ISSN No: 2309-4893 International Journal of Advanced...

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ISSN No: 2309-4893 International Journal of Advanced Engineering and Global Technology Vol-1, Issue-5, December 2013 REMOVAL OF HEAVY METAL RADIONULCIDE CONTAMINANTS BY PLANTS FROM URANIUM MILL TAILINGS C.Muralidhar Rao * and G.Sudhakar ** *Officer on Special Duty, Environmental management cell Atomic Minerals Directorate for Exploration & Research, Hyderabad Email: [email protected] ** Former Director, Environmental Protection Training and research Institute, Hyderabad. Email: [email protected] ABSTRACT: Uranium mill tailings are the crushed rock residues of the uranium extraction process from Uranium Oxide ores. The tailings effluent and tailings solids from the mill are discharged as slurry to a waste retention pond, the tailing pond. Natural radionuclides and trace metals are present in mine tailing/soil in varying concentrations, some of these are found in elevated concentrations in uranium waste tailings. Radionuclide and metal pollution is a global environmental problem and the number of contaminants entering the environment has increased greatly in recent times and this is due to increased mining activities. A study was undertaken for three years to evaluate the potential of native plant species for the removal of residual heavy metals and radionuclides from tailing ponds of Uranium mines, Jaduguda, Jharkhand. Sampling stations: three at Jaduguda, one at Turamdih were selected. pH, Electrical conductivity (EC) 12 metals (- Al, V, Cr, Mn, Fe, Ni, Cu, Zn, As, Se, Cd, Pb) and 3 radionuclides - Co, Sr and U) of the tailings were analysed. From the analysis of sediment/soil / water/effluent of tailing ponds, 8-elements (Al,U, Mn, V, Fe, Ni, Cu and Zn) were found to be significantly in higher concentrations in tailing soils. U and Mn were found to be the predominant contaminants. 26 plant species were screened for their ability to accumulate and remediate the contaminated soils. Significant hyperaccumulants are [Sacchurum spontaneum(U 8ppm),Pteris vittata(U 4ppm), Cyprus compressus(U 2ppm), Lantana camara(U 4ppm) and Typha latifolia(U 3ppm)], S.spontaneum(Cr16ppm), Ricinus communis(Cr 19ppm) and Typha latifolia(Cr 18ppm)] and for Sr[Alstonia scholaris(98ppm), Buchanania lanzan(81ppm) and Cassia alata(77ppm). Considering various factors of suitability of the plant species for phytoremediation, 4 species viz;Sacchurum spontaneum, Typha latifolia, Pteris vittata and Cyprus compressus found to hold good potential as phytoaccumulants of heavy metals and radionuclides in tailings of uranium mines. KEYWORDS: URANIUM; TAILING POND; BIOREMEDIATION; PHYTOACCUMULATION, PHYTOREMEDIATION; NUCLEAR WASTES; RADIONUCLIDE; TRACE METALS 288 WWW.IJAEGT.COM

Transcript of ISSN No: 2309-4893 International Journal of Advanced...

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ISSN No: 2309-4893

International Journal of Advanced Engineering and Global Technology Vol-1, Issue-5, December 2013

REMOVAL OF HEAVY METAL RADIONULCIDE CONTAMINANTS BY PLANTS FROM URANIUM MILL TAILINGS

C.Muralidhar Rao*and G.Sudhakar**

*Officer on Special Duty, Environmental management cell Atomic Minerals Directorate for Exploration & Research, Hyderabad

Email: [email protected] ** Former Director, Environmental Protection Training and research Institute, Hyderabad.

Email: [email protected]

ABSTRACT: Uranium mill tailings are the crushed rock residues of the uranium extraction process from Uranium Oxide ores. The tailings effluent and tailings solids from the mill are discharged as slurry to a waste retention pond, the tailing pond. Natural radionuclides and trace metals are present in mine tailing/soil in varying concentrations, some of these are found in elevated concentrations in uranium waste tailings. Radionuclide and metal pollution is a global environmental problem and the number of contaminants entering the environment has increased greatly in recent times and this is due to increased mining activities. A study was undertaken for three years to evaluate the potential of native plant species for the removal of residual heavy metals and radionuclides from tailing ponds of Uranium mines, Jaduguda, Jharkhand. Sampling stations: three at Jaduguda, one at Turamdih were selected. pH, Electrical conductivity (EC) 12 metals (- Al, V, Cr, Mn, Fe, Ni, Cu, Zn, As, Se, Cd, Pb) and 3 radionuclides - Co, Sr and U) of the tailings were analysed. From the analysis of sediment/soil / water/effluent of tailing ponds, 8-elements (Al,U, Mn, V, Fe, Ni, Cu and Zn) were found to be significantly in higher concentrations in tailing soils. U and Mn were found to be the predominant contaminants. 26 plant species were screened for their ability to accumulate and remediate the contaminated soils. Significant hyperaccumulants are [Sacchurum spontaneum(U 8ppm),Pteris vittata(U 4ppm), Cyprus compressus(U 2ppm), Lantana camara(U 4ppm) and Typha latifolia(U 3ppm)], S.spontaneum(Cr16ppm), Ricinus communis(Cr 19ppm) and Typha latifolia(Cr 18ppm)] and for Sr[Alstonia scholaris(98ppm), Buchanania lanzan(81ppm) and Cassia alata(77ppm). Considering various factors of suitability of the plant species for phytoremediation, 4 species viz;Sacchurum spontaneum, Typha latifolia, Pteris vittata and Cyprus compressus found to hold good potential as phytoaccumulants of heavy metals and radionuclides in tailings of uranium mines.

KEYWORDS: URANIUM; TAILING POND; BIOREMEDIATION; PHYTOACCUMULATION, PHYTOREMEDIATION; NUCLEAR WASTES; RADIONUCLIDE; TRACE METALS

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International Journal of Advanced Engineering and Global Technology Vol-1, Issue-5, December 2013

Introduction Environmental pollution by organic compounds, metals and radionuclide became extensive as mining and industrial activities increased in the 21st century and have intensified since then. Environmental pollutants containing heavy metals and radionuclides is in the form of effluent/stream released from industrial activities and in contrast with organic materials they cannot be degraded and therefore accumulate in water, soil, bottom sediments and living organism also. The grade of the uranium ore dug in uranium mines in India is remarkably low. Uranium mines in the world usually produce low grade ores containing 0.1 – 0.3% U3O8

[2]; the average grade in India having still lower about 0.06%. Thus the uranium industry generates large quantities of waste. Almost the entire mined ore comes out as waste after recovery[3].

Fig-1: Map showing Uranium occurrence in Jharkandh, India

In India, Uranium Corporation of India (UCIL) who have the monopoly over Uranium mining and mineral processing is operating 4 underground mines and one opencast mine, in addition to, two ore processing units in Singhbhum district of Jharkhand state(Fig-1) [1]. Another three uranium mining and processing units have been planned in the states of Andhra Pradesh (Tummalapally) and Meghalaya in the next 5 years. Of the above, Jaduguda, Bhatin, Narwapahar, Turamdih are underground mines and Banduhurang mine is an opencast one. Once the uranium ore is processed at the mill and converted through acid leaching to Sodium diuranate -yellowcake, it is sent to the Nuclear Fuel Complex in Hyderabad for further processing. Yellowcake is 80% rich in uranium oxide U3O8 and is used to make fuel rod for nuclear reactors on enrichment . In the process of mining to milling , leaching and final production of yellow cake ,it generates large quantity of hazards waste that are disposed off in vast area of land called tailing pond adjoining the UCIL mill. In underground mines, wastes generated from the mine are used as the filling material for the void created by excavation of ore. Whereas the coarser fraction is used for filling, the finer fraction is disposed off in tailings ponds. Though major portion of uranium present in the ore is extracted, a fraction though quantitatively small, remains unextracted and is finally discharged with the tailings [8]. The supernatant water after decantation and treatment in the Effluent Treatment Plant(ETP) is released into local stream. The release of radionuclides and heavy metals from Uranium mine beneficiation/ waste sites and their subsequent mobility in the environment is a subject of intense public concern. Release of heavy metal without proper treatment into soil, water and air systems posses a significant threat to public health and ecosystem because of its persistence, biomagnification and accumulation in food chain. Natural radionuclides and trace metals are present in soil in varying concentrations, some of these are found in elevated concentrations in uranium waste tailings [3,4]. No level of radiation exposure above background radiation can be deemed ‘safe’ [5] because of the

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presence half-life of various radionuclides ranging from 14 billion years to 3.1minutes. Heavy metals and their precursors, such tailings constitute a long term hazard [6]. This paper evaluates the quantity of uranium (U) and selected trace metal (Sr, Cs, Cr and Hg) mobilization in water, soil and level of metal accumulation in plant species collected from the tailing pond sites of uranium mines and rate of metal transfer from soil to plant species called transfer factor. Finally screening the candidate phytoremediating plant species is intended. The work presented and discussed here is part of the BRNS funded research project to identify native primary colonizing plant/biological species for remedying metal and radionuclide contamination in soils/sediments from uranium mining and milling sites in India. Materials and Method: Study area: The position of uranium tailing pond (Fig-2)[11], in which the research was carried out is located near uranium deposit (Latitude: 220 43” Longitude: 860 12”) is located in Singhbhum East district of Jharkhand state. It is about 6 km south of Tatanagar railway station, the nearest railhead on Howrah-Mumbai line. Jaduguda, the well-known underground uranium mine of UCIL is situated at about 25 km southeast of this deposit. The deposit falls under Survey of India Toposheet No.73 J/2. The deposit is well connected by all weather metal road with Jamshedpur and Jaduguda. The area around Turamdih uranium deposit exhibits a flat and moderately undulating topography lying within hill ranges in northern and southern side. The drainage pattern of the area is mainly controlled by streamlets feeding to nearby Kharkari River, a tributary of the Subernrekha river. The vegetation is nearly scanty comprising of bushes and a few small trees on the hill slopes.[1]There are three tailing ponds (Fig-3) (Tp-1, Tp-2 and Tp-3) in which Tp-1 is abandoned and not covered with soil and Tp-2 is abandoned and has been covered with 30cm layer of soil. The tailing pong-3 is presently being filled and having half full of water body.

Fig-2: Satellite Photograph around Jadugoda(the location of the study area) Field sampling and processing: Sampling point: Upstream sampling site:

- Rankini mandeer - Bhatin Tailing pond: - Tailing pond No.1

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- Tailing pond No.2 - Tailing pond No.3 Downstream: - Tilaitand - Dungridhi UCIL colony(control) away from the tailings.

17-Plant, 10-soil and 7-water samples (Fig-4) collected during March,2009 –April,2011 from in and around selected sites of Uranium tailing ponds of Jadugoda. 10 sample points are chosen (one sample sites each in abandoned tailing ponds i.e. Tp-1 and Tp-2, two sample sites in present working Tp-3, two upstream sample sites in the distance of 1Km, two sample sites from mining area and two down stream samples in the distance of 1Km and 2Km).

Fig-3: Locations of sampling points. Laboratory analysis: Preparation of Sample solution: Water: Stagnated water from tailing ponds as well as running water samples from natural streams were collected from selected sites in Poly Propylene bottles, the water samples received were filtered using whatman-40 filter paper .The water samples were preserved by maintaining acidity of 1 M with respect to acetic acid following standard procedure [12 to 16]. for metal analysis. Soil: Samples were collected in polythene bags at a depth of 25-30 cm (from surface). Soil samples were crushed, mixed thoroughly and air-dried for 5 to 6 days then dried in hot air oven for 24 hrs at 65oC and finally ground in to fine powder to pass through 2 mm sieve. Plant: Harvested samples are cleaned with tap water to remove any contaminates(on site). The root and shoot parts of individual plant species were separated, weighed (fresh weight) and placed in separate paper bags. In lab the samples were again cleaned with distilled water, air dried and kept at 65º C for 2 days in hot air oven and dry weight were taken. After taking dry weight the samples were ground into fine powder with Wiley

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mill followed by coffee grinder (Kenstar mixer grinder MG 0411) which was carefully cleaned between samples. to pass through a 2 mm sieve. Analysis: Soil pH was measured by mixing 10 gram of freshly soil sample and 50ml of distilled water and stirred for 20 minutes in a 100 ml beaker using magnetic stirrer. The soil-water mixture was kept overnight and taken the reading with the help of digital pH meter (Systronics 335). pH and EC were measured in water (Following APHA 4500H and B and 2510B protocols) and soil (following AOAC SW 846 9040 and SW 846 9050 protocols) samples. All metals were analysed by Inductively Coupled Plasma Mass Spectrometry (ICPMS).

Water :Before collecting the samples, containers were cleaned by soaking in 2 N HNO3 overnight, rinsed with pure water, and then air dried in fume hood. Samples were fixed with 8N HNO3 (Friel, J.K., et al.). Water samples were analysed for pH and Electrical Conductivity (EC). All metals were analysed by Inductively Coupled Plasma Mass Spectrometry (ICPMS). Standards and blanks were run con-currently. Approximately 0.5 g of the plant samples were weighed accurately and transferred to a Teflon container. 5 ml of 65% HNO3 and 1 ml 30% H2O2 added. After microwave/hotplate digestion cycle, digested samples were made upto 25 ml with de ionized water. (Yasemin S et al 2007). All metals were analysed by Inductively Coupled Plasma Mass Spectrometry (ICPMS).

Determination of Transfer Factor (TF) The uptake of radionuclides or elements by plants from the soil is normally described as transfer factor (TF), the ratio of concentration of radionuclide or element in plant tissue and soil (in Bq.kg-1 or mg.kg-1) (A.G. Hegde et.al. 2004)

Metal concentration in Plant tissue (Dry weight)

TF = ----------------------------------------------------------------------------- Metal concentration in Soil (Dry weight) from where the plant was grown.

Quality assurance and checking of inter laboratory data The results generated for metals and radionuclides were compared with previous published works (V.N.Jha et al 2007). The same samples were sent to Lucid Laboratories Pvt. Ltd, Hyderabad, for inter lab comparisons. Results and Discussion pH, EC and metal concentrations in soil and water samples and metal concentrations of plant samples were recorded for two years. All water samples have shown pH ranging between 5.62 to 7.24. The Tailing Pond1 (TP1) ,Tailing Pond 3 (TP3),Effluent treatment plant(ETP)and TTP(Turamdih Tailing pond, water samples were found to be slightly acidic in nature (pH =5.62), PL being Permissible limits (Figure: 4a & b). The pH of the soil collected from all the sampling points were less than the pH of the control. Soil samples collected away from tailing ponds considered as control. All the samples (Soil and water) were found to have higher levels of EC and are more than the permissible limit [Water: 2250 µmohs/cm (CPCB); Soil: 292] (Figure: 4b).

Fig:4a

TP1 TP3 TTP ETP PL*

6.93 6.78 6.32 6.45 6.13 5.98 5.62 6.60 7.24 7.50

pH Values of the samples pH Soil pH Water

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Fig:4b

Table-1 metal concentration in

Water samples(units in ppm)(PL=Permissible limits)

Higher level of uranium and trace metals are concentrated in tailing pond and downstream of tailing pond sampling point (Table-1 and Table-). Plant, soil and water sample which are collected from tailing pond showed the higher concentration level of uranium (i.e. plant: 38mg/kg, soil: 69mg/kg and water:78mg/L) and chromium (i.e. plant: 86mg/kg and soil: 262mg/kg), but the concentration level of chromium in all water samples which are collected from upstream of tailing pond and downstream of tailing pond showed below detection limit of instrument or very low level of Cr(<10ppb) as the uranium and chromium are more of originated from the ore. Higher concentration level of strontium was present in the samples which are collected from downstream of tailing pond(i.e.1.35mg/L). The analysis result of cesium in all samples (plant: <10mg/kg, soil: <10mg/kg and water: <20mg/kg) are at a very low concentration level or below detection limit of the instrument. Because of the volatile nature of the mercury, the analysis was done only in the water samples and all water samples which are collected from upstream, tailing pond and downstream of tailing

TP1 TP3 TTP ETP PL*

1365 1920 1310

1053 292

6103 6039 5428

3654

2250

EC values of the sample EC Soil EC Water

Water TP1 TP3 TTP ETP Control PL

Al 0.020 3.624 3.624 0.212 0.554 0.2

V 0.002 0.007 0.002 0.004 0.020 0.2

Cr 0.007 0.007 0.007 0.007 0.027 2.0

Mn 7.103 2.800 2.511 2.535 0.839 2.0

Fe 0.501 0.544 0.671 0.356 2.909 0.3

Ni 0.048 0.713 0.108 0.020 0.047 3.0

Co 0.004 0.087 0.027 0.027 0.123 1.0

Cu 0.004 0.060 0.234 0.006 0.010 1 .5

Zn 0.018 0.079 0.043 0.043 0.156 15.0

As 0.005 0.008 0.008 0.008 0.032 0.05

Se 0.001 0.054 0.004 0.028 0.121 0.05

Sr 0.587 0.762 0.593 0.295 0.098 4.0

Cd 0.001 0.001 0.001 0.001 0.001 2.0

Pb 0.001 0.036 0.001 0.027 0.082 0.1

U 26.388 78.973 16.444 0.283 0.003 0.015

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pond showed concentration of mercury(<2ppb) in below detection limit of instrument or no mercury content in the samples.

Fig .5.Trends of metals in water samples(units ppm, * permissible limits)

Metals in Soil: The average metal concentration in tailing ponds and its affected areas show significantly higher levels (Table– 2) of heavy metals- Al, Mn and Fe than the other metals and radionuclides Eight elements - Al (16553.4ppm), V (118.8ppm), Mn (3446.9ppm), Fe (34719.6ppm), Ni (200.9ppm), Cu (221.2ppm), Zn (175.3ppm) and U (50.8ppm) were recorded in higher concentrations. The concentrations of other metals are significantly in low concentration. Based on the control (threshold) values, eight elements (U, Mn, V, Fe, Ni, Cu and Zn) have been Identified to be higher than the threshold values (Figure: 6) and also considered as major contaminants - need to be remedied.

Fig.6: comparison of identified contaminant levels between two sampling sites (Jadugoda tailing pond and Turamdih tailing pond)(*C=control/ Threshold).

Table.2 Metal Concentration in Soil samples in ppm(*C= control/ Threshold)

Soil TP1 TP3 TTP ETP TP2 C* Al 15557 19516 15392 12664 19639 12529 V 101 147 77 161 107 10 Cr 191 176 119 165 229 170

3.62

Saturation

0.54 0.97 0.53

2.51

0.67

5.53

0.2

2

0.3 0.02 0.2

2

0.3 0.02

Al Mn Fe U Al Mn Fe U

Jaduguda tailing pond (ppm) Turamdih tailing pond (ppm)

Trends of metals in water Avg *PL

147

3430

237 231 217 75 77

2994

191 408 166 37 10 510

6414

89 69 92 4 10 510

6414

89 69 92 4

V Mn Fe Ni Cu Zn U V Mn Fe Ni Cu Zn U

Jaduguda tailing pond (in ppm) Turamdih tailing pond (in ppm)

Trend of metals in soil Metal *C

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Mn 5466 3430 2994 4524 821 510 Fe 39757 41735 49195 36384 6528 6414 Ni 245 237 190 151 181 89 Co 157 64 44 43 51 23 Cu 153 231 408 134 179 69 Zn 174 217 166 209 109 92 As 9 12 7 7 17 13 Se 1 1 0.2 1 4.7 6.3 Sr 79 50 37 98 41 69 Pb 25 30 19 24 22 20 U 69 75 37 67 6 3

Figure – 7: Comparison of metal concentrations in soil from five sampling sites [Jaduguda uranium mine tailing pond (TP1, TP2 & TP3), Turamdih uranium mine tailing pond (TTP) and Effluent Treatment Plant external channel (ETP).

Plants Metal Analysis

A total of 26 major plant species were screened for phytoaccumulation. The average metal concentrations values in plant samples collected from tailing ponds are compared with those of the were shown in table-3 and figure-8 Table-3. Metal accumulation (in ppm) in plant samples

Sl No Plant species Al V Cr Mn Fe Ni

Co Cu Zn

As

Se Sr Cd Pb U

1 Pteris vittata 71 1 1 211

109 2 1 1 2 1 0 1 0 4 4

2 Typha latifolia 22 0 2 68 46 1 0 3 9 0 0 2 0 3 3 3 Saccharum

spontaneum 54 0 16 31 71 1 0 4 17 0 0 2 0 3 8 4 Paspalidium spp 18 0 1 38 23 1 0 1 2 0 0 0 0 1 0 5 Bicopa monnieri 5 0 1 51 6 0 0 1 1 0 0 0 0 2 0 6 Eichhornia crassipes 11 0 1 49 73 0 0 5 23 0 0 0 0 4 1 7 Lantana camara 12 0 4 53 72 0 0 9 49 0 0 8 0 6 2 8 Agiratum conyzoides 19 0 2 44 38 1 0 4 6 0 0 3 0 4 1 9 Hyptis suaveolens 21 0 1 49 32 1 0 2 2 0 0 1 0 13 4 10 Cenchrus ciliaris 31 0 1 52 43 1 0 4 3 0 0 1 0 1 1 11 Encephalartos ferox 12 0 3 51 12 0 0 1 2 0 0 1 0 0 0 12 Pannicum

miliaceum 27 0 3 30 39 1 0 3 2 0 0 1 0 0 0

15557 101 191 5466 39757 245

157

153 175 10 1 79 1 25 69

19516 147 176 3430

41735 237

64

231 217 12

1 50

0 30

75 15392 77 119

2994 49195 190 44

408 166 7

0

38 0

19 37

12664 161 165

4524 36384 151

43 134 209

7

1

98

0

24

67 19639 107 229 821 6528

181 51 179 109 17

5

41

1

21 6

Al V Cr Mn Fe Ni Co Cu Zn As Se Sr Cd Pb U

Comparision of metal conc. between sampling points TP1 TP3 TTP ETP TP2

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13 Vitex negundo 21 0 4 56 94 0 0 9 52 0 0 8 0 3 0 14

Calotropis procera 83 1 0 3 100 1 0 1 1 0 0 0 0 25 0

15 Croton bonplandianum 12 0 0 4 15 0 0 1 2 0 0 2 0 1 0

16 Pongamia pinnata 0 0 4 126

188 0 0 23 74 0 0 24 0 0 0

17 Dichanthium annulatum 57 0 3 148 88 4 0 3 2 0 0 1 0 0 0

18 Combretum decandrum 38 0 1 21 46 1 0 1 1 0 0 1 0 11 1

19 Wisteria floribunda 0 0 4 77

147 0 0 14 41 0 0 19 0 0 0

20 Breynia vitisidea 0 0 5 97

112 0 0 22 94 0 0 16 0 0 1

21 Azadirachta indica 0 0 6 122

160 0 0 21 50 0 0 9 0 0 0

22 Penstemon digitalis 0 0 2 55 71 1 0 7 22 0 0 6 0 0 0 23 Cyprus compressus 34 0 1 76 28 2 0 2 3 0 0 1 0 1 2 24 Persicaria

hydropiper 33 0 1 75 42 2 0 2 3 0 0 2 0 1 1 25 Ipomea spp 24 0 3 16 20 1 0 2 4 0 0 3 0 1 0 26 Colocasia esculenta 10 0 0 31 9 0 0 2 6 0 0 1 0 2 0

Figure – 8: Average metal concentrations in plant samples collected from Uranium mine tailing pond

Terrestrial plant samples collected in the tailing ponds namely D. annulatum (V, Mn and Ni), P. pinnata, (Mn, Fe, Cu and Zn), A. indica (Mn, Fe, Cu and Zn) B. vitisidea (Mn, Fe, Cu and Zn) and W. floribunda (Fe and Cu) have also shown significantly higher concentration of metals (Figure: 8). Ten plant species from tailing pond have been identified as hyperaccumulants, namely P. vittata (V, Mn, Fe, Ni and U), S. spontaneum (U), L. camera (Cu and Zn), V. negundo (Zn), T. latifolia (Ni and U), C. procera (V) and H. suaveolens (U) P. hydropiper (V and Ni), Eichornia spp (V), C.compressus (Ni and U) Among all the plant samples collected from tailing ponds, P. vittata has shown significant higher concentration levels of all metals. 3 Plants species with highest metal and radionuclide accumulators were identified among 26 plant species and are presented below in the descending order:

0.7 0.2 0.3 0.1 0.0 0.1 0.1 0.1 0.1 0.2 0.2 0.3 0.1 0.5 0.0 0.2 0.3 0.3 0.1 0.0 0.1 0.4 0.2 0.0 0.0 0.0

211

68 31 38 51 49 53 44 49 52 51

30 56

3

55 76 75

16 31

126

4

148

21

77 97 122 109

46 71

23 6

73 72 38 32 43

12 39

94 100 71

28 42 20 9

188

15

88

46

147 112

160

1.90 0.89 0.50 0.62 0.45 0.30 0.07 0.59 0.70 0.79 0.20 0.83 0.08 0.78 0.64 1.68 1.72 0.71 0.29 0.00 0.23 3.55 0.76 0.00 0.00 0.00 1 3 4 1 1 5 9 4 2 4 1 3 9 1 7 2 2 2 2 23

1 3 1 14 22 21 2 9 17 2 1

23 49

6 2 3 2 2

52

1 22

3 3 4 6

74

2 2 1

41

94

50

4.3 2.5 8.1 0.3 0.4 0.7 1.5 0.6 3.9 0.6 0.0 0.1 0.4 0.4 0.0 1.8 1.0 0.0 0.3 0.0 0.0 0.2 1.2 0.0 1.0 0.0

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T. la

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S. sp

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Pasp

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B. m

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I. ca

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A. c

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C. c

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E. fe

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W. f

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Tailing pond ETP Control

Plant average metal conc. (ppm) V Mn Fe Ni Cu Zn U

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ISSN No: 2309-4893

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• V: P. vittata (0.7ppm) > C. procera (0.5ppm) > D. annulatum (0.4ppm) • Mn: P. vittata (211ppm) > D. annulatum (148ppm) > P. pinnata (126ppm) • Fe: P. pinnata (188ppm) > A. indica (160ppm) > W. floribunda (147ppm) • Ni: D. annulatum (3.6ppm) > P. vittata (1.9ppm) > C. compressus (1.7ppm) • Cu: P. pinnata (2.3ppm) > B. vitisidae (2.2ppm) > A. indica (2.1ppm) • Zn: B. vitisidae (94ppm) > P. pinnata (74ppm) > V. negundo (52ppm) • U: S. spantanium (8ppm) > P. vittata (4.3ppm) > H. suaeulance (3.9ppm)

Comparison of mean TF of identified contaminants in plant species

The Transfer Factor (TF) of metal and radionuclide from soil to plants of collected samples were determined based on dry weight. Only Hyperaccumulation of 6 metals by plants have shown significant TF values.The average metal TF of plant sample collected from tailing ponds and its downstream areas are placed in table-4 and fig-9 below

Table-4. Transfer factor on Dry weight basis

Sl No Plant species Mn Fe Ni Cu Zn U 1 Pteris vittata 0.080 0.000 0.030 0.010 0.010 0.170 2 Typha latifolia 0.080 0.000 0.000 0.020 0.420 0.060 3 Saccharum

spontaneum 0.030 0.010 0.000 0.020 0.190 0.670 4 Paspalidium spp 0.050 0.000 0.010 0.010 0.010 0.010 5 Bicopa monnieri 0.000 0.000 0.000 0.010 0.010 0.000 6 Eichhornia crassipes 0.000 0.000 0.000 0.010 0.020 0.050 7 Lantana camara 0.030 0.010 0.000 0.050 1.000 0.100 8 Agiratum conyzoides 0.090 0.010 0.000 0.030 0.260 0.050 9 Hyptis suaveolens 0.730 0.000 0.010 0.020 0.010 0.320 10 Cenchrus ciliaris 0.020 0.000 0.010 0.010 0.030 0.020 11 Encephalartos ferox 0.320 0.000 0.000 0.010 0.010 0.000 12 Pannicum

miliaceum 0.010 0.000 0.000 0.000 0.010 0.000 13 Vitex negundo 0.090 0.010 0.000 0.040 0.470 0.040 14 Calotropis procera 0.000 0.020 0.000 0.010 0.010 0.060 15 Croton

bonplandianum 0.000 0.000 0.000 0.010 0.020 0.000 16 Pongamia pinnata 0.040 0.000 0.010 0.020 0.030 0.030 17 Dichanthium

annulatum 0.200 0.000 0.010 0.010 0.010 0.010 18 Combretum

decandrum 0.000 0.000 0.010 0.020 0.010 0.080 19 Wisteria floribunda 0.020 0.000 0.010 0.030 0.010 0.000 20 Breynia vitisidea 0.020 0.000 0.000 0.010 0.060 0.000 21 Azadirachta indica 0.220 0.030 0.000 0.510 0.940 0.000 22 Penstemon digitalis 0.030 0.000 0.010 0.010 0.010 0.000 23 Cyprus compressus 0.060 0.000 0.000 0.010 0.010 0.420 24 Persicaria

hydropiper 0.060 0.020 0.000 0.040 0.760 0.000 25 Ipomea spp 0.070 0.020 0.000 0.070 1.730 0.010 26 Colocasia esculenta 0.090 0.020 0.000 0.060 0.920 0.000

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The results clearly indicate the differences in V, Mn, Fe, Ni, Cu, Zn and U accumulation among tailing ponds and controls. Plants collected from tailing ponds have shown significantly higher ranges of TF values: V (0.000 to 0.005), Ni (0.00 to 0.03) and U (0.0 to 0.7). In contrast, controls have shown significantly low TF values except for few species, which have shown much higher TF values of Fe (0.00 to 0.03), Cu (0.01 to 0.51), and Zn (0.0 to 1.7) (Figure: 9C, E and F).In case of Manganese, only H. suaeulance (TF: 0.7) and E. ferox (TF: 0.3) from tailing ponds, C. compressus (TF: 0.2) and P. pinnata (TF: 0.2) from control site have the maximum TF value and none of the other plant samples collected from all the sampling sites have shown significant TF .Only B. vitisidae (Zn TF: 1.73) collected from control site has the TF value more than 1. Plant species with high TF values for individual metals were screened and identified species for remediation are presented in the table below (Table-5).

Figure – 9: Comparison of each individual contaminant (metal and radionuclide) mean TF values in plants samples from uranium tailing ponds. Table –5 Plants identified for accumulation of major contaminants in Uranium tailing ponds

S.NO. Suggested Plants Metal Accumulators

Single Dual Multiple

1 H. suaveolens

Mn - Mn, Ni, U

E. ferox - -

2 P. pinnata

Fe Fe, Cu Fe, Cu, Mn, Zn

A.indica - Fe, Cu, Zn 3 S.spontaneum U - -

0.08

1

0.07

6

0.02

5

0.05

0

0.00

3

0.00

4

0.02

7

0.09

0

0.72

8

0.01

6 0.32

3

0.00

8

0.09

2

0.00

4

0.00

1

0.03

6

0.19

8

0.00

3

0.01

7

0.01

9 0.22

0

0.02

6

0.05

6

0.05

7

0.07

1

0.09

0

P. v

ittat

a

T. la

tifol

ia

S. sp

anta

nium

Pasp

alid

ium

spp

B. m

oner

i

I. ca

rnea

L. c

amar

a

A. c

onyn

zoid

es

H. su

aeul

ance

C. c

elea

ris

E. fe

rox

P. m

iliac

eum

V. n

egun

do

C. p

roce

ra C.…

P. d

egita

lis

C. c

ompr

essu

s

P. h

ydro

pipe

r

Icor

nia

spp

C. e

scul

enta

P. p

inna

ta

D. a

nnul

atum

C. d

ecan

drum

W. f

lorib

unda

B. v

itisid

ae

A. in

dica

Tailing pond ETP Control

Mn

0.02

8

0.00

3

0.00

4

0.00

8

0.00

2

0.00

2

0.00

0

0.00

4 0.01

3

0.00

6

0.00

1

0.00

4

0.00

1

0.00

4

0.00

1 0.01

3

0.00

7

0.00

6

0.00

8

0.00

2

0.00

0 0.01

3

0.00

4

0.00

0

0.00

0

0.00

0

P. v

ittat

a

T. la

tifol

ia

S. sp

anta

nium

Pasp

alid

ium

spp

B. m

oner

i

I. ca

rnea

L. c

amar

a

A. c

onyn

zoid

es

H. su

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ance

C. c

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E. fe

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P. m

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V. n

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C. p

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ra

C. b

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andi

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P. d

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C. c

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P. h

ydro

pipe

r

Icor

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C. e

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enta

P. p

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ta

D. a

nnul

atum

C. d

ecan

drum

W. f

lorib

unda

B. v

itisid

ae

A. in

dica

Tailing pond ETP Control

Ni

0.17

4

0.06

5

0.66

8

0.01

5

0.00

1

0.04

9

0.10

2

0.04

5 0.32

5

0.01

6

0.00

0

0.00

1

0.04

0

0.06

3

0.00

0

0.03

2

0.01

4

0.08

0

0.00

2

0.00

5

0.00

0

0.00

2

0.42

4

0.00

0

0.00

7

0.00

0

P. v

ittat

a

T. la

tifol

ia

S. sp

anta

nium

Pasp

alid

ium

spp

B. m

oner

i

I. ca

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L. c

amar

a

A. c

onyn

zoid

es

H. su

aeul

ance

C. c

elea

ris

E. fe

rox

P. m

iliac

eum

V. n

egun

do

C. p

roce

ra

C. b

unpl

andi

anus

P. d

egita

lis

C. c

ompr

essu

s

P. h

ydro

pipe

r

Icor

nia

spp

C. e

scul

enta

P. p

inna

ta

D. a

nnul

atum

C. d

ecan

drum

W. f

lorib

unda

B. v

itisid

ae

A. in

dica

Tailing pond ETP Control

G. Mean TF of U in plant samples

U

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C.decondrum -

4 P.vittata V

V, Ni V, Ni, U C. bunplandianus - -

5 P. vittata Ni

Ni, V V, Ni, U P.digitalis Ni, V -

6 P. pinnata Cu

Cu, Fe Cu, Fe, Mn, Zn B. vitisidea Cu, Zn Cu, Zn, Fe

7 B. vitisidea Zn

Zn, Cu Zn , Cu, Fe L. camara - Zn, Cu, U

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Uranium(U): Out of 26 plant species collected, only 5 species(i.e. S. spontaneum, Typha latifolia, Lantana camara, Ageratum conyzoides, Breynia vitisidae) which are collected from tailing pond are showed the accumulation of Uranium and remaining plant species which are collected from upstream, tailing pond and downstream samples are having <1mg/kg concentration of U. The higher accumulation of U is seen in the root (38mg/kg), stem and leaf (4mg/kg) parts of S. spontaneum, fallowed by root part of Typha latifolia(3mg/kg) and leaf sample of Lantana camera(3mg/kg). The increased order of U accumulation in the collected plant samples (Table-6) are as follows: (S. spontaneum) > (Typha latifolia) > (Lantana camara) > (Ageratum conyzoides) > (Breynia vitisidae)

Table-6: Sl

No. Scientific Name Type of sample

Plant U(mg/kg)

Soil U(mg/kg) TF value

1 Saccharum spontaneum Root 38 69 0.550

2 S. spontaneum Stem & Leaf 4 69 0.057

3 Typha latifolia Root 3 4 0.75 4 Lantana camara Leaf 3 35 0.085 5 S. spontaneum Root 2 35 0.057

6 S. spontaneum Stem & Leaf 2 35 0.057

7 Lantana camara Root 2 35 0.057

8 Ageratum conyzoides Leaf 1 35 0.028

9 Breynia vitisidae Root 1 35 0.028 Chromium(Cr): There are only 4 species (i.e. S. spontaneum, Typha latifolia, Ageratum conyzoides, Lantana camara) which are collected from tailing pond and 2 species(i.e. Ricinus communis, Alstonia scholaris) which are collected from downstream samples showed higher accumulation of Chromium than upstream samples and remaining all other plant species are having <10mg/kg concentration of Cr. The higher accumulation of Cr is seen in the root (37 to 86mg/kg), stem and leaf (28mg/kg) parts of S. spontaneum, fallowed by root part of Ricinus communis (19mg/kg) and root part of Typha latifolia (18mg/kg). The increased order of Cr accumulation in the collected plant samples (Table-7) are as follows: (S. spontaneum) > (Ricinus communis) > (Typha latifolia) > (Ageratum conyzoides) > (Alstonia scholaris) > (Lantana camara)

Table-7:

Sl.No. Scientific Name Type of sample

Plant Cr(mg/kg

)

Soil Cr(mg/kg

) TF value Site of

sample

1 S. spontaneum Root 86 88 0.977 Tailing pond

2 S. spontaneum Root 37 165 0.224 Tailing pond 3 S. spontaneum Stem &

Leaf 28 88 0.318

4 Ricinus communis Root 19 227 0.083 Downstream

5 Typha latifolia Root 18 158 0.113 Tailing pond 6 Ageratum conyzoides Flower 16 165 0.096

7 T. latifolia Leaf 15 165 0.090

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8 Alstonia scholaris Leaf 15 120 0.125 Downstream

9 S. spontaneum Stem & Leaf 13 165 0.078 Tailing

pond 10 Lantana camara Leaf 12 165 0.072 11 Ageratum conyzoides Root 12 165 0.072

Strontium (Sr): There are only 3 species (i.e. Buchanania lanzan, Cassia alata and B. monosperma) which are collected from upstream sample and 2 species(i.e. Alstonia scholaris and Ricinus communis) which are collected from downstream samples showed higher accumulation of strontium than tailing pond samples and remaining all other plant species are having <48mg/kg concentration of Sr. The higher accumulation of Sr is seen in the fruit(98mg/kg) and stem(87mg/kg) parts of Alstonia scholaris, fallowed by root part of Buchanania lanzan (81mg/kg) and leaf part of Cassia alata(77mg/kg). The increased order of Sr accumulation in the collected plant samples (Table-8) are as follows: (Alstonia scholaris) > (Buchanania lanzan) > (Cassia alata) > (B. monosperma) > (Ricinus communis)

Table-8:

Sl No. Scientific Name Type of sample

Plant Sr(mg/kg

)

Soil Sr(mg/kg) TF value Site of

sample

1 Alstonia scholaris Fruit 98 143 0.685 Down stream 2 Alstonia scholaris Stem 87 143 0.608

3 Buchanania lanzan Root 81 98 0.826

Upstream

4 Cassia alata Leaf 77 98 0.785 5 Buchanania lanzan Stem 65 98 0.663 6 B. monosperma Stem 61 98 0.622 7 Cassia alata Stem 60 98 0.612 8 B. monosperma Root 53 98 0.540 9 Buchanania lanzan Leaf 52 98 0.530

10 Ricinus communis Leaf 49 74 0.662 Down stream 11 Alstonia scholaris Leaf 49 143 0.342

Conclusion This study provides evidence of elevated and potentially toxic radionuclides and trace metals concentrated in uranium tailing ponds and may contaminate soil, water and its surrounding. Phytoaccumulation of U, Cr and Sr in the foliage of certain natural species in the immediate downstream vicinity of the Uranium tailing pond near Jadugoda, Jharkhand. Of the 26 species examined,Pteris vittata, S. spontaneum, Typha latifolia and Lantana camara appeared to have the greatest potential to serve as a Phytoaccumulators for U and Cr contamination,Cyprus compressus and Pongamia pinnata for Mn while Ricinus communis, Alstonia scholaris and Buchanania lanzan, had the greatest potential as a Phytoaccumulators for Sr. A significantly positive correlation was found between the accumulation of various heavy metals in plants and their availability in soil. Among various sampling sites of plants, soil and water(Upstream, Tailing pond and Downstream), the maximum level of various heavy metals (i.e. U, Sr and Cr) except Cs, and Hg, was detected in tailing pond plants followed by Downstream while the lowest level of all the metals was recorded in upstream samples. However, in plant analysis of root, shoot

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and leafs separately, results indicate that most of the metals remained concentrated heavily in roots, while few plants showed significant translocation of metals from roots to shoots. Acknowledgements

Authors are thankful to Uranium Corporation of India Ltd and Dr. A.K. Shukla, Bhabha Atomic Research Centre for their constant coordination in sample collection. Grateful to Atomic Minerals Directorate for Exploration & Research and Environment Protection Training & Research Institute, Hyderabad for the radionuclide analysis facilities provided. Authors are greatful to the Board of Research in Nuclear Science(BRNS) of Dept of Atomic Energy ,Govt of India for their financial assistance for the research project. References 1. http://www.amd.gov.in/regions/er_m2.htm 2. A. K. Sarangi, D. R. Dash and P. P. Sharma Uranium Corporation of India Ltd.

Jaduguda, Singbhum East, Jharkhand SOME OBSERVATIONS ON URANIUM MINERALISATION AT TURAMDIH ,2006 (http://www.ucil.gov.in/web/PapersSarangi/Observations%20on%20U%20mineralisation%20at%20Turamdih.pdf) accessed on 29-11-2013.

3. Hiroaki KOIDE, Research Reactor Institute, Kyoto University Radioactive contamination around Jadugoda uranium mine in India, April 27, 2004

4. S.K. Basu, V.N. Jha and A.H. Khan, Health Physics unit, Jadugoda, Environment Assesment Division(Radionuclide Safety systems division), Bhaba Atomic Research Centre. Proc. Nat. Symp. On Environment, B’lore Univ., June, 2000 pp. 138-141)

5. Bastias, J. G., Retreatment of radioactive gold bearing tailings and rehabilitation of mill and tailings dump sites at Rockhole and Moline, Northern Territory (a personal view). Australian Mining Industry Council Environment Workshop Papers (Adelaide, 21–25 September 1987), Australian Mining Industry Council, Canberra. Proceedings of Conference ‘Reclamation, A Global Perspective’, Calgary, Alberta, 27–31 August 1989, pp. 319–346.

6. The Queensland Conservation Council and Friends of the Earth Brisbane and made possible by the Beyond Nuclear Initiative www.nuclearfreequeensland.org

7. E. R. Landa U.S. Geological Survey, 430 National Center, Reston, Virginia 20192, USA (Received April 18, 2002)Journal of Radioanalytical and Nuclear Chemistry, Vol. 255, No. 3 (2003) 559–563

8. John M. Zachara1, Calvin C. Ainsworth1, Gordon E. Brown Jr.2, and Jeffrey G. Catalano2 1Pacific Northwest National Laboratory, Richland, WA 2Stanford University, Stanford, CA. “Chromium Speciation and Mobility in a High Level Nuclear Waste Vadose Zone Plume”, Science Highlight – March 2004

9. Lal Singh and Prafulla Soni, Ecology and Environment Division, Forest Research Institute, Dehradun 248 006, India. Concentration of radionuclides in uranium tailings and its uptake by plants at Jaduguda, Jharkhand, India. CURRENT SCIENCE, VOL. 98, NO. 1, 10 JANUARY 2010

10. CMP-24EDIT2 (13July04).doc. Chemicals from industrial activities. Economopoulos AP (1993). Environmental technology series: Assessment of sources of air, water, and land pollution: A guide to rapid source inventory techniques and their use in formulating environmental control strategies, Part one: Rapid inventory techniques in environmental pollution, World Health Organization, Geneva.

11. http://www.gisdevelopment.net/application/health/planning/mwf09_aditya.htm 12. Soil, Plant and Water analysis” by. P.C. Jaiswal . ISBN: 8127232262 ISBN-13: 9788127232269, 978-8127232269 Binding:

Paperback Publishing Date: 2006 Publisher: Kalyani Publishers / Lyall Bk Depot 13. “Practical Environmental Analysis” by Miroslav Radojecic Miroslav Radojević, Vladimir Nikolaevich Bashkin, Royal

Society of Chemistry (Great Britain) 14. Association of Official Analytical Chemists (AOAC) 15. Standard method American Public Health Association (APHA), American Water Works Association (AWWA) and Water

Environment Federation (WEF) 16. Standard method SW846-7471A (USEPA/SW/846, Rhodes, J.D (1982), Subbaiah and Asija (1956), W & O Method, Hanway

and Heidel (1952).) 17. Kolthoff, I.M. and Elving, P.J., Treatise on Analytical Chemistry, part II, Vol. 9 (1962)

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