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1.
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   

2.
Monthly plutonium and thorium depositions at Tsukuba (28 m asl) and Mt. Haruna (1370 m asl) were measured during 2006 and 2007 (Jan 2006-Dec 2007 at Tsukuba, Nov 2006-Dec 2007 at Mt. Haruna). The monthly 239,240Pu depositions ranged from 0.044 to 2.67 mBq m−2 at Tsukuba and from 0.05 to 0.9 mBq m−2 at Mt. Haruna during the measurement periods. Monthly 239,240Pu deposition did not differ markedly between the two sites except in April 2007. Seasonal pattern of monthly 239,240Pu depositions at both sites showed high in spring and low in summer, and typical of seasonal variations in northeastern Asia. Thorium deposition at Tsukuba was higher than that at Mt. Haruna except in May and June 2007. 230Th/232Th activity ratios were used to partition deposition samples into locally and remotely derived fractions. The results revealed that a major proportion of total 239,240Pu and Th deposits are derived from remote sources, especially in spring.  相似文献   

3.
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   

4.
The concentrations of 238Pu, 239,240Pu, 241Am and 244Cm were determined in sediment samples from five streams and two ponds on the Savannah River Plant (SRP) and in four sediment samples from the Savannah River above and below the plant site. The following concentration ranges were determined: 238Pu, 0·07–386 fCi g−1; 239,240Pu, 0·37–1410 fCi g−1; 241Am, 0·1–4360 fCi g−1; 244Cm, <0·01–392 fCi g−1. Comparisons of the elemental and isotopic ratios of the sediments show that the majority of the sediments studied have been impacted upon by plant operations and that sediments outside the plant boundary in the Savannah River have only been influenced by aerial releases. Atom ratios of 240Pu/239Pu indicate that up to 86% of the Pu in these sediments is derived from plant operations. However, comparisons of the concentration data with values for other impacted sediments near nuclear facilities indicate that the levels are relatively small. Finally, <13% of the Pu, Am or Cm in pond sediments is associated with humic or fulvic acids, indicating that little of the material should be remobilized in oxic environments through organic complexation.  相似文献   

5.
234U and 238U activity concentrations and their relative effective doses have been determined in 10 bottled mineral waters in Tunisia. Alpha spectrometry was used as technique to measure uranium isotopes. The obtained isotopic ratio 234U/238U varies between 1.1 and 3 which means that the two isotopes are not in radioactive equilibrium. Measured activity concentration varies between 3.2 and 40 mBq/l for 234U and between 1.5 and 26.3 mBq/l for 238U. Effective doses (assuming 2 litres per day of water consumption) coming from this two isotopes are found to vary between 0.16 and 2.02 μSv/a which is lower than the maximum recommended dose level by the WHO.  相似文献   

6.
The aim of this work was to determine the concentrations and isotopic compositions of plutonium and uranium in environmental samples for safeguards purposes. An analytical method was developed with a plutonium and uranium separation procedure based on extraction chromatography (using 2 mL TEVA and UTEVA columns) and detection with a quadrupole ICP-MS applying an ultra-sonic nebulizer coupled with a membrane desolvation system. Starting from blank swipes, the background equivalent concentration (BEC) was 8 fg for 239Pu and 1 ng 238U. The method was successfully applied to certified reference materials as well as to round robin samples obtained in the framework of the inter-laboratory exercise program, promoted by the Brazilian–Argentine Agency for Accounting and Control of Nuclear Materials (ABACC), together with the US Department of Energy (USDOE). After the introduction of an additional ion-exchange separation step, the methodology was applied to the IAEA-384 sediment reference sample with precise and accurate total plutonium and uranium, 240Pu/239Pu, 241Pu/239Pu, 234U/238U and 235U/238U atomic ratio results.  相似文献   

7.
Plutonium and americium have been measured in surface waters of the Greenland and Barents Seas and in the northern North Sea from 1980 through 1984. Measurements in water and biota, Fucus, Mytilus and Patella, were carried out in North-English and Scottish waters in 1982 and Fucus samples were collected from the Irish coast in 1983. Fallout is found to dominate as a source of 239+240Pu north of latitude 65°N, while for 238Pu a substantial fraction originates from European nuclear fuel reprocessing facilities. The 238Pu/239+240Pu isotope ratio provides clear evidence of the transport of effluent plutonium from the latter to Spitsbergen waters. Fallout plutonium in Arctic waters has a residence time of the order of several years, while for Pu from Sellafield we estimate mean residence times of 11–15 months in Scottish waters and, tentatively, 1·5-3 y during transport from the North Channel (north of the Irish Sea) to Spitsbergen. 241Am found in Arctic waters probably originates from the decay of fallout 241Pu and, like Pu, tentatively has a residence time of the order of several years. Americium from Sellafield has an estimated mean residence time of 4–6 months in Scottish waters.  相似文献   

8.
The total 239+240Pu activities and 240Pu/239Pu atom ratios in surface soil samples (0–5 cm) in the Kumtag Desert in western Gansu Province, and in a soil core sample in Lanzhou were investigated using a sector-field ICP-MS. In the surface soil samples, 239+240Pu activities in fine particles (<150 μm) were 1.3–2.1 times of those in coarse particles (150 μm–1 mm) which ranged from 0.005 to 0.157 mBq/g. Atom ratios of 240Pu/239Pu in the surface soils ranged from 0.168 to 0.192 with a mean of 0.182 ± 0.008. The mean ratio was similar to the typical global fallout value although the Kumtag Desert was believed to have received close-in fallout derived from Chinese nuclear weapons tests mainly conducted in the 1970s. Furthermore, the mean 240Pu/239Pu atom ratio observed in the soil core sample in Lanzhou was similar to the typical global fallout value. In the soil core sample, 239+240Pu activities in the various layers ranged from 0.012 to 0.23 mBq/g, and the inventory of 239+240Pu (32.4 Bq/m2, 0–23 cm) was slightly lower than that expected from global fallout (42 Bq/m2) at the same latitude. Rapid downward migration of Pu isotopes was observed in Lanzhou soil core sample layers. The contribution of the 10-cm deep top layers of surface soils to total inventory was only 17%, while the contribution of deeper layers (10–23 cm) was as high as 83%. The 239+240Pu activity levels and 240Pu/239Pu atom ratios in soils in Gansu Province, China are similar to those in atmospheric deposition samples collected in the spring in recent years in Japan.  相似文献   

9.
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.  相似文献   

10.
Concentrations of the anthropogenic 137Cs and 239,240Pu in surface water of the Sea of Japan were in the ranges of 2·7–3·8 mBq l-1 and 1·3–8·0 μBq l-1, respectively, in 1993–1994, which are in the same order of magnitude as those in the North Pacific. The time-series data indicated a marked increase of surface 137Cs in 1986 and 1987 after the major radioactive dumping and the Chernobyl fallout in 1986 and then rapidly decreased thereafter. The apparent half-residence time of 137Cs in the surface water was estimated to be about 3 years for excess 137Cs and 16 years for a rather long time-scale transport, respectively. For 239,240Pu in the surface water, no systematic temporal variation was observed over the past two decades, which may reflect rapid recycling of deeper Pu. The results revealed that most of the recent radioactivity in water columns of the Sea of Japan was of global fallout origin from atmospheric nuclear testing and partly the Chernobyl fallout. No clear signal about the effect of radioactivity from Russian dumping was observed.  相似文献   

11.
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   

12.
Monitoring of 239,240Pu in surface air of Prague started in 1986 in connection with the Chernobyl accident. Measurable activities of 10–28 μBq m−3 were found from 29 April 1986 to 5 May 1986. In the most of the monitoring periods of 1987–1996, activities of 239,240Pu in air were not measurable. Positive values for 239,240Pu and 238Pu in air could be obtained after installation of an aerosol sampler with higher flow-rate in 1997. Activity concentrations of 239,240Pu and 238Pu in Prague air in the most of quarters of 1997–2006 were in the range 0.53–5.06 and <0.16–1.10 nBq m−3, respectively. Seasonal fluctuations can be found in content of 239,240Pu in air. Activity ratios of 238Pu/239,240Pu in air are higher than those in top soil, so it can be supposed that 238Pu is coming to air of Prague also from other sources than resuspension of fallout from atmospheric nuclear tests.  相似文献   

13.
Natural background gamma radiation and radioactivity concentrations were investigated from 2003 to 2005 in Kinta District, Perak, Malaysia. Sample locations were distant from any ‘amang’ processing plants. The external gamma dose rates ranged from 39 to 1039 nGy h−1. The mean external gamma dose rate was 222 ± 191 nGy h−1. Small areas of relatively enhanced activity were located having external gamma dose rates of up to 1039 ± 104 nGy h−1. The activity concentrations of 238U, 232Th and 40K were analyzed by using a high-resolution co-axial HPGe detector system. The activity concentration ranges were 12–426 Bq kg−1 for 238U, 19–1377 Bq kg−1 for 232Th and <19–2204 Bq kg−1 for 40 K. Based on the radioactivity levels determined, the gamma-absorbed dose rates in air at 1 m above the ground were calculated. The calculated dose rates and measured dose rates had a good correlation coefficient, R of 0.94. To evaluate the radiological hazard of the natural radioactivity, the radium equivalent activity, the gamma-absorbed dose rate and the mean population weighted dose rate were calculated. An isodose map for the Kinta District was also produced.  相似文献   

14.
A study is presented on the distribution of 234U, 238U, 235U isotopes in surface water of the Llobregat river basin (Northeast Spain), from 2001 to 2006. Sixty-six superficial water samples were collected at 16 points distributed throughout the Llobregat river basin. Uranium isotopes were measured by alpha spectrometry (PIPS detectors). The test procedure was validated according to the quality requirements of the ISO17025 standard. The activity concentration for the total dissolved uranium ranges from 20 to 261 mBq L−1. The highest concentrations of uranium were detected in an area with formations of sedimentary rock, limestone and lignite. A high degree of radioactive disequilibrium was noted among the uranium isotopes. The 234U/238U activity ratio varied between 1.1 and 1.9 and the waters with the lowest uranium activity registered the highest level of 234U/238U activity ratio. Correlations between uranium activity in the tested water and chemical and physical characteristics of the aquifer were found.  相似文献   

15.
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   

16.
A shallow-land radioactive waste repository operated in boggy forest environment from 1963 to 1989. During the operation period, a considerable amount of technogenic radionuclides, in solidified state, was disposed into the vault established in the geological structure at the depth of up to 3 m. Environmental monitoring activities started after the closure of the repository in 1989. Recent investigations revealed transfer of radiocarbon and plutonium to the groundwater in the prevailing flow direction. Activity concentration of 239,240Pu in non-filtered fraction of the groundwater from observation well no. 4 determined by alpha-spectrometry was 6.4 × 10−5 Bq l−1 in 2005, and 3.2 × 10−4 Bq l−1 in 2006. Further analysis of colloid-facilitated transport of plutonium is planned. Variation of 14C activity concentration in the same well was monitored in 2006. It varied from 0.2 ± 0.1 Bq l−1 in October to 2.8 ± 0.6 Bq l−1 in June and July. Results imply further research into radiocarbon transfer to atmosphere and selected plant species.  相似文献   

17.
A pond which undergoes seasonal anoxia as a result of thermal stratification was studied to assess the possible release of actinide elements from anoxic sediments to the pond waters. Concentration profiles of 239,240Pu, 241Am, 232Th, iron and manganese in the water column show significant increases in concentration for all elements in the anoxic deep waters. However, calculated total inventories of the elements in the pond water indicate no apparent input of actinide elements to the system during summer stratification. Similar inventory calculations for 239,240Pu in a previously studied system support the results of this study. The lack of a significant increase in pond inventories of actinide elements coupled with a lack of correspondence of concentration profiles of the actinide elements to the seasonal Fe and Mn concentrations profiles argues that the increases in concentrations observed for these elements in anoxic bottom waters result from the downward transport of material already in the water column rather than release from the sediments.  相似文献   

18.
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   

19.
Caesium-137 and (239,240)PU were analysed in the water column along the Algerian coast. The (137)Cs activity concentration in surface water increased from the west to the east from 1.6 to 3.3 mBq L(-1), documenting a presence of Modified Atlantic Water (MAW) in the region. Higher concentrations observed in deep waters may be due to an intrusion of Levantine Intermediate Water (LIW), which has been carrying higher levels of (137)Cs from Chernobyl accident. The (239,240)Pu sub-surface concentration peaked at about 250 m water depth as a result of biogeochemical processes in the water column. The observed (239,240)Pu/(137)Cs activity ratio at the surface (0.003) was significantly lower than that in global fallout (0.04). This decrease exceeds that expected from radioactive decay of (137)Cs, and confirms that Pu due to its adsorption on sinking particles is more effectively removed from surface layers than is (137)Cs. An increase of the (239,240)Pu/(137)Cs activity ratio with depth suggests that (239,240)Pu, similarly as (137)Cs, should be also transported by advection to maintain the observed ratios in deep waters. An intrusion of LIW may enhance therefore both the (137)Cs and (239,240)Pu concentrations in deep waters. The average (238)Pu/(239+240)Pu activity ratio in seawater was 0.03+/-0.02, confirming a global fallout origin of Pu in the Algerian Basin. Caesium-137 and (239,240)Pu inventories in the water column were estimated to be from 2.7+/-0.5 kBq m(-2) to 3.8+/-0.7 kBq m(-2), and from 13.8+/-2.6 Bq m(-2) to 41+/-7B qm(-2), respectively. The (137)Cs massic activities in surface sediment were almost constant, the average activity was 9.0+/-0.8 Bq kg(-1). Sedimentation rates obtained using the (210)Pb method were from 0.1 to 0.7 cm y(-1), and resulting penetration depths of (137)Cs in the sediment cores were from 15 to over 40 cm. The (137)Cs peaks found in the sediment cores were associated with the Chernobyl accident (1986) and global fallout (1964). The (137)Cs inventories in the sediment were increasing from the west (180 Bq m(-2)) to the east (350 Bq m(-2)).  相似文献   

20.
The disequilibrium between 234U and 238U is commonly used as a tracer of groundwater flow. This paper aims to identify uranium contents and uranium isotopic disequilibria variation in groundwater sampled from deep Continental Intercalaire aquifer (southern Algeria and Tunisia). Large variations in both U contents (0.006–3.39 ppb) and 234U/238U activity ratios (0.4–15.38) are observed. We conduct a first assessment in order to verify whether the results of our investigation support and complete previous hydrogeological and isotopic studies. The dissolved U content and 234U/238U activity ratio data were plotted on a two-dimensional diagram that was successfully utilized on sharing the CI aquifer into different compartments submitted to different oxidising/reducing conditions and leads also to distinguished two preferential flow paths in the Nefzaoua/Chott Fejej discharge area. Uranium isotopes disequilibrium indicate that ranium chemistry is mainly controlled by water–rock interaction enhanced by long residence time recognised for this aquifer.  相似文献   

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