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.     

Vertical distribution and characteristics of soil humic substances affecting radionuclide distribution

The humic substances extracted from different soil depths are separated into humic (HA) and fulvic (FA) acids, and characterized for their chemical composition, proton exchange capacity, spectroscopic characteristics and binding properties to the europium ion. The chemical and spectroscopic results show that FA compared to HA has a relatively high O/C ratio, high acidic functional group contents and low aromatic contents. The synchronous fluorescence spectroscopic results show that the stability constant (K) of the soil humic substances with Eu(III) ion tends to increase as the soil depth becomes deeper, and HA has a slightly stronger binding ability than FA. The measured total site concentrations (C(L)) reveal that Eu(III) ion is loaded onto HA by 62-77% of the total acid sites, but FA is only approximately 50% covered by Eu(III) ion. Information could be useful in understanding the migration of radionuclides in soil layer.     

Behavior of heavy metals in model three-component soil systems

Model three-component soil systems including goethite (a mineral component) and a suspension of microorganisms (a biological component) have been used to study the interaction of Pb and Zn with the mineral surface. The results show that live microorganisms markedly reduced the adsorption of these metals, especially Pb, on the goethite shell surface. In the case of Pb, this is due to a decrease in the content of its nonexchangeable form; in the case of Zn, to a decrease in the content of its exchangeably bound compounds. An organic matter preparation obtained by autoclave treatment of microorganisms has a markedly weaker effect on metal adsorption, compared to the suspension of live microbial cells.     

Suitable gamma energy for gamma-spectrometric determination of U in surface soil samples of a high rainfall area in India

The paper presents a systematic study on suitability of various gamma lines for monitoring of ²³⁸U activity in soil samples around a uranium mineralized zone of Kylleng Pyndengsohiong Mawthabah (Domiasiat), Meghalaya in India. The area lies in a plateau region which recieves the highest average annual rainfall (12,000 mm) in the world. The geochemical behaviour of the uranium and its daughter products at such wet climatic conditions imposes restrictions to assess ²³⁸U through gamma lines of radon decay products. Soil samples were collected from nine locations around the uranium mineralization zone for analysis. The ratio of the concentration of uranium obtained from gamma energies of radium daughter products to the 63.29 keV of ²³⁴Th was found to vary from 1.01 to 2.07, which indicates a pronounced disequilibrium between uranium and radium daughters. The results obtained from various gamma energies were validated from the data generated by Instrumental Neutron Activation Analysis (INAA) technique. The ²³⁸U activities from the two analytical methods show a well fitted regression line with correlation coefficient 0.99 which validates the reliability of 63.29 keV energy for estimation of uranium in such conditions.     

Estimating the amount and distribution of radon flux density from the soil surface in China

Based on an idealized model, both the annual and the seasonal radon ((222)Rn) flux densities from the soil surface at 1099 sites in China were estimated by linking a database of soil (226)Ra content and a global ecosystems database. Digital maps of the (222)Rn flux density in China were constructed in a spatial resolution of 25 km x 25 km by interpolation among the estimated data. An area-weighted annual average (222)Rn flux density from the soil surface across China was estimated to be 29.7+/-9.4 mBq m(-2)s(-1). Both regional and seasonal variations in the (222)Rn flux densities are significant in China. Annual average flux densities in the southeastern and northwestern China are generally higher than those in other regions of China, because of high soil (226)Ra content in the southeastern area and high soil aridity in the northwestern one. The seasonal average flux density is generally higher in summer/spring than winter, since relatively higher soil temperature and lower soil water saturation in summer/spring than other seasons are common in China.     

Influence of microorganisms on the behavior of technetium and other elements in paddy soil surface water

Insolubilization patterns of technetium (Tc) and other trace elements (Sc, Co, Zn, Se, Rb, Sr, Y, Nb, Ce, Pm, Gd, Lu, Hf, and Re) in surface water covering paddy fields were compared to gain insight into the behavior of Tc in an agricultural environment. The insolubilization of Tc, which did not pass through a 0.2-microm-pore-size filter, was mainly caused by bacteria. Among the 14 other elements investigated, Nb was insolubilized by bacteria and the amounts of insoluble Nb were positively correlated with those of Tc. Although Re is a chemical analog of Tc, no similarity was observed. These results suggest that Tc behaves similarly to Nb in the insolubilization in surface water covering paddy fields.     

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.     

Sea to land transfer of anthropogenic radionuclides to the North Wales coast, Part I: external gamma radiation and radionuclide concentrations in intertidal sediments, soil and air

Previous projects specifically aimed at performing radiological assessments in the vicinity of North Wales, investigating the presence and transfer of radionuclides from sea to land, were in 1986 and 1989. Since then, changes have occurred in the radioactive discharges from the British Nuclear Group Sellafield site. Annual discharges of (137)Cs, (238)Pu, (239,340)Pu and (241)Am have decreased markedly whereas, up until recent years, discharges of (99)Tc have increased. It is therefore desirable to quantify current transfer processes of radionuclides in the North Wales region and thus provide an update on 15-year-old studies. A field campaign was conducted collecting soil samples from 10 inland transects and air particulates on air filters from three High Volume Air Samplers, along the northern coast of Wales at Amlwch, Bangor Pier and Flint. Complementary field data relating to external gamma dose rates were collected at the soil sites. The field data generated for (137)Cs, (238)Pu, (239,340)Pu and (241)Am were consistent with what had been reported 15 years previously. Therefore, there has been no increase in the supply of these Sellafield-derived radionuclides to the terrestrial environment of the North Wales coast. The (99)Tc data in sediments were consistent with reported values within annual monitoring programmes, however, a relatively high activity concentration was measured in one sediment sample. This site was further investigated to determine the reason why such a high value was found. At present there is no clear evidence as to why this elevated concentration should be present, but the role of seaweed and its capacity in accumulating (99)Tc and transferring it to sediment is of interest. The analysis of the field samples for (99)Tc, (137)Cs, (238)Pu, (239,240)Pu and (241)Am has provided a data set that can be used for the modelling of the transfer of anthropogenic radionuclides from sea to land and its subsequent radiological implications and is reported in an accompanying paper.     

Variability in background levels of surface soil radionuclides in the vicinity of the US DOE waste isolation pilot plant

Concentrations of radionuclides were measured in soils from a grid of locations surrounding the US Department of Energy Waste Isolation Pilot Plant (WIPP) in southeastern New Mexico and from a grid on a reference site approximately 20 km southeast of the WIPP site. Each of the two grids has 16 sampling locations (grid nodes) systematically distributed within an area of 16.580 ha. Sampling was conducted prior to the arrival of the first waste shipment at WIPP. Thus, the 137Cs and 23,240Pu in the soil are expected to have been deposited as global fallout, although the Gnome Site, 8.8 km southwest of the WIPP, is also a potential source of 239,240Pu and fission products. The reference grid has significantly higher concentrations of fallout and natural radionuclides than the WIPP grid. Up to 80% of the total variability in radionuclide concentrations across the two grids is attributable to differences between grid nodes. Differences between replicates within a location account for 44-50% of the variability in concentrations of the uranium isotopes, but only 11-17% of the variability in the concentrations of the other radionuclides. Samples having similar abundance of radionuclides were spatially aggregated across the terrain. The activity concentrations of the radionuclides were strongly correlated with the concentrations of Al and Pb, and with the percentages of sand, silt and clay in the soil. Normalizing radionuclide concentrations to the concentration of Al or percent fine particles can help adjust for differences in soil textures among samples and facilitate the detection of gradients or temporal changes in soil concentrations.     

Radioactivity level and soil radon measurement of a volcanic area in Cameroon

The radioactivity level of soils in a volcanic area in Cameroon was determined and discussed. Thirty soils samples were collected from Buea and Limbé cities located in the south-western Cameroon. These two regions are known for theirs volcanic grounds due to the presence of Mount Cameroon Mountain. The activity concentrations of natural radionuclides as well as that of the fission product were evaluated by gamma-ray spectrometry using a hyper-purity germanium detector (HPGe). The ranges of concentrations in the surveyed soils were 11-17 Bq kg(-1), 22-36 Bq kg(-1) and 43-201 Bq kg(-1) for (226)Ra, (232)Th and (40)K, respectively. The radioisotope (137)Cs was also found but in a very small amount. The outdoor absorbed dose rate 1m above ground with the corresponding annual effective dose rate, assuming a 20% occupancy factor was estimated. The radium equivalent and the external hazard index were also evaluated and results are compared with available data from other studies and with the world average value [United Nations Scientific Committee on the Effects of Atomic Radiation (UNSCEAR), 1988. Sources, Effects and Risks of Ionizing Radiation. Report to the General Assembly on the Effects of Atomic Radiation. United Nations, New York; UNSCEAR, 2000. Sources and Effects of Ionizing Radiations. Report to the General Assembly with Scientific Annexes. United Nations, New York]. A solid state nuclear track detector (SSNTD), LR-115 was used for soil radon measurements at a depth of 50 cm. The ranges of soil radon concentrations were 6.7-10.8 kBq m(-3) and 5.5-8.7 kBq m(-3) in Buea and Limbé, respectively. A positive correlation was found between concentrations of radium measured with gamma-spectrometry and the soil radon concentrations measured with the nitrate cellulose detectors. The results of this study provide the radioactivity level in soil of a volcanic area, which has been found to be within the safety limits. The south-western Cameroon can be considered as having normal natural background radiation.     

Behaviour and transport of radionuclides in soil and vegetation of a sand dune ecosystem

A sand dune ecosystem in the vicinity of the British Nuclear Fuels reprocessing plant at Sellafield, Cumbria, UK was used to examine the spatial, temporal and depth distributions of 134Cs, 137Cs, 238Pu, 239 + 240Pu and 241Am in soil and in two species of vegetation (Festuca rubra, Ammophila arenaria). Core samples showed evidence of the accumulation of radionuclides derived mainly from sea-to-land transfer. Accumulated deposits of radioactivity (0-0.1 m) lie within the range: 1.1-3.4 Bq kg-1 (134Cs), 260-440 Bq kg-1 (137Cs), 31-40 Bq kg-1 (238Pu), 150-215 Bq kg-1 (239 + 240Pu) and 190-240 Bq kg-1 (241Am). Soil profiles showed greater activity concentrations in their deeper regions and this is attributed to leaching of radionuclides in percolating drainage water accentuated by the coarse texture, low organic matter and clay mineral content of coastal sands. Radionuclide activity concentrations in F. rubra and A. arenaria were similar, in the ranges 20-70 Bq kg-1 (137Cs), 1-5 Bq kg-1 (238Pu), 10-30 Bq kg-1 (239 + 240Pu) and 10-65 Bq kg-1 (241Am). Clear temporal and spatial variations were observed in both species of vegetation, reflecting the weather conditions antecedent to the sampling period and the influence of sea-to-land transfer. Concentration ratios (vegetation:soil) for activity concentrations in the two species were similar, in the ranges: 0.05-0.14 (137Cs), 0.025-0.097 (238Pu), 0.022-0.057 (239 + 240Pu) and 0.025-0.212 (241Am).     

A 10-year study of the 137Cs distribution in soil and a comparison of Cs soil inventory with precipitation-determined deposition

During a 10-year period, 1988-1998, surface soil samples have been collected at Blentarp in southern Sweden and analysed for 137Cs from the Chernobyl accident and from the nuclear weapons tests. The distance between the sampling plots on the different sampling occasions has been no more than 3 m. The results show that the depth distribution of 137Cs is very similar for each of the sampling occasions, indicating that the caesium migration at this site is very small. The total activity measured in the soil cores is in agreement with the calculated activity of 137Cs deposited at the site after nuclear weapons tests and the Chernobyl accident, based on air activity concentration and the amount of precipitation. The calculated deposition of 137Cs originating from the bomb tests amounts to 1.41 kBq m-2 for the period 1962-1986, which is in agreement with the activity of nuclear weapons fallout measured in the soil samples (1.60 kBq m-2 as a mean value of the first four years of sampling). The calculated activity of 137Cs of Chernobyl origin was 0.79 kBq m-2, which agrees well with the value of 0.79 kBq m-2 measured in the soil samples in 1988.     

Distribution and migration of 95Zr in a tea plant/soil system

(95)Zr is a primary radionuclide in the radioactive liquid efflux from a pressurized water reactor and one of the main radionuclides released after nuclear accidents. The fission yield of (95)Zr is as high as 6.2%, however, its environmental behavior has not been well documented. An experiment was conducted to evaluate the accumulation and distribution of (95)Zr in a tea plant/soil system. (95)Zr was accumulated primarily in the trunk of tea plants after being taken up from the soil. The radioactivity concentration of (95)Zr in the trunk increased slowly with time, then it reached a dynamic equilibrium 14 days after application. The radioactivity concentration of (95)Zr in the other parts of the tea plant was very low; only slighter greater than the detection limit. The results indicated that (95)Zr was not readily translocated in the tea plant. About 98.9% of applied (95)Zr was found to concentrate in the upper 5 cm layer after being sprayed onto the soil surface. The results indicated that (95)Zr could not readily move downwards with percolating water due to strong adsorption to surface soil.     

Effect of biosurfactants on crude oil desorption and mobilization in a soil system

Microbially produced biosurfactants were studied to enhance crude oil desorption and mobilization in model soil column systems. The ability of biosurfactants from Rhodococcus ruber to remove the oil from the soil core was 1.4-2.3 times greater than that of a synthetic surfactant of suitable properties, Tween 60. Biosurfactant-enhanced oil mobilization was temperature-related, and it was slower at 15 degrees C than at 22-28 degrees C. Mathematical modelling using a one-dimensional filtration model was applied to simulate the process of oil penetration through a soil column in the presence of (bio)surfactants. A strong positive correlation (R(2)=0.99) was found between surfactant penetration through oil-contaminated soil and oil removal activity. Biosurfactant was less adsorbed to soil components than synthetic surfactant, thus rapidly penetrating through the soil column and effectively removing 65-82% of crude oil. Chemical analysis showed that crude oil removed by biosurfactant contained a lower proportion of high-molecular-weight paraffins and asphaltenes, the most nonbiodegradable compounds, compared to initial oil composition. This result suggests that oil mobilized by biosurfactants could be easily biodegraded by soil bacteria. Rhodococcus biosurfactants can be used for in situ remediation of oil-contaminated soils.     

A new generic sub-model for radionuclide fixation in large catchments from continuous and single-pulse fallouts, as used in a river model

This paper presents a new general sub-model for fixation in catchment areas to be used within the framework of a river model for substances such as radionuclides and metals from continuous and single-pulse fallouts. The model has been critically tested using data from 27 European river sites covering a very wide geographical area and contaminated by radiocesium and radiostrontium from the Chernobyl accident and from the nuclear weapons tests (NWT fallout). This modelling approach gives radionuclide concentrations in water (total, dissolved and particulate phases) at defined sites on a monthly basis. The overall river model is based on processes in the upstream river stretch and in the catchment area. The catchment area is differentiated into inflow (approximately dry land) areas and outflow (approximately wetland) areas. The model has a general structure, which can be used for all radionuclides or substances. It is simple to apply in practice since all driving variables may be readily accessed from maps and standard monitoring programs. The driving variables are: latitude, altitude, catchment area, mean annual precipitation and fallout. Note that for large catchments, this model does not require data on the characteristic soil type or the percentage of outflow areas (wet lands) in the catchment, as in most previous models, since in practice it is very difficult to obtain reliable data on characteristic soil type or percentage of outflow areas, especially in large and topographically complex catchments. Modelled values have been compared to empirical data from rivers sites covering a wide domain (catchment areas from 3000 to 3,000,000 km2, precipitation from 400 to 1700 mm/year; fallouts from 1600 to 280,000 Bq/m2; altitudes from 0 to 1000 m.a.s.l. and latitudes from 41 degrees to 72 degrees N). The river model with its sub-model for fixation predicts close to the uncertainty factors given by the empirical data, which have been shown to be about a factor of 1.6 for 137Cs and a factor of 2.2 for 90Sr in river water. The obtained characteristic uncertainty factors for 137Cs from the Chernobyl fallout is 2.4, for 137Cs from the NWT fallout it is 1.3 and for the 90Sr results from the NWT fallout it is 3 using the new model.     

Deposition and distribution of Chernobyl fallout fission products and actinides in a Russian soil profile

In this article the distribution of fission products and actinides in a soil profile from Novo Bobovicky in Russia, which was contaminated due to the Chernobyl nuclear power plant accident, is described. The ground deposition of long-lived fission products determined by gamma-spectrometry was (recalculated to 26 April 1986) 1600 kBq (137)Cs/m(2), 900 kBq (134)Cs/m(2) and 60 kBq (125)Sb/m(2). Of these radionuclides (137)Cs shows the dominating activity at the present time. After 6.5 years 90% of the Cs and Sb activity was contained in the upper 4 cm. A (239,240)Pu ground deposition of 77.4+/-8.0 Bq/m(2) was determined by alpha-spectrometry. The (238)Pu/(239,240)Pu activity ratio of 0.30+/-0.03 and (241)Pu/(239,240)Pu activity ratio of 115+/-14 (in 1986) measured in the soil profile, indicates that the analysed Pu originates mainly from the Chernobyl accident. The average (234)U/(238)U activity ratio of 1.06+/-0.29 indicates that the uranium in this soil is dominated by naturally occurring uranium.The alpha- and beta-autoradiography revealed that the activity is mainly present in particulate form. It could further be observed that the spots containing alpha- or beta-activity originated from different particles. A comparison of alpha-autoradiography with the bulk Pu and Am activity showed that 92% of the alpha-activity was present as clearly detectable alpha-spots.The beta-active particles, located by beta-autoradiography were correlated with gamma-spectrometric measurements and contained only (137)Cs. These hot spots ranged from 0.02 to 0.15 Bq.It could be concluded that the vertical transport of (137)Cs and fuel fragments occurs mainly by movement of particles through the soil. It could also be concluded that the fuel fragments found, in this soil were depleted in respect to Cs, Sb and Eu.Comparison of the analysed (238)Pu/(239,240)Pu, (241)Pu/(239,240)Pu and (241)Am/(239,240)Pu ratios with the ratios calculated with ORIGEN-S code gave an estimate of the average burn-up of the fuel particles to be in the range of 11-12 GWd/tU.The results presented in this article are valid for this single soil profile and should not be generalised unless validated in a more rigorous study of a larger number of soil profiles.     

Chlorpyrifos in surface waters before and after a federally mandated ban

Samples collected from rural and urban streams in the City of Denton, Texas, USA were analyzed for the organophosphorus pesticides diazinon and chlorpyrifos during the years preceding and following a United States Environmental Protection Agency ban on many chlorpyrifos uses. A network of 70 monitoring stations, based mainly on topography and hydrological considerations, were established within the three main watersheds of Denton. Monitoring stations were sampled monthly from March through August during periods of normal flow (baseflow), resulting in a total of 308 samples and 311 samples collected during 2001 and 2002, respectively. Pesticide concentrations were determined using commercially available enzyme-linked immunosorbent assays (ELISA) specific for each pesticide. Results from this temporally and spatially dense monitoring effort were used to illustrate the impacts of a ban on most chlorpyrifos sales that was imposed in December 2001. The total number of samples exhibiting concentrations above method lower limits of detection (LLD) decreased between 2001 and 2002 for both chlorpyrifos and diazinon. The total number of sites exhibiting at least one sample with concentrations above the LLD for chlorpyrifos, however, significantly decreased (Fisher's exact test, p<0.0001, n=70) when comparing 2001 (before the ban) with 2002 (after the ban). Similar analyses indicated no significant difference (Fisher's exact test, p=0.50, n=70) in the number of sites exhibiting detectable diazinon concentration between 2001 and 2002. Our results indicate that the cessation of retail chlorpyrifos sales at the end of 2001 resulted in a highly significant decrease in the surface water occurrences of this pesticide during 2002.