Distribution and mobilization of U, Th and 226Ra in the plant-soil compartments of a mineralized uranium area in south-west Spain

The activity concentrations of natural uranium isotopes (238U and 234U), thorium isotopes (232Th, 230Th and 225Th) and 226Ra were studied in soil and vegetation samples from a disused uranium mine located in the Extremadura region in the south-west of Spain. The results allowed us to characterize radiologically the area close to the installation and one affected zone was clearly manifest as being dependent on the direction of the surface water flow from the mine. The activity concentration mean values (Bq/kg) in this zone were: 10,924, 10,900, 10,075 and 5,289 for 238U, 234U, 230Th and 226Ra, respectively, in soil samples and 1,050, 1,060, 768 and 1,141 for the same radionuclides in plant samples. In an unaffected zone, the activity concentration mean values (Bq/kg) were: 184, 190, 234 and 7251 for 235U, 234U, 230Th and 226Ra, respectively, in soil samples and 28. 29, 31 and 80 in plant samples. The activity concentrations obtained for 232Th and 228Th showed that the influence of the mine was only important for the uranium series radionuclides. The relative radionuclide mobilities were determined from the activity ratios. Correlations between radionuclide activity concentrations and stable element concentrations in the soil samples helped to understand the possible distribution paths for the natural radionuclides.     

Uptake of uranium and thorium by native and cultivated plants

Large part of available literature on biogeochemistry of uranium and thorium refers to the studies performed either in highly contaminated areas or in nutrient solutions that have been artificially ‘spiked’ with radionuclides. Effects of background levels of natural radioactivity on soil-grown plants have not been studied to the same extent. In this paper, we summarised results of greenhouse and field experiments performed by the author from 2000 to 2006. We examined some of the factors affecting transfer of U and Th from soil to plants, differences in uptake of these radionuclides by different plants, relationships between U and Th in soil and in plants, and temporal variations of U and Th in different plant species. Concentrations of radionuclides (critical point for experimental studies on biogeochemistry of U and Th - rare trace elements in non-contaminated regions) and essential plant nutrients and trace elements were determined by instrumental neutron activation analysis.     

Plant/soil concentration ratios for paired field and garden crops, with emphasis on iodine and the role of soil adhesion

In the effort to predict the risks associated with contaminated soils, considerable reliance is placed on plant/soil concentration ratio (CR) values measured at sites other than the contaminated site. This inevitably results in the need to extrapolate among the many soil and plant types. There are few studies that compare CR among plant types that encompass both field and garden crops. Here, CRs for 40 elements were measured for 25 crops from farm and garden sites chosen so the grain crops were in close proximity to the gardens. Special emphasis was placed on iodine (I) because data for this element are sparse. For many elements, there were consistent trends among CRs for the various crop types, with leafy crops > root crops ≥ fruit crops ≈ seed crops. Exceptions included CR values for As, K, Se and Zn which were highest in the seed crops. The correlation of CRs from one plant type to another was evident only when there was a wide range in soil concentrations. In comparing CRs between crop types, it became apparent that the relationships differed for the rare earth elements (REE), which also had very low CR values. The CRs for root and leafy crops of REE converged to a minimum value. This was attributed to soil adhesion, despite the samples being washed, and the average soil adhesion for root crops was 500 mg soil kg⁻¹ dry plant and for leafy crops was 5 g kg⁻¹. Across elements, the log CR was negatively correlated with log Kd (the soil solid/liquid partition coefficient), as expected. Although, this correlation is expected, measures of correlation coefficients suitable for stochastic risk assessment are not frequently reported. The results suggest that r ≈ −0.7 would be appropriate for risk assessment.     

Variation among chlorine concentration ratios for native and agronomic plants

Variation among plant/soil concentration ratios (CRs) for important radionuclides requires attention because it is a major source of uncertainty in nuclear environmental safety assessments. For agronomic plants, variation among plant species is easy to deal with because there are relatively few species. In natural settings, there are vastly more species and the question becomes how to develop representative statistical distributions of CRs. Chlorine (Cl) is a good element with which to address this problem, because ³⁶Cl is a key radionuclide in nuclear waste disposal and yet stable Cl is easily measured in the environment. We measured CRs (dry weight basis) for Cl among edible parts of agronomic plants at one site, and found a geometric mean (GM) of 10, a geometric standard deviation (GSD) of 1.9 and a range of 5–66. When the GM was weighted by the relative contributions of the various plants to the human diet, it rose to 16. Among native plants at five sites, each site representative of a specific environment, the GMs were 4.0–13 and the GSDs were 2.9–6.2. The CRs for individual species ranged from 0.8 to 170. However, when weighted by relative contributions of the plants to selected animal diets, the GMs were as high as 50. The conclusions are that: the variation in CR for agronomic plants is a subset of the variation among native or all plants, variation among species (the GSD) can be sixfold, and variation among species is large enough that typical diets of specific animals could expose them to several-fold higher amounts of Cl (or ³⁶Cl) than expected from generic CR values.     

Uptake and distribution of natural radioactivity in wheat plants from soil

The uptake of naturally occurring uranium, thorium, radium and potassium by wheat plant from two morphologically different soils of India was studied under natural field conditions. The soil to wheat grain transfer factors (TF) were calculated and observed to be in the range of 4.0 x 10(-4) to 2.1 x 10(-3) for 238U, 6.0 x 10(-3) to 2.4 x 10(-2) for 232Th, 9.0 x 10(-3) to 1.6 x 10(-2) for 226Ra and 0.14-3.1 for 40K. Observed ratios (OR) of radionuclides with respect to calcium have been calculated to explain nearly comparable TF values in spite of differences in soil concentration of the different fields. They also give an idea about the discrimination exhibited by the plant in uptake of essential and nonessential elements. The availability of calcium and potassium in soil for uptake affects the uranium, thorium and radium content of the plant. The other soil factors such as illite clays of alluvial soil which trap potassium in its crystal lattice and phosphates which form insoluble compounds with thorium are seen to reduce their availability to plants. A major percentage (54-75%) of total 238U, 232Th and 226Ra activity in the plant is concentrated in the roots and only about 1-2% was distributed in the grains, whereas about 57% of 40K activity accumulated in the shoots and 16% in the grains. The intake of radionuclides by consumption of wheat grains from the fields studied contributes a small fraction to the total annual ingestion dose received by man due to naturally existing radioactivity in the environment.     

Transfer of (40)K, (238)U, (210)Pb, and (210)Po from soil to plant in various locations in south of Syria

Transfer factors of (40)K, (238)U, (210)Pb, and (210)Po from soil to some agriculture crops in various locations in south of Syria (Dara'a and Assuwaydaa districts) have been determined. Soil and vegetable crops (green pepper, cucumber, tomato, and eggplant), legumes crops (lentil, chickpea, and broad bean), fruit trees (apple, grape, and olives) and cereals (barley and wheat) were collected and analyzed for (238)U, (210)Pb, and (210)Po. The results have shown that higher transfer factors (calculated as Bqkg(-1) dry wt. plant material per Bqkg(-1) dry wt. soil) for (210)Po, (210)Pb and (238)U were observed in vegetable leaves than fruits and cereals leaves; the highest values of transfer factor (TF) for (238)U were found to be 0.1 for straw of chickpea. Transfer factors for (210)Po varied between 2.8x10(-2) and 2 in fruits of eggplant and grain of barley, respectively. In addition, several parameters affecting transfer factors of the radionuclides were evaluated. The results can be considered as base values for TF of natural radionuclides in the region.     

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.     

Soil to plant transfer of 238U, 226Ra and 232Th on a uranium mining-impacted soil from southeastern China

Both soil and plant samples of nine different plant species grown in soils from southeastern China contaminated with uranium mine tailings were analyzed for the plant uptake and translocation of 238U, 226Ra and 232Th. Substantial differences were observed in the soil-plant transfer factor (TF) among these radionuclides and plant species. Lupine (Lupinus albus) exhibited the highest uptake of 238U (TF value of 3.7x10(-2)), while Chinese mustard (Brassica chinensis) had the least (0.5x10(-2)). However, in the case of 226Ra and 232Th, the highest TFs were observed for white clover (Trifolium pratense) (3.4x10(-2)) and ryegrass (Lolium perenne) (2.1x10(-3)), respectively. 232Th in the tailings/soil mixture was less available for plant uptake than 226Ra or 238U, and this was especially evident for Chinese mustard and corn (Zea mays). The root/shoot (R/S) ratios obtained for different plants and radionuclides shown that Indian mustard had the smallest R/S ratios for both 226Ra (5.3+/-1.2) and 232Th (5.3+/-1.7), while the smallest R/S ratio for 238U was observed in clover (2.8+/-0.9).     

The influence of a coal-fired power plant operation on radionuclide concentrations in soil

Fifty-two soil samples in the vicinity of a coal-fired power plant (CFPP) in Figueira (Brazil) were analyzed. The radionuclide concentration for the uranium and thorium series in soils ranged from <9 to 282 Bq kg(-1). The range of 40K concentration in soils varied from <59 to 412 Bq kg(-1). The CFPP (10 MWe) has been operating for 35 years and caused a small increment in natural radionuclide concentration in the surroundings. This technologically enhanced natural radioactivity (TENR) was mainly due to the uranium series (234Th, 226Ra and 210Pb) and was observable within the first kilometer from the power plant. The CFPP influence was only observed in the 0-25 cm soil horizon. The soil properties prevent the radionuclides of the 238U-series from reaching deeper soil profiles. The same behavior was observed for 40K as well. No influence was observed for 232Th, which was found in low concentrations in the coal.     

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.     

Trace element and radionuclide mass balances at a coal-fired electric generating station

Coal, bottom ash, and fly ash from Milliken Station, a coal-fired 270 MW power plant, were analyzed for 20 elements (Ag, Al, As, Be, Cd, Co, Cr, Cu, Ga, Hg, Mn, Ni, Pb, Sb, Se, Sn, Te, Tl, V, and Zn) and the major natural radionuclides (²³⁸U series, ²³²Th series, and ⁴⁰K). Mass balance calculations showed that most of the Hg, and some of the Sb and Se, were unaccounted for by ash collection, suggesting their possible discharge into the atmosphere. Silver, As, Hg, Pb, Cd, and Zn were more concentrated in the fly ash than in the bottom ash while all of the other elements were equally distributed, by concentration, between the ash fractions. The radionuclides showed a 46% higher concentration in fly ash than in bottom ash, and ²¹⁰Pb was enriched in the fly ash relative to the other radionuclides by a factor of 2.4. Mass balance calculations indicated a balance within statistical error for the radionuclides, except for ²¹⁰Pb.     

Influence of soil texture on the distribution and availability of 238U, 230Th, and 226Ra in soils

The influence of soil texture on the distribution and availability of (238)U, (230)Th, and (226)Ra in soils was studied in soil samples collected at a rehabilitated uranium mine located in the Extremadura region in south-west Spain. The activity concentration (Bqkg(-1)) in the soils ranged from 60 to 750 for (238)U, from 60 to 260 for (230)Th, and from 70 to 330 for (226)Ra. The radionuclide distribution was determined in three soil fractions: coarse sand (0.5-2mm), medium-fine sand (0.067-0.5mm), and silt and clay (<0.067 mm). The relative mobility of the natural radionuclides in the different fractions was studied by comparison of the activity ratios between radionuclides belonging to the same radioactive series. The lability of these radionuclides in each fraction was also studied through selective extraction from the soils using a one-step sequential extraction scheme. Significant correlations were found for (238)U, (230)Th, and (226)Ra between the activity concentration per fraction and the total activity concentration in the bulk soil. Thus, from the determination of the activity concentration in the bulk soil, one could estimate the activity concentration in each fraction. Correlations were also found for (238)U and (226)Ra between the labile activity concentration in each fraction and the total activity concentration in bulk soil. Assuming that there is some particle-size fraction that predominates in the process of soil-to-plant transfer, the parameters obtained in this study should be used as correction factors for the transfer factors determined from the bulk soil in previous studies.     

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.     

Fallout distribution in Padua and Northeast Italy after the chernobyl nuclear reactor accident

The radioactive cloud from the Chernobyl nuclear reactor accident arrived in northeast Italy on 30 April 1986. Ground-level air activities detected in Padua reached maximum values of 28·6, 19·2, 3·3, 1·7 and 7·5 Bq m⁻³ for ¹³¹I, ¹³²Te(¹³²I), ¹³⁷Cs and ¹⁰³Ru, respectively, on 1 May; about 10 days later, the activities had fallen to less than 1% of peak values. Considerations of cloud homogeneity are reported.The distribution of fallout radionuclides in Padua was evaluated on the basis of radioactivity detected on natural surfaces. The average committed dose equivalent to the thyroid for adult people in Padua through ¹³¹I inhalation was estimated at 0·37 mSv. Soil activity was monitored daily in samples collected in Padua during the first weeks of May 1986. Fallout deposition over northeast Italy was measured on 75 surface soil samples collected during June 1986 and long-lived radionuclide distribution maps were derived.     

Invariance of isotope ratios of lithogenic radionuclides: more evidence for their use as sediment source tracers

Activities of radionuclides in the 238U (230Th, 226Ra, 210Pb) and 232Th (232Th, 228Th, 228Ra) decay series were determined in sediments from an east Texas watershed and examined with isotope ratios and compared to particulate organic carbon (POC), % fines (<63 microm) and total concentrations of Al, Fe and Mn. The objective was to elucidate the presence or absence of relationships affecting the effectiveness of these radionuclides in modeling sediment transport. Strong positive correlations were observed between radionuclides and Mn (Th) and % fines (Ra and Th). Isotope ratios effectively reduce these influences, supporting the contention that isotope ratios offset extrinsic variability in terrestrial sediments. Strong associations of 210Pbxs (excess 210Pb) and 226Ra/230Th with POC agree with data from marine and terrestrial settings, indicating that the role of POC in isotope fractionation, transport and sequestration merits further investigation.     

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.     

Primordial radionuclides in Canadian background sites: secular equilibrium and isotopic differences

A literature review and field sampling were done to obtain information on primordial (natural-series) radionuclide concentrations in terrestrial environments in diverse locations across Canada. Of special interest was the degree of secular equilibrium among members of decay series. The analytes measured in soils and plants were (nat)U by neutron activation-delayed neutron counting, (228)Th, (230)Th, (232)Th, (226)Ra and (210)Po by alpha spectroscopy, (210)Pb by gas flow proportional counting, (228)Ra by beta counting and (137)Cs by gamma spectroscopy. In addition, ICP-MS was used to obtain concentrations of about 50 analytes including elemental U, Pb, and Th. Samples were from seven representative background sites with a total of 162 plant samples from 38 different species. These data were supplemented by a review that gathered a large portion of the similar data from published sources. The sites chosen were semi-natural, far from any nuclear industry, although several were specifically located in areas with slightly elevated natural U concentrations. As might be expected, there were many cases of non-detectable concentrations. However, certain trends were evident. The activity ratio (210)Po/(210)Pb was unity in soils and non-annual plant tissues such as lichens. It was about 0.6 in annual plant tissues. These results are consistent with the time required for ingrowth of (210)Po to reach secular equilibrium. There was evidence from several sources that (210)Pb in plants came predominantly from deposition of (210)Pb from air after the decay of airborne (222)Rn. This was expected. Somewhat unexpected was the observation that (228)Th seemed to be much more plant available than (232)Th, even though both are in the same decay series and should be chemically similar. The difference was attributed to the combined effects of ingrowth from (228)Ra in the plant and effects of alpha recoil in mobilizing (228)Th in the soil. In general, the results of this study will benefit risk assessment, both in providing background concentrations, but also some indication of where isotope activity ratios can and cannot be used to estimate concentrations.     

Radiological characteristics and investigation of the radioactive equilibrium in the ashes produced in lignite-fired power plants

Coal- and lignite-fired power plants produce significant amounts of ashes, which are quite often being used as additives in cement and other building materials. In many cases, coal and lignite present high concentrations of naturally occurring radionuclides, such as 238U, 226Ra, 210Pb, 232Th and 40K. During the combustion process, the produced ashes are enriched in the above radionuclides. The different enrichment of the various radionuclides within a radioactive series, such as that of 238U, results in the disturbance of radioactive secular equilibrium. An extensive research project for the determination of the natural radioactivity of lignite and ashes from Greek lignite-fired power plants is in progress in the Nuclear Engineering Department of the National Technical University of Athens (NED-NTUA) since 1983. This paper presents detailed results for the natural radioactivity, the secular radioactive equilibrium disturbance and the radon exhalation rate of the fly-ash collected at the different stages along the emission control system of a lignite-fired power plant as well as of the bottom-ash. From the results obtained so far, it may be concluded that 226Ra radioactivity of fly-ash in some cases exceeds 1 kBq kg(-1), which is much higher than the mean 226Ra radioactivity of surface soils in Greece (25 Bq kg(-1)). Furthermore, the radioactivity of 210Pb in fly-ash may reach 4 kBq kg(-1). These results are interpreted in relation to the physical properties of the investigated nuclides, the temperature in the flue-gas pathway, as well as the fly-ash grain size distribution. It is concluded that towards the coldest parts of the emission control system of the power plant, the radioactivity of some natural nuclides is gradually enhanced, secular radioactive equilibrium is significantly disturbed and the radon exhalation rate tends to increase.     

Significant radioactive contamination of soil around a coal-fired thermal power plant

Soil samples were collected around a coal-fired power plant from 81 different locations. Brown coal, unusually rich in uranium, is burnt in this plant that lies inside the confines of a small industrial town and has been operational since 1943. Activity concentrations of the radionuclides 238U, 226Ra, 232Th, 137Cs and 40K were determined in the samples. Considerably elevated concentrations of 238U and 226Ra have been found in most samples collected within the inhabited area. Concentrations of 235U and 226Ra in soil decreased regularly with increasing depth at many locations, which can be explained by fly-ash fallout. Concentrations of 235U and 226Ra in the top (0-5 cm depth) layer of soil in public areas inside the town are 4.7 times higher, on average, than those in the uncontaminated deeper layers, which means there is about 108 Bq kg(-1) surplus activity concentration above the geological background. A high emanation rate of 222Rn from the contaminated soil layers and significant disequilibrium between 238U and 226Ra activities in some kinds of samples have been found.     

The assumption of linearity in soil and plant concentration ratios: An experimental evaluation

We have evaluated one of the main assumptions in the use of concentration ratios to describe the transfer of elements in the environment. The ratios examined in detail were the ‘concentration ratio’ (CR) of leaf to soil and the ‘partition coefficient’ of (K_d) of solid- to liquid-phase concentrations in soil. The ‘translocation ratio’ of berry to leaf was also computed when possible. Use of these ratios implies a linear relationship between the concentrations. Soil was experimentally contaminated to evaluate this linearity over more than a 1000-fold range in concentration. A secondary objective was to determine CR and K_d values in a long-term (2 y) outdoor study using a peat soil and a slow-growing native plant species, specifically blueberries (Vaccinium angustifolium). The elements I, Se, CS, Pb and U wer chosen as environmentally important elements expected to provide a broad range in CR and K_d values. the reuslts indicated that relationships of leaf and leachate concentrations were not consistently linearly related to the total soil concentrations for each of the elements. The modelling difficulties implied by these concentration dependencies can be partially offset by including in the models the strong negative correlation between CR and K_d. The error introduced by using a mean value of the ratios for Se or U resulted in up to a ten-fold increase in variability for CR and a three-fold increase for K_d.