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1.
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   

2.
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   

3.
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   

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.
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   

6.
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   

7.
Concentrations of the natural radionuclides 238U, 226Ra, 232Th and 40K have been measured by γ-ray spectrometry in 796 topsoil samples from the Pearl River Delta Zone (PRDZ) of Guangdong, China. The mean concentrations for 238U, 226Ra, 232Th and 40K were found to be 140 ± 37 Bq kg−1, 134 ± 41 Bq kg−1, 187 ± 80 Bq kg−1 and 680 ± 203 Bq kg−1 dry mass, respectively. These values were all higher than the mean values in soil for China and the world. Outdoor air-absorbed dose rates, calculated from activity concentrations of 226Ra, 232Th and 40K, ranged from 86 to 237 nGy h−1, with a mean value of 165 ± 46 nGy h−1. The corresponding annual outdoor effective dose rate per person was estimated to be between 0.11 and 0.29 mSv y−1, with a mean value of 0.20 ± 0.06 mSv y−1, which was also higher than the world mean value of 0.07 mSv y−1. The radium equivalent activity (Raeq) and the external hazard index (Ir) resulted from the natural radionuclides in soil, were also calculated and found to vary from 230 to 676 Bq kg−1 and from 0.6 to 1.8, respectively. The Raeq and the Ir in all the investigated regions were up to 75% higher than the set limits of 370 Bq kg−1 and 1.0, respectively.  相似文献   

8.
We investigated the vertical profiles of 239+240Pu, 137Cs, and excess 210Pb (210Pbex) in sediment core samples obtained from two freshwater lakes and two brackish lakes situated near the first commercial spent nuclear fuel reprocessing plant in Rokkasho, Japan, before the final test of the plant using actual spent nuclear fuel. The inventory of 239+240Pu in those lakes was larger than that in soil in Rokkasho, which indicated the inflow of 239+240Pu from the catchment area in addition to direct deposition on the lake surfaces. The 137Cs inventory in sediments of the brackish lakes was lower than that in the soil, which showed that part of the 137Cs was removed from the sediments by the brackish water or that it was not deposited into the sediments, because of the high solubility of Cs in brackish water. The 137Cs inventory in sediments of the freshwater lakes was higher than that of the brackish lakes, and comparable with that in soil except for one core sample out of four. The 239+240Pu/137Cs ratio in freshwater lake sediments was higher than that in soil, and that indicated that part of the 137Cs was lost from the sediments. The low inventory of 137Cs may be attributable to competition for absorption sites in sediments with ammonium ions formed in the reducing environment which occurs from summer to fall in the sediments. Those data will be used as background data on the artificial radionuclides in the lakes to assess the effect of released radionuclides on their concentrations.  相似文献   

9.
A field experiment using rare earth elements (REEs) as tracers was conducted to investigate soil erosion processes on slope surfaces during rainfall events. A plot of 10 m × 2 m × 0.16 m with a gradient of 20° (36.4%) was established and the plot was divided into two layers and four segments. Various REE tracers were applied to the different layers and segments to determine sediment dynamics under natural rainfall. Results indicated that sheet erosion accounted for more than 90% of total erosion when the rainfall amount and density was not large enough to generate concentrated flows. Sediment source changed in different sections on the slope surface, and the primary sediment source area tended to move upslope as erosion progressed. In rill erosion, sediment discharge mainly originated from the toe-slope and moved upwards as erosion intensified. The results obtained from this study suggest that multi-REE tracer technique is valuable in understanding the erosion processes and determining sediment sources.  相似文献   

10.
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   

11.
Sequential extraction techniques have been developed to assess partitioning of anthropogenic radionuclides (240Pu, 239Pu, and 237Np), originating from a variety of sources, as identified by using bulk sediment isotopic composition. Sediments were leached sequentially with a series of six chemical treatments designed to approximate different environmental processes that may occur or to selectively extract trace metals contained in different solid phases of the sediments (i.e., exchangeable, reducible, carbonate, organic, acid leachable, and refractory). Results indicate the majority of Pu and Np is similarly distributed within many of the extracted fractions, with the largest percentage (66–97%) of both elements being observed in sediments treated with buffered citrate dithionite (CDB), which targets easily reduced constituents such as Mn and Fe hydrous oxides. While these results do indicate an association of Pu and Np with redox sensitive elements, the environmental implications are unclear given that the CDB treatment is more extreme than naturally occurring conditions. Minor amounts of Np partition differently from Pu in sediments. The NH4-acetate treatment, which is designed to liberate trace metals that are loosely adsorbed onto the surfaces of sedimentary materials such as hydrated iron oxides and humic substances, or present at exchangeable sites in clay minerals, mobilized ∼12% of the total Np while Pu levels were below detection. The H2O2 treatment, which is designed to liberate trace metals bound to organic matter, mobilized ∼8 and ∼1% of Np and Pu, respectively. These results indicate that a minor portion of the total Np may be affected by environmental conditions that have little or no effect on Pu. Between 7 and 24% of the Pu was observed in treatments designed to liberate Pu and Np that are tightly bound to lithogenic phases or refractory silicates. The 240Pu/239Pu observed in accessible and refractory fractions ranged between 0.11 and 0.18. With the exception of one sample, the 240Pu/239Pu isotope ratios measured in the refractory fractions are essentially identical having a mean ratio value of 0.123 ± 0.001 (1σ). The 240Pu/239Pu ratios provide isotopic evidence that suggests a portion of non-fallout contamination has a refractory nature. The presence of similarly low 240Pu/239Pu ratios in refractory fractions of sediments from the Ob and Irtysh Rivers suggests the existence of a source of refractory Pu which is consistent with refractory “hot particles” derived from surface tests at the Semipalitinsk test site.  相似文献   

12.
The role of puddle sediments as a final depot of 137Cs horizontal migration within the urban landscape is studied using the example of Ekaterinburg city, Russia. Radioactive contamination in the city appeared due to fallout after atmospheric testing of nuclear weapons and nuclear accidents. Contamination density of 137Cs in the region was assessed from archive data to be about 5.1 kBq/m2, of which the maximum activity concentration (<30 Bq/kg) is associated with the upper 15 cm soil layer. Results of the survey reported here indicate a mean 137Cs activity concentration in puddle sediments of 80 Bq/kg, with a maximum value of 540 Bq/kg. It is estimated that horizontal migration has led to about a fourfold concentration of 137Cs in puddle sediments.  相似文献   

13.
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   

14.
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   

15.
The present study applied sequential extraction techniques to investigate the binding and mobility of plutonium (Pu) in sediments from the rivers and estuaries of the Ob and Yenisey. As a study site, the Ob and Yenisey are particularly interesting as both rivers have weapons-grade Pu sources in their catchment areas, including the Russian Pu production and reprocessing plants at Mayak, Tomsk-7 and Krashnoyarsk, and the Semipalantinsk nuclear weapons testing site in Kazakhstan. Plutonium activity and 240Pu/239Pu ratios were determined using accelerator mass spectrometry (AMS). Sequential extractions showed that between 47 and 80% of the Pu in Yenisey River sediments and 35–53% of the Pu in soils around the Techa River are mobilized with weak oxidising agents, which can indicate that Pu is bound to organic material. In contrast, Pu in Ob and Yenisey Estuarine sediments was more strongly bound, with 60–100% being found in the HNO3-extractable fraction. This change in speciation could reflect either that Pu bound to organic material in the Techa and Yenisey River sediments becomes more fixed to the sediments with time, or that organic-bound Pu is mobilized and released to the water when the sediments encounter the more saline water of the Ob and Yenisey estuaries. In general, 240Pu/239Pu ratios were relatively consistent between different extraction fractions, although, in whole sediments, an increase in ratio was observed with distance from the source. This reflects the increased influence of weapon fallout from catchment runoff within the river systems, as compared to the weapons-grade sources close to the production and reprocessing plants. Knowledge of Pu speciation in the Ob and Yenisey Rivers, and the processes controlling its behaviour in estuarine systems, can improve predictions of its transfer and subsequent environmental impact to Arctic Seas.  相似文献   

16.
The release of tritiated water (HTO) to the atmosphere during the winter can contribute significantly to snow contamination and to water-soil-plant contamination after the spring thaw. The dose significance of such a release depends on the persistence of tritiated water in the snowpack, which is primarily controlled by the HTO diffusion process in snow and the rate of re-emission into the atmosphere from the snowpack surface. Monitoring data collected after an acute winter release at Chalk River Laboratories and data obtained in winter over a chronically contaminated area were analyzed to estimate the diffusion coefficient of HTO in the snowpack. Under conditions of cold and dry snow, the diffusion coefficient lay in the range 1-2 × 10−10 m2 s−1, an order of magnitude lower than diffusion in water but an order of magnitude higher than self-diffusion in ice. These results confirm the theoretical predictions (Bales, 1991). Values up to six times higher were found for warmer periods and just before spring melt, when other processes contribute to profile evolution. The low diffusion rate of tritium in cold, dry snow means that tritium remains in the snowpack throughout the winter, to be released during spring thaw to potentially contaminate surface water, soil and crops.  相似文献   

17.
Impact of water quality parameters on the sorption of U(VI) onto hematite   总被引:2,自引:0,他引:2  
In this study, the sorption of U(VI) from aqueous solution on hematite was studied as a function of various water quality parameters such as contact time, pH, ionic strength, soil humic acid (HA) or fulvic acid (FA), solid content and temperature by using a batch technique. The results demonstrated that the sorption of U(VI) was strongly dependent on ionic strength at pH < 6.0, and outer-sphere surface complexation may be the main sorption mechanism. The sorption was independent of ionic strength at pH > 6.0 and the sorption was mainly dominated by inner-sphere surface complexation. The presence of HA/FA increases U(VI) sorption at low pH, whereas decreases U(VI) sorption at high pH. The thermodynamic parameters (ΔH0, ΔS0, and ΔG0) were calculated from the temperature dependent sorption isotherms, and the results suggested that U(VI) sorption was a spontaneous and endothermic process. The results might be important for the application of hematite in U(VI) pollution management.  相似文献   

18.
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   

19.
The objective of this paper is to report on the results of a study of 238Pu, 239 + 240Pu and 241Am inventories onto Blelham Tarn in Cumbria (UK). The atmospheric fallout inventory was obtained by analysing soil cores and the results are in good agreement with the literature: 101 Bq m(-2) for 239 + 240Pu; 4.5 Bq m(-2) for 238Pu and 37 Bq m(-2) for 241Am. The sediment core inventory for the whole lake is compared to the atmospheric fallout inventory. The sediment activity is 60-80% higher than the estimated fallout activity, showing a catchment area contribution and in particular the stream input.  相似文献   

20.
The vertical distribution of 137Cs activity in peat soil profiles and 137Cs activity concentration in plants of various species was studied in samples collected at two sites on a raised bog in central Sweden. One site (open bog) was in an area with no trees and only a few sparsely growing plant species, while the other (low pine) was less than 100 m from the open bog site and had slowly growing Scots pine, a field layer dominated by some ericaceous plants and ground well-covered by plants. The plant samples were collected in 2004–2007 and were compared with samples collected in 1989 from the same open bog and low pine sites. Ground deposition of 137Cs in 2005 was similar at both sites, 23?000 Bq m−2. In the open bog peat profile it seems to be an upward transport of caesium since a clear peak of 137Cs activity was found in the uppermost 1–4 cm of Sphagnum layers, whereas at the low pine site 137Cs was mainly found in deeper (10–12 cm) layers. The migration rate was 0.57 cm yr−1 at the open bog site and the migration centre of 137Cs was at a depth of 10.7, while the rate at the low pine site was 0.78 cm yr−1 and the migration centre was at 14.9 cm. Heather (Calluna vulgaris) was the plant species with the highest 137Cs activity concentrations at both sites, 43.5 k Bq−1 DM in 1989 decreasing to 20.4 in 2004–2007 on open bog and 22.3 k Bq kg−1 DM in 1989 decreasing to 11.2 k Bq−1 DM by the period 2004–2007 on the low pine site. 137Cs transfer factors in plants varied between 0.88 and 1.35 on the open bog and between 0.48 and 0.69 m2 kg−1 DM at the low pine site.  相似文献   

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