Measurement of natural radioactive nuclide concentrations in various metal ores used as industrial raw materials in Japan and estimation of dose received by workers handling them

Natural resources such as ores and rocks contain natural radioactive nuclides at various concentrations. If these resources contain high concentrations of natural radioactive nuclides, workers handling them might be exposed to significant levels of radiation. Therefore, it is important to investigate the radioactive activity in these resources. In this study, concentrations of radioactive nuclides in Th, Zr, Ti, Mo, Mn, Al, W, Zn, V, and Cr ores used as industrial raw materials in Japan were investigated. The concentrations of ²³⁸U and ²³²Th were determined by inductively coupled plasma mass spectrometry (ICP-MS), while those of ²²⁶Ra, ²²⁸Ra, and ⁴⁰K were determined by gamma-ray spectrum. We found the concentrations of ²³⁸U series, ²³²Th series, and ⁴⁰K in Ti, Mo, Mn, Al, W, Zn, V, and Cr ores to be lower than the critical values defined by regulatory requirements as described in the International Atomic Energy Agency (IAEA) Safety Guide. The doses received by workers handling these materials were estimated by using methods for dose assessment given in a report by the European Commission. In transport, indoor storage, and outdoor storage scenarios, an effective dose due to the use of Th ore was above 4.3 × 10⁻² Sv y⁻¹, which was higher than that of the other ores. The maximum value of effective doses for other ores was estimated to be about 4.5 × 10⁻⁴ Sv y⁻¹, which was lower than intervention exemption levels (1.0 × 10⁻³ Sv y⁻¹) given in International Commission of Radiological Protection (ICRP) Publication 82.     

Uranium isotopes in Tunisian bottled mineral waters

²³⁴U and ²³⁸U activity concentrations and their relative effective doses have been determined in 10 bottled mineral waters in Tunisia. Alpha spectrometry was used as technique to measure uranium isotopes. The obtained isotopic ratio ²³⁴U/²³⁸U varies between 1.1 and 3 which means that the two isotopes are not in radioactive equilibrium. Measured activity concentration varies between 3.2 and 40 mBq/l for ²³⁴U and between 1.5 and 26.3 mBq/l for ²³⁸U. Effective doses (assuming 2 litres per day of water consumption) coming from this two isotopes are found to vary between 0.16 and 2.02 μSv/a which is lower than the maximum recommended dose level by the WHO.     

Radiological monitoring: terrestrial natural radionuclides in Kinta District,Perak, Malaysia

Natural background gamma radiation and radioactivity concentrations were investigated from 2003 to 2005 in Kinta District, Perak, Malaysia. Sample locations were distant from any ‘amang’ processing plants. The external gamma dose rates ranged from 39 to 1039 nGy h⁻¹. The mean external gamma dose rate was 222 ± 191 nGy h⁻¹. Small areas of relatively enhanced activity were located having external gamma dose rates of up to 1039 ± 104 nGy h⁻¹. The activity concentrations of ²³⁸U, ²³²Th and ⁴⁰K were analyzed by using a high-resolution co-axial HPGe detector system. The activity concentration ranges were 12–426 Bq kg⁻¹ for ²³⁸U, 19–1377 Bq kg⁻¹ for ²³²Th and <19–2204 Bq kg⁻¹ for ⁴⁰ K. Based on the radioactivity levels determined, the gamma-absorbed dose rates in air at 1 m above the ground were calculated. The calculated dose rates and measured dose rates had a good correlation coefficient, R of 0.94. To evaluate the radiological hazard of the natural radioactivity, the radium equivalent activity, the gamma-absorbed dose rate and the mean population weighted dose rate were calculated. An isodose map for the Kinta District was also produced.     

Distribution of uranium isotopes in surface water of the Llobregat river basin (Northeast Spain)

A study is presented on the distribution of ²³⁴U, ²³⁸U, ²³⁵U isotopes in surface water of the Llobregat river basin (Northeast Spain), from 2001 to 2006. Sixty-six superficial water samples were collected at 16 points distributed throughout the Llobregat river basin. Uranium isotopes were measured by alpha spectrometry (PIPS detectors). The test procedure was validated according to the quality requirements of the ISO17025 standard. The activity concentration for the total dissolved uranium ranges from 20 to 261 mBq L⁻¹. The highest concentrations of uranium were detected in an area with formations of sedimentary rock, limestone and lignite. A high degree of radioactive disequilibrium was noted among the uranium isotopes. The ²³⁴U/²³⁸U activity ratio varied between 1.1 and 1.9 and the waters with the lowest uranium activity registered the highest level of ²³⁴U/²³⁸U activity ratio. Correlations between uranium activity in the tested water and chemical and physical characteristics of the aquifer were found.     

Preliminary assessment of current radiation doses to the population of Brodokalmak from contamination of the Techa River

Significant quantities of liquid radioactive waste were discharged to the Techa River in the southern Urals region of Russia in the early years of operation of the Mayak PA plant (1948–1951). A collaborative project is underway under contract to the European Commission to consider the radiological impact of radioactive contamination in the Southern Urals. Part of this project involves the calculation of radiation doses currently received by the population of Brodokalmak on the Techa river. The assessment made use of local data on the habits of the population and measurements of radionuclide activity concentrations in food and water. Exposure pathways included in the assessment were ingestion of foods and external exposure to gamma radiation from radionuclides deposited on the banks of the river. A range of doses was calculated for different age groups, firstly, assuming that the restrictions in place are retained and, secondly, assuming that there are no restrictions. These restrictions include bans on drinking river water, fishing and bathing in the river and the prohibition of use of the river and surrounding flood plains by humans and cattle. With restrictions the highest dose estimated was 0.56 mSv y⁻¹ for the most exposed adults and without restrictions this increased to 3.4 mSv y⁻¹.     

Long-term investigation of anthropogenic and naturally occurring radionuclides at reference sites in western Sweden

In case of an accidental release of radioactive substances into the environment, it is important to quickly and reliably estimate the radiation dose received by people in the affected area, and to determine the extent of the contamination. Measurements of the extent of the release and the subsequent contamination can be facilitated if there are predetermined reference sampling sites with known background radiation and inventory of radionuclides. Since 1996, 34 reference sites for soil sampling, field gamma, and intensimeter measurements have been established in western Sweden. Time series data for dose rates and radioisotope inventory have been collected at these sites, allowing for the investigation of changes in these parameters over time. The mass activity densities for the uranium and thorium series elements varied approximately between 10 and 50 Bq/kg and between 10 and 40 Bq/kg, respectively. The mass activity density of ⁴⁰K was approximately in the range 300–800 Bq/kg. The radiation exposure due to ¹³⁷Cs was rather small in this area. The dose rates calculated from in situ measurement data showed that the contribution to the total dose rate was almost entirely due to naturally occurring radionuclides. The measured dose rate was about twice as high as the calculated rate, even after subtracting the contribution from cosmic radiation. This may be explained by the fact that intensimeters generally are calibrated to measure the quantity ambient dose equivalent, which should not underestimate the effective dose.     

Radiological hazards of TENORM in the wasted petroleum pipes

Disposal petroleum pipes containing sludge and scale as a technically enhanced natural occurring radioactive material (TENORM) leads to internal and external radiation hazards and then a significant radiation dose to the workers. In order to contribute to a future waste management policy related to the presence of TENORM in the disposal sites of wasted petroleum pipes, scale and sludge as TENORM wastes are collected form these disposal pipes for radiometric analysis. These pipes are imported from onshore oilfields at south Sinai governorate, Egypt. The highest mean ²²⁶Ra and ²²⁸Ra concentrations of 519 and 50 kBq/kg respectively, were measured in scale samples. Sludge lies within the normal range of radium concentration. The average absorbed dose caused by the exposure to the wasted pipes equal to 4.09 μGy h⁻¹ from sludge and 262 μGy h⁻¹ from scale. This is much higher than the acceptable level of 0.059 μGy h⁻¹. Due to radon inhalation, important radon related parameters are calculated which advantage in internal dose calculation. Fairly good correlation between real radium content and radon exhalation rate for sludge samples is obtained. The hazards from sludge come from its high emanation power for radon which equal to 3.83%. The obtained results demonstrate the need of screening oil residues for their radionuclide content in order to decide about their final disposal.     

Exposure of workers in mineral processing industries in Brazil

The mining, milling and processing of uranium and thorium bearing minerals may result in radiation doses to workers. A preliminary survey pilot program, that included six mines in Brazil (two coal mines, one niobium mine, one nickel mine, one gold mine and one phosphate mine), was launched in order to determine the need to control the radioactive exposure of the mine-workers. Our survey consisted of the collection and analysis of urine samples, complemented by feces and air samples. The concentrations of uranium, thorium and polonium were measured in these samples and compared to background data from family members of the workers living in the same dwelling and from residents from the general population of Rio de Janeiro. The results from the coal mines indicated that the inhalation of radon progeny may be a source of occupational exposure. The workers from the nickel, gold and phosphate mines that were visited do not require a program to control internal radiological doses. The niobium mine results showed that in some areas of the industry exposure to thorium and uranium might occur.     

Natural radioactivity in refractory manufacturing plants and exposure of workers to ionising radiation

This paper shows the results of a survey carried out at some refractory manufacturing plants. During the first part of the survey, the concentration of natural radioactivity in raw materials and end-products, coming from four plants, was assessed. Several raw materials and, as a consequence, some end-products as well have shown activity concentrations exceeding a few hundreds of Bq kg⁻¹ of ²³⁸U and ²³²Th. In some important raw materials, such as bauxite and corundums, a remarkable radioactive disequilibrium was observed; this is probably due to the high temperature processes undergone by these materials. The second part of the survey focussed on the measurements of ambient equivalent dose rates, airborne dust concentrations and radon indoor. On the basis of results obtained, the effective dose for the standard worker was estimated. Two different types of refractory plants were investigated. Effective doses for both plants were lower than 1 mSv y⁻¹.     

The importance of physico-chemical parameters on the speciation of natural radionuclides in riverine ecosystems

External gamma radiation levels were measured in the catchment areas of the Sharavathi River and the dose rates in air were found to be in the range 26.0-61.0 nGy h⁻¹. Soil and sediment samples of the riverine environment were analysed for natural radionuclides such as ²²⁶Ra, ²³²Th and ⁴⁰K using a NaI(Tl) gamma spectrometer. The activity concentration of ²¹⁰Pb and ²¹⁰Po in soil and sediment samples was determined by radiochemical separation techniques. Evaluation of the activity concentration of radionuclides with grain size revealed an increase in the activity of ²²⁶Ra, ²³²Th and ⁴⁰K towards fine grain size. The activity concentrations for all isotopes in all samples were not significantly correlated with pH. However, the activity of ²¹⁰Po and ²¹⁰Pb in sediment showed a moderate positive correlation with organic matter content and a good correlation with clay content of sediment.     

Radium geochemistry in Na-Cl type groundwater in Niigata Prefecture, Japan

Radium isotopes in 23 Na-Cl type groundwater sampled mainly from deep wells in Niigata Prefecture, which is the site of the largest oil- and gas-fields in Japan, were measured along with U isotopes, chemical components and hydrogen and oxygen isotope ratios to elucidate the distribution and behavior of Ra in a brackish environment underground. Also analyzed were U and Th isotopes in 38 rock samples collected from outcrops at 17 locations. Ra-226 concentrations (8.86-1637 mBq kg⁻¹) of groundwater samples roughly correlated with total dissolved solid (TDS) concentrations and other alkaline earth contents. Their ²²⁸Ra/²²⁶Ra activity ratios (0.32-5.2) were similar to or higher than the ²³²Th/²³⁸U activity ratios (0.6-1.7) in the rocks. The most likely transport mechanism of Ra isotopes into groundwater was due to their α-recoil from the solid phase, probably from the water-rock interface where Th isotopes had accumulated, and adsorption/desorption reaction based on the increase in ²²⁶Ra contents with TDS.     

Multi-group approximation, scattering and calibration coefficients, uncertainty estimates and detection limits of a NaI(Tl)-based gamma spectrometry set-up for low-level activity analysis

This paper describes a quantitative radioactivity analysis method especially suitable for environmental samples with low-level activity. The method, consisting of a multi-group approximation based on total absorption and Compton spectra of gamma rays, is coherently formalized and a computer algorithm thereof designed to analyze low-level activity NaI(Tl) gamma ray spectra of environmental samples. Milk powder from 1988 was used as the example case. Included is a special analysis on the uncertainty estimation. Gamma sensitiveness is defined and numerically evaluated. The results reproduced the calibration data well, attesting to the reliability of the method. The special analysis shows that the uncertainty of the assessed activity is tied to that of the calibration activity data. More than 77% of measured 1461-keV photons of ⁴⁰K were counted in the range of clearly lower energies. Pile-up of single line photons (¹³⁷Cs) looks negligible compared to that of a two-line cascade (¹³⁴Cs). The detection limit varies with radionuclide and spectrum region and is related to the gamma sensitiveness of the detection system. The best detection limit always lies in a spectrum region holding a line of the radionuclide and the highest sensitiveness. The most radioactive milk powder sample showed a activity concentration of 21 ± 1 Bq g⁻¹for ¹³⁷Cs, 323 ± 13 Bq g⁻¹ for ⁴⁰K and no ¹³⁴Cs.     

Variation of radiation level and radionuclide enrichment in high background area

Significantly high radiation level and radionuclide concentration along Quilon beach area of coastal Kerala have been reported by several investigators. Detailed gamma radiation level survey was carried out using a portable scintillometer. Detailed studies on radionuclides concentration in different environmental matrices of high background areas were undertaken in the coastal areas of Karunagapalli, Kayankulam, Chavara, Neendakara and Kollam to study the distribution and enrichment of the radionuclides in the region. The absorbed gamma dose rates in air in high background area are in the range 43-17,400 nGyh⁻¹. Gamma radiation level is found to be maximum at a distance of 20 m from the sea waterline in all beaches. The soil samples collected from different locations were analysed for primordial radionuclides by gamma spectrometry. The activity of primordial radionuclides was determined for the different size fractions of soil to study the enrichment pattern. The highest activity of ²³²Th and ²²⁶Ra was found to be enriched in 125-63 μ size fraction. The preferential accumulation of ⁴⁰K was found in <63 μ fraction. The minimum ²³²Th activity was 30.2 Bq kg⁻¹, found in 1000-500 μ particle size fraction at Kollam and maximum activity of 3250.4 Bq kg⁻¹ was observed in grains of size 125-63 μ at Neendakara. The lowest ²²⁶Ra activity observed was 33.9 Bq kg⁻¹ at Neendakara in grains of size 1000-500 μ and the highest activity observed was 482.6 Bq kg⁻¹ in grains of size 125-63 μ in Neendakara. The highest ⁴⁰K activity found was 1923 Bq kg⁻¹ in grains of size <63 μ for a sample collected from Neendakara. A good correlation was observed between computed dose and measured dose in air. The correlation between ²³²Th and ²²⁶Ra was also moderately high. The results of these investigations are presented and discussed in this paper.     

Cesium isotope ratios as indicators of nuclear power plant operations

There are multiple paths by which radioactive cesium can reach the effluent from reactor operations. The radioactive ¹³⁵Cs/¹³⁷Cs ratios are controlled by these paths. In an effort to better understand the origin of this radiation, these ¹³⁵Cs/¹³⁷Cs ratios in effluents from three power reactor sites have been measured in offsite samples. These ratios are different from global fallout by up to six fold and as such cannot have a significant component from this source. A cesium ratio for a sample collected outside of the plant boundary provides integration over the operating life of the reactor. A sample collected inside the plant at any given time can be much different from this lifetime ratio. The measured cesium ratios vary significantly for the three reactors and indicate that the multiple paths have widely varying levels of contributions. There are too many ways these isotopes can fractionate to be useful for quantitative evaluations of operating parameters in an offsite sample, although it may be possible to obtain limited qualitative information for an onsite sample.     

Deposition of gamma emitters from Chernobyl accident and their transfer in lichen–soil columns

Lichen–soil column samples were taken from several locations in the Southern Finland between 1986 and 2006. Columns were divided into three parts, upper lichen, lower lichen and underlying soil, and their gamma emitting radionuclides, ¹³⁴Cs, ¹³⁷Cs, ¹⁰³Ru, ⁹⁵Zr, ¹⁰⁶Ru, ^110mAg, ¹²⁵Sb and ¹⁴⁴Ce, were measured with gamma spectrometry. Deposition values were calculated as Bq/m² for each sampling site. Distribution of various radionuclides in the three compartments as a function of time was determined. Both effective and ecological half-lives of all radionuclides were calculated for upper lichen, whole lichen and whole lichen–soil column. A linear relation was derived between the physical half-lives and effective half-lives for whole lichen and for whole lichen–soil column. Reindeer meat activity concentrations of various radionuclides and ensuing radiation doses to reindeer-herding people were also estimated for a hypothetical case where a similar high radioactive pollution, as was taken place in the Southern Finland, would have occurred in the reindeer-herding areas in the Finnish Lapland.     

Characterization of phosphogypsum wastes associated with phosphoric acid and fertilizers production

The present work is directed to characterize the phosphogypsum (PG) wastes associated with phosphoric acid produced by the wet process in industrial facility for the production of fertilizers and chemicals in Egypt. The PG waste samples were characterized in terms of spectroscopic analysis (X-ray diffraction, X-ray fluorescence, IR spectra) and radiometric analysis (γ- and α-measurements). The γ-ray measurements showed that the average activity concentrations are 140 ± 12.6, 459 ± 36.7, 323 ± 28.4, 8.3 ± 0.76 and 64.3 ± 4.1 Bq/kg for U-238, Ra-226, Pb-210, Th-232 and K-40, respectively. The α-particle measurements of uranium isotopes showed that the average activity concentrations of U-238, U-235 and U-234 were 153 ± 9.8, 7 ± 0.38, 152 ± 10.4 Bq/kg, respectively. The average radiochemical recovery (%) of the destructive α-particle measurements is ∼70% with a resolution (FWHM) of ∼30 keV. Activity ratios of U-238/Ra-226 and U-238/Pb-210 were less than unity (i.e., <1) and equal to 0.31 ± 0.02 and 0.47 ± 0.16, respectively. The isotopic ratios of U-238/U-235 and U-238/U-234 (in PG and PR samples) were close to the normal values of ∼21.7 and ∼1, respectively and are not affected by the wet processing of phosphate rock (PR). The obtained results of PG waste samples were compared with phosphate rock (PR) samples. The radiation hazard indices are namely, radium activity index (Ra-Eq > 370 Bq/kg), total absorbed gamma dose rate (D_γr > 5 nGy/h) and radon emanation fraction (Rn-EF > 20%). Uncertainty of the sample counting was 95% confidence level of σ. The results indicated the necessity to find suitable routes to decrease and/or redistribute the radionuclide of environmental interest (i.e., Ra-226) in PG wastes, consequently to reduce its radiation impacts in the surrounding environment.     

High background radiation investigated by gamma spectrometry of the soil in the southwestern region of Cameroon

The aim of this work is to determine the radioactivity concentration of ²²⁶Ra, ²³²Th and ⁴⁰K in sub-surface (0-5 cm) soil samples collected from Awanda, Bikoué, Ngombas in the southwestern region of Cameroon, to assess their contribution to the external dose exposure relative to the United Nation Scientific Committee on Effects of Atomic Radiation (UNSCEAR) data. An HPGe p-type detector coupled to a multichannel analyzer was used to perform measurements and data processing. The activity concentrations of ²²⁶Ra varied from 0.06 ± 0.01 to 0.27 ± 0.02 kBq kg⁻¹ with a mean value of 0.13 ± 0.01 kBq kg⁻¹ wet weight. The activity concentrations of ²³²Th varied from 0.10 ± 0.01 to 0.70 ± 0.05 kBq kg⁻¹ with a mean value of 0.39 ± 0.03 kBq kg⁻¹ wet weight, and ⁴⁰K concentrations varied from 0.37 ± 0.02 to 1.53 ± 0.11 kBq kg⁻¹ with a mean value of 0.85 ± 0.07 kBq kg⁻¹ wet weight, respectively. The mean value of outdoor annual effective doses were estimated to be 0.48 mSv y⁻¹, 0.39 mSv y⁻¹ and 0.38 mSv y⁻¹ from Ngombas, Awanda and Bikoué, respectively. The studied areas can be said to have a high background radiation level.     

Occupational exposure to radon and natural gamma radiation in the La Carolina, a former gold mine in San Luis Province, Argentina

Radon and gamma radiation level measurements were carried out inside the La Carolina mine, one of the oldest gold mining camps of southern South America, which is open for touristic visits nowadays. CR-39 track-etch detectors and thermoluminescent dosimeters of natural CaF₂ and LiF TLD-100 were exposed at 14 points along the mine tunnels in order to estimate the mean ²²²Rn concentration and the ambient dose equivalent during the summer season (November 2008 to February 2009). The values for the ²²²Rn concentration at each monitoring site ranged from 1.8 ± 0.1 kBq m⁻³ to 6.0 ± 0.5 kBq m⁻³, with a mean value of 4.8 kBq m⁻³, indicating that these measurements exceed in about three times the upper action level recommended by ICRP for workplaces. The correlations between radon and gamma radiation levels inside the mine were also investigated. Effective doses due to ²²²Rn and gamma rays inside the mine were determined, resulting in negligible values to tourists. Considering the effective dose to the mine tourist guides, values exceeding 20 mSv of internal contribution to the effective doses can be reached, depending on the number of working hours inside the mine.     

Natural radionuclide content in building materials and gamma dose rate in dwellings in Cuba

An extensive research project to investigate the radioactive properties of Cuban building materials was carried out because there is a lack of information on the radioactivity of such materials in Cuba. In the framework of this project 44 samples of commonly used raw materials and building products were collected in five Cuban provinces. The activity concentrations of natural radionuclides were determined by gamma ray spectrometry using a p-type coaxial high purity germanium detector and their mean values were in the ranges: 9-857Bqkg(-1) for (40)K; 6-57Bqkg(-1) for (226)Ra; and 1.2-22Bqkg(-1) for (232)Th. The radium equivalent activity in the 44 samples varied from 4Bqkg(-1) (wood) to 272Bqkg(-1) (brick). A high pressure ionisation chamber was used to measure the indoor absorbed dose rate in 543 dwellings and workplaces in five Cuban provinces. The average absorbed dose rates in air ranged from 43nGyh(-1) (Holguín) to 73nGyh(-1) (Camagüey) and the corresponding population-weighted annual effective dose due to external gamma radiation was estimated to be 145+/-40microSv. This value is 51% lower than the effective dose due to internal exposure from inhalation of decay products of (222)Rn and (220)Rn and it is 16% higher than the calculated value for the typical room geometry of a Cuban house.     

Radionuclide content of building materials and associated gamma dose rates in Egyptian dwellings

Studies have been carried out to determine the natural radioactivity in some building materials (bricks, tiles, marble and ceramics) and their associated radiation hazard. The radioactivity concentrations of ²²⁶Ra ²³²Th and ⁴⁰K were measured using a gamma spectrometer with a Hp–Ge detector. The activities of ²³⁸U and ²³⁴U were measured using an alpha-spectrometer with a surface barrier detector after applying a radiochemical procedure. The ²³⁴U/²³⁸U isotopic ratios were calculated. The radium equivalent activities and the radiation hazard index associated with the natural radionuclides were calculated. A computer program was developed and applied to calculate the dose rate a person will receive from the walls of a room constructed from the studied building materials.