Measurement of natural radionuclides in U.K. diet

The levels of radium-226, lead-210 and polonium-210 in the U.K. diet have been determined. The important food groups contributing to the intake of these radionuclides have been identified. Seventy-five percent of the daily intake of radium-226 is derived from beverages, cereals, other vegetables, bread, sugars and preserves. Seventy-five percent of the intake of lead-210 and polonium-210 is derived from bread, milk, cereals, beverages, other vegetables, sugars and preserves, and meat products. The average daily intakes of these radionuclides are tentatively calculated to be 30 mBq for radium-226 and 82 mBq for both lead-210 and polonium-210. These levels are compared with data from other countries. The annual effective dose equivalents resulting from the intakes are approximately 3 muSv for radium-226 and 54 muSv from lead-210 and polonium-210 together. The differences between these doses and other current estimates are discussed.     

About the assumption of linearity in soil-to-plant transfer factors for uranium and thorium isotopes and 226Ra

The linearity assumption for soil and plant concentrations of radionuclides is usually a good approximation for use in food-chain models. To verify this assumption, different samples of plant and substrate were collected from a granitic zone located near a disused uranium mine in order to cover a large range of concentrations. In all of the samples, the activity concentration of 226Ra and of different isotopes of uranium (238U and 234U) and thorium (232Th, 230Th and 228Th) were determined. The results indicate that the linearity assumption can be considered valid when the range of concentrations taken into account is large (approx. two orders of magnitude). Otherwise, there is a clear deviation from linearity. Also, the influence of different stable elements on the soil-plant transfer factors was studied by using multivariate regression methods. The uptake of uranium, thorium and radium was found to be mainly associated with the concentration of iron in the plant and the phosphorus and alkaline earths in the substrate.     

Estimated dose to man from uranium millling via the beef/milk food-chain pathway

One of the major pathways of radiological exposure to man from uranium milling operations is through the beef/milk food chain. Studies by various investigators have shown the extent of uptake and distribution of ²³⁸U, ²³⁴U, ²³⁰Th, ²²⁶Ra, ²¹⁰Pb, and ²¹⁰Po in plants and cattle. These long0lived natural radioisotopes, all nuclides of the uranium decay series, are found in concentrated amounts in uranium mill tailings. In this paper, data from these investigations are used to estimate the dose to man from consumption of beef and milk from cattle that have fed on forage contaminated with the tailings. The estimated doses from this technologically enhanced source are compared with those resulting from average dietary intake of these radionuclides from natural sources.     

Radioactivity of fertilizers in Finland

Concentrating of ²³⁸U, ²²⁶Ra, ²²⁸Th, ²³⁵U and ⁴⁰K in 81 samples of Finnish fertilizer were measured with Ge (Li) spectrometers. The samples represented 28 different types of fertilizer including those for agriculture, forests and gardens. The ratios of activity concentrations of ²³⁸U to ²²⁶Ra in the samples varied from 1.0 to 67 with a geometric mean of 3.6 and the ratios of ²²⁸Th ²²⁸Ra varied from 0.95 to 9.5 with a geometric mean of 2.4. The weighted means of radionuclide concentrations per unit weight of phosphorus in fertilizers were estimated to be 3800 Bq/kgP of ²³⁸U, 1100 Bq/kgP of ²²⁶Ra, 78 Bq/kgP of ²²⁸Ra, 190 Bq/kgP of ²²⁸Th and 210 Bq/kgP of ²³⁵U. The weighted mean of the ⁴⁰K concentrations in fertilizers was 3500 Bq/kg. The estimated total activities spread on tilled soils during the 1982–1983 season were 260 GBq of ²³⁸U, 72 GBq of ²²⁶Ra, 5.3 GBq of ²²⁸Ra, 13 GBq of ²²⁸Th, 14 GBq of ²³⁵U and 3800 GBq of ⁴⁰K. The amounts of the uranium isotopes correspond to about 21 000 kg of natural uranium.     

Linearity assumption in soil-to-plant transfer factors of natural uranium and radium in Helianthus annuus L

The linearity assumption of the validation of soil-to-plant transfer factors of natural uranium and (226)Ra was tested using Helianthus annuus L. (sunflower) grown in a hydroponic medium. Transfer of natural uranium and (226)Ra was tested in both the aerial fraction of plants and in the overall seedlings (roots and shoots). The results show that the linearity assumption can be considered valid in the hydroponic growth of sunflowers for the radionuclides studied. The ability of sunflowers to translocate uranium and (226)Ra was also investigated, as well as the feasibility of using sunflower plants to remove uranium and radium from contaminated water, and by extension, their potential for phytoextraction. In this sense, the removal percentages obtained for natural uranium and (226)Ra were 24% and 42%, respectively. Practically all the uranium is accumulated in the roots. However, 86% of the (226)Ra activity concentration in roots was translocated to the aerial part.     

Elimination of natural uranium and (226)Ra from contaminated waters by rhizofiltration using Helianthus annuus L

The elimination of natural uranium and (226)Ra from contaminated waters by rhizofiltration was tested using Helianthus annuus L. (sunflower) seedlings growing in a hydroponic medium. Different experiments were designed to determine the optimum age of the seedlings for the remediation process, and also to study the principal way in which the radionuclides are removed from the solution by the sunflower roots. In every trial a precipitate appeared which contained a major fraction of the natural uranium and (226)Ra. The results indicated that the seedlings themselves induced the formation of this precipitate. When four-week-old seedlings were exposed to contaminated water, a period of only 2 days was sufficient to remove the natural uranium and (226)Ra from the solution: about 50% of the natural uranium and 70% of the (226)Ra were fixed in the roots, and essentially the rest was found in the precipitate, with only very small percentages fixed in the shoots and left in solution.     

Distribution of radionuclides in different parts of a mushroom: influence of the degree of maturity

Mushrooms are known to be bioaccumulators of radionuclides, but little is known about their distribution within the fruiting bodies or the influence of the degree of maturity on uptake. We carried out a series of cultures of the species Pleurotus eryngii under controlled laboratory conditions to analyze these variables. The maximal uptake of 134Cs and 85Sr was found to occur in mature fruiting bodies, and with the growth of the mushroom the distribution of radionuclides within the fruiting bodies became inhomogeneous. In particular, there was an exponential increase in the percentage of the total activity of 134Cs, 85Sr, and 60Co in the cap+gills as the fruiting bodies matured, accompanied by a complementary decrease in the stem. Radiocaesium, potassium, calcium, (239+240)Pu, (234,238)U, (228,230,232)Th, and 226Ra were assayed in the cap, gills, and stem of fruiting bodies of Tricholoma equestre collected in a natural ecosystem and cultured P. eryngii. Potassium and radiocaesium were mainly located in the cap+gills, and 226Ra in the gills. There was a disequilibrium between (230,232)Th and 228Th in the different parts of the fungi, probably due to uptake of 228Ra and subsequent decay to 228Th. Finally, the distribution pattern of (239+240)Pu, (234,238)U, and (230,232)Th seemed to be species dependent.     

Natural radionuclides in mineral waters

Concentration levels of natural radionuclides in mineral waters have been studied in several European countries. In the Federal Republic of Germany in recent years a nationwide investigation was carried out by several institutions.The concentrations of ²²⁶Ra, uranium isotopes, ²¹⁰Pb and ²¹⁰Po found are similar to those in other European countries. While for adults the health risk from drinking mineral water is comparable to the risk from terrestrial radiation, special consideration has to be given to the risk of infants when mineral water is used for preparing their food.     

Gamma-emitting natural and anthropogenic radionuclides in the terrestrial environment of Kongsfjord,Svalbard

This paper presents results obtained from a radiometric survey, conducted by the Norwegian Radiation Protection Authority, into the levels of gamma-emitting radionuclides, both anthropogenic and natural, in the terrestrial environment of Kongsfjorden, which lies on the North-Western Coast of Spitsbergen in the Arctic archipelago of Svalbard (79 degrees N, 12 degrees E). Samples of terrestrial matrices were taken during field campaigns conducted between 2000 and 2002 and analysed for a range of gamma-emitting radionuclides. The objectives of this study included an assessment of the levels of gamma-emitting radionuclides in the terrestrial environment of the region, identification of processes and activities that influence the accumulation and redistribution of such nuclides within the region and elucidation of the behaviour of such radionuclides within a high arctic environment. Results indicate a quite homogenous spatial distribution of such radionuclides within the study area and highlight the relatively low levels of contamination by the anthropogenic radionuclide, 137Cs, on Svalbard. Average values and ranges of the radionuclides activities in surface soils (0-3 cm) were: 238U 42 Bq/kg (17-134), 226Ra 43 Bq/kg (12-137), 232Th 21 Bq/kg (4-52), 40K 283 Bq/kg (31-564), 137Cs 35 Bq/kg (1-146). Average levels of these nuclides in avian faecal materials were 238U 63 Bq/kg, 226Ra 54 Bq/kg, 232Th 19 Bq/kg, 40K 365 Bq/kg, 137Cs 78 Bq/kg. Enrichment of radionuclides is apparent in soils taken from locations close to bird colonies in the locale, maximum levels of the radionuclides being found in samples associated with such colonies. The results indicate that this is due to concentration of such radionuclides within the faecal material of the birds and subsequent enrichment of the nearby soils either via direct incorporation of the faeces into the soil or by leaching processes. The results indicate that this process may result in contamination of non-related species, such as Svalbard reindeer (Rangifer tarandus playrhynchus), via pathways other than the traditionally accepted route of atmospheric deposition-vegetation-reindeer.     

Radium migration through clay liners at waste disposal sites

The migration of 226Ra through the bottom compacted clay liner of the wastewater disposal reservoirs of an industrial plant that processes uranium ore was evaluated. An instrumental method for 226Ra analysis in soils, consisting of detector calibration, the determination of detector counting efficiency, cumulative counting of both background and soil samples in regular counting intervals, and photo-peak smoothing was developed. The 226Ra was analyzed by means of its granddaughter 214Bi, at a photo-peak of 609 keV. The results showed that most of the 226Ra which diffused from the solution into the soil was retained in the upper layer of the sample, and that just a small percentage migrated to the subjacent layers. This methodology is adequate for the assessment of the migration of radionuclides through soil layers and for environmental impact studies related to contamination of soils by radionuclides.     

Natural radionuclides in industrial and rural soils

Radium-226, lead-210, uranium and thorium are dispersed in the environment by fly ash emitted by coal fuelled power stations. Concentrations of these nuclides have been determined in fly ash from three power stations and in soils collected in six industrial and twenty rural regions. In industrial areas the concentrations of natural radionuclides, in a 5 cm thick surface soil layer, were found to be higher than in lower layers. With the exception of lead-210 this effect was not observed in rural soils, which contained less of radium-226, uranium and thorium. It was found that the type of coal, or combustion technology, influences the amount of radium-226 dispersed in the environment which is accessible to plants.     

Performance assessment model development and parameter acquisition for analysis of the transport of natural radionuclides in a Mediterranean watershed

This paper describes the methodology developed to construct a model for predicting the behaviour of the natural radioisotopes of U, Th and Ra in a Mediterranean watershed. The methodology includes the development of the performance assessment model, obtaining water flow and radiological parameters based on experimental data and analysis of results. The model, which accounts for both water flows and mass balances of the radionuclides in a semi-natural environment, provides assessments of radionuclide behaviour in grassland and agricultural soils, rivers and reservoirs, including the processes of radionuclide migration through land and water and interactions between both. From field and laboratory data, it has been possible to obtain parameters for the driving processes considered in the model, water fluxes, source term definition, soil to plant transfer factors and distribution coefficient values. Ranges of parameter values obtained have shown good agreement with published literature data. This general methodological approach was developed to be extended to other radionuclides for the modelling of a biosphere watershed in the context of performance assessment of a High Level Waste (HLW) repository under Mediterranean climate conditions, as well as for forecasting radionuclide transport under similar Mediterranean conditions that will occur in the future in other areas. The application of sensitivity and uncertainty analysis was intended to identify key uncertainties with the aim of setting priorities for future research. The model results for the activity concentration in the reservoir indicate that for (238)U and (230)Th the most relevant parameter is the initial concentrations of the radionuclides in the reservoir sediments. However, for (226)Ra the most important parameter is the precipitation rate over the whole watershed.     

Heterogeneous distribution of radionuclides, barium and strontium in phosphogypsum by-product

Phosphogypsum (PG) is a high volume by-product of the phosphate fertilizer industry which is composed mainly of CaSO₄·2H₂O. Impurities in PG include F, trace elements and naturally-occurring radionuclides. Radium-226 content is sufficiently high in some PGs that it has limited PG usage in building materials and as an amendment to agricultural soils. Radium likely exists in PG as a sulfate solid solution with Ba, and possibly Sr. This study determined the distribution of ²²⁶Ra, Ba, Sr, U, Th and ²¹⁰Pb among three size fractions (fine: <20 μm; medium: 20–53 μm; coarse: >53 μm) in PGs derived from three different phosphate rock sources. All chemical species, except for Sr in PG derived from Idaho rock, were enriched in the <20-μm fraction relative to the other size fractions and relative to unfractionated PG. On average, fine fraction ²²⁶Ra and ²¹⁰Pb contents were enriched approximately sixfold over unfractionated PG. ²²⁶Ra was enriched in the fine fraction to a greater degree than were Ba or Sr, indicating that Ra behavior in PG is distinct from these other elements. The combination of (i) particle sorting during PG deposition, and (ii) non-uniform distribution of radionuclides in PG, may contribute to radionuclide heterogeneity at PG repositories.     

Consumption of homegrown products does not increase dietary intake of arsenic, cadmium, lead, and mercury by young children living in an industrialized area of Germany

The dietary intake of arsenic (As), cadmium (Cd), mercury (Hg), and lead (Pb) was studied among young German children with different food consumption behaviour (consumption of own grown foodstuffs and of products from the supermarket). The study area comprised an industrialized and a rural area of West Germany. Dietary intake of contaminants was measured by the duplicate method according to the WHO guideline. A total 588 duplicate portions were collected daily from 84 individuals between May and September 1998. Intake of food groups was calculated from dietary records. Determination of As, Cd, Hg, and Pb was performed following high-pressure digestion of lyophilized samples by atomic absorption spectrometry (AAS). Geometric mean weekly intake [microg/(kgbw x week)] was as follows: As 1.4, Cd 2.3, Hg 0.16, and Pb 5.3. Geometric mean intake corresponded to the percentage of the provisional tolerable weekly intake (PTWI) as follows: As 9.7%, Cd 32%, Hg 3.3%, Pb 21%. As and Hg intake were mainly influenced by fish consumption. The amount of cereals and bakery wares mainly determined the Cd and Pb intake. Children living in the industrialized area with a substantial food consumption of own grown vegetables or products from domestic animals products had no increased dietary intake of the metals.     

Pre-operational environmental survey at the uranium mine and mill site,Poços de Caldas,Minas Gerais,Brazil

The first Brazilian uranium mine and mill are located on the Poços de Caldas plateau, in the Central State of Minas Gerais. The pre-operational environmental survey was carried out over a period of two years by the Brazilian Nuclear Energy Commission (CNEN), through the Instituto de Radioproteção e Dosimetria (IRD). The selection of the materials to be monitored, the sampling points and the radionuclides to be analysed were based on critical parameters taking into account the meteorological and hydrological characteristics of the site as well as land use. The results obtained are sufficient to characterize the environmental background of the area, and will allow an assessment of the environmental impact due to the operation of the facility and an evaluation of the adequacy of the effluent emmission control measures. In relation to their contribution to the population dose, the results indicated that ²²⁶Ra and ²¹⁰Pb will be the important radionuclides.     

Effect of water purification on its radioactive content

We have analyzed the dissolved activity of various radionuclides of natural origin (226Ra and (234,235,235)U) and artificial origins (90Sr and (239+240)Pu), together with other non-radioactive physico-chemical parameters (pH, conductivity, dry residue, [Ca2+], [Mg2+], [K+] and [Fe(2+,3+)], in both pre-potable and potable water from 17 treatment plants in Extremadura (Spain). We have established a series of criteria and complementary techniques to the traditional methods of purification, aimed at the quantitative elimination of the presence in solution of the mentioned radionuclides. We highlight: (a) the increment of the mineral content of the water in its treatment succeeds in eliminating 226Ra, until reaching values close to 70%; (b) the increment of the mineralization of the water by addition of chemical reagents, conducted within the pH values 7.1 and 7.8, succeeds in eliminating up to 90% of the total uranium in dissolution; (c) the elimination of 90Sr during the purification is poor, in general, reaching average levels of only 15% when the purification process is practiced within concrete ranges for potable water (pH > 7, conductivity > 150 microS/cm, dry residue > 150 mg/l, [Ca2+] > 10 mg/l and [Mg2+] > 1.2 mg/l), and finally, (d) the decrease of the solubility of the iron, as low as it can get during the purification process, together with an increase of the conductivity associated, in principle, to parallel increments of other variables not analyzed in this work, such as SO4(2-), CO3(2-), etc., the activity of dissolved (239+240)Pu decreases to 90%. The application of the traditional processes of water purification outside the ranges and criteria formulated can increase the presence in dissolution up to 400%, for some radionuclides, largely the consequence of its redissolution from the non-soluble fraction of the water.     

Assessment of daily intake of trace elements due to consumption of foodstuffs by adult inhabitants of Rio de Janeiro city

Concentrations of Al, Cd, Cr, Cu, Mn, Ni, Pb, U and Zn were determined in vegetables (leafy vegetables, fruit, root, grain and cereal), derived products (sugar, coffee, manioc flour, wheat flour, corn flour, and pasta) and animal products (meat, fish, milk) most frequently consumed by adult inhabitants of Rio de Janeiro city. A total of 90 samples were analyzed using inductively coupled plasma mass spectrometry (ICPMS) as the principal method following sample dissolution by dry and wet ashing. Generally, highest contributions for the intake of micronutrients (Cu, Mn, Ni and Zn) arise from bean, rice and wheat flour consumption. Meat, cow milk and the flours, wheat and manioc, are major sources of Al, Cd, Pb and U intake. The daily intake of nine elements via foodstuffs was estimated as: 3.4x10(-4) mg of U, 1.8x10(-3) mg of Cd, 2.8x10(-2) mg of Pb, 2.3x10(-2) mg of Cr, 8.9x10(-2) mg of Ni, 1.12 mg of Cu, 2.5 mg of Mn, 3.5 mg of Al and 4.8 mg of Zn. The intake of toxic elements ranged between 2.7% (Cd) and 30% (U) of the provisional tolerable daily intake and reference dose values indicating that food consumption is, at present, no critical factor for the uptake of these toxic metals, in the population studied here. Concerning micronutrients, the recommended values of daily intake of Cu and Mn are conveniently supplied by the diet; however, for Cr and Zn they are lower than the recommend daily allowance. Due to high metal concentrations and consumption rates, black bean is the foodstuff that provided the highest ingestion rates of Cu, Mn, Ni and Zn (36-60% of the reference dose), being therefore a very important source of micronutrient supply.     

Assimilation of thorium isotopes into terrestrial vegetation

Vegetation and root zone soil from 17 locations within and near the boundaries of a former thorium processing plant were collected and analyzed for 232Th, 228Th and 230Th in order to evaluate the degree of movement of these radionuclides from soil to root tissue, as well as the extent of their translocation into above-ground plant compartments. Concentration ratio (CR) values ranged as follows: 232Th: 0.0003-0.3218 (shoots), 0.0065-0.9057 (roots); 228Th: 0.0038-0.3300 (shoots), 0.0183-0.7335 (roots); 230Th: 0.0007-0.4560 (shoots), 0.0076-1.252 (roots). Root/shoot ratios were 1.03-85.6 (232Th), 1.54-45.8 (228Th) and 1.36-54.5 (230Th). In nearly all instances, the CR values for 228Th exceeded those for 232Th, with the average 228Th/232Th CR ratios being 3.36 and 1.68 for shoots and roots, respectively. No discernable difference was observed between 230Th and 232Th concentration patterns. The increased 228Th/232Th CR ratio observed is presumably due to the intake of 228Ra into the plant structure, leading to subsequent production of 228Th, through decay, within the plant. It is estimated that approximately 80% of the resident 228Th in above-ground vegetation originates through this mechanism.     

The effect of exposure to employees from mining and milling operations in a uranium mine on lead isotopes--a pilot study

Potential exposure during mining and milling of uranium ore has resulted in the industry being highly regulated. Exposure can arise from inhalation of the daughter product radioactive gas radon (222Rn), inhalation of radioactive dust particles from mining and milling, direct irradiation from outside the body, and ingestion of radionuclides (e.g. uranium or radium) in food or water. Making use of the highly unusual lead isotopic signature for uranium ores (high 206Pb/204Pb from the high uranium content, low 208Pb/204Pb from the low Th/U ratio), we undertook a pilot study of nine male mine employees and three controls from the Ranger uranium mine in the Northern Territory Australia to determine if it was feasible to use lead isotopes in blood to identify exposure to uranium-derived materials. The lead isotopic data for the mine employees and controls plot in two distinct fields which are consistent with predicted isotopic patterns. Assuming retention of 10% of the ingested lead, then the increases seen in 206Pb represent intakes of between 0.9 and 15 mg, integrated over the years of exposure. The small amount of lead does not affect blood lead concentrations, but appears to be sufficient to be detectable with sensitive isotopic methods. Further studies, including those on urine, should be undertaken to confirm the veracity of the lead isotope method in monitoring exposure of uranium industry employees.     

Distribution,cycling and mean residence time of 226Ra, 210Pb and 210Po in the Tagus estuary

Results for dissolved and particulate ²²⁶Ra, ²¹⁰Pb and ²¹⁰Po in the Tagus river, estuary and coastal sea system show different distribution and chemical behaviour patterns for these radionuclides in the three aquatic environments. ²²⁶Ra from riverborne particles dissolves in the estuary and contributes to increased concentrations of dissolved ²²⁶Ra in estuarine water. In the estuary, dissolved ²¹⁰Pb and ²¹⁰Po from river discharge and atmospheric deposition are scavenged by suspended matter, which in turn becomes enriched in these nuclides in comparison with riverborne particles. As a result of these processes, the estuarine water flowing into the coastal sea contains enhanced concentrations of dissolved ²²⁶Ra, but is depleted in dissolved ²¹⁰Pb and ²¹⁰Po. Under average river flow conditions, mass balance calculations for dissolved ²¹⁰Po and ²¹⁰Pb in the estuary allowed their mean residence times to be estimated as 18 and 30 days, respectively. Due to the rapid sorption of these radionuclides on to settling particles, bottom sediments in the estuary represent a sink for ²¹⁰Pb and ²¹⁰Po from both natural sources and industrial waste releases. Results also suggest that partial re-dissolution of these radionuclides from bottom sediments and intertidal mudflats is likely to occur in the mid- and low-estuary zones. Nevertheless, box-model computations indicate that the discharge of ²¹⁰Pb and ²¹⁰Po into the coastal sea takes place mainly with the transport of sediment, whereas the discharge in the dissolved fraction can only account for one third of the activities entering the estuary in the soluble phase. Implications of these results to the cycling of radionuclides in phosphate waste releases into estuarine environments are discussed.