154.4

0.62 0.22 0.05 0.16

D ¼ AF where D is the annual effective dose (mSv y21); A the activity concentration of uranium (Bq l21); F the effective dose per unit intake via ingestion (4.51025 mSv Bq21). The annual effective dose from the collected drinking water samples is found to vary from 0.33 to 37.78 mSv, which is well within the recommended limit of 0.1 mSv y21(17). The cumulative dose calculated from these water samples has been found to vary from 69.3 to 2644.6 mSv in Punjab and from 23.1 to 597.8 mSv in Himachal Pradesh. The

corresponding excess cancer risk is found to vary from 0.07 to 2.761026 in Punjab and from 0.02 to 0.621026 in Himachal Pradesh, which is quite less than 1025, and is calculated by multiplying the risk factor of 7.31022 per Sv with a reference dose level (RDL) equal to 0.1 mSv annual exposure via drinking water(17). The values of the uranium concentration in drinking water samples obtained in the present investigations in the study areas are also compared with those available in the literature worldwide. The uranium concentration in water samples in south Greenland lies in the range of 0.5–1.0 mg l21 as reported by Brown et al.(19). The average values of uranium in drinking ground water were found to be 3 mg l21(2) with ranges of 0.015–973 mg l21 in domestic supplies in the USA(20). Kumru(21) has reported uranium concentration in water samples from Turkey in the range of 0.24–17.65 mg l21. Bansal et al.(22, 23) have reported uranium concentration in range of 0.67 to 471.27 mg l21 in the Aligarh (in Uttar Pradesh state of India) tube well water and the domestic Indian water supplies. Mehra et al.(9) has reported uranium concentration in water samples from Malwa region of Punjab, India in the range of 5.41–43.39 mg l21. Kansal et al. (24) has reported uranium concentration in water samples from Western Haryana, India in the range of 6.37–43.31 mg l21. The uranium concentration in water samples in Kulu area of Himachal Pradesh lies in the range from 0.26 to 2.56 mg l21 as reported by Singh et al.(25). Rani et al.(7) has reported uranium concentration in water samples from some areas of Punjab and Himachal Pradesh, India in the range of 1.39–98.25 mg l21. Avery wide range of uranium concentration of 0.04–1400 mg l21 in drinking water supplies in Jordon has been reported by Gedeon et al.(26) and Smith et al.(27). The uranium values obtained in the water samples in the present investigations lie in the range reported by other investigators. CONCLUSION The range of uranium in the water samples from Punjab varies from 1.24 to 45.42 mg l21 with an

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district these values ranges from 0.64 mg l21 (Aut) to 5.65 mg l21 (Hanogi Mata) with an average value of 2.17 mg l21, for Kullu district these values ranges from 0.56 mg l21 (Durgaghaat) to 2.63 mg l21 (Tattapani) with an average value of 1.60 mg l21 and the values for Shimla district ranges from 0.61 mg l21 (Bhararhi Ghaat) to 10.11 mg l21 (Panahatti) with an average value of 2.74 mg l21. The uranium concentration lies in the range of 1.24–45.42 mg l21 with a mean value of 14.91 mg l21 in drinking water samples from Punjab and 0.56–10.11 mg l21 with a mean value of 2.17 mg l21 in Himachal Pradesh. The measured uranium content in 4 % water samples from Punjab has been found to be higher than the recommended limit of 30 mg l21(14, 15) and thus was not suitable for drinking purposes. However, the uranium concentration in all the water samples from Himachal Pradesh is well below the recommended limit of 30 mg l21. The uranium activity concentration was calculated by using the unit conversion factor (0.02528 Bq l21 ¼1 mg l21 uranium). The calculations for dose rate, cumulative dose and average life time fatality risk are made by using the conversion factors given by ICRP 72(16) and WHO(17) for public exposed to natural uranium. The cumulative dose has been calculated for an average life of 70 y and cancer risk has been predicted by using risk factor of 7.31022 per Sv(17, 18). The annual effective dose value from drinking water samples due to ingestion of the uranium concentration in 2 l of water for the age group .17 y are calculated using the following equation:

URANIUM ESTIMATION IN PUNJAB AND HIMACHAL PRADESH

average value of 14.91 mg l21. The measured uranium content in 4 % water samples from Punjab has been found to be higher than the recommended limit of 30 mg l21(14, 15). However, the uranium concentration in all the water samples from Himachal Pradesh is well below the recommended limit of 30 mg l21. The annual effective dose from drinking water samples of these areas is in the range of 0.33–37.78 mSv, which is safe from the health hazard point of view.

12.

13.

14.

The authors are thankful to the residents of the study area for their cooperation during the fieldwork, and Department of Physics, Guru Nanak Dev University (GNDU), Amritsar and National Geophysical Research Institute (NGRI), Hyderabad for providing experimental facilities.

15.

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