j. environ. res. develop. journal of environmental...

J. Environ. Res. Develop. Journal of Environmental Research And Development Vol. 8 No. 2, October-December 2013

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ASSESSMENT OF URANIUM LEVELS IN ATMOSPHERIC PARTICULATE MATTER (PM10) IN AND AROUND THE

TUMMALAPALLE URANIUM MINING SITE, ANDHRA PRADESH, INDIA

Murad Basha A., Yasovardhan N., Satyanarayana S.V. *1 , Subba Reddy G.V.2, Padma Savitri P. , Vishwa Prasad K.3 and Vinod Kumar A.4

1. Department of Chemical Engineering, JNTUACE, Anantapur, Andhra Pradesh (INDIA) 2. Department of Chemistry, JNTUACE, Pulivendula, Andhra Pradesh (INDIA) 3. HPU Division, Nuclear Fuel Complex, Hyderabad (INDIA) 4. Environmental Assessment Division, BARC, Mumbai (INDIA)

Received July 10, 2013 Accepted October 15, 2013

ABSTRACT Recently, there is a rapid increase of nuclear based generated power, associated industries and its mining activities in India. This has raised the questions concerning a possible increase of uranium levels over that existing in the environment. The present work explores the evaluation of ambient air quality with respect to the Atmospheric Particulate Matter (PM10) and Uranium concentration in PM10 at Tummallapalle Uranium mining site as well as its surrounding villages. In order to monitor ambient air quality, ten PM10 Air Samplers (10 locations) were installed in and around 30 km radial distance from Uranium mining site. Air Samples were collected twice in a month for one year duration. The uranium concentration in PM10 was estimated using UV-Flourimetry technique after acid digestion of PM10 present on the glass fiber/EPM 2000 filter paper. The Uranium concentration was found to be in the range of 5 - 30 ng/m3. These values are found to be normal compared with the reported literature values which are in the range of 20 - 200 ng/m3.

Key Words : Nuclear power, Uranium, PM10, UV–Flourimetry, Air quality

INTRODUCTION In present days, the world uses a great deal of energy and the usage of it is increasing dramatically, particularly in developing countries. Uranium is a best alternative source in the production of electricity through nuclear technology to meet the world’s demand. In view of importance of uranium in the generation of electricity with the help of nuclear technology, Government of India (UCIL-Uranium Corporation of India Limited) has established the extraction and processing of Uranium from its ore at Tummalapalle, Pulivendula, Andhra Pradesh, India. Uranium (U) is naturally occurring heavy metal and is found at an average concentration of 0.0003% (3 mg/kg) in the earth’s crust. It occurs in numerous minerals and is also found in lignite, monazite sands,

phosphate rock and phosphate fertilizers.1,2 Since, uranium is naturally occurring element, it is present in the environment in ultra trace levels, interacts with its surroundings and may reach the humans through inhalation, food and drinking water.3 There is always a chance of release of Uranium into the atmosphere in various stages in the nuclear fuel cycle, including mining, milling, reining, fuel fabrication and fuel reprocessing. Basically uranium is both chemically and radio logically toxic. The literature survey reveals that uranium toxicity primarily affects the kidney, causing damage to the proximal tubule. Further, this metal has been also identified as a potential reproductive toxicant.4,5 Particular Matter in air (both Air - PM10 and PM>10 micron) have been recognized with great environmental significance. Particulate matter is the carrier of many harmful trace *Author for correspondence


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metals (such as As, Be, Cd, Cr, Cu, Hg, Mn, Ni, Pb, Sb, Se, V, Zn, U etc), and can be deposited into the human respiratory system. 6-9 The most essential step of figuring out the distribution characteristics of PM10 in the industrial complex area is to establish long-term concentration profiles of PM10 and the associated components including toxic metals. The workers and residents in and around industrial complexes are assumed to be exposed to elevated levels of the toxic metals associated with the PM10 compared to residents who are living further away from the industrial areas.10-15

AIMS AND OBJECTIVES To analyze the Uranium concentration in ambient air associated with PM10 and exclusively focused on quantitative estimation and variation of uranium in PM10 at Tummalapalle Uranium mining site and its surrounding villages. The study area Tummalaplle, Andhra Pradesh, India lies and confined in the tropical region where the climate is characterised by very hot summers, mild winters and monsoon rains. In summer season, a temperature ranges from maximum 46°C during daytime to a minimum of 15°C at night. In winter maximum temperature during day goes up to 40.6°C and minimum temperature at night becomes as low 10.6°C.10,16

MATERIAL AND METHODS All reagent used for the analysis were of analytical grade and Milli – Q water is used for distilled water prior to use. The sampling was all dilutions. All the glassware was cleaned by soaking in dilute nitric acid and was rinsed with performed around the 30 km radial distance from the Uranium mining site. The sampling locations were fixed on the basis of wind roses and locations were distributed according to the radial distances from the site as follows. : 5 locations within 5 km radial distance, considered as Core Zone 3 locations between 5-10 km radial distance, considered as Buffer Zone 1 2 locations between10-30 km, considered as Buffer Zone 2 The sampling locations and its longitude and latitudes were measured through GPS locator and the values are given in Table 1. The location map is shown in Fig.1. The samples of PM10 were collected twice in a month from November - 2010 to February - 2012. The Envirotech High Volume air sampler Model APM 460 BL was used to collect the samples by running the equipment for a period of 24 hours with an average flow rate of 1.3 LPM (lit/min). The samples of the particulate matter with aerodynamic diameter less than 10 μm (PM10) were collected by passing air over pre-weighed glass fiber/EPM 2000 filter paper.

Table 1 : Showing location names, latitudes/longitudes and distances from the mining site

S/N Location Zones Radial distance from the site (km) Latitude/ Longitude

1 L1

Core Zone

0.53 14°19'09.25"/78°16'08.22" 2 L2 1.17 14°19'37.61"/78°15'20.28" 3 L3 3.74 14°18'24.12"/78°17'46.38" 4 L4 3.93 14°19'50.64"/78°18'05.94" 5 L5 4.55 14°21'52.14"/78°16'11.76" 6 L6

Buffer Zone-1 6.64 14°22'56.58"/78°15'11.94"

7 L7 7.85 14°22'14.46"/78°19'13.26" 8 L8 9.90 14°22'10.44"/78°21'29.46" 9 L9 Buffer Zone-2

14.28 14°26'55.74"/78°14'04.50" 10 L10 17.70 14°10'49.68"/78°11'30.06"


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Fig. 1 : Geographical distribution of the sampling locations

The wind rose for Tummalapalle uranium mining site collected for the period September – 2011 to June – 2012 is shown in Fig. 2. The filter papers used for the collection of PM10 were pre – conditioned (24 h in a dessicator under the following conditions: temperature of 15 – 30 °C and humidity less than 40%). They were pre –

weighed and after the particulates collected, the filters were reconditioned for another 24 h in the dessicator and reweighed for mass of PM10. All the procedures during handling of filters were strictly quality controlled to avoid any possible contamination and followed the guidelines of CPCB, India.17,18

Fig. 2 : Wind rose for Tummalapalle uranium mining site

Uranium analysis The PM10 sample was collected on glass fiber/EPM 2000 filter paper which was digested in several stages. Initially, the digestion was carried out by taking approximately 20 ml of aquaregia (HNO3: HCl - 1:3) until dryness on hotplate. Then, around 20 ml of HClO4: HNO3 (1:4) was added and digested on hotplate till complete dryness of the sample. Finally, the resultant sample was

digested 2-3 times with Conc. HNO3 on the hot plate until to dryness. The digest was rinsed with 4N HNO3 and filtered off on Whatmann 41 filter paper. The filtrate was kept on the hot plate up to dryness. To the final residue, 10 ml of 4N HNO3 and 10 ml of aluminum nitrate were added. From this mixture, the uranium is extracted using ethyl acetate by solvent extraction process. The separated organic layer is subjected to evaporation. The residue

Wind Rose Tummalapalle, AWS-ISRO602, September 22, 2011-June 20, 2012


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containing Uranium is dissolved in 4N HNO3 and analyzed with the help of UV-Flourimetry using platinum plancheting.

RESULTS AND DISCUSSION PM10 (µg/m3) concentration and Uranium (ng/m3) concentration in PM10 sample at different sampling villages with its sampling dates, annual Minimum (Min), Geometric Mean (GM) and Maximum (Max) values are given in Table 2. Air – PM10 concentration The PM10 concentrations were observed in the range of 30.2 – 87.1 µg/m3 at L1; 22.9 – 109.6 µg/m3 at L2; 13.5 – 64.7 µg/m3 at L3; 24.3 – 78.1 µg/m3 at L4; 19.2 – 99.0 µg/m3 at L5; 15.4 – 134.4 µg/m3 at L6; 24.7 – 82.5 µg/m3 at L7; 15.2 – 67.6 µg/m3 at L8; 22.5 – 75.1 µg/m3 at L9; and 4.5 – 13.5 µg/m3 at L10. It has been observed that L6 is showing high Air - PM10 concentration (134.44 µg/m3) with GM value of 45.8 µg/m3, which was sampled in the season of winter. This concentration is higher than the maximum concentration reported in all other sampling locations. The observed Air – PM10 value has exceeded once during the observation period, the limit of daily (24 hrs) - Indian National Ambient air quality standards of Air - PM10 (100 µg/m3) value.19 This site is at a radial distance of 6.64 km from the mining site and the mining operation cannot be the cause to these high values. It was found that there exists an operating stone crushing mill near to the L6 sampling location. The location is also situated beside Pulivendula to Kadapa highway, where huge vehicular movement takes place. The minimum Air - PM10 (13.5 µg/m3) concentration has been observed at L3 with GM value of 37.5 µg/m3. The reported value is low even comparing with minimum values at all other sampling locations where it was sampled in the season of monsoon. This sampling site is located in core zone at a radial distance of 3.74 km from the mining site. The sampling locations L1, L2, L6 and L7 were comparatively showed higher concentrations of PM10 (GM of 52.9, 52.0, 45.8 and 52.2 respectively). The locations L1 and L2 are located in Core Zone and having the radial distance of 0.53 and 1.17 km, respectively. Dust generation due to movement of tipper

Lorries carrying ore and other vehicles for local public transportation may be the reason for the elevated values. The locations L6 and L7 are located in Buffer Zone – 1 at radial distance of 6.64 and 7.85 km, respectively. These sampling locations are located beside Pulivendula to Kadapa highway, catering to huge vehicular movement. In addition both the sampling locations there exists stone crushing mills. The sampling location L10 frequently observed low concentration of PM10 with the GM of 28.1. The location is located in Buffer Zone – 2 having the radial distance of 17.7 km from the mining site. This location is far away from the mining site, and also situated at other side of hill area and can be considered as a control pint for future studies as impact of transport of particulate matter including dust from the mining site, if any will be minimal. The high values of PM10 concentration were observed in winter season (i.e., from December to February) in all the sampling locations due to enhanced combustion activities of the villager. In addition lot of agricultural crops are cultivated in winter season, adding to possible dust load generation. Uranium concentration in air – PM10 Uranium concentration in PM10 were observed in the range of 3.8 – 32.2 ng/m3 at L1; 1.6 – 27.8 ng/m3 at L2; 1.8 – 22.9 ng/m3 at L3; 3.9 – 31.6 ng/m3 at L4; 1.5 – 30.6 ng/m3 at L5; 2.2 – 31.7 ng/m3 at L6; 3.1 – 28.6 ng/m3 at L7; 1.2 – 31.9 ng/m3 at L8; 1.5 – 24.9 ng/m3 at L9; and 4.5 – 13.5 ng/m3 at L10. By considering samples individually, a maximum concentration value (32.2 ng/m3) was found in a sampling location L1 with a GM of 13.5 ng/m3 and these values marginally varied throughout the sampling period when compared with the other sampling location. This location is situated in core zone with the radial distance of 0.53 km from the mining site. Since, the location is very near to the mining site, transportation of ore from one place to other for processing and re suspension of the deposited dust due to vehicular movement for transportation of public may be the possible reason for these elevated values. The GM’s of the all locations is below 11 ng/m3 except the location L1, where it is 13.5 ng/m3. However, the concentration of Uranium reported in


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Table 2 : Air – PM10 (µg/m3) concentration and Uranium (ng/m3) concentration in Air – PM10 of different sampling villages with its

sampling dates

Date of sampling

Filter Paper

L1 L2 L3 L4 L5 L6 L7 L8 L9 L10

PM10 U PM10 U PM10 U PM10 U PM10 U PM10 U PM10 U PM10 U PM10 U PM10 U

25-Nov-10

GF-1 Filter Paper

NS NS NS NS 36.6 14.3 24.8 29.8 52.1 16.3 35.6 31.7 51.0 19.3 28.3 17.7 NS NS 37.1 12.9

13-Dec-10 NS NS NS NS 22.6 7.9 31.5 13.5 67.8 29.8 134.4 11.7 61.6 13.5 45.4 12.6 NS NS 35.7 12.6

06-Jan-11 87.1 9.5 74.0 23.3 64.7 10.6 59.7 9.3 99.0 13.5 64.7 12.1 68.6 10.4 47.3 14.4 57.1 12.1 56.6 12.2

29-Jan-11 82.1 16.8 53.4 1.6 42.1 13.2 49.5 6.1 44.8 3.3 44.7 6.3 28.7 4.4 45.0 15.5 35.2 11.5 24.1 10.6

13-Feb-11 55.8 9.5 67.2 6.0 63.6 5.6 78.1 13.4 79.4 7.5 38.0 4.9 82.5 4.6 54.5 12.9 45.9 2.2 NS NS

04-Mar-11 42.7 3.8 59.8 5.1 28.6 9.7 46.1 4.5 62.6 7.2 35.9 2.2 66.9 3.1 41.1 8.3 68.6 5.5 NS NS

08-Apr-11 79.9 8.1 84.7 6.5 38.2 6.3 57.2 17.5 19.2 26.3 76.8 7.4 64.0 28.6 35.2 1.2 60.2 9.0 NS NS

15-Apr-11 72.7 13.1 56.2 10.7 52.4 3.4 33.7 31.1 37.7 14.1 40.1 23.9 64.4 6.4 43.2 2.0 54.1 6.3 27.5 7.2

29-Apr-11 49.3 32.2 71.0 27.8 43.9 5.7 55.6 31.6 26.9 30.6 44.6 26.7 82.2 10.4 15.2 31.9 75.1 24.9 32.7 6.6

13-Jun-11 57.1 18.3 31.5 7.8 51.1 22.9 24.4 7.8 28.2 17.8 36.1 26.4 51.7 16.2 46.4 28.4 54.9 10.3 23.5 9.7

03-Jul-11 47.2 19.7 109.6 7.4 39.7 12.4 27.5 8.1 33.4 12.6 33.3 15.3 42.0 12.3 67.6 15.9 37.3 9.3 28.0 4.5

16-Jul-11 53.8 19.5 33.7 3.5 50.5 14.3 25.0 9.7 31.3 12.8 29.4 14.5 38.1 12.8 35.5 22.1 30.8 3.8 32.6 4.9

06-Aug-11 30.2 12.5 60.0 6.9 13.5 1.8 62.0 8.6 25.3 3.2 15.4 7.9 24.7 8.2 21.6 12.1 22.5 13.4 24.7 5.4

07-Sep-11 44.5 14.7 55.3 7.8 25.0 13.7 32.5 14.3 49.0 19.6 45.1 17.9 41.9 12.4 30.3 3.2 27.3 1.5 19.6 8.6

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21-Oct-11 72.1 15.4 54.0 9.1 49.1 9.3 76.2 4.7 55.9 6.8 57.6 6.9 59.7 3.2 47.7 14.7 48.8 12.8 26.2 10.6

06-Dec-11

EPM 2000

36.3 12.3 22.9 1.6 35.1 3.2 24.3 8.1 76.0 1.5 61.9 3.6 72.3 12.9 44.5 13.8 38.2 12.4 28.4 10.7

28-Dec-11 75.8 14.5 64.1 3.6 39.3 12.1 69.8 13.2 43.7 3.6 91.9 12.4 75.7 12.7 51.7 14.5 40.3 12.4 29.8 10.5

20-Jan-12 33.9 13.5 31.8 7.9 27.9 14.5 29.1 12.3 27.8 7.9 38.3 12.4 41.6 16.5 27.9 17.8 31.2 14.5 23.6 12.7

08-Feb-12 31.6 17.6 28.4 4.9 34.0 8.5 34.5 3.9 31.9 6.8 45.8 16.5 32.0 12.4 21.7 12.7 34.3 14.8 16.8 13.5

Minimum 30.2 3.8 22.9 1.6 13.5 1.8 24.3 3.9 19.2 1.5 15.4 2.2 24.7 3.1 15.2 1.2 22.5 1.5 16.8 4.5

Geometric Mean 52.9 13.5 52.0 6.4 37.5 8.5 40.7 10.8 42.6 9.6 45.8 11.0 52.2 9.9 37.2 10.9 42.5 8.6 28.1 9.1

Maximum 87.1 32.2 109.6 27.8 64.7 22.9 78.1 31.6 99.0 30.6 134.4 31.7 82.5 28.6 67.6 31.9 75.1 24.9 56.6 13.5

Note: U – Uranium, NS – Not Sample

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all the locations were found to be very low when compared with the standard value 150 µg/m3 (regulatory standard for Ontario) based on the toxicity associated with this Uranium and Uranium related compounds for 24 hr average in Air – PM10.20 Further, as per National Emissions Standard for Hazardous Air Pollutants Radionuclide (NESHAPs) for U-238 is 350 ng/m3 (Fig. 3).

The PM10 and Uranium concentration of location 4, L2, L6 and L7 were not showing any significant correlation, throughout the sampling duration from Nov.2010 to Feb.2012. Hence, both Air- PM10 and Uranium concentrations are independent with each other and the graphical representation is shown in Fig. 4(a) to Fig. 4(d).

Fig. 3 : Annual GM of Air – PM10 and Uranium concentration in Air – PM10

Daily intake The daily intake of Uranium concentration through inhalation is calculated based on 20 m3 of air per day is inhaled by an adult of study area. The daily intake of Uranium in respective locations is tabulated in Table 3. On examining the content in Table 3, the daily intake of Uranium concentration has been

observed 0.27 µg/day for L1, 0.13 µg/day for L2, 0.17 µg/day for L3, 0.22 µg/day for L4, 0.19 µg/day for L5, 0.22 µg/day for L6, 0.20 µg/day for L7, 0.23 µg/day for L8, 0.17 µg/day for L9 and 0.23 µg/day for L10. The calculated daily intake of uranium is below the standard permissible daily intake limit of uranium concentration (1.5 µg/day).21

Fig. 4(a) : PM10 and Uranium concentration in PM10 for UCIL-Mining site

0.010.020.030.040.050.060.070.080.090.0

100.0

06-J

an-1

129

-Jan

-11

13-F

eb-1

104

-Mar

-11

08-A

pr-1

115

-Apr

-11

29-A

pr-1

113

-Jun

-11

03-J

ul-1

116

-Jul

-11

06-A

ug-1

107

-Sep

-11

21-O

ct-1

106

-Dec

-11

28-D

ec-1

120

-Jan

-12

08-F

eb-1

2

Con

cent

ratio

n

Sampling date

L1Air-PM10

U

PM10

0102030405060

PM10 Uranium in PM10PM10 (µg/m3)

Con

cent

ratio

n

No. of days

PM10 (µg/m3)


221

Fig. 4(b) : PM10 and Uranium concentration in PM10 for Tummalapalle

Fig. 4(c) : PM10 and Uranium concentration in PM10 for Bestuvaripalle

Fig. 4(d) : PM10 and Uranium concentration in PM10 for Vemula

Table 3 : Daily intake of uranium concentration in different location

Location Daily intake of Uranium (µg/day) L1 0.27 L2 0.13 L3 0.17 L4 0.22 L5 0.19 L6 0.22 L7 0.20 L8 0.23 L9 0.17 L10 0.23

0.020.040.060.080.0

100.0120.0

06-J

an-1

129

-Jan

-11

13-F

eb-1

104

-Mar

-11

08-A

pr-1

115

-Apr

-11

29-A

pr-1

113

-Jun

-11

03-J

ul-1

116

-Jul

-11

06-A

ug-1

107

-Sep

-11

21-O

ct-1

106

-Dec

-11

28-D

ec-1

120

-Jan

-12

08-F

eb-1

2Con

cent

ratio

n

Sampling date

L2Air-PM10

U

PM10

0.0

50.0

100.0

150.0

25-N

ov-1

013

-Dec

-10

06-J

an-1

129

-Jan

-11

13-F

eb-1

104

-Mar

-11

08-A

pr-1

115

-Apr

-11

29-A

pr-1

113

-Jun

-11

03-J

ul-1

116

-Jul

-11

06-A

ug-1

107

-Sep

-11

21-O

ct-1

106

-Dec

-11

28-D

ec-1

120

-Jan

-12

08-F

eb-1

2

Con

cent

ratio

n

Sampling date

L6Air-PM10

UPM10

0.020.040.060.080.0

100.0

25-N

ov-1

013

-Dec

-10

06-J

an-1

129

-Jan

-11

13-F

eb-1

104

-Mar

-11

08-A

pr-1

115

-Apr

-11

29-A

pr-1

113

-Jun

-11

03-J

ul-1

116

-Jul

-11

06-A

ug-1

107

-Sep

-11

21-O

ct-1

106

-Dec

-11

28-D

ec-1

120

-Jan

-12

08-F

eb-1

2Con

cent

ratio

n

Sampling date

L7Air-PM10

U

PM10


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CONCLUSION The ambient air quality with respect to PM10 at Tummalapalle Uranium mining site and its surrounding located villages, along with quantitative estimation of Uranium concentration in PM10 were evaluated. The observed values at all the sampling locations found to be within the permissible limit of 150 ng/m3 (Ontario standard – 150 ng/m3 and NESHAPs – 350 ng/m3). No abnormal change of PM10 in and around the mining plant was observed. The daily intake of uranium is below the standard permissible daily intake limit of uranium concentration (1.5 µg/day). Hence, these levels may not cause any imminent danger to individuals who inhale this air. Further, there was no correlation between the PM10 and Uranium concentrations observed in all the sampling locations, indicating that they are independent to each other.

ACKNOWLEDGEMENT The authors greatly acknowledge BRNS, DAE for providing financial assistance (Ref No. 2008/36/77-BRNS/4010) to carry out this research work. Authors convey their gratitude to HPU Division, NFC, Hyderabad, India for their support in the analysis of Uranium and UCIL, Tummalapalle, Andhara Pradesh, India for their help in collection of samples.

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