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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.
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   

3.
Measured monthly atmospheric depositional fluxes of cosmogenically produced 7Be ranged from 1 to 67 mBq/cm2 in Boston, Massachusetts between September 2000 and August 2007. These fluxes exhibited seasonality and supported a decay-corrected 7Be atmospheric depositional running inventory that ranged from 36 to 144 mBq/cm2. Annual 7Be deposition exhibited an increasing trend that may reflect a general decrease in solar activity and a general increase in precipitation over the 7-year sampling period. To investigate short-term sediment dynamics and accumulation patterns in the Neponset River estuary, we collected six sediment cores in July 2006 and measured 7Be sediment inventories ranging from 48 to 546 mBq/cm2 Comparisons of these sediment inventories with the 7Be running inventory from atmospheric deposition (101 mBq/cm2) at the time of core collection indicated a large degree of spatial heterogeneity in sediment accumulation patterns and its potential use as a tool for assessing the impacts of environmental restoration activities in estuarine environments.  相似文献   

4.
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   

5.
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   

6.
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   

7.
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   

8.
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   

9.
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   

10.
Recent advancements in analytical technology make it possible for artificial radionuclides released from nuclear explosions to be detected in Arctic ice core layers. The fission product, 137Cs, and the unexpended fission material, 239+240Pu, originating from the Nagasaki A-bomb of August 1945, were measured by collecting 10 ice cores on the Agassiz ice cap, Ellesmere Island, Canada. The deposition rates were 0·020 mBq cm-2 for 137Cs and 0·0016 mBq cm-2 for 239+240Pu, originating from Nagasaki. Assuming the radionuclides, excluding the amount fissioned from the explosion and deposi-ted as local fallout, are deposited evenly throughout the Northern Hemisphere, 67% of the expected amount of 137Cs reached the Arctic while 1·1% of 239+240Pu reached the Arctic. The results suggest that different transport mechanisms exist for various contaminants in the global transport system.  相似文献   

11.
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   

12.
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   

13.
Plutonium isotopes, 239Pu and 240Pu, were measured in liver samples from Surume squid using a sector-field high resolution ICP-MS after radiochemical purification. Surume squid samples were obtained from nine landing ports in Japanese inshore during fishery season from September to December 2002. Concentrations of 239Pu and 240Pu ranged from 1.5 to 28 mBq kg(-1) and 1.1 to 24 mBq kg(-1), respectively. Plutonium (239,240Pu) concentrations in liver were several thousand times higher than levels found in seawater. The concentration factor (CF) compared to seawater for 239,240Pu and 13 other elements ranged from 10(0) to 10(7). The CF values for 239,240Pu, V and Th were 10(2)-10(4). Pu had an intermediate CF between conservative and scavenged elements. 240Pu/239Pu atomic ratios in the squid liver ranged from 0.177 to 0.237 which were slightly higher than 0.178+/-0.014 for global fallout. The variations of 240Pu/239Pu atomic ratios in ocean currents with different source functions are important for interpreting high 240Pu/239Pu atomic ratios in Surume squid liver. It seems likely that Pu with high 240Pu/239Pu atomic ratio is continuously transported through the solubilization and seawater transport from the North Equatorial Current to Kuroshio and its branch, Tsushima Current. By assuming that Pu found in Surume squid liver is a mixture of global fallout Pu (0.178) and close-in fallout Pu with high 240Pu/239Pu atomic ratio (0.30-0.36) around Bikini Atoll, Pu contribution from Bikini close-in fallout Pu accounts for close to 35% of the whole plutonium in Surume squid liver. These results highlight that Surume squid is a useful organism for evaluating environmental Pu levels of larger sea area and facilitate the development of models to understand oceanic transport of close-in fallout Pu from Bikini Atoll.  相似文献   

14.
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   

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.
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   

17.
The 7Be wet deposition has been intensively investigated in a semiarid region at San Luis Province, Argentina. From November 2006 to May 2008, the 7Be content in rainwater was determined in 58 individual rain events, randomly comprising more than 50% of all individual precipitations at the sampling period. 7Be activity concentration in rainwater ranged from 0.7 ± 0.3 Bq l−1 to 3.2 ± 0.7 Bq l−1, with a mean value of 1.7 Bq l−1 (sd = 0.53 Bq l−1). No relationship was found between 7Be content in rainwater and (a) rainfall amount, (b) precipitation intensity and (c) elapsed time between events. 7Be ground deposition was found to be well correlated with rainfall amount (R = 0.92). For the precipitation events considered, the 7Be depositional fluxes ranged from 1.1 to 120 Bq m−2, with a mean value of 32.7 Bq m−2 (sd = 29.9 Bq m−2). The annual depositional flux was estimated at 1140 ± 120 Bq m−2 y−1. Assuming the same monthly deposition pattern and that the 7Be content in soil decreases only through radioactive decay, the seasonal variation of 7Be areal activity density in soil was estimated. Results of this investigation may contribute to a valuable characterization of 7Be input in the explored semiarid ecosystem and its potential use as tracer of environmental processes.  相似文献   

18.
In order to study the deposition on vegetation of plutonium arising from the testing of nuclear weapons and discharges from nuclear facilities, sheep faeces were collected from the South-west and North of England. The plutonium content of faeces has been shown to be a reproducible and sensitive indicator of deposition on herbage and, with this technique, plutonium discharged from the Sellafield Works of British Nuclear Fuels LImited can be detected 60 km from the site. On moorland pastures the concentration of 239+240Pu in faeces, expressed as activity per gram of ash, is roughly equal numerically to the deposit of plutonium on 1 m2 of vegetation.Some of the plutonium ingested by a grazing sheep is absorbed and the highest concentrations are found in liver. The liver of a sheep grazing on pasture where the 239+240Pu concentration in faeces was about 2 pCi (74 mBq) g−1 of ash, was found to contain <1% of the Generalised Derived Limit for mutton and offal, and the meat <0·001%.  相似文献   

19.
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   

20.
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   

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