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1.
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   

2.
Fractionation of plutonium isotopes (238Pu, 239,240Pu) in environmental samples (i.e. soil and sediment) and bio-shielding concrete from decommissioning of nuclear reactor were carried out by dynamic sequential extraction using an on-line sequential injection (SI) system combined with a specially designed extraction column. Plutonium in the fractions from the sequential extraction was separated by ion exchange chromatography and measured using alpha spectrometry. The analytical results show a higher mobility of plutonium in bio-shielding concrete, which means attention should be paid to the treatment and disposal of nuclear waste from decommissioning.  相似文献   

3.
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.  相似文献   

4.
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   

5.
Pu concentrations in surface sediments of the Ligurian Sea are about ten times higher than in adjacent river sediments and are highly correlated with sediment porosities. The integrated inventory of 239,240Pu in a sediment core is calculated to be 3·5 mCi km?2, nearly twice the average input from fallout at these latitudes, apparently because Pu is removed from seawater by particle scavenging.The sedimentation rate is calculated from the depth of the 239,240Pu maximum to be 0·52 ± 0·06 cmy?1.  相似文献   

6.
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   

7.
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   

8.
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   

9.
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.  相似文献   

10.
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   

11.
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.  相似文献   

12.
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   

13.
Modelling the distribution of plutonium in the Pacific Ocean   总被引:2,自引:0,他引:2  
An Oceanic General Circulation Model (OGCM) including a plutonium scavenging model as well as an advection-diffusion model has been developed for modelling the distribution of plutonium in the Pacific Ocean. Calculated 239, 240Pu water profile concentrations and 239, 240Pu inventories in water and sediment of the Pacific Ocean have showed a reasonable agreement with the experimental results. The presence of local fallout plutonium in central North Pacific waters has been confirmed. The observed 240Pu/239Pu mass ratios confirm that plutonium originating from local fallout from nuclear weapons tests carried out at Bikini and Enewetak Atolls is more rapidly removed from surface waters to deeper waters than plutonium originating from global fallout. The developed OGCM can be used for modelling the dispersion of other non-conservative tracers in the ocean as well.  相似文献   

14.
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   

15.
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   

16.
In a sediment core of Nishiyama reservoir at Nagasaki city, depth profiles of (240)Pu/(239)Pu isotopic ratio, (239+240)Pu and (137)Cs activities were determined. Sediments containing plutonium and (137)Cs, which were deposited immediately after a detonation of Nagasaki atomic bomb, were identified in the core. Observed below the sediments were macroscopic charcoals, providing evidence for initial deposit of the fallout of the Nagasaki atomic bomb. This is the first entire depositional records of plutonium and (137)Cs released from the Nagasaki atomic bomb together with those from atmospheric nuclear tests.  相似文献   

17.
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   

18.
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   

19.
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   

20.
New data are reported on the concentrations, isotopic composition and speciation of americium, plutonium and uranium in surface and ground waters in the Sarzhal region of the Semipalatinsk Test Site, and an adjacent area including the settlement of Sarzhal. The data relate to filtered water and suspended particulate from (a) streams originating in the Degelen Mountains, (b) the Tel′kem 1 and Tel′kem 2 atomic craters, and (c) wells on farms located within the study area and at Sarzhal. The measurements show that 241Am, 239,240Pu and 238U concentrations in well waters within the study area are in the range 0.04–87 mBq dm−3, 0.7–99 mBq dm−3, and 74–213 mBq dm−3, respectively, and for 241Am and 239,240Pu are elevated above the levels expected solely on the basis of global fallout. Concentrations in streams sourced in the Degelen Mountains are similar, while concentrations in the two water-filled atomic craters are somewhat higher. Suspended particulate concentrations in well waters vary considerably, though median values are very low, at 0.01 mBq dm−3, 0.08 mBq dm−3 and 0.32 mBq dm−3 for 241Am, 239,240Pu and 238U, respectively. The 235U/238U isotopic ratio in almost all well and stream waters is slightly elevated above the ‘best estimate’ value for natural uranium worldwide, suggesting that some of the uranium in these waters is of test-site provenance. Redox analysis shows that on average most of the plutonium present in the microfiltered fraction of these waters is in a chemically reduced form (mean 69%; 95% confidence interval 53–85%). In the case of the atomic craters, the proportion is even higher. As expected, all of the americium present appears to be in a reduced form. Calculations suggest that annual committed effective doses to individual adults arising from the daily ingestion of these well waters are in the range 11–42 μSv (mean 21 μSv). Presently, the ground water feeding these wells would not appear to be contaminated with radioactivity from past underground testing in the Degelen Mountains or from the Tel′kem explosions.  相似文献   

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