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1.
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   

2.
Results for naturally occurring 7Be, 210Pb, 40K, 214Bi, 214Pb, 212Pb, 228Ac and 208Tl and anthropogenic 137Cs in airborne particulate matter in the Barcelona area during the period from January 2001 to December 2005 are presented and discussed. The 212Pb and 208Tl, 214Bi and 214Pb, 7Be and 210Pb radionuclide levels showed a significant correlation with each other, with correlation coefficients of 0.99, 0.78 and 0.69, respectively, suggesting similar origin/behaviour of these radionuclides in the air. Caessium-137 and Potassium-40 were transported to the air as resuspended particle from the soil. The 7Be and 210Pb concentrations showed similar seasonal variations, with a tendency for maximum concentrations during the summer months. An inverse relationship was observed between the 7Be, 210Pb, 40K and 137Cs concentrations and weekly rainfall, indicating washout of atmospheric aerosols carrying these radionuclides.  相似文献   

3.
Soil inventories of anthropogenic radionuclides were investigated in altitudinal transects in 2 French regions, Savoie and Montagne Noire. Rain was negligible in these 2 areas the days after the Chernobyl accident. Thus anthropogenic radionuclides are coming hypothetically only from Global Fallout following Atmospheric Nuclear Weapon Tests. This is confirmed by the isotopic signatures (238Pu/239+240Pu; 137Cs/239+240Pu; and 241Am/239+240Pu) close to Global Fallout value. In Savoie, a peat core age-dated by 210Pbex confirmed that the main part of deposition of anthropogenic radionuclides occurred during the late sixties and the early seventies. In agreement with previous studies, the anthropogenic radionuclide inventories are well correlated with the annual precipitations. However, this is the first time that a study investigates such a large panel of annual precipitation and therefore of anthropogenic radionuclide deposition. It seems that at high-altitude sites, deposition of artificial radionuclides was higher possibly due to orographic precipitations.  相似文献   

4.
Ribeira Bay is located approximately 130 km south of the city of Rio de Janeiro and receives discharges of liquid effluent from the Angra dos Reis nuclear power plant (NPP) site, where two pressurized water reactors are located. To test whether the presence of anthropogenic radionuclides in sediments in Ribeira Bay could be correlated to the NPP operations, we sampled seven sediment cores and determined accumulation rates and chronologies. Only one sediment core did not exhibit a superficial mixing layer; this sample was used for dating purposes. Cesium-137 and 207Bi were observed in this sediment profile, but their presence was associated with atmospheric fall-out rather than the nearby NPP. The exponential decay of 210Pb concentration with sediment layer depth was verified below a superficial mixing layer for all other sediment cores. Calculated accumulation rates ranged from 1.2 mm y−1 in the inner bay to 6.2 mm y−1 close to its entrance.  相似文献   

5.
In case of an accidental release of radioactive substances into the environment, it is important to quickly and reliably estimate the radiation dose received by people in the affected area, and to determine the extent of the contamination. Measurements of the extent of the release and the subsequent contamination can be facilitated if there are predetermined reference sampling sites with known background radiation and inventory of radionuclides. Since 1996, 34 reference sites for soil sampling, field gamma, and intensimeter measurements have been established in western Sweden. Time series data for dose rates and radioisotope inventory have been collected at these sites, allowing for the investigation of changes in these parameters over time. The mass activity densities for the uranium and thorium series elements varied approximately between 10 and 50 Bq/kg and between 10 and 40 Bq/kg, respectively. The mass activity density of 40K was approximately in the range 300–800 Bq/kg. The radiation exposure due to 137Cs was rather small in this area. The dose rates calculated from in situ measurement data showed that the contribution to the total dose rate was almost entirely due to naturally occurring radionuclides. The measured dose rate was about twice as high as the calculated rate, even after subtracting the contribution from cosmic radiation. This may be explained by the fact that intensimeters generally are calibrated to measure the quantity ambient dose equivalent, which should not underestimate the effective dose.  相似文献   

6.
Caesium-137 activity concentration in the water columns of the Gulf of Patras (Central Greece) and the North-Eastern Aegean Sea (easterward to Lemnos Island) was investigated in selected sampling stations during the period September 2004–June 2006. The methodology followed was based on the sorption of caesium (Cs) on cotton wound cartridge filters impregnated by Cu2[Fe(CN)6] via in-situ pumping. In terms of the horizontal and vertical records, the activity concentrations of 137Cs in the Gulf of Patras ranged between 1.2 and 6.7 Bq m−3, depending on the sampling period and the prevailing physicochemical regime at the sampling station. The general pattern of the decreased activity concentrations of 137Cs with increasing depth was reversed in the Gulf of Patras during the cold period attributed to the prevailing advective processes of the area. The activity concentrations of 137Cs in the North-Eastern Aegean Sea ranged from 2.6 to 12.8 Bq m−3, whereas significant stratified curves were observed during the warm period and also, in one station during the cold period. In terms of temporal variation, the discharges in the Gulf of Patras resulted in enhanced levels of 137Cs, whereas in the North Aegean Sea the incoming water masses form the Black Sea had an apparent influence throughout the year by increasing the 137Cs levels, hence presenting a weak seasonal variation. Comparing the two studied areas, one could say that the North Aegean Sea, as an open sea environment, presented higher concentrations due to the influence of the Black Sea water masses. The estimated inventories of 137Cs in the Gulf of Patras ranged 0.25 ± 0.03–0.79 ± 0.03 kBq m−2, whereas in the North-Eastern Aegean Sea they ranged 0.33 ± 0.02–0.92 ± 0.03 kBq m−2.  相似文献   

7.
External gamma radiation levels were measured in the catchment areas of the Sharavathi River and the dose rates in air were found to be in the range 26.0-61.0 nGy h−1. Soil and sediment samples of the riverine environment were analysed for natural radionuclides such as 226Ra, 232Th and 40K using a NaI(Tl) gamma spectrometer. The activity concentration of 210Pb and 210Po in soil and sediment samples was determined by radiochemical separation techniques. Evaluation of the activity concentration of radionuclides with grain size revealed an increase in the activity of 226Ra, 232Th and 40K towards fine grain size. The activity concentrations for all isotopes in all samples were not significantly correlated with pH. However, the activity of 210Po and 210Pb in sediment showed a moderate positive correlation with organic matter content and a good correlation with clay content of sediment.  相似文献   

8.
This study focuses on the cesium-137 (137Cs) contamination in grass and in different compartments of oak trees growing in ecosystems, located in the zone with sub-mediterranean climate in South Bulgaria, characterized with high summer temperatures, low precipitation and often periods of drought. In 2008, three experimental sites - PP1, PP2, PP3 - were sampled in oak ecosystems from Maleshevska Mountain at 900 m above sea level. Samples from grass species and oak tree leaves, branches with different diameter, wood disks and bark were analyzed for 137Cs activity with γ-spectrometry. The soil-to-plant transfer factor (TF) values for 137Cs were estimated differentiating different tree compartments. Our findings showed relatively high activity concentrations of 137Cs in oak trees even 22 years after the Chernobyl accident. The grass under oak was less contaminated compared with the oak trees. The different organs of oak trees could be distinguished according to the 137Cs contamination as follows: bark > branches (d < 1 cm) > leaves > branches (d > 3 cm) > wood. The relatively higher contamination of bark compared with the new-formed biomass suggested that a significant part of 137Cs was accumulated as a result of direct adsorption at the time of the main contamination event. The TF values obtained and the presence of 137Cs in the branches, leaves and in the wood formed after 1986 confirmed that 22 years after the contamination, the main mechanism of 137Cs entrance in tree biomass was the root uptake.  相似文献   

9.
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   

10.
Sources of anthropogenic radionuclides in the environment: a review   总被引:1,自引:0,他引:1  
Studies of radionuclides in the environment have entered a new era with the renaissance of nuclear energy and associated fuel reprocessing, geological disposal of high-level nuclear wastes, and concerns about national security with respect to nuclear non-proliferation. This work presents an overview on sources of anthropogenic radionuclides in the environment, as well as a brief discussion of salient geochemical behavior of important radionuclides. We first discuss the following major anthropogenic sources and current developments that have lead, or could potentially contribute, to the radionuclide contamination of the environment: (1) nuclear weapons program; (2) nuclear weapons testing; (3) nuclear power plants; (4) uranium mining and milling; (5) commercial fuel reprocessing; (6) geological repository of high-level nuclear wastes that include radionuclides might be released in the future, and (7) nuclear accidents. Then, we briefly summarize the inventory of radionuclides 99Tc and 129I, as well as geochemical behavior for radionuclides 99Tc, 129I, and 237Np, because of their complex geochemical behavior, long half-lives, and presumably high mobility in the environment; biogeochemical cycling and environment risk assessment must take into account speciation of these redox-sensitive radionuclides.  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.
Discharges from the Krasnoyarsk Mining and Chemical Industrial Complex (KMCIC) near Krasnoyarsk resulted in radioactive contamination of sediments of the River Yenisei. Between 1999 and 2006, 16 sediment cores were collected at different positions 15-1500 km downstream from the discharge point. The concentration of artificial gamma-emitting radionuclides (137Cs, 60Co, 152Eu, and 241Am) was determined with the objective to analyze the migration processes leading to the transport of these radionuclides along the river and to their vertical distribution within the sediment. In cores taken in the vicinity of the reactors, the average activity concentration of 137Cs, 152Eu, and 60Co was about 1000 Bq kg−1, and the activity concentration of 241Am was about 20 Bq kg−1. Contamination levels of artificial radionuclides were decreasing with increasing distance downstream the KMCIC: The fastest decrease of average activity by a factor of 10 over a distance of 300 km was observed for 241Am, whereas for 137Cs this decrease occurred over a distance of 1100 km. Sequential extraction experiments revealed that in all depths and at all distances the studied radionuclides were tightly bound to the sediment.To investigate the mechanisms of transport of the 137Cs and 60Co contamination, mathematical models have been used to describe the contamination in the river water and within the sediments.  相似文献   

13.
A microcosm laboratory experiment was conducted to determine the impact of biological reworking by the ragworm Nereis diversicolor on the redistribution of particle-bound radionuclides deposited at the sediment-water interface. Over the course of the 40-day experiment, as much as 35% of a 137Cs-labelled particulate tracer deposited on the sediment surface was redistributed to depths of up to 11 cm by the polychaete. Three different reworking models were employed to model the profiles and quantify the biodiffusion and biotransport coefficients: a gallery-diffuser model, a continuous sub-surface egestion model and a biodiffusion model. Although the biodiffusion coefficients obtained for each model were quite similar, the continuous sub-surface egestion model provided the best fit to the data. The average biodiffusion coefficient, at 1.8 ± 0.9 cm2 y−1, is in good agreement with the values quoted by other workers on the bioturbation effects of this polychaete species. The corresponding value for the biotransport coefficient was found to be 0.9 ± 0.4 cm y−1. The effects of non-local mixing were incorporated in a model to describe the temporal evolution of measured 99Tc and 60Co radionuclide sediment profiles in the eastern Irish Sea, influenced by radioactive waste discharged from the Sellafield reprocessing plant. Reworking conditions in the sediment column were simulated by considering an upper mixed layer, an exponentially decreasing diffusion coefficient, and appropriate biotransport coefficients to account for non-local mixing. The diffusion coefficients calculated from the 99Tc and 60Co cores were in the range 2-14 cm2 y−1, which are consistent with the values found by other workers in the same marine area, while the biotransport coefficients were similar to those obtained for a variety of macrobenthic organisms in controlled laboratories and field studies.  相似文献   

14.
Measurements of airborne radioactive aerosol concentration were carried out on the basis of 1-3 days samples after the Chernobyl disaster and during the period of 1992-2003. Transport of "hot" particles of different composition resulted in the high activity concentrations of (137)Cs, (238)Pu, (239,240)Pu and (241)Am in the atmosphere in Vilnius at the end of April 1986. The (240)Pu/(239)Pu atom ratio showed clear evidence of non-global plutonium originating from the Chernobyl accident in the atmosphere over Lithuania. The (240)Pu/(239)Pu atom ratio ranged from 0.14 to 0.40 in monthly samples in Vilnius in 1995-2003. An increase in activity concentration of (137)Cs by a factor of 100 (up to 300 microBq/m(3)) was found following forest fires in the Ukraine and Belarus. However, no transport of the Chernobyl plutonium was observed and the (240)Pu/(239)Pu atom ratio in samples collected during the forest fires was found to be 0.229 and 0.185, respectively. The exponential decrease in the (240)Pu/(239)Pu atom ratio from 0.30 to 0.19 (mean values) was observed in 1995-2003.  相似文献   

15.
A gamma-ray survey and analysis of 16 riverbed samples from the Reedy River watershed near Simpsonville, SC were conducted and compared with national and international studies of primordial radionuclides. The study reported here follows on a recent discovery of anomalously high uranium concentrations in several private well waters in the area. An HPGe spectrometer was used for quantification of gamma emitting radionuclides in the sediments. All sediments contained radionuclides from the uranium and thorium series as well as (40)K. Uranium-238 concentrations in sediment samples ranged from 11.1 to 74.2Bqkg(-1). The measured radionuclide concentrations were compared with data from UNSCEAR and NURE reports. The river and stream sediment data were augmented by in situ NaI(Tl) gamma-ray spectrometer measurements. Comparisons between the ex situ and in situ measurements indicate equivalently distributed uranium in the surface soils and stream sediments, the source of which is likely attributed to the monazite belts that are known to exist in the area.  相似文献   

16.
Data on content of (90)Sr, (137)Cs, (239,240)Pu and (3)H in water of the Tobol-Irtysh part of the Techa-Iset-Tobol-Irtysh-Ob river system (through which the "Mayak" PA radioactive wastes are transported) are presented and discussed. The data were received in 2004-2005 under the ISTC project on radioecological monitoring of the Tobol and Irtysh rivers. Monthly observations of (137)Cs, (90)Sr and (3)H content in water in the area of the Tobol and Irtysh confluence have been conducted starting from May 2004. To obtain information on the investigated river system as a whole, the radioecological survey of the Tobol and Irtysh rivers at the section from the mouth of the Iset River to the confluence with the Ob River was carried out in 2004. It is shown that the impact of "Mayak" PA waste transport by (90)Sr is distinctly traced as far as the area of the Irtysh and Ob confluence.  相似文献   

17.
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   

18.
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   

19.
The production and discharge of liquid radioactive wastes as excreta from patients undergoing Nuclear Medicine Diagnostic (NMD) in a hospital were studied. Instantaneous and accumulated activity, discharged from the hospital to the sewage system, has been estimated keeping in mind radionuclide decay. This study would enable estimation of the environmental impact due to NMD procedures. Annual accumulated activities of 2.2GBq ((131)I), 1.847GBq ((99m)Tc), 0.743GBq ((123)I), 0.337GBq ((67)Ga), 0.169GBq ((111)In) and 0.033GBq ((201)Tl) result from our model when applied to a European hospital. A comparison is made with calculations by other authors that do not consider the radionuclide decay and who overestimate by two orders of magnitude. Doses to critical people as sewage treatment workers are also significantly reduced. So, our results stress the importance of including the decay in the calculations.  相似文献   

20.
Several natural and anthropogenic radionuclides (210Pb, 226Ra and 137Cs) in guano-phosphatic coral sediments and pure guano particles collected from Ganquan, Guangjin, Jinqing and Jinyin Islands of the Xisha archipelago, South China Sea, were analyzed. The Constant Initial Concentration (CIC) model and the Constant Rate of Supply (CRS) model were applied for age calculation. The average supply rate of 210Pb was 126 Bq m−2 a−1, very close to the flux of northern hemisphere average (125 Bq m−2 a−1). The activities of anthropogenic radionuclides in the sediments were very low, indicating that human nuclear tests did not notably impact this region. The main source of radionuclides in the sediments was from atmospheric precipitation, and the organic matter derived from plant and produced by nutrient-rich guano could further enhance them.  相似文献   

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