risk assessment due to ingestion of natural radionuclides and heavy metals in the milk samples: a...

Environ Monit Assess (2011) 175:157–166DOI 10.1007/s10661-010-1502-8

Risk assessment due to ingestion of natural radionuclidesand heavy metals in the milk samples: a case studyfrom a proposed uranium mining area, Jharkhand

Soma Giri · Gurdeep Singh · V. N. Jha ·R. M. Tripathi

Received: 19 November 2009 / Accepted: 6 May 2010 / Published online: 21 May 2010© Springer Science+Business Media B.V. 2010

Abstract Ingestion of radionuclides and heavymetals through drinking water and food intakerepresents one of the important pathways forlong-term health considerations. Milk and milkproducts are main constituents of the daily diet.Radionuclides and heavy metals can be appre-hended in the ecosystem of the East Singhbhumregion which is known for its viable grades ofuranium, copper and other minerals. For the riskassessment studies, samples of milk were collectedfrom twelve villages around Bagjata mining areaand analysed for U(nat), 226Ra, 230Th, 210Po, Fe,Mn, Zn, Pb, Cu and Ni. Analysis of the resultsof the study reveals that the geometric mean ofU(nat), 226Ra, 230Th and 210Po was 0.021, 0.24,0.23 and 1.08 Bq l−1, respectively. The ingestiondose was calculated to be 12.34 μSvY−1 whichis reflecting the natural background dose via the

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S. Giri (B) · G. SinghCentre of Mining Environment, Departmentof Environmental Science and Engineering,Indian School of Mines, Dhanbad, 826004, Indiae-mail: [email protected]

V. N. Jha · R. M. TripathiEnvironmental Assessment Division, Bhabha AtomicResearch Centre, Mumbai, 400085, India

route of ingestion, and much below the 1 mSvlimit set in the new ICRP recommendations. Theexcess lifetime cancer risk was estimated to be1.72 × 10−4 which is within the acceptable excessindividual lifetime cancer risk value of 1 × 10−4.The geometric mean of Fe, Mn, Zn, Cu and Ni was4.91, 0.29, 4.77, 0.56 and 0.48 mgl−1, respectively;whereas the daily intake was computed to be 0.44,0.03, 0.43, 0.05 and 0.04 mg/day, respectively. Pbwas not detected in any of the samples. The hazardquotient revealed that the intake of the heavymetals through the ingestion of milk does not poseany apparent threat to the local people as none ofthe HQ of the heavy metals exceeds the limit of 1.

Keywords Radionuclides · Heavy metals · Milk ·Risk assessment · Intake · Ingestion dose ·Excess lifetime cancer risk · Hazard quotient

Introduction

At the sites in the vicinity of the nuclear fuel cyclefacilities involved in mining, milling, ore separa-tion, purification, etc. there is enrichment of ra-dionuclides and trace metals which find their wayinto the food chains. In these areas, mining activityis a chief source of metals entering into the en-vironment. In the process of mining exploitationand ore concentrating, mine tailing and wastewa-ters are created and dust is emitted. This results in

158 Environ Monit Assess (2011) 175:157–166

the potentially severe pollution of the surroundingenvironment. Leaching of these elements frommines, leakage from dumps of radioactive wastematerial, elevate the levels of the radionuclidesand the heavy metals in the environment whichgets into the soil and thus in the vegetation and ul-timately to mankind (Khan et al. 1997). The heavymetals and the radionuclides enter the humanbody mainly by two routes namely: inhalation andingestion. The intake through ingestion dependson the food habits.

Ingestion of radionuclides through food intakeaccounts for a substantial part of average radi-ation doses to various organs of the body andalso represents one of the important pathways forlong-term health considerations. Human dietarycomposition varies from place to place and fromone individual to another. Natural radionuclidesentering the food chain are mostly derived fromthe soil and, as a result, variation in soil radionu-clide content is a prime source of geographicvariability. Plant uptake also varies from speciesto species; hence the intake of different foodproducts forms a secondary source of variability(McDonald et al. 1999; Fernandez et al. 2004;Hernandez et al. 2004).

Milk is an important vector of radionuclidesand heavy metals to man that may get into theenvironment from the mining activities. The pas-sage of radionuclides and heavy metals is throughthe soil-feed/grass-cow-milk chain (Licata et al.2004). Milk is one of the important food for hu-man nutrition and contains all the macronutrientsnamely protein, carbohydrates, fat, vitamins (A, Dand B groups) and trace elements particularly cal-cium, phosphate, magnesium, zinc and selenium(Abollino et al. 1998; Buldini et al. 2002). Also,milk and milk products are main constituents ofthe daily diet, especially for vulnerable groupssuch as infants, school age children and old age(Davies et al. 1986). As far as the fundamentalcomposition of cow’s milk is known, its elementalcomposition is generally unknown. It has beenreported that the content of the main mineralcomponents, such as Ca, P, K, Na, Mg, Cl, S, isnot diversified and undergoes only slight changesdepending on the lactation phase and the qualityof nutrition (Brzoska et al. 1996), in particularunder the influence of applied mineral additives

or environmental conditions, mainly chemical pol-lutants (Schroeder 2003).

Low-grade uranium deposits are found inSinghbhum region of Jharkhand. Following thediscovery, mining and processing of uraniumore has been started in several parts of easternSinghbhum (Jaduguda, Bhatin and Narwapahar).However, with increasing requirement of nuclearenergy, by 2020, new sites of mining has beenproposed to be excavated for uranium. One of theproposed new sites in Singhbhum is at Bagjata,which is an underground mine. The mining atBagjata may lead to affect the pre-existing envi-ronmental status of the area. In this connection,the present study was being carried out to gener-ate baseline data for dietary components of theBagjata uranium mining area. As a part of thisbaseline study, milk from the adjoining areas wereanalysed for their exposure to radionuclides andheavy metals content.

Materials and methods

Description of the study area

Located in Jharkhand, the Singhbhum Thrust Beltis E–W trending 160 km long belt known for Cu–apatite–magnetite and kyanite deposits. Studies ofmineral paragenesis indicate that mineralizationalong the thrust belt took place over a long period,the minerals being deposited in two stages, thefirst to form being apatite and magnetite, closelyfollowed by uranium mineralization and the sul-phides including chalcopyrites were the last to bedeposited. Uranium–copper mineralization coex-ists in the area, along with Fe, Mn, etc., howeverdepending upon the viability, Cu, U and otherminerals is mined and processed. The Bagjatamining area is situated in the Bhalki–Kanyalukadeposit (Bhola et al. 1964).

Bagjata Mining Area is situated at latitudeof 22◦26′07′′N to 22◦28′34′′N and longitude of86◦25′16′′E to 86◦31′29′′E in Dalbhum sub divisionof East Singhbhum district in Jharkhand State.It is an underground uranium mine. There areseveral small villages surrounding the mining site.The location detail of the study area is given in theFig. 1 and sampling points are depicted in Fig. 2.

Environ Monit Assess (2011) 175:157–166 159

Fig. 1 Location map of the study area

Sample collection

Locally rearing cow’s milk samples were collectedfrom twelve villages around the Bagjata miningarea during the month of September 2007. Fromeach village, five samples were collected, thus atotal of 60 samples were analysed. Samples werecollected and immediately after collection sam-ples were preserved in 37% formaldehyde (3 ml/l)(Douglas 1967).

Laboratory analysis

Collected samples was taken and subjected to wetdigestion by the method as described by Richards(1968). After removal of organic matter (mixtureof nitric acid and perchloric acid treatment), sam-

ples were leached repeatedly with 8 N HNO3,filtered and the volume was made up to 100 ml byadding re-distilled water. Aliquots were preservedfor the analysis of heavy metals and radionuclides.

The 210Po was analysed by electrochemicalexchange technique followed by alpha counting(Figgins 1961). Estimation of U(nat) was carriedout fluorimetrically (Kolthoff and Elving 1962)while 226Ra was estimated using radon emanationtechnique (Ragjavayya et al. 1980). Analysis of230Th was carried out by separating it throughanion exchange resin followed by alpha counting(Hyde 1960). Heavy metals were analysed usingan atomic absorption spectrophotometer (GBCAvanta). For analytical quality assurance; the re-sult of each metal was corrected by subtracting thevalue from the blank. Also, after every five sample


Fig. 2 Sampling locationsfor milk in Bagjatamining area

readings, standards were run to make sure thatthe obtained results were within range. A standardair–acetylene flame was used.

Analysis of the data

For each radionuclide and heavy metal, the dis-tribution of the combined data was verified bythe curve of accumulated frequency (Miller andMiller 1989). As usually observed in environmen-tal samples, the concentrations of the radionu-clides and heavy metals were better representedby the log-normal distribution, and the central

tendency thus is represented by the geometricaverage (Wayne 1990).

Risk from the intake of radionuclides throughingestion: excess lifetime cancer risk

The excess lifetime carcinogenic risk can be esti-mated by multiplying average daily dose (ADD)with slope factor (SF) and the duration of life(75.2 years). The slope factors are taken fromHealth Effect Assessment Summary Tables ofUnited States Environmental Protection Agency(US-EPA 1989). The sum of the risks from all


radionuclides and pathways yields the lifetime riskfrom the overall exposure irrespective of the bodypart. In general, the US-EPA considers excesscancer risks that are below about 1 chance in1,000,000 (1 × 10−6) to be so small as to be neg-ligible, and risks above 1 × 10−4 to be sufficientlylarge that some sort of remediation is desirable.Excess cancer risks that range between 1 × 10−6

and 1 × 10−4 are generally considered to be ac-ceptable (US-EPA 1991).

The basic equation for calculating excess indi-vidual lifetime cancer risk is:

Risk = ADD × SFo × 27448 days(75.2 years

)

where: Risk = a unitless probability of an indi-vidual developing cancer over a lifetime; ADD =average daily dose [mg/kg day; pCi], SFo = slopefactor, expressed in [(mg/kg day)−1; pCi/risk].

The risk is related to doses but since US-EPA-Integrated Risk Information System (IRIS) data-base has provided slope factors in unit activity/riskwhich is specific for each radionuclide, the sameprocedure is adopted for the assessment. Theslope factors are given in the units of pCi/risk sothe activities are converted from Bq to pCi. Theconversion factor used is 1 Bq = 27 pCi.

Risk from the intake of heavy metals throughingestion: hazard quotient

Risk of the chemical toxicant may be charac-terised using a hazard quotient (HQ). This is the

ratio of the average daily dose (ADD; milligramsper kilogram body weight per day) of a chemicalto a reference dose (RfD, milligrams per kilogramper day) defined as the maximum tolerable dailyintake of a specific metal that does not result inany deleterious health effects:

HQ = ADDRfD

.

If HQ > 1.00, then the ADD of a particularmetal exceeds the RfD, indicating that there is apotential risk associated with that metal.

Results and discussion

Radiochemical analysis of milk

The result of radiochemical analysis of the milksamples are presented in Table 1. The range ofU(nat), 226Ra, 230Th and 210Po in the milk sampleswere 0.015–0.033, 0.07–1.17, 0.1–0.51 and 0.48–2.94 Bq l−1, respectively. The geometric mean ac-tivity of U(nat), 226Ra, 230Th and 210Po was foundto be 0.021, 0.24, 0.23 and 1.08 Bq l−1. Of all theradionuclides analysed, the activity of 210Po wasfound to be maximum while the activity of U(nat)was the minimum. Among the radionuclides, theconcentration of 210Po is generally higher thanthe other radionuclides in the dietary components.This may be attributed to the derivation of the ra-dionuclide from soil and air. The secondary decayof 210Pb present in the soil may also be a reason

Table 1 Radiochemicalanalysis of milk ofBagjata mining area(values corresponding toeach village is average of5 samples)

Code no. Location Uranium Bq l−1 Radium Bq l−1 Thorium Bq l−1 Polonium Bq l−1

1 Latia 0.024 0.07 0.17 1.962 Bagjata 0.020 0.12 0.25 1.233 Bhaduya 0.017 0.16 0.27 0.744 Bakra 0.019 0.09 0.12 0.495 Phuljhari 0.020 0.09 0.10 0.486 Gohala 0.015 0.19 0.28 1.217 Mosabani 0.022 0.91 0.51 1.238 Badia 0.024 0.26 0.38 2.949 Nimdih 0.033 1.17 0.15 0.7410 Madantola 0.028 0.34 0.29 1.7211 Katsakra 0.019 0.45 0.35 1.0512 Khariasai 0.020 0.39 0.21 0.97

Geomean 0.021 0.24 0.23 1.08(n = 60)


of the high 210Po content in the plant foodstuffs(Moore et al. 1976; Shacklette et al. 1978; Kabata-Pendias 2001), which may in turn be transferred tothe milk.

The activity of the radionuclides was found tobe higher than the values reported for the stud-ies in radioactive and nonradioactive regions bydifferent researchers. The may be attributed tothe fact that the study area falls in the uraniummineralised zone of East Singhbhum. The average210Po activity of 10 mBq l−1 in milk was reportedby Kannan et al. (2001) from Kalpakkam. Val-ues of 15, 97, 180 and 400 mBq l−1 have beenreported from Bombay (Khandekar 1977), Brazil(Amaral et al. 1992), Portugal (Carvalho 1995)and Syria (Othman and Yassine 1995) for 210Po inmilk. The mean 226Ra concentration of 0.006 and0.028 Bq l−1 in the milk samples from Bombayand Kerala was suggested by Chhabra (1966). Inanother study in the vicinity of Brown coal mine,Tusnica, the value of 226Ra in the milk sampleswas reported as 0.04 ± 0.01 Bq l−1 (Saracevic et al.2009). In the same study, the value of uraniumwas found to be 0.014 ± 0.006 Bq l−1. Uraniumestimated in the milk samples of Sulesian regionwas reported to be 0.035 Bq l−1 (Dobrzañski et al.2005).

Heavy metal analysis of milk

The geometric mean concentration of Fe, Mn, Zn,Cu and Ni in the samples of milk was found to be4.91, 0.29, 4.77, 0.56 and 0.48 mgl−1, respectively

(Table 2). In all the samples, the concentrationof Pb was below detection limit (0.05 mgl−1).Secretion of Pb into milk is rare unless an acutedose is ingested, since there is an exponentialrelationship between Pb intake and output in milk(Oskarsson et al. 1992). The range of Fe, Mn, Zn,Cu and Ni in the milk samples were 0.2–13.2, 0.14–0.95, 1.66–7.13, 0.23–2.03 and 0.31–0.7 mgl−1, re-spectively. Table 3 gives reported concentrationrange of heavy metals in cow milk by variousresearchers. It can be seen from the table thatthe concentration of Zn was found to be morethan the other metals which is in accordance toother studies (Enb et al. 2009; Lante et al. 2004;Dobrzañski et al. 2005). Fe was found to be muchhigher as compared to other studies. The averageconcentration of other heavy metals in the milkis also higher as compared to other studies. Thismay be attributed to the mineralisation of thearea. The study area falls in the Singhbhum Thrustbelt which is rich in Fe, Cu, Ni and other metals(Sarangi and Singh 2006). The contamination ofpastures and the accumulation of toxic metalsin grazing animals can occur on soils that arenaturally rich in metals (Martin and Coughtrey1982). The passage of heavy metals is throughthe soil–feed/grass–cow–milk chain. So the highconcentration of the metals in the soil will leadto appearance in the milk in more quantities ascompared to the other locations.

The recorded limits of International Dairy Fed-eration (IDF 1979) were 0.37, 0.10, 0.025, 3.280.049 and 0.026 mg/kg milk for Fe, Cu, Mn, Zn,

Table 2 Heavy metalanalysis of milk ofBagjata mining area(values corresponding toeach village is average offive samples)

ND not detected

Code no. Location Fe mgl−1 Mn mgl−1 Zn mgl−1 Pb mgl−1 Cu mgl−1 Ni mgl−1

1 Latia 5.06 0.5 5.75 ND 0.29 0.632 Bagjata 4.0 0.39 5.53 ND 1.47 0.333 Bhaduya 9.56 0.14 5.42 ND 0.62 0.394 Bakra 3.55 0.59 7.13 ND 2.03 0.315 Phuljhari 5.31 0.22 7.11 ND 0.23 0.76 Gohala 3.76 0.17 6.08 ND 0.34 0.47 Musabani 1.13 0.19 1.66 ND 0.47 0.428 Badia 0.2 0.24 3.15 ND 0.49 0.519 Nimdih 1.08 0.29 2.18 ND 0.54 0.5910 Madantola 13.2 0.34 3.68 ND 0.47 0.4111 Katsakra 5.81 0.18 4.25 ND 0.68 0.6312 Khariasai 6.23 0.25 5.31 ND 0.59 0.47

Geomean 4.91 0.29 4.77 0.56 0.48(n = 60)


Table 3 Comparison of heavy metals (mgl−1) in cow milk samples with other studies

S. no Location Fe Mn Zn Pb Cu Ni Reference

1 Bombay City (India) 3.177 0.0017 0.043 Tripathi et al. (1999)2 Burundi (South Africa) 4.1 0.07 Benemariya et al. (1993)3 Düsseldorf City (Germany) 2.1 0.033 Jochum et al. (1995)4 Germany (market) 3.73 0.04 Ostapczuk et al. (1987)5 Turkey (market) 0.03 0.02 0.03 0.02 Aksu et al. (2004)6 Bangalore City (India) 0.33 1.83 Lokeshwari and

Chandrappa (2006)7 Egypt (animal farms) 0.572 0.047 2.828 0.131 Enb et al. (2009)8 Italy (Calabria animal farms) 0.29 0.029 4.631 0.005 0.052 Lante et al. (2004)9 Silesia (industrialised and 0.101 3.163 0.089 0.053 Dobrzañski et al. (2005)

coal mining area)10 Bagjata 4.91 0.29 4.77 ND 0.56 0.48 Present study

Pb and Cd, respectively and it can be seen that inthe present study all the metals are exceeding thelimits.

Ingestion dose of the radionuclides

In order to calculate the ingestion dose of these ra-dionuclides, per day consumption of 90 ml of milk(Dang et al. 1994) is used to calculate the intake.Ingestion dose of these radionuclides is evaluatedusing dose conversion factors of 0.045 μSv Bq−1

for uranium, 0.28 μSv Bq−1 for radium, 0.21 μSvBq−1 for thorium and 0.24 μSv Bq−1 for polo-nium (ICRP-68 1994) and annual geometric meanconcentrations of these radionuclides have beenconsidered in the present study (Table 4).

The intake of the radionuclides due to con-sumption of milk was calculated to be 51.61 BqY−1, with a contribution of 0.69, 7.88, 7.56 and35.48 Bq Y−1, from U(nat), 226Ra, 230Th and 210Po.The ingestion dose was estimated to be 0.03, 2.21,1.59 and 8.51 μSv Y−1, respectively. The totaldose was assessed to be 12.34 μSv Y−1which isreflecting the natural background dose via theroute of ingestion, which is much below the 1 mSv

Table 4 Ingestion dose of radionuclides through the intakeof milk

U(nat) 226Ra 230Th 210Po

Geomean (Bq kg−1) 0.021 0.24 0.23 1.08Intake (Bq Y−1) 0.69 7.88 7.56 35.48Ingestion dose (μSvY−1) 0.03 2.21 1.59 8.51Total dose 12.34

limit set in the new ICRP (2007) recommenda-tions. It is negligible compared to the global av-erage annual radiation dose of 2,400 μSv to manfrom the natural radiation sources as proposed byUNSCEAR (2000).

The data has been used for the excess lifetimecancer risk assessment by US-EPA method (US-EPA 1993). The excess lifetime cancer risk wasestimated to be 1.72 × 10−4 which is within theacceptable excess individual lifetime cancer riskvalue of 1 × 10−4 (Table 5).

Daily intake estimate of heavy metalsand hazard quotient

Taking into account per day consumption of 90 mlof milk (Dang et al. 1994), the daily intake ofFe, Mn, Zn, Cu and Ni is computed to be 0.44,0.03, 0.43, 0.05 and 0.04 mg per day, respectively(Table 6). The tolerable daily intake limits of Znand Cu recommended by the UNEP, FAO, WHO(1992) for adults are 33,000 and 6,500 μg day−1,respectively, and the metals do not cross the limits.

Table 5 Cancer risk due to intake of milk

Radionuclide SFo(Slope Intakeb Cancer riskfactor oral)a

U(nat) 8.66 × 10−11 0.05 1.21 × 10−7

226Ra 5.14 × 10−10 0.58 8.23 × 10−6

230Th 1.19 × 10−10 0.56 1.83 × 10−6

210Po 2.25 × 10−9 2.63 1.62 × 10−4

Total risk 1.72 × 10−4

aSFo in risk/pCibDaily intake in pCi


Table 6 Intake and hazard quotient of heavy metals due to ingestion of milk

Heavy metals RfDo (Reference Geometric Intakeb ADD (average HQ (hazardoral dose)a mean daily dose)c quotient)

Fe 7.0 × 10−1 4.91 0.44 0.0085 0.012Mn 1.4 × 10−1 0.29 0.03 0.0005 0.004Zn 3.0 × 10−1 4.77 0.43 0.0083 0.028Cu 4.0 × 10−2 0.56 0.05 0.001 0.024Ni 2.0 × 10−2 0.48 0.04 0.0008 0.042aRfDo in mg/ kg body weight/daybIntake in mg/daycADD in mg/ kg body weight/day

The HQ was estimated for the heavy metalsby the intake of the milk. The average daily dosewas calculated by dividing the intake by the bodyweight of an average Indian man, i.e. 52 kg (Jainet al. 1995; Dang et al. 1996). The RfDo of all theheavy metals were considered from US-EPA.

The hazard quotient calculated revealed thatthe intake of the heavy metals through the inges-tion of milk does not pose any apparent threat tothe local people. None of the HQ of the heavymetals exceeds the limit of 1 as proposed by US-EPA (Table 6). The HQ ranges from 0.004 (Mn)to 0.042 (Ni).

Conclusions

The levels of heavy metals (Zn, Cu, and Pb) in themilk samples were within the permissible levelsgiven by WHO/FAO. The risk assessment studiesalso confirm no potential risk due to the intake ofheavy metals and radionuclides owing to the con-sumption of the milk. Both the hazard quotient forthe heavy metals and excess lifetime cancer riskfor radionuclides are within the acceptable limitsprovided by US-EPA. These amounts could betoxic and hazardous if taken in large quantities.Since the dietary intake of food may constitute amajor source of a long-term low-level body accu-mulation of radionuclides and heavy metals, thedetrimental impact becomes apparent only afterseveral years of exposure. The mining activitiesmay increase the levels of radionuclides and heavymetals in the soil which may be apparent in thehigher levels of the food chains. Concentration ofmetals in milk will provide baseline data and thereis a need for intensive sampling of the same for

quantification of the results. Regular monitoringof these radionuclides and the metals in milk andin other food materials is essential to preventexcessive build up of the metals in the food chain.

Acknowledgements Thanks are due to the Board of Re-search in Nuclear Sciences, Department of Atomic Energy,Government of India, New Delhi, for providing the nec-essary funding and laboratory facilities necessary for thestudy.

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