Can 239 + 240Pu replace 137Cs as an erosion tracer in agricultural landscapes contaminated with Chernobyl fallout?

Erosion studies often use 137Cs from the global fallout (main period: 1953-1964) as a tracer in the soil. In many European countries, where 137Cs was deposited in considerable amounts also by the Chernobyl fallout in 1986, the global fallout fraction (GF-Cs) has to be separated from the Chernobyl fraction by means of the isotope 134Cs. In a few years, this will no longer be possible due to the short half-life of 134Cs (2 yr). Because GF-Cs in the soil can then no longer be determined, the potential of using 239 + 240Pu as a tracer is evaluated. This radionuclide originates in most European countries essentially only from the global fallout. The activities and spatial distributions of Pu and GF-Cs were compared in the soil of a steep field (inclination about 20%, area ca. 3 ha, main soil type Dystric Eutrochrept), sampled at 48 nodes of a 25 x 25 m2 grid. The reference values were determined at 12 points adjacent to the field. Their validity was assured by an inventory study of radiocaesium in a 70 ha area surrounding the field sampling 275 nodes of a 50 x 50 m2 grid. In the field studied, the activity concentrations of GF-Cs and Pu in the Ap horizon were not correlated (Spearman correlation coefficient R = 0.20, p > 0.05), and the activity balance of Pu differed from that of GF-Cs. Whereas no net loss of GF-Cs from the field was observed as compared to the reference site, Pu was more mobile with an average loss of ca. 11% per unit area. In addition, the spatial pattern of GF-Cs and Pu in the field differed significantly. The reason may be that due to their different associations with soil constituents, Pu and Cs represent different fractions of the soil, exhibiting different properties with respect to erosion/deposition processes. This indicates that both radionuclides or one of them may not be appropriate to quantity past erosion. When tracer losses are used to calibrate or verify erosion prediction models, systematic deviations may not only stem from model shortcomings but also from tracer technique.     

Distribution of fallout radionuclides (7Be, 137Cs, 210Pb and 239,240Pu) in soils of Taiwan

Depth profiles and cumulative deposition of four fallout radionuclides (7Be, 137Cs, 210Pb and 239,240Pu) were determined in presumably undisturbed soils in Taiwan. Inventories of these radionuclides in different areas correlate significantly with each other (except 7Be) and with mean annual rainfall, providing a necessary condition for the development of soil erosion studies in Taiwan. However, the data show very large spatial variability between and within landscape units, reflecting the steep topographic and meteorological gradients in the island. Thus, the application of fallout radionuclides to study soil conservation in Taiwan is expected to be a demanding task; it will call for dense sampling even at undisturbed reference sites.     

Activity ratios of 137Cs, 90Sr and 239+240Pu in environmental samples

Both global and Chernobyl fallout have resulted in environmental contamination with radionuclides such as 137Cs, 90Sr and 239+240Pu. In environmental samples, 137Cs and 239+240Pu can be divided into the contributions of either source, if also the isotopes 134Cs and 238Pu are measurable, based on the known isotopic ratios in global and Chernobyl fallout. No analogous method is available for 90Sr. The activity ratios of Sr to Cs and Pu, respectively, are known for the actual fallout mainly from air filter measurements; but due to the high mobility of Sr in the environment, compared to Cs and Pu, these ratios generally do not hold for the inventory many years after deposition. In this paper we suggest a method to identify the mean contributions of global and Chernobyl fallout to total Sr in soil, sediment and cryoconite samples from Alpine and pre-Alpine regions of Austria, based on a statistical evaluation of Sr/Cs/Pu radionuclide activity ratios. Results are given for Sr:Cs, Sr:Pu and Cs:Pu ratios. Comparison with fallout data shows a strong depletion of Sr against Cs and Pu.     

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.     

Spatial and temporal distribution of Pu in the Northwest Pacific Ocean using modern coral archives

Historical ²³⁹Pu activity concentrations and ²⁴⁰Pu/²³⁹Pu atom ratios were determined in skeletons of dated modern corals collected from three locations (Chuuk Lagoon, Ishigaki Island and Iki Island) to identify spatial and temporal variations in Pu inputs to the Northwest Pacific Ocean. The main Pu source in the Northwest Pacific is fallout from atmospheric nuclear weapons testing which consists of global fallout and close-in fallout from the former US Pacific Proving Grounds (PPG) in the Marshall Islands. PPG close-in fallout dominated the Pu input in the 1950s, as was observed with higher ²⁴⁰Pu/²³⁹Pu atom ratios (> 0.30) at the Ishigaki site. Specific fallout Pu contamination from the Nagasaki atomic bomb and the Ivy Mike thermonuclear detonation at the PPG were identified at Ishigaki Island from the ²⁴⁰Pu/²³⁹Pu atom ratios of 0.07 and 0.46, respectively. During the 1960s and 1970s, global fallout was the major Pu source to the Northwest Pacific with over 60% contribution to the total Pu. After the cessation of the atmospheric nuclear tests, the PPG again dominated the Pu input due to the continuous transport of remobilised Pu from the Marshall Islands along the North Equatorial Current and the subsequent Kuroshio Current. The Pu contributions from the PPG in recent coral bands (1984 onwards) varied over time with average estimated PPG contributions between 54% and 72% depending on location.     

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.     

Distribution of Np and Pu in Swedish lichen samples (Cladonia stellaris) contaminated by atmospheric fallout

The activity concentrations of (237)Np and the two Pu isotopes, (239)Pu and (240)Pu, were determined in lichen samples (Cladonia stellaris) contaminated by fallout from atmospheric nuclear test explosions and the Chernobyl accident. The samples were collected at 18 locations in Sweden, from north to south, between 1986 and 1988 and analysed with high-resolution inductively coupled plasma mass spectrometry (HR-ICP-MS) and alpha spectrometry. Data on the activity ratios (238)Pu/(239+240)Pu and (134)Cs/(137)Cs measured previously were also included in this study for comparison. The (237)Np activity concentration ranged from 0.08 +/- 0.01 to 2.08 +/- 0.17 MBq kg(-1), depending on the location of the sampling site and time of collection. The (239+240)Pu activity concentration ranged from 0.09 +/- 0.01 to 4.09 +/- 0.15 Bq kg(-1), with the (240)Pu/(239)Pu atomic ratio ranging between 0.16 +/- 0.01 and 0.44 +/- 0.03, the higher ratios indicating a combination of weapons test fallout and Chernobyl fallout. The (237)Np/(239)Pu atomic ratios ranged between 0.06 +/- 0.01 and 0.42 +/- 0.04, the lower ratios indicating combination of weapons test fallout and Chernobyl fallout. At a well-defined sampling site at Lake Rogen (62.32 degrees N, 12.38 degrees E), additional lichen samples were collected between 1987 and 1998 to study the distribution of Np and Pu in different layers. The concentrations of the two elements follow each other quite well in the profile.     

Assessment of the global fallout of plutonium isotopes and americium-241 in the soil of the central region of Saudi Arabia

A radiochemical technique for determination of plutonium isotopes and 241Am in soil samples is tested against IAEA-standard reference materials to determine its accuracy and precision for reliable results. The technique is then used in the investigation of topsoil samples, collected from the natural environment of the central region of Saudi Arabia, to assess the effect of fallout accumulation of these radionuclides in the region. Plutonium and americium were sequentially separated from all other components of the sample by anion-exchange chromatography and co-precipitated with Nd3+ as fluorides. The precipitates were mounted on membrane filters and measured using a high-resolution alpha-spectrometer. The results of the analysis of the reference materials showed satisfactory sensitivity and precision of the technique. The results of the analyzed soil samples show activity levels ranging from < LLD to 0.089 and from 相似文献   

A modelling study on 137Cs and 239,240Pu behaviour in the Alborán Sea, western Mediterranean

A model for simulating the dispersion processes of 137Cs and 239,240Pu in the Alborán Sea is described. The model consists of two hydrodynamic models: a 2D depth-averaged model and a two-layer model which provide tidal and geostrophic currents, respectively; a sediment transport model which provides suspended particle concentrations and sedimentation rates over the domain; and the radionuclide dispersion model including interactions of dissolved radionuclides with suspended particles and bed sediments. These processes are formulated using kinetic transfer coefficients. The hydrodynamic and sediment models are run and validated in advance, and their results are then used to simulate the dispersion of 137Cs and 239,240Pu, which are introduced from atmospheric fallout. Radionuclide concentrations in the water column and distributions in bed sediments have been compared with measurements in the sea. Both set of data are, in general, in agreement. The model has also been applied to calculate radionuclide fluxes through the Strait of Gibraltar. These computed fluxes have been compared with previous estimations as well.     

Vertical distribution of radionuclides in soil of a grassland site in Chernobyl exclusion zone

Five soil profiles from a site about 8 km SE of the Chernobyl NPP were investigated for the vertical distribution of radionuclides. The average (137)Cs-inventory at the site is about 2.6 MBq/m(2) (reference date 1 May 1986). Apart from (137)Cs, the following radionuclides have been identified (their activity ratios to (137)Cs in brackets): (134)Cs (0.537), (125)Sb (0.068), (60)Co (0.0022), (154)Eu (0.016), (155)Eu (0.020), (94g)Nb (9.5E-5), (239/240)Pu (0.0088), (238)Pu (0.040), (90)Sr (0.30) and (241)Am (0.011). Apparent vertical migration velocities are between 0.14 and 0.26 cm/a, apparent dispersion coefficients range from 0.02 to 0.13 cm(2)/a. The rankings of the velocities v for different radionuclides are (Sr, Cs, Sb, Co, Pu)< Am < Eu and Sr < (Cs, Nb), for D, the following rankings have been found: (Nb, Sr, Cs) < Am < Eu, Cs相似文献   

Modelling of a large-scale urban contamination situation and remediation alternatives

The Urban Remediation Working Group of the International Atomic Energy Agency's EMRAS (Environmental Modelling for Radiation Safety) program was organized to address issues of remediation assessment modelling for urban areas contaminated with dispersed radionuclides. The present paper describes the first of two modelling exercises, which was based on Chernobyl fallout data in the town of Pripyat, Ukraine. Modelling endpoints for the exercise included radionuclide concentrations and external dose rates at specified locations, contributions to the dose rates from individual surfaces and radionuclides, and annual and cumulative external doses to specified reference individuals. Model predictions were performed for a “no action” situation (with no remedial measures) and for selected countermeasures. The exercise provided a valuable opportunity to compare modelling approaches and parameter values, as well as to compare the predicted effectiveness of various countermeasures with respect to short-term and long-term reduction of predicted doses to people.     

Plutonium as a chronomarker in Australian and New Zealand sediments: a comparison with Cs

The construction of high resolution chronologies of sediment profiles corresponding to the last 50-100 years usually entails the measurement of fallout radionuclides ²¹⁰Pb and ¹³⁷Cs. The anthropogenic radionuclide, ¹³⁷Cs, originating from atmospheric nuclear weapons testing can provide an important “first appearance” horizon of known age (1954-1955), providing much-needed validation for the sometimes uncertain interpretations associated with ²¹⁰Pb geochronology. However, while ¹³⁷Cs usually provides a strong signal in sediment in the northern hemisphere, total fallout of ¹³⁷Cs in the southern hemisphere was only 25% that of the north and the low activities of ¹³⁷Cs seen in Australian and New Zealand sediments can make its horizon of first appearance somewhat arguable. Low ¹³⁷Cs fallout also limited the size of the 1963-1964 fallout peak, a peak that is usually seen in northern hemisphere sediment profiles but is often difficult to discern south of the equator.This paper shows examples of the use of nuclear weapons fallout Pu as a chronomarker in sediment cores from Australia (3 sites) and New Zealand (1 site). The Pu profiles of five cores are examined and compared with the corresponding ¹³⁷Cs profiles and ²¹⁰Pb geochronologies. We find that Pu has significant advantages over ¹³⁷Cs, including greater measurement sensitivity using alpha spectrometry and mass spectrometric techniques compared to ¹³⁷Cs measurements by gamma spectrometry. Moreover, Pu provides additional chronomarkers associated with changes in the Pu isotopic composition of fallout during the 1950s and 1960s. In particular, the ²³⁸Pu/^239+240Pu activity ratio shows distinct shifts in the early 1950s and the mid to late 1960s, providing important known-age horizons in southern hemisphere sediments. For estuarine and near-shore sediments Pu sometimes has another significant advantage over ¹³⁷Cs due to its enrichment in bottom sediment relative to ¹³⁷Cs resulting from the more efficient scavenging of dissolved Pu in seawater by sediment particles.     

Concentration and characterization of plutonium in soils of Hubei in central China

To study the Pu concentration and isotope ratio distributions present in China, the ^239+240Pu total activities and ²⁴⁰Pu/²³⁹Pu atom ratios in core soil samples from Hubei Province in central China were investigated using Accelerator Mass Spectrometry (AMS). The activities ranged from 0.019 to 0.502 mBq g⁻¹ and the ^239+240Pu inventories of 45 and ∼55 Bq m⁻² agree well with that expected from global fallout. The ²⁴⁰Pu/²³⁹Pu atom ratios in the soil ranged from 0.172 to 0.220. The ratios are similar to typical global fallout values. Hence, any close-in fallout contribution from the Chinese nuclear weapons tests, mainly conducted in the 1970s, must have either been negligible or had a similar ²⁴⁰Pu/²³⁹Pu ratio to that of global fallout. The top 10 cm layer of the soil contributes ∼90% of the total inventory and the maximum concentrations appeared in the 2-4 cm or 4-6 cm layers. It is suggested that climatic conditions and organic content are the two main factors that affect the vertical migration of plutonium in soil.     

Comparative analysis of (239)Pu, (137)Cs, (210)Pb and (40)K spatial distributions in the top soil layer at the Baltic coast

This paper presents the results of an investigation into the spatial distribution of radionuclides of artificial ((239,240)Pu, (137)Cs) and natural ((210)Pb, (40)K) origins in the upper (0-5 cm) soil layers on the Baltic coastline of Lithuania ( approximately 5 km(2) area). The samples were analysed by gamma ray spectrometry and combined radiochemical procedures. The highest (210)Pb, (239,240)Pu and (137)Cs activity concentrations were determined in the forest samples, whereas (40)K activity was rather homogeneous across the study area. Relatively high (239,240)Pu and (40)K activity concentrations were determined along the surf zone. The (210)Pb and (137)Cs activity concentrations showed a gradual increase from the surf zone to the forest. The average activity concentrations of (239,240)Pu, (137)Cs, (210)Pb and (40)K in the beach and forest samples, respectively, were as follows: 0.32+/-0.08 and 0.74+/-0.14; 50+/-4 and 1190+/-50; 4.7+/-2.0 and 48+/-6; 186+/-15 and 216+/-17 Bq/kg.     

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.     

Radiological impact of coal-fired power generation

A radiological impact assessment was carried out at the 4000 MW Nanticoke Thermal Generating Station on the north shore of Lake Erie and at an ash disposal site in Metropolitan Toronto, both operated by Ontario Hydro. Analyses were performed on feed coal, fly ash and bottom ash and on samples of air filters, precipitation, water, soil and vegetation in the vicinity of the generating station. The measured radionuclide levels in the vicinity of the generating station showed no evidence of enhancement from station emissions. There were no indications that leaching of radionuclides or emanation of radon gas from ash disposal sites would be a problem. There was evidence, however, of higher radionuclide concentrations on the finer ash particles. Furthermore, the use of fly ash in building materials could lead to enhanced radiation levels. Atmospheric dispersion and radiation dose calculations were also carried out. Predicted concentrations in air were all less than 1% of background values. The committed dose equivalent from one year of operation was estimated to be 0·27 μSv at the site boundary and 0·11 μSv at 10 km east of the site.     

Studies of Np and Pu in the marine environment of Swedish-Danish waters and the North Atlantic Ocean

The long-lived anthropogenic radionuclides (237)Np, (239)Pu and (240)Pu were determined in marine environmental samples (seaweed and seawater) collected from Swedish-Danish waters and the North Atlantic Ocean at various locations on different occasions during the period 1991-2001. The measurements were performed with sector field Inductively Coupled Plasma Mass Spectrometry (ICP-MS) and conventional alpha spectrometry. The (237)Np activity concentrations in Fucus vesiculosus and surface seawater from the Swedish west coast and Danish waters ranged from 0.16+/-0.02 to 1.02+/-0.09 mBq kg(-1) (dry weight) and 0.65+/-0.02 to 1.69+/-0.02 mBq m(-3), respectively, depending on the location and sampling year. Most of the (237)Np in these waters is believed to originate from the Sellafield nuclear reprocessing plant, with some contribution from global fallout. The (240)Pu/(239)Pu atomic ratios in F. vesiculosus samples are reported in this study with an overall average of 0.17+/-0.03. The (237)Np and (239)Pu activity concentrations observed in surface seawater collected in North Atlantic waters ranged from 0.16+/-0.01 to 0.62+/-0.08 mBq m(-3) and from 0.64+/-0.05 to 4.27+/-0.08 mBq m(-3), respectively, and the (237)Np/(239)Pu atomic ratios were a good indicator of conservative behaviour of Np in marine waters.     

Sources and distributions of Cs, Pu, Pu radionuclides in the north-western Barents Sea

Sediment deposits are the ultimate sink for anthropogenic radionuclides entering the marine environment. The major sources of anthropogenic radionuclides to the Barents Sea are fallout from nuclear weapons tests, long range transport from other seas, and river and non-point freshwater supplies. In this study we investigated activity concentrations, ratios, and inventories of the anthropogenic radionuclides, ¹³⁷Cs, ²³⁸Pu, ^239,240Pu in dated sediment cores collected along a north-south transect in the northwestern Barents Sea. The data were used to evaluate the influence of different sources on the derived spatial and temporal patterns of anthropogenic radionuclides in seafloor sediment deposits. Activity concentrations of ¹³⁷Cs ranged from <0.1 Bq/kg to 10.5 Bq/kg while ^239,240Pu ranged from <0.01 Bq/kg to 2.74 Bq/kg and ²³⁸Pu activity concentrations ranged from <0.01 Bq/kg to 0.22 Bq/kg. Total inventories of ¹³⁷Cs ranged from 29.5 ± 1.5 Bq/m² to 152.7 ± 5.6 Bq/m² and for ^239,240Pu inventories (6 sediment layers only) ranged from 9.5 ± 0.3 Bq/m² to 29.7 ± 0.4 Bq/m². Source contributions varied among stations and between the investigated radionuclides. The ²³⁸Pu/^239,240Pu ratios up to 0.18 indicate discharges from nuclear fuel reprocessing plants as a main contributor of plutonium. Based on ²³⁸Pu/^239,240Pu ratio, it was calculated that up to 19-27% of plutonium is supplied from sources other than atmospheric global fallout. Taking into account Atlantic current flow trajectories and that both activity concentrations and inventories of plutonium negatively correlate with latitude, Sellafield is a major source for the Barents Sea. Concentrations and inventories of ¹³⁷Cs correlate positively with latitude and negatively with distance from the Svalbard archipelago. The ¹³⁷Cs concentrations are highest in an area of intensive melting of sea ice formed along the Siberian coast. Thus, sea ice and supplies from Svalbard may be important source of ¹³⁷Cs to the Barents Sea seafloor.     

A comparative study of (239,240)Pu in soil near the former Rocky Flats Nuclear Weapons Facility, Golden, CO

The Rocky Flats Nuclear Weapons Plant near Golden, CO released plutonium into the environment during almost 40 years of operation. Continuing concern over possible health impacts of these releases has been heightened by lack of public disclosure of the US Department of Energy (DOE) activities. A dose reconstruction study for the Rocky Flats facilities, begun in 1990, provided a unique opportunity for concerned citizens to design and implement field studies without participation of the DOE, its contractors, or other government agencies. The Citizens Environmental Sampling Committee was formed in late 1992 and conducted a field sampling program in 1994. Over 60 soil samples, including both surface and core samples, were collected from 28 locations where past human activities would have minimal influence on contaminant distributions in soil. Cesium-137 activity was used as a means to assess whether samples were collected in undisturbed locations. The distribution of plutonium (as (239,240)Pu) in soil was consistent with past sampling conducted by DOE, the Colorado Department of Public Health and Environment, and others. Elevated levels of (239,240)Pu were found immediately east of the Rocky Flats Plant, with concentrations falling rapidly with distance from the plant to levels consistent with background from fallout. Samples collected in areas south, west, and north of the plant were generally consistent with background from fallout. No biases in past sampling due to choice of sampling locations or sampling methodology were evident. The study shows that local citizens, when provided sufficient resources, can design and implement technical studies that directly address community concerns where trust in the regulated community and/or regulators is low.