Precipitation scavenging of 7Be and 137Cs radionuclides in air

Atmospheric depositional fluxes of the naturally occurring 7Be of cosmogenic origin and 137Cs from fallout of the Chernobyl accident were measured over a 6-year period (January 1987-December 1992) at Thessaloniki, Greece (40 degrees 38'N, 22 degrees 58'E). Total precipitation accumulation during 1987-1992 varied between 33.7 cm and 65.2 cm, reflecting a relatively dry (precipitation-free) climate. The activity concentrations of 7Be and 137Cs in rainwater depended on the precipitation rate, being higher for low precipitation rates and lesser for high precipitation rates. 137Cs was removed by rain and snow more efficiently than 7Be. Snowfall was more efficient than rainfall in removing the radionuclides from the atmosphere. The annual bulk depositional fluxes of 7Be varied between 477 and 1133 Bq m(-2) y(-1) and this variability was attributed to the amount of precipitation and the variations of the atmospheric concentrations of 7Be. The annual bulk depositional fluxes of 137Cs showed a significant decrease over time from 1987 to 1992, resulting in a removal half-life of 1.33 years. The presence of 137Cs in air, and therefore in rainwater and snow, long after the Chernobyl accident (26 April 1986) was mainly due to the resuspension process. The normalized depositional fluxes of both radionuclides showed maximal values during the spring season where the maximum amount of precipitation occurred. The relatively high positive correlation between 7Be and 137Cs normalized depositional fluxes indicates that the scavenging process of local precipitation controlled the fluxes of both radionuclides. The dry depositional flux of 7Be was less than 9.37% of total (wet and dry) depositional flux. The fraction of dry-to-total depositional flux of 137Cs was much higher than that of 7Be, due to the resuspended soil.     

Establishment of control site baseline data for erosion studies using radionuclides: a case study in East Slovenia

The aim of the present study was to establish a reference site and its soil characteristics for use of fallout radionuclides in erosion studies in Slovenia. Prior to this study, no reference site and baseline data existed for Slovenia for this purpose. In the agricultural area of Gori?ko in East Slovenia, an undisturbed forest situated in Šalamenci (46°44’N, 16°7’E), was selected to establish the inventory value of fallout ¹³⁷Cs and to establish a baseline level of multi-elemental fingerprint (major, minor, trace elements including heavy metals) and naturally occurring radionuclides in soils. A total of 20 soil profiles were collected at four 10 cm depth increments for evaluation of baseline level of ¹³⁷Cs inventory. An exponential distribution for ¹³⁷Cs was found and the baseline level inventory was established at 7300 ± 2500 Bq m⁻² with a coefficient of variation of 34%. Of this mean present-day inventory, approximately 45% is due to the Chernobyl contribution.The physical degradation of soils through erosion is linked with biochemical degradation. This study introduces an approach to establishment of the naturally occurring radionuclide and elemental fingerprints baseline levels at a reference site which can provide comparative data to those from neighbouring agricultural fields for assessment of soil redistribution magnitude using fallout radionuclides. In addition, this information will be used to determine the impact of soil erosion processes and agricultural practices on soil quality and redistribution within agricultural landscapes in Slovenia.     

Comparative advantages and limitations of the fallout radionuclides (137)Cs, (210)Pb(ex) and (7)Be for assessing soil erosion and sedimentation

The fallout radionuclides (FRNs) (137)Cs, (210)Pb(ex) and (7)Be are increasingly being used as a means of obtaining quantitative information on soil erosion and sediment redistribution rates within agricultural landscapes, over a range of different timescales, and they are frequently seen to represent a valuable complement to conventional measurement techniques. The recent development of the (7)Be method has greatly extended the timescale over which FRNs can be used, by permitting assessment of short-term soil erosion linked to individual events and changing soil management practices. This paper aims to review the advantages and limitations of each of the three FRNs and to identify key knowledge gaps linked to their use. In addition, guidelines for selecting the most appropriate FRN and associated approach, in order to deal with a range of spatial and temporal scales and to investigate specific sets of agro-environmental problems, are provided. Key requirements for future work, related to the application of FRNs in soil erosion investigations, are also identified. These include the upscaling of the approach to the catchment scale and a shift from use of the approach as a research tool to a decision support tool.     

Formation of radioactivity enriched soils in mountain areas

A field study was carried out in the Mercantour Mountains at 2200 m altitude to investigate the processes of soil enrichment in atmospheric Chernobyl (137)Cs. Soils with high (137)Cs activities have been collected in the pasture areas with frequently measured (137)Cs activity values of the order of 7000 Bq m(-2). At some single spots (about 6% of the studied area), activity in soils reached 300000 Bq m(-2), which represents 44% of the (137)Cs of the total area. Data further showed that spatial distribution of Cs depends widely on its origin: Chernobyl Cs is mainly concentrated in "enriched" soils, whereas older Cs and (241)Am fallout from nuclear weapons tests (NWTs) and natural atmospheric (210)Pb in soils is less heterogeneously distributed.In order to elucidate the processes which have led to the enrichment in Chernobyl (137)Cs in the Alps in May of 1986, we have studied the repartition of atmospheric (7)Be isotope (half-life=53.3 d) in the pasture compartments (soil, litter, grass, and snow). Snow (7)Be data give evidence that fallout enrichment is related to snow accumulation (snow drift). The transfer of beryllium occurs rapidly to the grass and litter, where the strongest pollutant accumulations were measured. However, (7)Be transport to the soil required more than 8 months.     

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.     

Vertical distributions of 210Pb excess, 7Be and 137Cs in selected grass covered soils in Southeast Queensland, Australia

Net accumulated areal activity densities and profiles of (210)Pb(ex), (7)Be and (137)Cs in the surface 10 cm of the soil are reported for eight sites in Southeast Queensland, Australia. Areal activity densities of (210)Pb(ex) and (7)Be varied from 1,080 to 4,100 Bqm(-2) and from 176 to 778 Bqm(-2), respectively. A significant (p < 0.001) portion of the variance (R(2) > 0.99) in their vertical distributions was explained by depth in the profile using an exponential function. Around 85% of accumulated (210)Pb(ex) was present in the surface 10 cm of the soil. Beryllium-7 was mainly confined to the grass and surface 2 cm of the soil. Average penetration half-depths of 3.6 +/- 0.2 and 0.3 +/- 0.1cm were determined for (210)Pb(ex) and (7)Be, respectively. Areal activity densities of global fallout (137)Cs varied from 10 to 361 Bqm(-2). Its signal was well mixed within the surface 10 cm. Comparison of the measured (137)Cs values to the estimated input value for the region ( approximately 490 Bqm(-2)) and profiling of a 1m deep soil core suggests a vertical migration of (137)Cs over the past decades. The paleo-radon activity flux determined from the (210)Pb(ex) areal activity density (5.1 +/- 0.9 mBqm(-2) s(-1)) was not statistically different to that measured using activated charcoal cups (5.5 +/- 0.4 mBqm(-2) s(-1)), tending to suggest that Southeast Queensland is neither a net source nor a net sink of (210)Pb-bearing aerosols.     

The temporal variations of (7)Be, (210)Pb and (210)Po in air in England

We have conducted measurements of naturally occurring radionuclides (7)Be, (210)Pb and (210)Po in air at ground level at Chilton, Oxfordshire, England. The sampling and analysis regime for the latter two isotopes has been optimised to minimise uncertainties in measurement due to decay of (210)Po and in-growth of (210)Pb during the sampling and analysis period. Analysis times were reduced by using Cerenkov counting to assay the (210)Bi daughter of (210)Pb. Monthly data collected over a four-year period are presented and discussed. (7)Be activity concentrations appear to peak in spring. (210)Pb activity concentrations also follow a seasonal trend reflecting different (222)Rn emanation rates from soil during winter and summer. Data for (210)Po show no such trend.     

Geographical mapping and associated fractal analysis of the long-lived Chernobyl fallout radionuclides in Greece

Immediately after the Chernobyl accident, a soil sampling programme was undertaken in order to detect and quantitatively analyse the long-lived radionuclides in the Chernobyl fallout. Soil samples (1242 in number) of 1 cm thick surface soil were collected in Greece during the period from May-November 1986. The samples were counted and analysed using Ge detector set-ups. The 137Cs fallout data have already been analysed, mapped and published. In an attempt to improve this analysis and also to extent it to other fallout radionuclides, an in-house unix-based data base/geographical information system (DBGIS) was developed. Multifractal analyses of the deposition patterns have also been performed. In the present work, an analysis of the results of the deposition of 137Cs, 134Cs, 144Ce, 141Ce, 125Sb, 110mAg, 106Ru, 103Ru, 95Zr and 54Mn are presented together with relevant fractal analysis and three characteristic contour maps. The maximum detected values of the above-mentioned radionuclides were 149.5 +/- 0.1, 76.1 +/- 0.1, 32.9 +/- 0.2, 46 +/- 2, 4.56 +/- 0.02, 7.98 +/- 0.02, 79.1 +/- 0.4, 337 +/- 2, 20.1 +/- 0.2 and 3.02 +/- 0.02 kBq m-2, respectively. Furthermore, a statistical technique to compare contour maps was introduced and applied to explain the differences which appeared in the maps of the above-mentioned radionuclides.     

Radiostrontium hot spot in the Russian Arctic: ground surface contamination by (90)Sr at the "Kraton-3" underground nuclear explosion site

Strontium-90 activity concentrations in surface soils and areal deposition densities have been studied at a site contaminated by an accidental release to atmosphere from the underground nuclear explosion "Kraton-3" conducted near the Polar Circle (65.9 degrees N, 112.3 degrees E) within the territory of the former USSR in 1978. In 2001-2002, the ground surface contamination at 14 plots studied ranged from 20 to 15 000 kBq m(-2), which significantly exceeds the value of 0.44 kBq m(-2) deduced for three background plots. The zone with substantial radiostrontium contamination extends, at least, 2.5 km in a north-easterly direction from the borehole. The average (137)Cs/(90)Sr ratio in the ground contamination originated from the "Kraton-3" fallout was estimated to be 0.55, which is significantly different from the ratio of 2.05 evaluated for background plots contaminated mostly from global fallout. Although vertical migration of (90)Sr in all undisturbed soil profiles studied is more rapid than that for (137)Cs, the depth of percolation of both radionuclides into the ground is mostly limited to the top 10-20 cm, which may be explained, primarily, by permafrost conditions. The horizontal migration rate of radiostrontium in the aqueous phase exceeds the radiocaesium migration rate by many times. This phenomenon seems to be a reason for the significant enrichment of the soil surface layers by radiostrontium at some sites, with variations occurring in accordance with small-scale irregularities of landscape.     

南京地区7Be沉降特征

7Be是研究大气科学与地球化学的核元素之一，对研究短期过程的地表土壤颗粒迁移具有较大价值。为了解南京地区利用7Be进行土壤侵蚀示踪研究的合适时机，于2010年1月~2011年12月收集南京地区各月的7Be沉降样品，经实验室化学实验处理和γ谱仪测量，计算7Be沉降通量，并分析7Be大气沉降的季节性变化趋势。结果表明：南京地区平均7Be沉降量为1 62178 Bq/（m2·a），沉降通量为066～1449 Bq/（m2·d），平均沉降通量为444 Bq/（m2·d）；7Be沉降通量的季节变化呈现双峰型趋势，冬末春初和夏季是两个高值区；7Be沉降的а值冬春季较大，夏季最低；降雨量大小与沉降量存在明显的正相关     

A simplified 137Cs transport model for estimating erosion rates in undisturbed soil

(137)Cs is an artificial radionuclide with a half-life of 30.12 years which released into the environment as a result of atmospheric testing of thermo-nuclear weapons primarily during the period of 1950s-1970s with the maximum rate of (137)Cs fallout from atmosphere in 1963. (137)Cs fallout is strongly and rapidly adsorbed by fine particles in the surface horizons of the soil, when it falls down on the ground mostly with precipitation. Its subsequent redistribution is associated with movements of the soil or sediment particles. The (137)Cs nuclide tracing technique has been used for assessment of soil losses for both undisturbed and cultivated soils. For undisturbed soils, a simple profile-shape model was developed in 1990 to describe the (137)Cs depth distribution in profile, where the maximum (137)Cs occurs in the surface horizon and it exponentially decreases with depth. The model implied that the total (137)Cs fallout amount deposited on the earth surface in 1963 and the (137)Cs profile shape has not changed with time. The model has been widely used for assessment of soil losses on undisturbed land. However, temporal variations of (137)Cs depth distribution in undisturbed soils after its deposition on the ground due to downward transport processes are not considered in the previous simple profile-shape model. Thus, the soil losses are overestimated by the model. On the base of the erosion assessment model developed by Walling, D.E., He, Q. [1999. Improved models for estimating soil erosion rates from cesium-137 measurements. Journal of Environmental Quality 28, 611-622], we discuss the (137)Cs transport process in the eroded soil profile and make some simplification to the model, develop a method to estimate the soil erosion rate more expediently. To compare the soil erosion rates calculated by the simple profile-shape model and the simple transport model, the soil losses related to different (137)Cs loss proportions of the reference inventory at the Kaixian site of the Three Gorge Region, China are estimated by the two models. The over-estimation of the soil loss by using the previous simple profile-shape model obviously increases with the time period from the sampling year to the year of 1963 and (137)Cs loss proportion of the reference inventory. As to 20-80% of (137)Cs loss proportions of the reference inventory at the Kaixian site in 2004, the annual soil loss depths estimated by the new simplified transport process model are only 57.90-56.24% of the values estimated by the previous model.     

Plutonium contamination from accidental release or simply fallout: study of soils at Palomares (Spain)

The activity concentration of plutonium in an environmental sample does not usually constitute sufficient information to determine if it is due only to fallout. Alpha and gamma spectrometry are used here conjointly in the study of environmental soil samples to distinguish between samples showing plutonium contamination due to fallout exclusively, and samples contaminated with plutonium from another source. The method was applied to soil samples collected in Palomares (Spain), where an accidental release of aerosols contaminated with plutonium occurred. The two contributions (fallout and accidentally released plutonium) were separated by means of the activity ratios between various radionuclides present in the samples analyzed. The fallout level was estimated from the 239 + 240Pu/137Cs activity ratio. For samples showing contamination due to the accident, the 238Pu/239 + 240Pu and 239Pu/240Pu activity ratios were also calculated to determine the grade of plutonium of this contamination.     

Classification of soil samples according to their geographic origin using gamma-ray spectrometry and principal component analysis

A principal component analysis (PCA) was used for classification of soil samples from different locations in Serbia and Montenegro. Based on activities of radionuclides ((226)Ra, (238)U, (235)U, (40)K, (134)Cs, (137)Cs, (232)Th and (7)Be) detected by gamma-ray spectrometry, the classification of soils according to their geographical origin was performed. Application of PCA to our experimental data resulted in satisfactory classification rate (86.0% correctly classified samples). The obtained results indicate that gamma-ray spectrometry in conjunction with PCA is a viable tool for soil classification.     

Availability and immobilization of 137Cs in subtropical high mountain forest and grassland soils

To understand the behavior of (137)Cs in undisturbed soils after nuclear fallout deposition between the 1940s and 1980s, we investigated the speciation of (137)Cs in soils in forest and its adjacent grassland from a volcano and subalpine area in Taiwan. We performed sequential extraction of (137)Cs (i.e., fractions readily exchangeable, bound to microbial biomass, bound to Fe-Mn oxides, bound to organic matter, persistently bound and residual). For both the forest and grassland soils, (137)Cs was mainly present in the persistently bound (31-41%) and residual (22-62%) fractions. The proportions of (137)Cs labile fractions--bound to exchangeable sites, microbial biomass, Mn-Fe oxides, and organic matter--were lower than those of the recalcitrant fractions. The labile fractions in the forest soils were also higher than those in the grassland soils, especially in the volcanic soil. The results suggest that the labile form of (137)Cs was mostly transferred to the persistently bound and resistant fractions after long-term deposition of fallout. The readily exchangeable (137)Cs fraction was higher in soils with higher organic matter content or minor amounts of 2:1 silicate clay minerals.     

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.     

The geographic distribution of radionuclide deposition across the continental US from atmospheric nuclear testing

For the first time, calculations for the more than 3000 counties of the US have been completed that estimate the average deposition density (Bq m(-2)) of more than 40 radionuclides in fallout from atmospheric nuclear weapons tests conducted in the US (1951-1962) and 19 radionuclides from tests conducted elsewhere in the world (1952-1963). The geographic pattern of deposition across the US, as well as the amount of fallout deposited, varied significantly depending on whether the tests were conducted within or outside of the US. Fallout deposited from the Nevada Test Site (NTS) varied geographically as a result of dispersion and dilution in the atmosphere, the wind patterns following each test, and the occurrence of localized rainfall events. In general, states immediately east of the NTS received the highest deposition from tests conducted there. In contrast, the variation in deposition across the country from global fallout was less than for NTS fallout primarily reflecting variations in annual precipitation across larger regions. Hence, in the eastern and mid-western US, where rainfall is above the national average, higher levels of global fallout were deposited than in the more arid southwestern states. This paper presents a summary of the methods used and findings of our studies on fallout from NTS and global fallout, with emphasis on two of the most important radionuclides, (131)I and (137)Cs.     

Distribution and flux of 238Pu, 239,240Pu, 241Am, 137Cs and 210Pb to high arctic lakes in the Thule district (Greenland)

Environmental samples (soil, sediment and lake water) in the Thule area (NW Greenland) have been studied to assess the contamination of radionuclides originating from a nuclear weapons accident (the Thule accident in 1968). Four lakes were chosen at different distances from the point of impact with the Thule air base community situated in between. The sedimentation rates in the lakes varied from 0.4 mm a(-1) (5 mg cm(-2) a(-1)) to 1.6 mm a(-1) (82 mg cm(-2) a(-1)). With these sedimentation rates, it is not possible to resolve the (239,240)Pu global fallout peak from a possible (239,240)Pu "accident" peak in the sediment depth profiles. However, the (239,240)Pu/(137)Cs and the (238)Pu/(239,240)Pu ratios agreed well with global fallout ratios, indicating that plutonium originating from the accident had not reached these lakes. This also indicates that the Thule air base community has probably only been exposed to radionuclides from the accident to a very limited extent. A limited study showed that (210)Pb could not be used as a normalizing nuclide to explain the transport of transuranic elements from the catchment area to the lake, i.e. (210)Pb has a different transport mechanism from that of the transuranic elements studied in this investigation.     

Intra-cultivar variability of the soil-to-grain transfer of fallout 137Cs and 90Sr for winter wheat

Differences between the root uptake of fallout radionuclides by different cultivars ('inter-cultivar' variability) growing on the same field may be influenced not only by genetic differences of the cultivars, but also by the spatial variability of the soil-to-grain transfer within the cultivation area of each cultivar. This 'intra-cultivar' variability was investigated in 2001 and 2002 for 137Cs and 90Sr using three winter wheat cultivars with four replicates for each cultivar at three different sites in Bavaria, Germany. The intra-cultivar variability proved to be in the same range as the inter-cultivar variability which was determined earlier at the same sites for both radionuclides. An ANOVA of the 137Cs data set revealed that the variability of the 137Cs soil-to-grain transfer was caused by the soil and climate (year) at the field sites and the interaction of cultivar and field. A significant contribution of the factor 'cultivar' alone to the variability could not be detected. This may be due to the complex environmental conditions to which plants are exposed in field experiments. To find wheat cultivars with minimal uptake of fallout radionuclides it may be better to examine the molecular mechanisms of their root uptake in order to identify targets for breeding "safer" plants.     

Biomagnification of 7Be, 234Th, and 228Ra in marine organisms near the northern Pacific coast of Japan

Enrichment of natural radionuclides of thorium, radium and beryllium in several kinds of marine organisms was investigated near the Pacific coast of Miyagi Pref., Japan. The radioactivity of 7Be, 210Pb, 234Th, 238U, 228Ra and 137Cs was measured using gamma spectrometry. High concentrations of 234Th were observed in ascidian livers (50-400 Bq/kg dry) and excrement (2000-2900 Bq/kg dry), although the parent 238U concentrations were less than 3 Bq/kg dry. Such extreme disequilibrium between 238U and 234Th activity was observed in other organisms (barnacles, mussels and brown algae). Relatively high concentrations of 228Ra were detected in ascidian livers and were observed to decrease according to its half-life (5.75 year), suggesting disequilibrium with its parent 232Th. High concentrations (about 1900-5000 Bq/kg dry) of 7Be were detected in ascidian liver. Possible mechanisms for the observed biomagnification and bioaccumulation of these radionuclides in the organisms analyzed were proposed.