CHAPTER VI RADIOACTIVITY IN VEGETABLES AND WATER. Vegetables are essential components of human diet as they

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1 CHAPTER VI RADIOACTIVITY IN VEGETABLES AND WATER 6.1. Introduction. Vegetables are essential components of human diet as they contribute starch, protein, vitamins, iron, calcium and other minerals. (Thompson and Kelly, 1990). They act as a buffering agent for acidic substances secreted during digestion. Vegetables and crops grown in active area can pick up a small fraction of the soil activity along with other minerals through root uptake (Eisenbud et al., 1997). Accumulation and transfer of radionuclide from one environmental compartment to another through root uptake in biological systems depend upon the availability of nuclides in soil. A series of studies in high background radiation areas have revealed interesting information on accumulation in plants (Paul et al., 1998). Kua et al., (1997) have evaluated the 226 Ra activity and estimated the dose of the residents of Taiwan. Leafy vegetables accumulated more 226 Ra than other vegetables and Kua et al (1997) have related the concentration of 226 Ra in all vegetables to that of the 107

2 soils in which they grow. The radionuclides 226 Ra and 228 Ra and their decay products are responsible for the major fraction of the dose received by humans from the naturally occurring internal emitters. Ghiassi Nejad et al., (2002) have evaluated the intake of 226 Ra in the city of Ramsar in Iran and found the maximum uptake of 226 Ra in leafy vegetables and the minimum in root vegetables. The vegetable to soil concentration ratio (CR) for 226 Ra shows the highest value of and the lowest value of for leafy and root vegetables respectively. Ross et al., (2007) have assessed the natural radionuclides in vegetables and fruits around Kudankulam Nuclear Power Project and found that 228 Ra activities in vegetables are at a much lower level than that of the high background radiation areas in Brazil but a little higher than those recorded around Kalpakkam Reactor Sites. Radium-226 activity concentration was high in leafy vegetables when compared to that of non-leafy vegetables and tubers. Shanthi et al., (2009) have compared the activity concentration of radionuclides in different vegetables and the effective dose in low and high background areas of Kanyakumari District in Tamil Nadu. The activity concentration of radionuclides such as 226 Ra, 228 Th, 238 U and 40 K was found to be higher in HBRAs compared to LBRAs. The daily intake of radioinuclides from food 108

3 crops grown and consumed was Bq and the daily internal dose resulting from ingestion of radionuclides in food was 2.3 µsv y -1. The south west coast of the Indian peninsula is a radioactive `hotspot` with its high activity due to thorium and uranium nuclides as reported from earlier studies (Rajamonickam, 2000) along the Manavalakurichi, and Midalam coasts in Kanyakumari extended to the Chavara region, in Kerala. The presence of primordial radionuclides such as 238 U and 232 Th in the biotic systems has been widely experimented (Lalit and Shukla, 1982). There is a definite link between the plant and the substrate soil, where the radionuclide if present may appear in the plant organs along the roots. The distribution of these radionuclides in different parts of the plant depends on the biogeochemical characteristics of the soil. The elevated levels of radionuclide in the soil often results in the proportionate uptake by the plants which in turn will result in increased radiation dosage in the herbivores, through their food chain (Varughese et al., 2008). Studies on the radioactivity of consumable items assume importance in view of its necessity to estimate the ingestion dose passed on to the consumer. The present study undertakes at least in part, to reveal the link between the activity of the plant and the soil 109

4 and an evaluation of the possible biological hazards in the consumption of vegetables in terms of effective dose and transfer factor Materials and Methods Type of Vegetables. The vegetables collected for radionuclide estimation can be classified into four categories namely leafy vegetables, root vegetables, non-leafy vegetables and fleshy vegetables. Leafy vegetables studied include red spinach (Amaranthus viridis) and drumstick leaves (Moringa olefera) whereas non leafy vegetables are ladies finger (Abelmoschus esculentus), drumstick (Moringa olejfera), gooseberry (Phyllanthus emblica) and coconut (Cocos nuczfera). Fleshy vegetables such as cucumber (Cucumis sativus), tomato (Solanum lycopersicun), papaya (Carica papaya) and tapioca (Manihot esculenta), the only root vegetable are selected for this study Sample collection and pre-concentration. Representative soil samples were collected from the root regions of the plants from a depth of about 150 cm in the high activity stations of the Kadiapattinum, Chinnavilai and Manavalakurichi, coastal villages viz (Fig.1.1) along the south west coast of India already identified as a high background radiation area (UNSCEAR, 2000). Three samples from each area were collected and 110

5 crushed into fine powder by using agate mortar. Before measurement the soil samples were dried in an air- oven at a temperature of 110ºC for 24 hours. Each sample was packed and sealed in a polythene bag that was kept in an air tight container. The sealed samples were stored for about four weeks before gamma analysis was performed, to allow 226 Ra and its short- lived progenies to attain equilibrium. Fresh vegetables and fruits grown in this area collected in fresh polythene bags and brought to the lab, were first washed in tap water and then in distilled water, to remove all attached sand and dust particles. The initial wet weight of the samples were noted. They were first dried in an electric oven at a temperature of 150 o C for about 48 hours and then ashed in a silica crucible using Muffle furnace at 700 o C, for 8 hours Radioactivity measurements. The concentration of gamma ray emitting radio isotopes in the samples were measured by employing high efficiency 48 mm 48 mm NaI (Tl) detector. The detector has a resolution of about 7% and an energy of 662 kev. The 238 U and 228 Th activities were calculated through 1764 kev of 214 Bi and kev of 208 Tl respectively and 40 K activity was calculated through 1460 kev from the net area under each photo peak after deducting the background activity. The gamma spectrum was recorded using a PC based multi channel 111

6 analyzer and processed using the NETSWIN software (Shanthi et al., 2009). From the net area within peak, the activity concentrations in the samples were obtained using the equation. where Ac = C / (m Pγ ε) Ac is the activity concentration Bq kg -1 of the radionuclide in the sample. C is the count rate obtained under the corresponding peak (s -1 ) m is the sample mass (kg) Pγ the emission probability and ε is the detection efficiency at a specific energy. The gamma radiation absorbed dose rate in air D R ngy h -1 was calculated as D R = C Th C U C K where C Th, C U and C K are the activity concentrations Bq kg -1 of thorium, uranium and potassium in the soil samples. The annual effective dose (HR) was calculated using the following equation that converts the absorbed dose rate ngy h -1 in air to effective dose msv HR = DR x 8760 h x 0.2 x 0.7 Sv Gy

7 Activity concentration in soil and vegetables. The variation in activity levels in soils of different places may be attributed to the wide variations on geological formation of different types of soils. The activity concentration of soils of ten different sampling stations and the total effective dose are as recorded in (Table.6.1). All the soil samples exhibit appreciable levels of uranium, thorium and potassium activity compared to the global average of 25.0 Bq kg -1, 35.0 Bq kg -1 and Bq kg -1 respectively (UNSCEAR, 2000). The highest values (23.5 ± 0.9 Bq kg -1, ± 0.3 Bq kg -1 and 1021 ± 0.1 Bq kg -1 for 238 U, 232 Th and 40 K respectively are recorded in station-1 (Fig.6.1.) whereas the mean values in this area are 17.8 Bq kg -1, Bq kg -1 and Bq kg -1 respectively. The absorbed dose rate (D R) at the ten different sampling stations in the study area, ranges between ngy h -1 and ngy h -1. The ariel dose rates (Hand survey) also follow a similar order (63 ngyy -1 to 258 ngy y -1 ) obviously under the impact of the soil radionuclides. The annual effective dose (outdoor) vary from 0.07 to 0.25 with the mean value of 0.15 msv y -1. This is too high compared to the world average of 0.07 msv y -1. The annual effective dose (indoor) also varies from 0.29 to 0.96 msv y -1 with the mean value of 0.64 msv y -1. The vegetable samples too exhibit proportionately high thorium activity especially in tubers and leafy vegetables. Tapioca, 113

8 papaya and red spinach have recorded the maximum values (17.35 Bq kg -1, Bq kg -1, and Bq kg -1 ) with correspondingly higher values for uranium (Fig.6.1 & 6.2) Concentration Factor. Radionuclide in the soil can reach human body through food, air and water. Vegetables and crops grown in active area can absorb a small fraction of the soil activity along with other minerals through the root system. The ability of various plant species to absorb radionuclides from soil or other substrates expressed in terms of concentration ratio (CR) is determined by (Lima and Penna-France 1988; Morredt, 1994). CR = Concentration of radionuclide in dried vegetables (Bq kg -1 ) Concentration of radionuclide in dried soil substrate (Bq kg -1 ) Concentration Factor in vegetables is a simple ratio between the concentration of an element in individual species to the concentration in the medium in which it grows. These factors can be of immense help for quick environmental impact assessment and implementation of counter measures. It is also used for assessing the consequences of radiation exposure to non human biota (Choi et al., 2008). 114

9 Table.6.3. shows the concentration factor for the respective nuclides in vegetables due to root uptake through food and water. The intake of 238 U and 232 Th through dietary item is significant as indicated by the high concentration ratio in many vegetables. Not surprisingly the uptake factor for potassium is found to be uniformly high in all the vegetables, as it is one of the major nutrients for plants. Whereas tapioca, papaya, ladies finger and cucumber have a high intake of 232 Th from the soil, drumstick, red spinach, coconut and tomato exhibit a higher tendency to absorb 238 U. But, the activity concentration of 232 Th in vegetables is one order higher in all samples compared to that of 238 U (Table.6.2). Thus thorium contributes more to the effective dose in vegetables than that of uranium. Potassium-40 absorption by the plant though one order higher compared to even that of thorium, the dose rate depends mainly on the 232 Th concentration in vegetables due to its large conversion factor (0.623). Moreover, the proportional intake of thorium and uranium in plants ( 232 Th / 238 U) follows the same order as that in the soil (8.01). However thorium activities in soil and vegetables are in direct correlation in tapioca, red spinach, coconut, cucumber and ladies finger as observed (Fig. 6.3.) from the highly significant correlation coefficient (r =0.8727). 115

10 Papaya and tubers in general, tapioca in particular have recorded the highest gamma activity. The high transfer factor reported here for tapioca and papaya reveals the high intake of radionuclide through their root system with multiplied thin hair roots spread all over the surface soil and hence tapioca and papaya grown in this area have high activity and transfer factor. A succulent fruit like papaya has the highest transfer factor indicating the vulnerability of the consumer. Cucumber and ladies finger consumption could be safer as noticed from their relatively low activity and transfer factor Activity of water. Among the three essential media of life, water is fundamental to all forms of life making up a larger percentage of weight of plants, animals and the human body, as all biological functions and cell metabolism occur under this medium. Agricultural operation and drinking water needs are satisfied by the ground water sources which get polluted fast due to natural and anthropogenic activities. Water systems that are vulnerable to radioactive contamination are required to undergo extensive monitoring to ensure safety. However, the contribution due to primordial radionuclides which are the constituents of soil in this area where the present studies are undertaken needs to be investigated. The aim of this study is to determine the activity concentration of these radionuclides in the 116

11 drinking water sources such as well water and bore water consumed by the local inhabitants, in order to ascertain the possible contribution to health effects. Ground water contamination occurs when hazardous substances come into contact and dissolve in the water that has soaked the soil. Advection, diffusion, dispersion and adsorptions of contaminants are the different modes of contamination of ground water. The most prevalent human activities that cause ground water contamination are agricultural activities, waste disposal, storage and transport of commercial materials, mining operations etc. Measurements of natural radioactivity in drinking water have been performed in many parts of the world, mostly for assessment of the risk resulting from consuming water. It was found that most activity is from 222 Rn, whose levels showed some variation from place to place and also with the sources of the water. The levels of 222 Rn were found in the ranges kbq m -3 in Nigeria (Farai and Sanni 1992), kbq m -3 in Slovania (Kobal et al. 1990), 1-29 kbq m -3 in Poland (Grzybowska et al. 1983), kbq m -3 in Bulgaria (Karamihailova and Zheku 1976), kbq m -3 in France (Bizollon et al. 1971), and up to 4.8 MBq m -3 in Finland (Asikainen et al. 1980). 117

12 It was also found that the second source of radioactivity in drinking water was 226 Ra. The levels of 226 Ra were found to range between Bqm -3 in each of the Slovania (Kobal et al. 1990), France (Bizollon et al. 1971), and Poland (Grzybowska et al., 1983), but this levels were much higher in the USA (Holbort et al. 1995), and Finland (Asikainen et al. 1980), where they reached a few kbq m -3. The uranium level in drinking water has been reported by several authors, ranging between Bqm -3 in Slovania (Kobal et al., 1990), Bqm -3 in France (Bizollon et al., 1971), Bqm -3 in the USSR (Shchepak 1970), and Bqm -3 in Finland (Asikainen et al. 1980). The determination of radionuclides in drinking water became increasingly important within these HBRAs, since water is very important to all forms of life making up a larger percentage of the weight of all plants, animals and human body. The limit for the uptake of radionuclides via drinking water has been established in the form of a total indicative dose of 0.1 msv y -1. However, the total indicative dose cannot be measured directly but has to be calculated from the summed up contribution of each natural or artificial radionuclides present in water. The parameters of choice are the gross-alpha and gross-beta activity concentration. If the gross-alpha 118

13 activity in a tap water sample is lower than 0.1 Bq l -1 and the grossbeta activity does not exceed 1.0 Bq l -1 it is understood that the annual total indicative dose of adults is less than 0.1mSv y -1. It has been found that uranium and radium are the major contributors for gross-alpha activity in drinking water (Wisser 2003). Ten liters of water (well water) collected from each sampling station in plastic carboys was filtered with Whatman filter paper, precipitated with dihydrogen ortho phosphate, calcium carrier (2 ml) and little ammonia and the precipitate of calcium ortho phosphate was kept undisturbed for a full night. Then the supernatant liquid was decanted, the precipitate was dissolved with concentrated HCl and was heated in an electric furnace to reduce the volume. Concentrated H 2SO 4 and 1ml of Barium carrier was added with the liquid and barium sulphate precipitate was obtained. Then the solution was centrifuged. BaSO 4 precipitate was taken in a clear aluminum planchat and dried in hot air oven at a temperature of C for two hours and cooled. The gross alpha, gross beta and the concentration of different radionuclides were determined using alpha, beta and gamma detectors. The gross alpha, gross beta activities and the activity concentration of the primordial radionuclides (Table.6.4.) such as 238 U, 232 Th and 40 K are not significantly high. The gross alpha activity 119

14 ranges from 0.02 to 0.05 Bq l -1 with the mean value of 0.02 Bq l -1 while the gross beta activity varies from 0.02 to 0.09 Bq l -1 with a mean value of 0.05 Bq l -1. The gross beta activity is found to be higher than gross alpha in almost all the sampling stations. This is probably due to the presence of 228 Ra a beta emitter with considerable activity. Previous studies too have indicated the presence of this isotopes (Wisser, 2003). The concentration of 232 Th, 238 U and 40 K are in the range of 1.02 to Bq l -1 (mean 6.23 Bq l -1 ), 1.11 to 2.31 Bq l -1 (mean 1.30 Bq l -1 ) and 0.03 to Bq l -1 (mean 5.10 Bq l -1 ) respectively. As expected the activity concentration level of 232 Th is more pronounced than the concentration level of 238 U and 40 K. Moreover the activity is comparatively high in Kadiapattinam, Chinnavilai and Periavilai which are areas of known high background radiation as reported elsewhere in the thesis. The resulting trend however shows that radiological health burden with respect to water on the human populace is very minimal and bound to have neither health implications nor contributing significant to background radiation. 120

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