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.     

Determination of concentration factors for Cs-137 and Ra-226 in the mullet species Chelon labrosus (Mugilidae) from the South Adriatic Sea

Concentration factors for Cs-137 and Ra-226 transfer from seawater, and dried sediment or mud with detritus, have been determined for whole, fresh weight, Chelon labrosus individuals and selected organs. Cesium was detected in 5 of 22 fish individuals, and its activity ranged from 1.0 to 1.6 Bq kg⁻¹. Radium was detected in all fish, and ranged from 0.4 to 2.1 Bq kg⁻¹, with an arithmetic mean of 1.0 Bq kg⁻¹. In regards to fish organs, cesium activity concentration was highest in muscles (maximum - 3.7 Bq kg⁻¹), while radium was highest in skeletons (maximum - 25 Bq kg⁻¹). Among cesium concentration factors, those for muscles were the highest (from seawater - an average of 47, from sediment - an average of 3.3, from mud with detritus - an average of 0.8). Radium concentration factors were the highest for skeleton (from seawater - an average of 130, from sediment - an average of 1.8, from mud with detritus - an average of 1.5). Additionally, annual intake of cesium and radium by human adults consuming muscles of this fish species has been estimated to provide, in aggregate, an effective dose of about 4.1 μSv y⁻¹.     

226Ra bioavailability to plants at the Urgeiriça uranium mill tailings site

Large amounts of solid wastes (tailings) resulting from the exploitation and treatment of uranium ore at the Urgeiri?a mine (north of Portugal) have been accumulated in dams (tailing ponds). To reduce the dispersion of natural radionuclides into the environment, some dams were revegetated with eucalyptus (Eucalyptus globolus) and pines (Pinus pinea). Besides these plants, some shrubs (Cytisus spp.) are growing in some of the dams. The objective of this study is to determine the 226Ra bioavailability from uranium mill tailings by quantifying the total and available fraction of radium in the tailings and to estimate its transfer to plants growing on the tailing piles. Plant and tailing samples were randomly collected and the activity concentration of 226Ra in plants (aerial part and roots) and tailings was measured by gamma-spectrometry. The exchangeable fraction of radium in tailings was quantified using one single step extraction with 1 mol dm-3 ammonium acetate (pH = 7) or 1 mol dm-3 calcium chloride solutions. The results obtained for 226Ra uptake by plants show that 226Ra concentration ratios for eucalyptus and pines decrease at low 226Ra concentrations in the tailings and appear relatively constant at higher radium concentrations. For shrubs, the concentration ratios increase at higher 226Ra solid waste concentrations approaching a saturation value. Percentage values of 16.0 +/- 8.3 and 12.9 +/- 8.9, for the fraction of radium extracted from the tailings, using 1 mol dm-3 ammonium acetate or calcium chloride solutions, respectively, were obtained. The 226Ra concentration ratios determined on the basis of exchangeable radium are one order of magnitude higher than those based on total radium. It can be concluded that, at a 95% confidence level, more consistent 226Ra concentration ratios were obtained when calculated on the basis of available radium than when total radium was considered, for all the dams.     

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.     

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.     

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.     

Foliar uptake of Cs from the water column by aquatic macrophytes

A transplant experiment was performed to determine the relative importances of root uptake from the sediments and foliar uptake from the water column in determining the accumulation of ¹³⁷Cs by aquatic macrophytes. Uncontaminated individuals of three species, Brasenia schreberi, Nymphaea odorata and Nymphoides cordata, were transplanted into pots containing either contaminated sediments (i.e. 1.2 Bq ¹³⁷Cs g⁻¹ dry mass) or uncontaminated sediments (i.e. < 0.1 Bq g⁻¹ dry mass) and immersed in Pond B, a former reactor cooling pond where ¹³⁷Cs concentrations in surface waters range from 0.4 to 0.8 Bq liter⁻¹. The plants in uncontaminated sediments rapidly accumulated ¹³⁷Cs from the water column and after 35 days of immersion had ¹³⁷Cs concentrations in leaves that were: (1) not statistically significantly different from those for plants in contaminated sediments; and (2) similar to those for the same species growing naturally in Pond B. The similarity in ¹³⁷Cs concentrations between naturally-occurring plants and those in pots with uncontaminated sediments suggests that foliar uptake from the water column is the principal mode of Cs accumulation by these species in Pond B.     

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.     

Distribution of long-lived radionuclides of the 238U series in the sediments of a small river in a uranium mineralized region of Spain

A study is presented on the distribution and mobilization of the natural U isotopes (238U and 234U), 230Th, and 226Ra in the sediments of a small river crossing an uranium mineralized zone where a disused uranium mine is located. Due to the preferential directions for surface run-off waters and to the mine's situation, one sampling point along the river bed was identified as a point of accumulation of radionuclides. The average values of the activity concentrations (Bq/kg) in this sediment sample were 5,025, 5,055, 5,915 and 1,694 for 238U, 234U, 230Th and 226Ra, respectively, while the respective average values of the activity concentrations (Bq/kg) for the sediment sample considered to give the background level were 125, 124, 131 and 370. Isotopic ratios between the descendants of 238U served to clarify some paths of distribution, involving the soils nearest to the sampling points and the location of these points with respect to the disused mine. The differences in behaviour found between the uranium, thorium and radium isotopes were associated to the mobility of these radionuclides in the fluvial system studied. Correlations between the radionuclide activity concentration ratios and stable element concentrations in the sediment samples were also investigated.     

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.     

Soil to plant transfer of Radium-226

A study of the uptake of ²²⁶Ra by vegetables was carried out in zones contaminated by wastes from an abandoned radium salts factory and from uranium mines and in uncontaminated regions of purely natural radioactivity. Radium-226 uptake depends on its concentration in the soil, the logarithm of its concentration in the vegetables being a linear function of the logarithm of the concentration in the soil. Concentration factors for ²²⁶Ra uptake by cabbage leaves range from 0·007 to 0·11; for herbage, they range from 0·09 to 0·5.     

Environmental impact studies of barium and radium discharges by produced waters from the "Bacia de Campos" oil-field offshore platforms,Brazil

Produced water samples from different E&P offshore petroleum platforms, belonging to the Bacia de Campos oil field, Brazil, were analyzed for barium, 226Ra and 'Ra. The concentrations measured are in the range of 0.36-25.7 mg l(-1) for barium, 0.012-6.0 Bq l(-1) for 226Ra and <0.05-12.0 Bq l(-1) for 1Ra. A strong correlation between the concentration of barium and radium isotopes was observed (226Ra: r2=0.926: 228Ra: r2=0.785). Additionally, seawater and sediment samples were taken at different distances (from 250 to 1,000 m) from the two selected platforms. Water samples were analyzed for dissolved and particulate barium, 226Ra and 225Ra and the sediment samples for total and leachable barium, 226Ra and 228Ra. The results showed that even for the shortest sampling distance (250 m) from the discharge point, barium, 226Ra and 228Ra concentrations are similar to the local background, indicating that dispersion by local currents is enough to minimize environmental impacts.     

Indoor air quality: Radon—Report on a WHO working group

The WHO Regional Office for Europe organized a working group in Dubrovnik, Yugoslavia, on 26–30 August 1985, which discussed radon as a pollutant affecting indoor air quality. Much of the natural background radiation to which the general public is exposed comes from the decay of ²²⁶Ra which produces radon gas and other products. Because radium is a trace element in most rock and soil, indoor concentrations of radon can come from a wide variety of substances, such as building materials and the soil under building foundations. Tap water taken from wells or underground springs may be an additional source. Radon daughter concentrations are considerably higher indoors than outdoors and are of the order of 2–5 Bq m⁻³ equilibrium equivalent radon (EER) concentration. It has been estimated that current exposure to radon gas could account for as much as 5–15% of all lung cancer deaths. It was recommended that, in general, buildings with concentrations of more than 100 Bq m⁻³ EER, as an annual average, should be considered for remedial action to lower such concentrations if simple measures are possible.     

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.     

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.     

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.     

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.     

Contamination of settling ponds and rivers as a result of discharge of radium-bearing waters from Polish coal mines

Saline waters from underground coal mines in Poland often contain natural radioactive isotopes, mainly 226Ra from the uranium decay series and 228Ra from the thorium series. Approximately 40% of the total amount of radium remains underground as radioactive deposits, but 225 MBq of 226Ra and 400 MBq of 228Ra are released daily into the rivers along with the other mine effluents from all Polish coal mines. Technical measures such as inducing the precipitation of radium in gobs, decreasing the amount of meteoric inflow water into underground workings, etc. have been undertaken in several coal mines, and as a result of these measures, the total amount of radium released to the surface waters has diminished by about 60% during the last 5-6 years. Mine water can have a severe impact on the natural environment, mainly due to its salinity. However, associated high levels of radium concentration in river waters, bottom sediments and vegetation have also been observed. Sometimes radium concentrations in rivers exceed 0.7 kBq/m3, which is the permitted level for waste waters under Polish law. The extensive investigations described here were carried out for all coal mines and on this basis the total radium balance in the effluents has been calculated. Measurements in the vicinity of mine settling ponds and in rivers have given us an opportunity to study radium behaviour in river waters and to assess the degree of contamination. Solid waste materials with enhanced natural radioactivity have been produced in huge amounts in the power and coal industries in Poland. As a result of the combustion of coal in power plants, low-radioactive waste materials are produced, with 226Ra concentration seldom exceeding a few hundreds of Bq/kg. A different situation is observed in coal mines, where, as a result of precipitation of radium from radium-bearing waters, highly radioactive deposits are formed. Sometimes the radioactivity of such materials is extremely high; precipitates from coal mines may have radium concentrations of 400,000 Bq/kg--equivalent to 3% uranium ore. Usually, such deposition takes place underground, but sometimes co-precipitation of radium with barium takes place on the surface, in settling ponds and in rivers. Therefore management of solid waste with technologically enhanced natural radioactivity (TENR) is a very important subject.     

210Pb-dating of a lake sediment core from Lough Carra (Co. Mayo, western Ireland): use of paleolimnological data for chronology validation below the 210Pb dating horizon

The chronologies and sediment accumulation rates for a lake sediment sequence from Lough Carra (Co. Mayo, western Ireland) were established by applying the constant initial concentration (CIC) and constant rate of supply (CRS) hypotheses to the measured ²¹⁰Pb_excess profile. The resulting chronologies were validated using the artificial fallout radionuclides ¹³⁷Cs and ²⁴¹Am, which provide independent chronostratigraphic markers for the second half of the 20th century. The validity of extrapolating the derived CIC and CRS dates below the ²¹⁰Pb dating horizon using average sedimentation rates was investigated using supplementary paleolimnological information and historical data. Our data confirm that such an extrapolation is well justified at sites characterised by relatively stable sedimentation conditions.     

Bioaccumulation and lack of oxidative stress response in the ragworm H. diversicolor following exposure to Ra in sediment

The main effluent from oil and gas production, produced water, from some platforms in the North Sea contains elevated concentrations of ²²⁶Ra. The aim of this study was to investigate whether ²²⁶Ra in sediment would accumulate in and affect sediment-dwelling organisms. In addition, we wanted to determine if the bioavailability would be modulated by the presence of a scale inhibitor which is used during oil and gas production. Hediste diversicolor was therefore exposed to different levels of ²²⁶Ra (30–6600 Bq kg⁻¹) in combination with scale inhibitor in the sediments in a flow through system. The levels of radioactivity in the exposures were close to levels that can be measured in proximity to oil/gas production facilities. ²²⁶Ra spiked to natural sediment partitioned into pore water and accumulated in the sediment-dwelling polychaete following a four-week exposure period. The results suggest that ²²⁶Ra did not bind strongly to sediment (low sediment:water partitioning coefficient), but it was not shown to bioaccumulate in any great extent (bioaccumulation factors of 0.019–0.022). Exposure of H. diversicolor in sediments with up to 6600 Bq kg⁻¹²²⁶Ra had no measurable effect on the total oxyradical scavenging capacity of the organisms compared to control. So although they accumulated the alpha-emitter, the treatments did not appear to cause oxidative stress in polychaete tissues.