EPJ Nuclear Sci. Technol.
Volume 8, 2022
|Number of page(s)||7|
|Published online||09 August 2022|
The activity concentrations of radionuclides 226Ra, 232Th and 40K of soil samples in the case of Metekel Zone, Ethiopia
Department of Physics, Debre Tabor University,
Debre Tabor, Ethiopia
* e-mail: email@example.com
Received in final form: 4 April 2022
Accepted: 22 June 2022
Published online: 9 August 2022
In this paper, we have studied the concentration levels and corresponding radiological hazard indices of natural radioactive elements such as radium-226, thorium-232, and potassium-40 in soil samples collected from Metekel Zone, Ethiopia. We have determined the concentration levels with the help of gamma ray spectrometry. Accordingly, we obtained the average values for radioactive concentrations of radium, thorium, and potassium to be 64 Bq/kg, 70 Bq/kg, and 330 Bq/kg, respectively. The radiological hazard has been also determined from the pertinent concentration levels of radium, thorium and potassium isotopes. Therefore, we obtained that the radioisotopes have heterogeneous distribution which must be caused by the nature and types of the soil in the area where this investigation was conducted for.
© T. Abate, Published by EDP Sciences, 2022
This is an Open Access article distributed under the terms of the Creative Commons Attribution License (https://creativecommons.org/licenses/by/4.0), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.
Man is continuously exposed to natural radiations that are present on earth since its creation. The knowledge of radionuclides distribution and radiation levels in the environment is important for assessing the effects of radiation exposure due to both terrestrial and extraterrestrial sources . Terrestrial radiation is due to the radioactive nuclides present in the varying amounts in soils, building materials, water, rocks and atmosphere while the extraterrestrial radiation originates from the outer space as primary cosmic rays . Natural radiations arises mainly from primordial nuclides such as 40K and the radionuclides from 226Ra and 232Th series and their decay products which occur at trace levels in all ground formations [1,3]. Soil, being the major source of natural radioactivity, is the raw material for buildings used in Metekel Zone.
Natural radioactivity present in soil produces gamma radiations in the environment and changes the background radiations level. Everyone in the planet is exposed to these background levels of ionizing radiations. External exposure occurs as a result of irradiation and internal exposure because of inhalation and ingestion . Since the natural radiation is the largest contributor to the external dose of world population, the assessment of gamma radiation dose from natural sources is of particular importance [4–6].
Thus, Radon is decay product of radium (226Ra) that is the part of uranium (238U) decay chains. Radon and its progenies are the major contributor in the atmosphere which is responsible for about half of radiation dose received by general population [1,2]. Radon is also the second major cause of lung cancer after smoking [5,6]. Indoor radon concentration depends upon the existence of natural radioactivity in the underlying soil or rock of a dwelling [5–7]. So, it is important to assess the radiation hazards arising due to use of soil samples in construction of dwellings . Many researchers have estimated the natural radioactivity levels and associated health hazards in the world [8–13].
In this study, the natural radioactivity levels in the soil samples of Metekel Zone are measured by gamma ray spectrometery using p–type high purity germanium semiconductor detector. The work in the study area has been carried out for the first time and will be of general interest to the inhabitants as the knowledge of radioactivity levels in the soil samples will provide awareness among them about the safety guiedrule development and radiological effects on their health. The results of this study have also been compare with the corresponding results found across the world.
Benishangul Gumuz is one of the regions of Ethiopia in North west part of it. Metekel zone is therefore found in this region and covers two–third of the total area of the region . It is bordered on the south and southwest by Kamashi, on the west by Sudan, and on the north and east by the Amhara Region. The Abay River defines the Zone’s boundaries with Kamashi, while the Dinder River defines part of its boundary with the Amhara Region as shown in Figure 1 . The administrative center of Metekel Zone is Gilgil Beles. The highest point is Mount Belaya which has 3,131 meters and is part of the Dangur range .
Map of the study sites in Benishangul Gumuz province, Ethiopia. The astriks shown the areas (districts) where the samples were collected .
The study sites are highly mineral rich (specially gold rich) areas and the income of the population around these places is traditional gold mining in addition to bamboo and crop production. Also, Metekel Zone is the location of seven districts (woredas): Guba, Dangur, Pawe, Mandura, Wenbera, Bulen, and Dibate. All the soil types such as Sandy loam, Sands, Silt, Clay, Silty clay, Clay loam, and so on are found in these districts . For this study, six different types of soil samples: Sandy loam, Sands, Silt, Clay, Silty clay and Clay loam were collected from each distric. Specifically, We have taken 24 samples from Dangur and Wombera, 4 samples from each soil types, and 18 samples from Bullen and Guba woredas in which 3 samples from six soil types. However, a total of 12 samples were taken from each of Pawe, Mandura and Dibate districts and 2 from each soil types based on the area of districts as shown in Figure 1. During sample collection, we have taken the samples from the surface of the earth at some depth and from predpared soils for constructions equivalently. The total of 120 representative samples, from North West Ethiopia were collected using a grab sampling method. When we have sampled selected soil samples, the depth of holes below the surface of earth were 0.5 m, which helps to obtain a better mineral content that could give the expected results. In addition, we used a distance of 2–3 m between samples based on the area of study sites, which allowed us to take proposed samples. These samples were collected in a new and transparent plastic bag containers from the soil surface of depth 0.5 m and cataloged according to location and type where they collected. A total of one hundred twenty samples were collected in seven Districts of Metekel Zone based on the geographical location.
Each sample was grained and dried in a temperature controlled oven at the temperature of 115 °C for about 15 hours to remove moisture, and also sieved through 200 µm mesh to obtain the fine powder of a homogeneous sample. About 100 g of samples were packed in gas tight, radon impermeable, cylindrical plastic containers (Marinelli beakers) which has 7 cm diameter and 10 cm height for gamma activity analysis . Before measurements, radon sealing is done by placing the sample container into an aluminum-lined bag and evacuating it using a Henkovac Mini Eco commercial vacuum packaging machine. The containers were kept packed for thirty two days in order to ensure that the short lived progeny of 226Ra and 222Rn have arrived equilibrium with their respective parent radionuclides.
Gamma ray spectrometery measurements were conducted with 45% efficiency p–type high purity germanium detector coupled to a multichannel analyzer was used for radioactivity measurements [4–6]. The selected detector has a high efficiency for typical samples, the high purity germanium detector is the Canberra Broad Energy Germanium (CBEGe) which exhibits lower background than typical coaxial detectors since it is more transparent to high energy gamma from naturally occurring radionuclides such as 40K and the Thorium series of 208Tl . The detector was shielded in a 5 cm thick lead on all sides including top to reduce background due to cosmic ray component by almost 98% and the inner sides of the lead lined with 2 mm copper foils. The spectrum acquisition and processing were made possible by coupling the detector output to an ORTEC Multi-Channel Analyzer (MCA) alongside a PC equipped with Genie 2000 evaluation software that matches gamma energies to a library of possible isotopes. Prior to counting the samples, efficiency and energy calibrations of the detector were carried out for various energies of interest in the selected sample geometry following the calibration procedures described by the International Atomic Energy Agency . The efficiency calibration was achieved by using a 450 g mixed Canberra soil standard containing 125Sb, 155Eu, 54Mn, 65Zn, and 40K in Marinelli beaker in the energy range of 35.5 keV to 1460.8 keV. The standard soil sample container and those of the experimental samples were geometrically identical. Point sources of241 Am (59.54 keV), 137Cs (661.66 keV) and 60Co (1173.24 and 1332.49 keV) from IAEA were used for the energy calibration. The background count was determined by counting an empty beaker container having the same dimensions with those carrying the samples. The background spectrum was subtracted from the measured sample spectra to obtain the net radionuclide activities. The counting time of each sample and background was obtained at 40,000 seconds since the spectrum was clearly distinct at this time with good statistics. Considering the low-intensity photons emission and slow decay rates, the activities of 226Ra and 232Th are hard to detect directly from the detector, therefore, under radioactive secular equilibrium condition, the photo peaks of their short-lived decay products were used to assess and evaluate the activity concentration of 226Ra and 232Th [17–22]. Weighted average activity was considered for a nuclide having more than one peak in the spectrum. The gamma-ray photopeak of 228Ac (911.1 keV) and 208Tl (583.1 keV) were used to determine the activity of232 Th while 214Bi (1120.3 and 609.3 keV) and 214Pb (351.9 keV) were used for the activity of 226Ra [22,23]. The activity of 40K was determined from its single gamma line of 1460.8 keV . The specific activity concentrations of 226Ra, 232Th, and 40K in each samples, in Bq kg−1, were then computed using equation [22–24]
where W is the net counts of gamma-ray, є is the photo peak efficiency of a detector, P is the absolute transition of gamma decay, t is counting time in seconds and M mass of the final prepared and dried sample in kilogram which is stored in the cylindrical plastic container for the purpose of experiment.
The specific activities of the natural radionuclides of the 226Ra, 232Th and 40K were evaluated by using gamma–ray spectrometry in 120 different soil samples collected from the districts in the Metekel Zone. All results including the minimum, maximum and mean values, of the above natural radioisotopes are depicted for the different districts in Table 1. The results taken from the samples prepared for constructions and taken from the ground including the same soil types were almost uniformly distributed in all districts.
The activity levels ( ± SD) for 226Ra, 232Th and 40K in all soil samples ranged from 10 ± 1 to 146 ± 2 Bq kg−1 with a mean of 64 ± 16 Bq kg−1, 26±4 to 167 ± 4 Bq kg−1 with a mean of 70 ± 19 Bq kg−1 and 94 ± 13 to 540 ± 28 Bq kg−1 with a mean of 330 ± 120 Bq kg−1, respectively. The world’s mean values of 226Ra, 232Th and 40K are 35, 30 and 400 Bq kg−1, respectively . The mean of 40K observed in this study was significantly lower than the world’s mean values, whereas the mean concentrations of 226Ra and 232Th were higher than the world’s mean values of 35 and 30 Bq kg−1, respectively.
As can be seen from Table 1, the highest mean activity of 226Ra was determined in the Bulen district and the Mandura district showed the lowest mean levels of 226Ra, the Guba and Wenbera districts showed the lowest value (43 ± 16 Bq kg−1) and the highest (84 ± 25 Bq kg−1) activity concentrations of 232Th, respectively. The activity concentrations of radioisotope 40K were found to be minimum in the Dibate (209 ± 60 Bq kg−1) and maximum in the Bulen (468 ± 70 Bq kg−1) areas.
Almost all the mean activity concentrations of 226Ra and 232Th in soil types of samples were higher than the world average value, on average, the activities of 40K were lower than the worldwide proposed values. Sandy loam samples showed the lowest 226Ra and 232Th activity concentration values and Clay samples have had the lowest 40K activity concentration values and all these values were lower than reported international’s mean values .
Sampled studied levels tabulated for reported data of other countries for comparison are given in Table 2. For example, the 226Ra the measured mean values for soil samples was higher than the concentration for Dhanbad city (Jharkhand), Turkey, Rize Province–Turkey, Istanbul, Kuwait, Northern Jordan, Eastern Yunnan China, Iran, Thai Lemongras, Saudi Arabia, Iraqi Kurdistan Region, Northern Regions of Oman and Niabi Faisalabad (Pakistan), and it was lower than the activity concentration of Sahiwal–Pakistan, North Cyprus, Malaysia, Southern Kenya, India, Penang–Pakistan and Kaduna State Nigeria. For the case of 232Th concentrations, the obtained value was higher than for Dhanbad city (Jharkhand), Turkey, Sahiwal–Pakistan, Turkey, Istanbul, Kuwait, Northern Jordan, Eastern Yunnan China, Iran, Thai Lemongras, Saudi Arabia, Iraqi Kurdistan Region, Northern Regions of Oman and Niabi Faisalabad (Pakistan), whereas it was lower than Malaysia, Kaduna State Nigeria, Southern Kenya and India. The obtained mean concentration value of 40K was 330 Bq kg−1. This was exactly higher than for Turkey, Northern Jordan, Eastern Yunnan China, Kaduna State Nigeria and Northern Regions of Oman.
According to our results, the spread out of 226Ra, 232Th and 40K in soils was not the same. The situation which makes different distribution across the study places with respect to exposure to radiation was defined in terms of radium equivalent activity (Raeq) in Bq kg−1 to compare the specific activity of materials containing different amounts of 226Ra, 232Th and 40K . The radium equivalent activity was estimated through the following relation :
where ARa, ATh and AK are concentrations of 226Ra, 232Th and 40K in Bq kg−1, respectively. The computed mean Raeq values are presented in Table 3 for the different soil types and the different districts where they are collected. The minimum 133 Bq kg−1 and the maximum (229 Bq kg−1) values of Raeq were found in Silt and Silty clay soil types in the Guba, Wenbera and Bulen districts, respectively. While the mean Raeq values of all the measured soil samples were lower than the limit value of 370 Bq kg−1 requested by Organization for Economic Cooperation and Development (OECD) .
The number of indices dealing with the assessment of the excess gamma radiation emitting from construction materials such as outdoor and indoor hazard indices and gamma concentration indices has been given by several researchers [1,2,27–29]. In this study, the gamma index (Iγ) was computed as recommended by the European Commission (EC) and used by [5,30]:
where ARa, ATh and AK are the activity concentrations of 226Ra, 232Th and 40K, respectively. The values of Iγ calculated from the studied values of 226Ra, 232Th and 40K are shown in Table 3 for different soil types and the districts where they were collected. The average values of Iγ for the studied samples varied in the range between 0.48 and 0.81 for types of soil and 0.52 and 0.79 for the districts which were less than the critical value of 1.
At this particular time, many alpha indices have been presented to assess the exposure level due to radon inhalation originating from construction materials . The alpha index was calculated by using formula:
where ARa is the concentration of 226Ra in the unit of Bq kg−1 that assumed in equilibrium with 238U. The recommended lower and upper level of 226Ra activity concentrations in soil are 100 and 200 Bq kg−1, respectively, as requested by International Commitee on Radiation Protection (ICRP) . This implies that, when the materials are used for construction, the recommended level of lower and upper limits concentration of 226Ra 100 Bq kg−1 and 200 Bq kg−1, for which Iα = 1. The mean calculated Iα values for the studied soil samples are given in Table 3 for the different soil types and the districts where they were collected. The values of Iα ranged from 0.25 to 0.47, with the mean value of 0.37. For the safely use of soil in the building of dwellings and for production of crops, Iα should be less than unity. Accordingly, our result shows the mean values calculated for Iα indices were less than unity for all study sites.
There is concern that some of the buildings will cause too much radiation doses to the human body due to gamma rays emitted by 214Pb and 214Bi progeny of 226Ra and 232Th decay chains, respectively and the contribution of 40K to the total body radiation dose is not ignored. The absorbed dose rate in indoor air due to gamma ray release from concentrations of 226Ra and 232Th and 40K was estimated using the formula recommended by EC  and United Nations Scientific Committee on the Effects of Atomic Radiation (UNSCEAR) . In the UNSCEAR and the European Commissions reports, the dose conversion coefficients were calculated for the standard room center. Dimensions of the room were 4 m × 5 m × 2.8 m. Thicknesses of walls, floor and ceiling and density of the structures were 20 cm and 2350 kg m−3 (soil), respectively.
where D is indoor absorbed dose rate and α, β and γ are the dose rates per unit activity concentrations of Ra, Th and K (nGyh−1 / Bq kg−1), respectively. The values of α, β and γ were taken to be 0.92, 1.1 and 0.08, respectively . By identifying the soil types and number of districts, we have collected the samples and measured the required terms. As a country, we do not have safety rules or guidelines for radiation protection and housing standards. Therefore, we used the EC room standard for this investigation.
The absorbed dose rates in indoor air calculated from the measured activities in different soil samples are also provided in Table 3 (column 5) for the different soil types and the study areas where they were collected. The measure intake dose rate in indoor air was found to vary from 116 to 196 nGyh−1 with a mean of 172 nGyh−1. It was higher than the world mean populated weight value of 84 nGyh−1. Results depicted in Table 3 tells that the lower and the higher received dose rates in air are produced by Sandy loam and Silty clay, respectively.
It is not common to use to use natural ventilation of the houses, as the local community uses the old method of house building. The houses they build are very narrow, have no windows, and no fresh air moving easily. As a result, they are more susceptible to various health problems. To estimate the periodical effective dose in indoor, it must be to consider that: (a) the conversion coefficient (0.7 Sv Gy−1) from absorbed dose in air to effective dose and (b) the indoor habitable factor (~80% for population). Therefore, the successful dose rate in mSv y−1 unit was estimated by using the relation
The calculated values for the annual effective dose (AED) ranged from 0.60 to 0.96 mSv, with a mean value of 0.85 mSv. The corresponding annual effective dose rate from Sandy loam, Sands, Silt, Clay, Silty clays and Clay loam was slightly below the dose criterion of 1 mSv y−1. In general, the average result of AED is approximate to 1 mSvy−1.
The measured concentrations (Bq kg−1) of 226Ra, 232Th and 40K in selected soil samples according to different districts in Metekel and types.
Comparison of mean activity concentrations (Bq kg−1 with studied results in soil samples from some selected countries.
The calculated results for radiological health indices parameters in the different districts in Metekel and the soil types.
The activities of the naturally ability radionuclides of the 226Ra, 232Th and 40K in the soil samples collected from agricultural and collected for building in North West Ethiopia were measured by using the technique of gamma ray spectrometry with HPGe detector. The calculated results may be useful in the assessment of the exposures and the radiation doses due to the naturally occurring radioactive material contents in soil samples. The overall average concentrations of 226Ra, 232Th and 40K were 64, 70 and 330 Bq kg−1, respectively. The obtained mean concentrations of 226Ra and 232Th in the studied soil samples are above the world’s quoted values of 35 and 30 Bq kg−1, respectively, however, the mean concentration of 40K in the samples is lower than the corresponding typical value of 400 Bq kg−1 .
The results presented in this work show that the mean values of Raeq, Iγ, Iα, the indoor absorbed dose rate and the annual effective dose rate in soil samples are 201 Bq kg−1, 0.71, 0.37, 172 nGyh−1 and 0.85 mSvy−1, respectively. Although, Ethiopia has been a member of the international Atomic Energy Agency (IAEA) since 2011, it does not yet have a radiation protection policy. Thus, the results of this study will be important as supportive materials for future to establish the country’s common radiation safety guiderules policy for the case of radiation protection and assessments of the impact of radioactive hazards.
The authors would like to thank Assosa University for supporting this research through fund. We are also grateful for our colleague staffs and offices who support us to realize this research work.
Conflict of Interests
The authors declared that there is no conflict of interest with respect to this research.
This Research did not Receive any Specific Funding.
Data Availability Statement
Data associated with this article cannot be disclosed due to legal reason.
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