Uptake of 226Ra and 210Pb by food crops cultivated in a region of high natural radioactivity in Brazil

The Poços de Caldas Plateau is a deeply weathered alkaline igneous intrusion of about 35 km diameter, in which several radioactive anomalies exist. The first Brazilian uranium mine and mill are located in this region. A study is in progress to assess the edible vegetable uptake of the most abundant natural radionuclides in the local environment and this paper reports the results for ²²⁶Ra and ²¹⁰Pb. In farm soils, both nuclides have similar concentrations. The minimum values are comparable to those found in areas of normal radioactivity but the maximum concentrations are ten-fold higher. ‘Exchangeable’ radium in soils ranges from 2·3% to 34·5% of the total. No statistical correlation was found between the ‘exchangeable’ ²²⁶Ra and several physico-chemical soil parameters. In the vegetables analyzed, ²²⁶Ra concentrations are slightly higher than those of ²¹⁰Pb and the maximum values are also one order of magnitude greater than in normal regions. For both radionuclides, the average soil-to-plant concentration factors are of the order of 10⁻³ and 10⁻², when related to total and to ‘exchangeable’ contents in soils, respectively. For each vegetable, no statistical correlation was observed between the ²²⁶Ra or ²¹⁰Pb concentrations in the plant (fresh weight) and concentrations in the soil, either total or ‘exchangeable’. The ‘exchangeable’ Ca in soils does not seem to influence radium uptake by plants in a defined way.     

Radium and uranium levels in vegetables grown using different farming management systems

Vegetables grown with phosphate fertilizer (conventional management), with bovine manure fertilization (organic management) and in a mineral nutrient solution (hydroponic) were analyzed and the concentrations of ²³⁸U, ²²⁶Ra and ²²⁸Ra in lettuce, carrots, and beans were compared. Lettuce from hydroponic farming system showed the lowest concentration of radionuclides 0.51 for ²²⁶Ra, 0.55 for ²²⁸Ra and 0.24 for ²³⁸U (Bq kg⁻¹ dry). Vegetables from organically and conventionally grown farming systems showed no differences in the concentration of radium and uranium. Relationships between uranium content in plants and exchangeable Ca and Mg in soil were found, whereas Ra in vegetables was inversely correlated to the cation exchange capacity of soil, leading to the assumption that by supplying carbonate and cations to soil, liming may cause an increase of U and a decrease of radium uptake by plants. The soil to plant transfer varied from 10⁻⁴ to 10⁻² for ²³⁸U and from 10⁻² to 10⁻¹ for ²²⁸Ra.     

Migration of radium from the thorium ore deposit of Morro do Ferro,Poços de Caldas,Brazil

A large thorium ore deposit is located in Morro do Ferro, a hill in the Poços de Caldas Plateau, Minas Gerais, Brazil, which contains an estimated 30 000 t of Th and 100 t of U in a highly weathered matrix exposed to erosion and leaching. ²²⁸Ra and ²²⁶Ra were analyzed in surface waters collected at various points in the drainage basin and in groundwaters from wells drilled through and around the ore body. The concentrations in groundwater demonstrated that radium is markedly leached by rainwater percolating through the ore body. In its transit underground, radium is removed from groundwater by sorption on soil particles and this natural process greatly reduces the radium discharged to the environment. In dry weather, the concentration of dissolved ²²⁸Ra in the main stream draining the Morro do Ferro is 7·0 ± 1·1 mBq litre⁻¹ and in a control stream 1·6 ± 0·3 mBq litre⁻¹. The estimated ²²⁸Ra mobilization rate by solubilizations is of the order of 10⁻⁷ y⁻¹.     

Study of soil-plant transfer of 226Ra under greenhouse conditions

A soil-plant transfer study was performed using soil from a former uranium ore processing factory in South Bohemia. We present the results from greenhouse experiments which include estimates of the time required for phytoremediation. The accumulation of ²²⁶Ra by different plant species from a mixture of garden soil and contaminated substrate was extremely variable, ranging from 0.03 to 2.20 Bq ²²⁶Ra/g DW. We found differences in accumulation of ²²⁶Ra between plants from the same genus and between cultivars of the same plant species. The results of ²²⁶Ra accumulation showed a linear relation between concentration of ²²⁶Ra in plants and concentration of ²²⁶Ra in soil mixtures. On the basis of these results we estimated the time required for phytoremediation, but this appears to be too long for practical purposes.     

Soil radium, soil gas radon and indoor radon empirical relationships to assist in post-closure impact assessment related to near-surface radioactive waste disposal

Least squares (LS), Theil’s (TS) and weighted total least squares (WTLS) regression analysis methods are used to develop empirical relationships between radium in the ground, radon in soil and radon in dwellings to assist in the post-closure assessment of indoor radon related to near-surface radioactive waste disposal at the Low Level Waste Repository in England. The data sets used are (i) estimated ²²⁶Ra in the <2 mm fraction of topsoils (eRa226) derived from equivalent uranium (eU) from airborne gamma spectrometry data, (ii) eRa226 derived from measurements of uranium in soil geochemical samples, (iii) soil gas radon and (iv) indoor radon data. For models comparing indoor radon and (i) eRa226 derived from airborne eU data and (ii) soil gas radon data, some of the geological groupings have significant slopes. For these groupings there is reasonable agreement in slope and intercept between the three regression analysis methods (LS, TS and WTLS). Relationships between radon in dwellings and radium in the ground or radon in soil differ depending on the characteristics of the underlying geological units, with more permeable units having steeper slopes and higher indoor radon concentrations for a given radium or soil gas radon concentration in the ground. The regression models comparing indoor radon with soil gas radon have intercepts close to 5 Bq m⁻³ whilst the intercepts for those comparing indoor radon with eRa226 from airborne eU vary from about 20 Bq m⁻³ for a moderately permeable geological unit to about 40 Bq m⁻³ for highly permeable limestone, implying unrealistically high contributions to indoor radon from sources other than the ground. An intercept value of 5 Bq m⁻³ is assumed as an appropriate mean value for the UK for sources of indoor radon other than radon from the ground, based on examination of UK data. Comparison with published data used to derive an average indoor radon: soil ²²⁶Ra ratio shows that whereas the published data are generally clustered with no obvious correlation, the data from this study have substantially different relationships depending largely on the permeability of the underlying geology. Models for the relatively impermeable geological units plot parallel to the average indoor radon: soil ²²⁶Ra model but with lower indoor radon: soil ²²⁶Ra ratios, whilst the models for the permeable geological units plot parallel to the average indoor radon: soil ²²⁶Ra model but with higher than average indoor radon: soil ²²⁶Ra ratios.     

Activity concentrations of 226Ra, 228Ra, 210Pb, 40K and 7Be and their temporal variations in surface air

Activity concentrations of the long-lived natural radionuclides ²²⁶Ra, ²²⁸Ra, ²¹⁰Pb, ⁴⁰K and of ⁷Be in surface air were measured twice monthly at a semi-rural location 10 km north of Munich (FRG) for at least three years. For the time interval 1983–1985, all values were found to be distributed log-normally, with geometric means (in μBq m⁻³) of 1·2 for ²²⁶Ra, 0·5 for ²²⁸Ra, 580 for ²¹⁰Pb, 12 for ⁴⁰K and 3500 for ⁷Be. Reflecting their common origin, the activity concentrations of ²²⁶Ra and ⁴⁰K are correlated with surface air dust concentrations (geometric mean 59 μg m⁻³). Seasonal variations of ²¹⁰Pb and ⁷Be air activity concentrations are established for the time interval 1978–1985.The contribution of local soil activity to the air activity concentrations of these radionuclides and of natural uranium is discussed. Resuspension factors are found to be of the order of 10⁻⁹m⁻¹.     

The plant/soil concentration ratio for calcium,radium, lead,and polonium: Evidence for non-linearity with reference to substrate concentration

Evidence exists from both the literature and our own observations that plant nuclide uptake for a variety of plants and elements is a non-linear function of substrate concentration. The uptake response to increasing substrate concentration is usually in the form of a single or multi-phasic saturation curve. For some plant types and elements the uptake response may also take the form in which a threshold of soil activity is necessary before uptake is measurable. We present a generic uptake response curve and the resulting concentration ratio function determined by computer simulation. Data describing the uptake response of plants to ²²⁶Ra, ²¹⁰Pb and ²¹⁰Po as well as for calcium and stable lead are discussed. Functions are also presented for these elements to describe the uptake response and the concentration ratio and their mathematical forms are compared to the generic model.     

Plant uptake of neptunium-237 and technetium-99 under field conditions

Plant uptake of ⁹⁹Tc freshly added to soils was compared with uptake of ⁹⁹Tc ‘aged’ in soil for more than a decade. A combination of alkaline soil and freshly added ⁹⁹Tc resulted in elevated uptake into radish foliage (plant/soil concentration ratios ranged from 37 to 46). Neptunium-237 was freshly added to all soils. Neptunium uptake via plant roots into foliage was strongly affected by soil pH. Neptunium uptake was greatest from acidic soils. The observed plant/soil concentration ratios for ²³⁷Np under field conditions were approximately 10⁻² from acidic soils (pH 5·6–5·7) and were comparable to field concentration ratios for ²³⁹Pu, that is 10⁻³, from a basic soil (pH 7·5).     

Transfer and uptake of radium in a natural and in a technologically modified radiation environment

Differentiation in the geochemical transfer and uptake of the nuclides ²²⁸Ra and ²²⁶Ra is observed to give high nuclide activity ratios, of ²²⁸Ra to ²²⁶Ra, ranging from 20 to 200 in sediment humus collected from a river subject to pollution. Differentiation of this nature is also observed in the non-ionic non-dialysable fraction of the Ra activity in river water and may be attributed to preferential complexing of ²²⁸Ra relative to ²²⁶Ra. Biological uptake of the activities produces a similar effect. The ratios are higher in a natural radiation environment than in a technologically enhanced one, indicating the influence of nuclide availability.     

Simulation of biological uptake of uranium and radium in an industrially polluted area

Distribution of ²³⁸U and ²²⁶Ra in soils and plants of an industrially polluted area are considered. The dependence between the biological uptake coefficients (BUCs) for the plant species studied and the radionuclide concentrations in soil can be approximated by a decreasing power function. Species differences in radionuclide uptake are demonstrated.     

The transfer of 137Cs and 60Co from feed to pork

The transfer of ¹³⁷Cs and ⁶⁰Co from fodder to meat and other organs was studied in growing pigs. The influence of two different feeding methods (potato and grain) commonly used in Germany was investigated. The radionuclides were transferred into plants by root uptake and these were fed once a day, all at once, to young pigs until they reached maturity. In this manner, the radioactivity was administered to the pigs in a similar chemical form as would occur after radioactive contamination of soil. It is demonstrated that the two feeding practices have only a minor influence on transfer coefficients, which were determined to be ≤0·002 days/kg for ⁶⁰Co in meat and in the ranges 0·18–0·26 (potato-feeding) and 0·17–0·33 days/kg (grain-feeding), respectively, for ¹³⁷Cs in different components of the meat: the transfer coefficients for ¹³⁷Cs into different organs range from 0·06 to 0·24 days/kg after potato-feeding and from 0·12 to 0·29 after grain-feeding.     

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.     

Bioaccumulation of Ra by plants growing in fresh water ecosystem around the uranium industry at Jaduguda, India

A field study has been conducted to evaluate the ²²⁶Ra bioaccumulation among aquatic plants growing in the stream/river adjoining the uranium mining and ore-processing complex at Jaduguda, India. Two types of plant group have been investigated namely free floating algal species submerged into water and plants rooted in stream & riverbed. The highest ²²⁶Ra activity concentration (9850 Bq kg⁻¹) was found in filamentous algae growing in the residual water of tailings pond. The concentration ratios of ²²⁶Ra in filamentous algae (activity concentration of ²²⁶Ra in plant Bq kg⁻¹ fresh weight/activity concentration of ²²⁶Ra in water Bq l⁻¹) widely varied i.e. from 1.1 × 10³ to 8.6 × 10⁴. Other aquatic plants were also showing wide variability in the ²²⁶Ra activity concentration. The ln-transformed filamentous algae ²²⁶Ra activity concentration was significantly correlated with that of ln-transformed water concentration (r = 0.89, p < 0.001). There was no correlation between the activity concentrations of ²²⁶Ra in stream/riverbed rooted plants and the substrate. For this group, correlation between ²²⁶Ra activity concentration and Mn, Fe, Cu concentration in plants were statistically significant.     

A study of radium bioaccumulation in freshwater mussels, Velesunio angasi, in the Magela Creek catchment, Northern Territory, Australia

Freshwater mussels, Velesunio angasi, along Magela Creek in Australia’s Northern Territory were examined to study radionuclide activities in mussel flesh and to investigate whether the Ranger Uranium mine is contributing to the radium loads in mussels downstream of the mine. Radium loads in mussels of the same age were highest in Bowerbird Billabong, located 20 km upstream of the mine site. Variations in the ratio of [Ra]:[Ca] in filtered water at the sampling sites accounted for the variations found in mussel radium loads with natural increases in calcium (Ca) in surface waters in a downstream gradient along the Magela Creek catchment gradually reducing radium uptake in mussels. At Mudginberri Billabong, 12 km downstream of the mine, concentration factors for radium have not significantly changed over the past 25 years since the mine commenced operations and this, coupled with a gradual decrease of the ²²⁸Ra/²²⁶Ra activity ratios observed along the catchment, indicates that the ²²⁶Ra accumulated in mussels is of natural rather than mine origin. The ²²⁸Th/²²⁸Ra ratio has been used to model radium uptake and a radium biological half-life in mussels of approximately 13 years has been determined. The long biological half-life and the low Ca concentrations in the water account for the high radium concentration factor of 30,000-60,000 measured in mussels from the Magela Creek catchment.     

Comparative study of natural radioactivity levels in soil samples from the Upper Siwaliks and Punjab,India using gamma-ray spectrometry

Natural radioactive materials under certain conditions can reach hazardous radiological levels. So, it becomes necessary to study the natural radioactivity levels in soil to assess the dose for the population in order to know the health risks and to have a baseline for future changes in the environmental radioactivity due to human activities. The natural radionuclide (²²⁶Ra, ²³²Th, and ⁴⁰K) contents in soil were determined for 26 locations around the Upper Siwaliks of Kala Amb, Nahan and Morni Hills, Northern India, using high-resolution gamma-ray spectrometric analysis. It was observed that the concentration of natural radionuclides viz., ²²⁶Ra, ²³²Th and ⁴⁰K, in the soil varies from 28.3 ± 0.5 to 81.0 ± 1.7 Bq kg⁻¹, 61.2 ± 1.3 to 140.3 ± 2.6 Bq kg⁻¹ and 363.4 ± 4.9 to 1002.2 ± 11.2 Bq kg⁻¹ respectively. The total absorbed dose rate calculated from activity concentration of ²²⁶Ra, ²³²Th and ⁴⁰K ranged from 71.1 to 162.0 nGy h⁻¹. The radium equivalent (R_eq) and the external hazard index (H_ex), which resulted from the natural radionuclides in soil, were also calculated and found to vary from 149.4 to 351.8 Bq kg⁻¹and from 0.40 to 0.95 respectively. These values in Upper Siwaliks area were compared with that from the adjoining areas of Punjab. The radium equivalent activities in all the soil samples were lower than the limit (370 Bq kg⁻¹) set in the Organization for Economic Cooperation and Development (OECD) report and the dose equivalent was within the safe limit of 1 mSv y⁻¹.     

Occupational dosimetric assessment (inhalation pathway) from the application of phosphogypsum in agriculture in South West Spain

Phosphogypsum (PG) has been traditionally applied as Ca-amendment in saline marsh soils in SW Spain, where available PG has 710 ± 40 Bq kg⁻¹ of ²²⁶Ra. This work assesses the potential radiological risk for farmers through ²²²Rn exhalation from PG-amended soils and by inhalation of PG-dust during its application. A three-year field experiment was conducted in a commercial farm involving two treatments: control and 25 t PG ha⁻¹ with three replicates (each 0.5 ha plots). The ²²²Rn exhalation rate was positively correlated with potential evapotranspiration, which explained 67% of the variability. Statistically significant differences between the control and PG treatments were not found for ²²²Rn exhalation rates, and mean values were within the lowest quartile of the typical range for ²²²Rn exhalation from soils. Airborne dust samples were collected during the application of PG and sugar-beet sludge amendments. The highest PG-attributable ²²⁶Ra concentration in the dust samples was 3.3 × 10² μBq m⁻³, implying negligible dose increment for exposed workers.     

Distributional U, Ra, Pb and Po in soil

A soil profile from 0 to 90 cm was collected in an undisturbeded area of Cape Cod, Massachusetts. Five centimeter increments of the profile were analyzed for ^234,238U, ²²⁶Ra, ²¹⁰Pb and ²¹⁰Po. The factors affecting the activity distribution of these naturally-occurring radionuclides are discussed for this particular soil type.     

Distributional 234,238U, 226Ra, 210Pb and 210Po in soil

A soil profile from 0 to 90 cm was collected in an undisturbeded area of Cape Cod, Massachusetts. Five centimeter increments of the profile were analyzed for ^234,238U, ²²⁶Ra, ²¹⁰Pb and ²¹⁰Po. The factors affecting the activity distribution of these naturally-occurring radionuclides are discussed for this particular soil type.     

Soil to leaf transfer factor for the radionuclides ²²⁶Ra, ⁴⁰K, ¹³⁷Cs and ⁹⁰Sr at Kaiga region, India

Transfer factors are the most important parameters required for mathematical modeling used for environmental impact assessment of radioactive contamination in the environment. In this paper soil to leaf transfer factor for the radionuclides ⁴⁰K, ²²⁶Ra, ¹³⁷Cs and ⁹⁰Sr is estimated for Kaiga region in Karnataka state, India. Among the plants in which study is carried out, ²²⁶Ra, ⁴⁰K, ¹³⁷Cs and ⁹⁰Sr activity in leaves of herbaceous plants is higher than that of tree leaves. Soil to leaf transfer factor for ²²⁶Ra, ⁴⁰K, ¹³⁷Cs and ⁹⁰Sr was found to be in the range of 0.03-0.65, 0.32-8.04, 0.05-3.03 and 0.42-2.67 respectively.     

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.