Radioactivity measurements and risk assessments in soil samples at south and middle of Qatar
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1 Radioactivity measurements and risk assessments in soil samples at south and middle of Qatar A. T. Al-Kinani*, M. A. Amr**, K. A. Al-Saad**, A. I. Helal***, and M. M. Al Dosari* *Radiation and Chemical protection Department, Ministry of Environment, P. O. Box 7634, Doha, Qatar. **Department of Chemistry and Earth Sciences, Qatar University, P. O. Box 2713, Doha, Qatar. ***Department of Nuclear Physics, NRC, Atomic Energy Authority, Cairo, 13759, Egypt. ABSTRACT Health risks associated with the exposure to the natural radioactivity present in soil materials have great concern all over the world. Thus soil samples were collected from an urban areas at south and middle of Qatar in order to measure natural radioactivity, 40 K, 226 Ra and 232 Th and the artificial 137 Cs using gamma-ray spectrometry method. The soil activity concentrations ranged from for 226 Ra, for 232 Th and for 40 K with mean values of 57, 87 and 207 Bq/ kg, respectively. The concentrations of these radionuclides were compared with the available data from other countries. The average and ranges of activity concentration of 226 Ra in Qatar soil areas are very much comparable to the world figures. However, the concentration for 232 Th is comparable to other Gulf area and lower than that for Egypt and the world figures. The concentration for 40 K is lower as compared with Egypt and Kuwait figures, but it was comparable to Oman figures. The radium equivalent activity (Ra eq ) in these soil samples ranges from Bq/kg to Bq/kg) with a mean value of 57.4 Bq/kg which is far below the safe limit (permissible) limit (370 Bq/kg). The calculated values for external hazard index H ex for the soil samples ranged from and the average concentration of was lower than other values reported. However, these values are lower than unity; therefore, the soil from these regions is safe and can be used as a construction material without posing any significant radiological threat to population. The absorbed dose rate calculated from activity of 226 Ra, 232 Th and 40 K ranges between , , and ngy/h, respectively, and the total average absorbed dose rate ngy/h was lower than the world wide average absorbed dose rate 51 ngy/h. The total absorbed dose in the study areas ranged from ngy/ h with an average value of ngy/h. The corresponding outdoor and indoor annual effective doses ranged from 49.5 to µsv and to µsv with an average value of and µsv, respectively. Whereas the world wide average annual effective dose is approximately 460 µsv. Key Words: Natural Radioactivity/ Hazard Index/ Risk Assessment. INTRODUCTION Human beings and other living matters have always been exposed to natural radiations arising from naturally occurring radioactive elements in the soil and rocks, cosmic rays from outer space and the internal exposure from radioactive elements in food, water and air. The natural radioactivity in soil primarily comes from 238 U and 232 Th series (and their decay progeny) and the primordial radionuclide 40 K. These radioisotopes contribute to the dose received by human being through external exposure -200-
2 and internal exposure due to their ingestion and inhalation. Because of the natural or artificial processes, radionuclides may accumulate and be concentrated in selected areas of the environment. The fallout resulting from the nuclear weapon tests are released into the atmosphere and they travels at great altitudes. They gradually fall to earth and are washed down in rain. 137 Cs, one of the fission products, is strongly absorbed and retained by soil particles as are the natural radionuclides. External gamma dose estimation due to the terrestrial sources is essential because it contributes to the collective dose. These doses vary depending upon the concentrations of the natural radionuclides series, and their daughter products and 40 K, present in the soils and rocks, which depend upon the local geology of the selected region. Background radiation due to local geology and geochemical effects cause enhanced levels of terrestrial radiation (UNSCEAR 2000). Therefore, measurements of natural radioactivity in soil are of a great interest for many institutions throughout the world. To evaluate the terrestrial gamma dose rate for outdoor occupation, it is very important to estimate the natural radioactivity level in soils. The present work was conducted to ascertain the overall contributions of fallout 137 Cs and natural 40 K, 226 Ra and 232 Th in the Quatrain soil samples. Which include measurement of radium equivalent activity (Ra eq ), the absorbed dose rate in the air (D) at height of 1m above the surface of ground and Radium Equivalent, External Hazard Index (H ex ), to assess possible radiological hazards to human health. Material and methods: Sampling EXPERIMENTAL Twenty one soil samples were collected from middle and south parts of Qatar. Most of investigated soil samples were collected near Saudi border. The geographic location of the study areas are between the latitude and longitude , as shown in Figure (1). The soil was collected at a depth of about 20 cm from the ground surface to get the natural soil. Soil samples were filled into labeled polyethylene bags and sealed. Fine quality of the sample is obtained using scientific sieve of 150 micron-mesh size. The samples were crushed into fine powder by using Mortar and Pestle to get rid of stones. Before measurement samples are dried in an oven at a temperature of 353 K for 24 h to ensure that any significant moisture was removed from the samples. Each soil sample is packed and sealed in an airtight PVC 200 or 1000 ml Marinelli beaker and kept inside refrigerator for about 4 weeks period to allow secular radioactive equilibrium among the daughter products of radon ( 222 Ra), thoron ( 220 Ra) and their short lived decay products. Table (1) shows the number, ID, coordinate, and weight of soil samples collected from investigated area. Measurements: Using coaxial hyper-pure germanium detector (HPGe) (Canberra) based on high-resolution gamma spectrometry system, the activity of samples is counted. Each soil samples was placed on the crystal detector and analyzed using a high-resolution, low-background gamma-ray spectroscopy. The detector has a resolution of 2.5 kev and relative efficiency of 20% for MeV gamma energy of 60 Co. The output of the detector is connected to PC. The spectral data is analyzed using the Genie 2000 Gamma Analysis Software package. Each spectrum was acquired for seconds (24 hours). The detector was surrounded by a lead shield lead on all sides to reduce the background radiation level of the system, and lined inside with copper sheets to minimize the X-rays emitted due to interaction of cosmic radiation with lead. The absolute photo-peak efficiency calibration of the system were carried out using standard 152 Eu because of its suitable half-life and the wide range of gamma ray energies produced during its decay process (121.8 kev kev) and mixed source containing ( 57 Co, 60 Co, 137 Cs, and 203 Hg) which have an identical geometry to the soil samples
3 Fig (1). Locations of samples collection. A Marinelli beaker with the same geometry filled with de-ionized water was used to determine the background spectrum observed by the germanium detector. The counting time of the ambient background spectrum was also for 24 hours. The samples were placed, in their Marinelli beakers, directly on to the front face of the detector. The counting geometry of the samples and the standard sources used for efficiency calibration were kept constant. A gamma-ray energy transitions lines ranging from ~100 kev up to MeV, associated with the decay products of the natural series were then analyzed independently to obtain more statistically significant overall results. These data were combined under the assumption of secular equilibrium of the radionuclides within these samples. The natural radioactivity in soil primarily comes from U and Th series and natural potassium. They are essential parameters in determining the natural radioactivity concentration levels and their behavior in -202-
4 the environment. Artificial radionuclides can also be present such as 137 Cs from the fallout of nuclear weapons testing and from accidents such as Chernobyl. Such data can be used as a baseline from which to detect any future artificial release of radioactive radionuclides. Table (1): Number, ID, Coordinate, and Weight of Sample collected from investigated area. NO Sample ID Weight of Sample (g). Longitude x Latitude y The activity levels for radionuclides in the measured samples are computed using the following equation: where A is the activity level of a certain radionuclide expressed in Bq/Kg dry weight, C is the net counting rate of sample subtracted from background (counts per seconds), ɛ is the counting efficiency of the used detector, P is the absolute transition probability of γ-decay and W is the dried sample weight expressed in Kg. The specific radioactivity of 226 Ra under the peak energy of kev are the sum of 235 U under the peak energy of kev and peak energy of 226 Ra alone. Thus the radioactivity of 226 Ra alone calculated by subtracting the specific radioactivity of 235 U which is calculated from the peak -203-
5 energy of kev from the total specific radioactivity calculated for 226 Ra. The measured activity concentrations for 232 Th series in the samples were calculated from 228 Ac and 212 Pb decay assuming equilibrium decays of 228 Ac and 212 Pb in the 232 Th series. The external hazard index is an evaluation of the hazard of the natural gamma radiation. The prime objective of this index is to limit the radiation dose to the admissible dose equivalent limit of 1 msv/y. The external hazard index should be below the unity for the radiation hazard to be negligible The external hazard index H ex can be calculated by the following equation cited by (Beretka and Mathew 1985): H ex = C Ra /370 + C Th /259 + C K / where C Ra, C Th and C K are the activity concentrations of 226 Ra, 232 Th and 40 K in Bq/kg, respectively. The values of this index must be less than one in order to keep the radiation hazard without posing any significant radiological threat to the population. The terms of radium equivalent activity (Ra eq ) in Bq/kg are used to compare the radiological effect or activity of material that contain 226 Ra, 232 Th and 40 K in soil. Ra eq is used to assess the radiation hazards associated with these materials that provide a guideline in regulation safety standards on radiation protection for general public living in the area under investigation. Ra eq is calculated by the following equation (Yu et al 1992): Ra eq = C Ra C Th C K where C Ra, C Th and C K are the activity concentrations of 226 Ra, 232 Th and 40 K, respectively in Bq/kg. Ra eq was calculated assuming that 370 Bq/kg of 226 Ra or 259 Bq/kg of 232 Th or 4810 Bq/kg of 40 K produce the same gamma dose rate. The total external terrestrial gamma radiation absorbed dose rate (D) in air due to gamma rays emitted by the 214 Pb, 214 Bi, 226 Ra, 232 Th decay chain and 40 K at 1 m above the ground level. Using the conversion factor of ngyh -1 /Bqkg -1 for 40 K, ngyh -1 /Bqkg -1 for 226 Ra, and ngyh - 1 /Bqkg -1 for 232 Th (UNSCEAR 1993). These conversion coefficients were originally determined from Monte Carlo calculation using mathematical phantoms UNSCEAR (1993). In the above conversion factors, it is assumed that all the decay products of 226 Ra and 232 Th are in radioactive equilibrium. The published maximal admissible (per missible) dose rate is 55 ngy/h. The following equation can be calculated by (Mehra et al 2007): D (ngy/h)=0.461 C Ra C Th C K where, C Ra, C Th andc k are the activity concentrations (Bq/kg) of radium, thorium and potassium in the samples. Assuming that 137 Cs and the 235 U decay series can be neglected as they contribute very little to the total dose from environmental background. Calculation of annual effective dose in the outdoor and indoor, account must take the conversion coefficient from absorbed dose in air to effective dose and (0.7 Sv/Gy) which is used to convert the absorbed rate to human effective dose equivalent. Annual estimated average effective dose equivalent received by a member is calculated using an indoor and outdoor occupancy factor of 80% and 20% respectively. The annual effective doses are determined as follows Mehra et al (1997): Indoor (nsv) = (Absorbed Dose) / ngy x 8760h x 0.8 x 0.7 Sv/Gy Outdoor (nsv) = (Absorbed Dos) / ngy x 8760h x 0.2 x 0.7 Sv/Gy -204-
6 RESULTS AND DISCUSSION Figure (2) shows the background-subtracted spectrum for sample number 2605 and clearly shows transitions associated with decays from the 226 Ra, 214 Pb, and 214 Bi isotopes associated with the 238 U decay chain, as well as 228 Ac and 212 Pb decay lines from the 232 Th series. Fig. (2): Background-subtracted gamma-ray spectrum associated with sample number Table (2) summarizes the results of measurements of natural radionuclide ( 226 Ra, 232 Th, and 40 K) concentrations in the collected soil samples. Analysis of the results indicates that there is some degree of a positive correlation between the activity concentrations of 232 Th and 40 K since the concentration of 40 K increases as the concentration of 232 Th increases in the soil samples. Table (2) shows the radium equivalent activity (Ra eq ) in these soil samples ranging from Bq/kg to Bq/ kg) with mean value of 57.4 Bq/kg, which is far below the safe (permissible) limit (370 Bq/kg) recommended by Bereka and Mathew (1985). Table (3) shows the calculated values for external hazard index H ex for the soil samples ranging from to 0.21 and average concentration was The absorbed dose rate calculated from activity concentration ranged between and ngy/h for 226 Ra and between and ngy/h for 232 Th, and between and ngy/h for 40 K. The average absorbed dose rate ngy/h was lower than the world wide average absorbed dose rate, 51 ngy/h UNSCEAR (2000)
7 Table (2): Activity concentration of 226 Ra, 232 Th, 40 K and 137 Cs using gamma ray spectrometry and H ex in the soil samples from Qatar. Sample No ID 226 Ra Radionuclide concentration Bq/kg 137 Cs 232 Th 40 K Ra eq (H ex ) ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± Average
8 Table (3): Air-absorbed dose rates and annual effective doses at some locations of Qatar. Sample No average 232 Th Absorbed dose (ngy/h) 226 Ra K Total Annual effective dose (µsv ) outdoor indoor
9 The total absorbed dose in the study area ranged from to ngy/h with an average value of ngy/h. The corresponding outdoor and indoor annual effective doses range from 49.5 to µsv and to 24.78µSv with an average value of and µsv respectively while the world wide average annual effective dose is approximately 460µSv UNSCEAR (2000). CONCLUSION The average activity concentration of 226 Ra in Qatar soil equal (32.02) is similar to the world figures (35 Bq/kg) reported in UNSCEAR (2000), and it is also very much similar to Oman, Spain, and Hungary concentration (29.7, 32, and 33 Bq/kg respectively). The average activity concentration of 232 Th in Qatar soil is equal 8.88 Bq/kg. This is similar to the activity concentration of Kuwait (10 Bq/kg) and lower than world figures ( 30 Bq/kg) depending on geological formation of soil. The average activity concentration of 40 K in Qatar soil ( Bq/kg) are very much similar to that of Oman and Kuwait (225 and 370 Bq/kg respectively). The calculated average value of external hazard index (H ex ) for Qatar soil sample is 0.164, which is lower than values compared to figures reported by (Mehra et al 2007). However, these values are lower than unity; therefore, the soil from these regions is safe and can be used as a construction material without posing any significant radiological threat to population (European Commission. Radiation Protection report). The average of the indoor and outdoor effective dose due to natural radioactivity of soil samples is lower than the average national and world recommended value of 1.0 msv/y. Artificial radionuclides can also be presented including 137 Cs from the fallout of nuclear weapons testing and from accidents such as Chernobyl are essential parameters in determining the natural radioactivity concentration levels and their behavior in the environment. Such data can be used as a baseline from which to detect any future artificial release of radioactive radionuclides. ACKNOWLEDGMENT This article was made possible by NPRP award [NPRP ] from the Qatar National Research Fund (a member of The Qatar Foundation). The statements made herein are solely the responsibility of the authors. REFERENCES (1) A. T. Al-Kinani; Iran J. Radiat. Res.; 4, 143 (2006). (2) K. A. Al-Saad, M. A. Amr, A. Ismail, A. I. Helal; J. Environ. Chem. and Ecotoxicol.; 2, 60 (2010). (3) WHO Depleted Uranium Sources, Exposure and Health Effects. World Health Organization, Vienna (2001). (4) R. Mehra, S. Singh, K. Singh, R. Sonkawade; Environ. Monit. Assess.; 134, 333 (1997)
10 (5) European Commission. Radiation Protection 112 Radiological protection principles concerning the natural radioactivity of building materials. Brussels: European Commission (1999). (6) UNSCEAR. United Nations Scientific Committee on the effects of atomic radiation. Effects and risks of ionizing radiations. New York: United Nation (2000). (7) UNSCEAR. Sources and Effects of Ionizing Radiation. United Nations Scientific Committee on the effect of atomic radiation. New York: United Nations (1993). (8) K. N. Yu, Z. J. Guan,, M. J. Stoks, E. C. Young; J. Environ. Radioact.; 17, 31 (1992). (9) J. Bereka, P. J. Mathew; Health Phys; 48, 87 (1985)
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