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1.
Monitoring of (239,240)Pu in surface air of Prague started in 1986 in connection with the Chernobyl accident. Measurable activities of 10-28muBqm(-3) were found from 29 April 1986 to 5 May 1986. In the most of the monitoring periods of 1987-1996, activities of (239,240)Pu in air were not measurable. Positive values for (239,240)Pu and (238)Pu in air could be obtained after installation of an aerosol sampler with higher flow-rate in 1997. Activity concentrations of (239,240)Pu and (238)Pu in Prague air in the most of quarters of 1997-2006 were in the range 0.53-5.06 and <0.16-1.10nBqm(-3), respectively. Seasonal fluctuations can be found in content of (239,240)Pu in air. Activity ratios of (238)Pu/(239,240)Pu in air are higher than those in top soil, so it can be supposed that (238)Pu is coming to air of Prague also from other sources than resuspension of fallout from atmospheric nuclear tests.  相似文献   

2.
A sediment core collected from the sub-aqueous delta of the Yangtze River estuary was subjected to analyses of 137Cs and plutonium (Pu) isotopes. The 137Cs was measured using γ-spectrometry at the laboratories at the Nanjing University and Pu isotopes were determined with Accelerator Mass Spectrometry (AMS), measurements made at the Australian National University. The results show considerable structure in the depth concentration profiles of the 137Cs and 239+240Pu. The shape of the vertical 137Cs distribution in the sediment core was similar to that of the Pu. The maximum 137Cs and 239+240Pu concentrations were 16.21 ± 0.95 mBq/g and 0.716 ± 0.030 mBq/g, respectively, and appear at same depth. The average 240Pu/239Pu atom ratio was 0.238 ± 0.007 in the sediment core, slightly higher than the average global fallout value. The changes in the 240Pu/239Pu atom ratios in the sediment core indicate the presence of at least two different Pu sources, i.e., global fallout and another source, most likely close-in fallout from the Pacific Proving Grounds (PPG) in the Marshall Islands, and suggest the possibility that Pu isotopes are useful as a geochronological tool for coastal sediment studies. The 137Cs and 239+240Pu inventories were estimated to be 7100 ± 1200 Bq/m2 and 407 ± 27 Bq/m2, respectively. Approximately 40% of the 239+240Pu inventory originated from the PPG close-in fallout and about 50% has derived from land-origin global fallout transported to the estuary by the river. This study confirms that AMS is a useful tool to measure 240Pu/239Pu atom ratio and can provide valuable information on sedimentary processes in the coastal environment.  相似文献   

3.
Measurements of airborne radioactive aerosol concentration were carried out on the basis of 1-3 days samples after the Chernobyl disaster and during the period of 1992-2003. Transport of "hot" particles of different composition resulted in the high activity concentrations of (137)Cs, (238)Pu, (239,240)Pu and (241)Am in the atmosphere in Vilnius at the end of April 1986. The (240)Pu/(239)Pu atom ratio showed clear evidence of non-global plutonium originating from the Chernobyl accident in the atmosphere over Lithuania. The (240)Pu/(239)Pu atom ratio ranged from 0.14 to 0.40 in monthly samples in Vilnius in 1995-2003. An increase in activity concentration of (137)Cs by a factor of 100 (up to 300 microBq/m(3)) was found following forest fires in the Ukraine and Belarus. However, no transport of the Chernobyl plutonium was observed and the (240)Pu/(239)Pu atom ratio in samples collected during the forest fires was found to be 0.229 and 0.185, respectively. The exponential decrease in the (240)Pu/(239)Pu atom ratio from 0.30 to 0.19 (mean values) was observed in 1995-2003.  相似文献   

4.
The vertical distribution of the 236U/238U isotopic ratio was investigated in soil samples from three different locations on La Palma (one of the seven Canary Islands, Spain). Additionally the 240Pu/239Pu atomic ratio, as it is a well establish tool for the source identification, was determined. The radiochemical procedure consisted of a U separation step by extraction chromatography using UTEVA® Resin (Eichrom Technologies, Inc.). Afterwards Pu was separated from Th and Np by anion exchange using Dowex 1x2 (Dow Chemical Co.). Furthermore a new chemical procedure with tandem columns to separate Pu and U from the matrix was tested. For the determination of the uranium and plutonium isotopes by alpha spectrometry thin sources were prepared by microprecipitation techniques. Additionally these fractions separated from the soil samples were measured by Accelerator Mass Spectrometry (AMS) to get information on the isotopic ratios 236U/238U, 240Pu/239Pu and 236U/239Pu, respectively. The 236U concentrations [atoms/g] in each surface layer (∼2 cm) were surprisingly high compared to deeper layers where values around two orders of magnitude smaller were found. Since the isotopic ratio 240Pu/239Pu indicated a global fallout signature we assume the same origin as the probable source for 236U. Our measured 236U/239Pu value of around 0.2 is within the expected range for this contamination source.  相似文献   

5.
The Mining and Chemical Industrial Combine, Zheleznogorsk (MCIC, previously known as Krasnoyarsk-26) on the River Yenisey has contaminated the surrounding environment with anthropogenic radionuclides as a result of discharges of radioactive wastes. The purpose of this study was to investigate the vertical distribution of anthropogenic contamination (137Cs and plutonium) within floodplain areas at different distances from the discharge point. Sites were chosen that display different characteristics with respect to periodic inundation with river water. Cs-137 activity concentrations were in the range 23–3770 Bq/kg (dry weight, d.w.); Pu-239,240 activity concentrations were in the range <0.01–14.2 Bq/kg (d.w.). Numerous sample cores exhibited sub-surface maxima which may be related to the historical discharges from the MCIC. Possible evidence indicating the deposition of earlier discharges at MCIC in deeper core layers was observed in the 238Pu:239,240Pu activity ratio data: a Pu signal discernible from global fallout could be observed in numerous samples. Cs-137 and Pu-239,240 activity concentrations were correlated with the silt fraction (% by mass <63 μm) though no significant correlation was observed between (grain-size) normalised 137Cs activity concentrations and distance downstream from the MCIC.  相似文献   

6.
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.  相似文献   

7.
Anthropogenic radionuclides in seawater have been used as transient tracers of processes in the marine environment. Especially, plutonium in seawater is considered to be a valuable tracer of biogeochemical processes due to its particle-reactive properties. However, its behavior in the ocean is also affected by physical processes such as advection, mixing and diffusion. Here we introduce Pu/137Cs ratio as a proxy of biogeochemical processes and discuss its trends in the water column of the North Pacific Ocean. We observed that the 239,240Pu/137Cs ratio in seawater exponentially increased with increasing depth (depth range: 100–1000 m). This finding suggests that the profiles of the 239,240Pu/137Cs ratios in shallower waters directly reflect biogeochemical processes in the water column. A half-regeneration depth deduced from the curve fitting the observed data, showed latitudinal and longitudinal distributions, also related to biogeochemical processes in the water column.  相似文献   

8.
Samples from a marine sediment core from the Irish Sea (54.416 N, 3.563 W) were analyzed for the isotopic composition of uranium, plutonium and americium by a combination of radiometric methods and AMS. The radiochemical procedure consisted of a Pu separation step by anion exchange, subsequent U separation by extraction chromatography using UTEVA® and finally Am separation with TRU® Resin.Additionally to radiometric determination of these isotopes by alpha spectrometry, the separated samples were also used for the determination of 236U/238U and plutonium isotope ratios by Accelerator Mass Spectrometry (AMS) at the VERA facility.  相似文献   

9.
The use of building materials containing naturally occurring radionuclides as 40K, 232Th, and 238U and their progeny results in external exposures of the residents of such buildings. In the present study, indoor dose rates for a typical Jordan concrete room are calculated using Monte Carlo method. Uniform chemical composition of the walls, floor and ceiling as well as uniform mass concentrations of the radionuclides in walls, floor and ceiling are assumed.Using activity concentrations of natural radionuclides typical for the Jordan houses and assuming them to be in secular equilibrium with their progeny, the maximum annual effective doses are estimated to be 0.16, 0.12 and 0.22 mSv a−1 for 40K, 232Th- and 238U-series, respectively. In a total, the maximum annual effective indoor dose due to external γ-radiation is 0.50 mSv a−1. Additionally, organ dose coefficients are calculated for all organs considered in ICRP Publication 74. Breast, skin and eye lenses have the maximum equivalent dose rate values due to indoor exposures caused by the natural radionuclides, while equivalent dose rates for uterus, colon (LLI) and small intestine are found to be the smallest. More specifically, organ dose rates (nSv a−1 per Bq kg−1) vary from 0.044 to 0.060 for 40K, from 0.44 to 0.60 for radionuclides from 238U-series and from 0.60 to 0.81 for radionuclides from 232Th-series.The obtained organ and effective dose conversion coefficients can be conveniently used in practical dose assessment tasks for the rooms of similar geometry and varying activity concentrations and local-specific occupancy factors.  相似文献   

10.
Anthropogenic Pu isotopes are important geochemical tracers for sediment studies. Their distributions and sources in the water columns as well as the sediments of the North Pacific have been intensively studied; however, information about Pu in the Southeast Asian seas is limited. To study the isotopic composition of Pu, and thus to identify its sources, we collected sediment core samples in the South China Sea and the Sulu Sea during the KH-96-5 Cruise of the R/V Hakuho Maru. We analysed the activities of 239+240Pu and the atom ratios of 240Pu/239Pu using isotope dilution sector-field inductively coupled plasma mass spectrometry (SF-ICP-MS). The 240Pu/239Pu atom ratios in the sediments of both areas (inventory weighted mean: 0.251 for the South China Sea and 0.280 for the Sulu Sea) were higher than the global fallout value (0.178 ± 0.019), suggesting the existence of Pu from the Pacific Proving Grounds in the North Pacific. Low inventories of 239+240Pu in sediments were observed in the South China Sea (3.75 Bq/m2) and the Sulu Sea (1.38 Bq/m2). Most of the Pu input is still present in the water column. Scavenging and benthic mixing processes were considered to be the main processes controlling the distribution of Pu in the deep-sea sediments of both study areas.  相似文献   

11.
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.  相似文献   

12.
The aim of the work was to estimate plutonium inflow from the Vistula River’s catchments area to the Baltic Sea. There were differences in plutonium activities depending on season and sampling site. The highest activities of 238Pu and 239+240Pu were transported from the Vistula River watershed to the Baltic Sea in spring and the lowest in summer. Annually, the southern Baltic Sea is enriched via the Vistula River with 10.3 MBq of 238Pu and 89.0 MBq of 239+240Pu. The enhanced concentration of plutonium in water from the Vistula River is the result of its runoff from the Vistula drainage area, mostly from snowmelt, enhanced rainfalls and leached materials from river bed.  相似文献   

13.
The concentrations and vertical distribution of 239,240Pu, 241Am and 137Cs in the bottom sediments and water samples of Lake Päijänne were investigated. This lake is important, since the Päijänne area received a significant deposition from the Chernobyl fallout. Furthermore Lake Päijänne is the raw water source for the Helsinki metropolitan area. In addition no previous data on the distribution of plutonium and americium in the sediment profiles of Lake Päijänne exist. Only data covering the surface layer (0–1 cm) of the sediments are previously available. In the sediments the average total activities were 45 ± 15 Bq/m2 and 20 ± 7 Bq/m2 for 239,240Pu and 241Am, respectively. The average 241Am/239,240Pu ratio was 0.45 ± 0.14. The 241Am/239,240Pu ratio is lowest in the surface layer of the sediments and increases as a function of depth. The 238Pu/239,240Pu ratio of the sediment samples varied between 0.012 ± 0.025 and 0.162 ± 0.079, decreasing as a function of depth. The average activity in water was 4.9 ± 0.9 mBq/m3 and 4.1 ± 0.2 mBq/m3 for 239,240Pu and 241Am, respectively. The 241Am/239,240Pu ratio of water samples was 0.82 ± 0.17. 239,240Pu originating from the Chernobyl fallout calculated from the average total activities covers approximately 1.95 ± 0.01% of the total 239,240Pu activity in the bottom sediments. The average total 137Cs activity of sediment profiles was 100 ± 15 kBq/m2 and 19.3 ± 1.4 Bq/m3 in water samples.  相似文献   

14.
The aim of the paper was plutonium (238Pu and 239+240Pu) determination in seabirds, permanently or temporarily living in northern Poland at the Baltic Sea coast. Together 11 marine birds species were examined: 3 species permanently residing in the southern Baltic, 4 species of wintering birds and 3 species of migrating birds. The obtained results indicated plutonium is non-uniformly distributed in organs and tissues of analyzed seabirds. The highest plutonium content was found in the digestion organs and feathers, the smallest in skin and muscles. The plutonium concentration was lower in analyzed species which feed on fish and much higher in herbivorous species. The main source of plutonium in analyzed marine birds was global atmospheric fallout.  相似文献   

15.
Natural radionuclides, such as 210Po and 210Pb were measured in the water samples collected from six stations at Kuala Selangor, Malaysia. Results for 210Po and 210Pb in dissolved and particulate phases have showed the difference in distribution and chemical behavior. The fluctuation activities of 210Po and 210Pb depend on wave action, geology and degree of fresh water input occurring at study areas and probably due to different sampling dates. The distribution coefficient, Kd, values of 210Po and 210Pb ranged from 2.0 × 103 l g−1 to 265.15 × 105 l g−1, and from 3.0 × 103 l g−1 to 558.16 × 105 l g−1, respectively. High Kd values of 210Po and 210Pb indicated that a strong adsorption of 210Po and 210Pb onto suspended particles, and the sinking of both nuclides on the seabed at study locations were controlled by the characteristics of suspended particles.  相似文献   

16.
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.  相似文献   

17.
A sediment core from a lake downwind of the Rocky Flats Plant, where nuclear weapons components are produced, was used to reconstruct a time pattern of off-site plutonium deposition. Core sections were dated by analyses of 137Cs, 239,240Pu, 238Pu, and 241Am fallout from nuclear testing and 238Pu fallout from a satellite failure. A peak in transuranic concentrations occurred in late 1969 which was attributable to the Plant. This was confirmed by mass isotopic analysis of plutonium isotopes in selected core segments where the global fallout and Plant contributions could be differentiated. The 18 nCi 239,240Pu per m2 from the Plant that had accumulated in the sediment is reasonable when compared to soil analyses.  相似文献   

18.
Data are presented here on the distribution of 239,240Pu in the pore waters of two cores taken from a seasonally anoxic lake. The pore water 239,240Pu profile exhibits a subsurface activity maximum of 230 ± 30 μBqkg?1 in the 3–6 cm interval in June, as compared to an activity of 5 ± 3 μBqkg?1 in the overlying water. The pore water 239,240Pu profile in June follows the solid phase distribution pattern of 239,240Pu and also the pore water distributions of Fe and Mn. Under more reducing conditions in August, pore water 239,240Pu activities drop off to undetectable levels at all depths. This rapid change in the pore water 239,240Pu activity reflects the dynamic nature of Pu diagenesis in these sediments. Potential diffusional fluxes of 239,240Pu into the lake's hypolimnion in June are calculated to be on the order of 2·5 μBq cm?2y?1. This flux would not be significant in altering the solid phase 239,240Pu inventory (2·8 × 104μBqcm?2).  相似文献   

19.
A radioactivity survey was launched in 1991 to determine the background levels of 239+240Pu in the marine environment off a commercial spent nuclear fuel reprocessing plant before full operation of the facility. Particular attention was focused on the 240Pu/239Pu atom ratio in seawater and bottom sediment to identify the origins of Pu isotopes. The concentration of 239+240Pu was almost uniform in surface water, decreasing slowly over time. Conversely, the 239+240Pu concentration varied markedly in the bottom water and was dependent upon the sampling point, with higher concentrations of 239+240Pu observed in the bottom water sample at sampling points having greater depth. The 240Pu/239Pu atom ratio in the seawater and sediment samples was higher than that of global fallout Pu, and comparable with the data in the other sea area around Japan which has likely been affected by close-in fallout Pu originating from the Pacific Proving Grounds. The 240Pu/239Pu atom ratio in bottom sediment samples decreased with sea depth. The land-originated Pu is not considered as the reason of the increasing 239+240Pu concentration and also decreasing the 240Pu/239Pu atom ratio with sea depth, and further study is required to clarify it.  相似文献   

20.
Results of groundwater and seawater analyses for radioactive (3H, 222Rn, 223Ra, 224Ra, 226Ra, and 228Ra) and stable (D and 18O) isotopes are presented together with in situ spatial mapping and time series 222Rn measurements in seawater, direct seepage measurements using manual and automated seepage meters, pore water investigations using different tracers and piezometric techniques, and geoelectric surveys probing the coast. This study represents first time that such a new complex arsenal of radioactive and non-radioactive tracer techniques and geophysical methods have been used for simultaneous submarine groundwater discharge (SGD) investigations. Large fluctuations of SGD fluxes were observed at sites situated only a few meters apart (from 0 cm d−1 to 360 cm d−1; the unit represents cm3/cm2/day), as well as during a few hours (from 0 cm d−1 to 110 cm d−1), strongly depending on the tidal fluctuations. The average SGD flux estimated from continuous 222Rn measurements is 17 ± 10 cm d−1. Integrated coastal SGD flux estimated for the Ubatuba coast using radium isotopes is about 7 × 103 m3 d−1 per km of the coast. The isotopic composition (δD and δ18O) of submarine waters was characterised by significant variability and heavy isotope enrichment, indicating that the contribution of groundwater in submarine waters varied from a small percentage to 20%. However, this contribution with increasing offshore distance became negligible. Automated seepage meters and time series measurements of 222Rn activity concentration showed a negative correlation between the SGD rates and tidal stage. This is likely caused by sea level changes as tidal effects induce variations of hydraulic gradients. The geoelectric probing and piezometric measurements contributed to better understanding of the spatial distribution of different water masses present along the coast. The radium isotope data showed scattered distributions with offshore distance, which imply that seawater in a complex coast with many small bays and islands was influenced by local currents and groundwater/seawater mixing. This has also been confirmed by a relatively short residence time of 1–2 weeks for water within 25 km offshore, as obtained by short-lived radium isotopes. The irregular distribution of SGD seen at Ubatuba is a characteristic of fractured rock aquifers, fed by coastal groundwater and recirculated seawater with small admixtures of groundwater, which is of potential environmental concern and has implications on the management of freshwater resources in the region.  相似文献   

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