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1.
In situ large volume filtration and chemisorption techniques were used to collect samples from the North Pacific for radiochemical analyses of fallout transuranics and 55Fe in filterable and filtered phases. The data cover several locations for surface collections and a detailed depth profile north of Hawaii at 30°N. The observed partition of these nuclides between suspended particulate and filtered phases is directly linked to the rates at which they are moved downward through the water column in association with sinking particles. Particulate phases in open ocean surface waters contain higher Pu (12–35%) than subsurface particulates (which average about 6%). 241Am was found to exhibit much stronger particle association—typically close to 50% in both surface and subsurface waters—in accord with its known greater particle reactivity. In the high Pu deep water layer, particle associated Pu dropped to close to 1% of total Pu concentration. Together with a correlated increase in the proportion of oxidized Pu in this layer close to the sediment-water interface, this is taken as clear evidence of remobilization Pu from particles at, or near to, the interface. 55Fe distributions on filtered particulates indicate a much deeper depth distribution relative to the transuranics. This may reflect both a higher particle association reactivity in respect to scavenging and a longer exposure history to scavenging (especially relative to 241Am—produced by in situ decay).  相似文献   

2.
The responses to pH of abiotic interactions between dissolved humic substances, iron and phosphate were investigated by examining redistributions of 55FeCl3 and 32PO43− added to epilimnetic lakewater from Lake Skjervatjern. The simultaneous movement of 55Fe and 32P to fractions of 10 000–20 000 and > 100 000 Daltons nominal molecular weight, as indicated by Sephadex gel filtration, diminished in response to decreasing pH. Variations in transformations to larger molecular size fractions with incubation time revealed by gel filtration were erratic, but indicated that transformations of added 55Fe and 32P are complete after circa 24 h. Movement of 32P to particle size fractions (>0.2 μm) was not dependent on pH, whilst transformations of 55Fe to material of particle size increased as pH was lowered. Precipitation of added 55Fe and 32P was minimal at all pH values tested. Responses of precipitation losses to pH were not coincident for both radionuclides.  相似文献   

3.
The use of ultra filtration in trace metal speciation studies in sea water   总被引:1,自引:0,他引:1  
During this work, size fractionation technique "ultra filtration" is used in speciation studies of trace elements in the coastal sea water. Filtration is the most commonly used method to fractionate trace metal species, but often only "dissolved" and "particulate" fraction. The purpose of the present study is to determine colloidal and suspended particulate concentrations of Fe, Zn, Cu, Ni, and Mn in sea water. Suspended particulate matter were separated in three different size groups namely (>2.7 microm, <2.7->0.45 microm and <0.45->0.22 microm) by suction filtration using cellulose acetate and nitrate filter membranes. Thereafter to concentrate the solution with colloidal particle <0.22 microm-1.1 nm (0.5 k Nominal Molecular Weight cut-off Limit {NMWL}), the solution obtained from filtration through <0.22 microm, is sequentially passed through the ultra-filtration membranes having pore diameters of 14 nm (300 k NMWL), 3.1 nm (50 k NMWL), 2.2 nm (30 k NMWL), 1.6 nm (10 k NMWL) and 1.1 nm (0.5 k NMWL) by using Stirred Ultra-filtration Cells, operating in concentration mode. The concentration of Fe, Zn, Cu, Ni, and Mn were measured in suspended and dissolved fraction by ion chromatography, ICP-AES and Atomic Absorption Spectrometer. The salinity of the solution in various dissolved fractions of sequential filtration varies between 30.89-34.22 parts per thousand. The maximum concentrations of colloidal Zn, Cu, Ni and Mn in dissolved fraction were in <2.2->1.6 nm fraction. In case of Fe, colloidal fractions <2.2->1.6 nm and <1.6-<1.1 nm shows higher concentration. The concentration of Zn, Cu, Ni and Mn increase with decrease in size in suspended particulate matter, while the reverse is observed in case of Fe. This size separation data that specifies the partitioning of metals between dissolved and suspended solid phases is necessary for developing physically based models of metal transport in aquatic system.  相似文献   

4.
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   

5.
An assessment has been made of the association of (239+240)Pu, 241Am and 210Po (in secular equilibrium with 210Pb) with iron minerals using a magnetic extraction technique. Grab samples of beach sand from the Cumbrian (UK) coastline were subjected to successive extractions with an approximately 0.1 T ferrite magnet and an approximately 0.3 T rare-earth magnet procedure to separate magnetic iron oxide minerals. Radionuclide concentrations in the magnetic extracts were enhanced (by approximately 4-6-fold) relative to the residue. Those in the approximately 0.1 T magnet extracts were broadly similar to those in the antiferromagnetic material extracted by the approximately 0.3 T magnet, despite the very large differences in magnetic property values between the two fractions (one to two orders of magnitude). The percentage of magnetic material in terms of mass was small and therefore, the majority of these radionuclides (on average 88%) were associated with the residue. Removal of stable Fe was incomplete. Given that the radionuclides may also bind to paramagnetic (nonmagnetic) Fe minerals, the data were extrapolated by normalising the results to quantitative Fe removal. This yielded average values of 37%, 45% and 46% for (239+240)Pu, 241Am and 210Po(210Pb), respectively, as upper limits for the fraction associated with magnetic + nonmagnetic Fe minerals. There are significant uncertainties inherent in quantifying data from this extraction technique. Nevertheless, it seems reasonable to conclude that radionuclide association with Fe minerals is unlikely to have a significant impact upon the physical dispersion of sediment contaminated by Sellafield discharges in the Irish Sea. However, it may be an important factor in governing Pu redox and redissolution behaviour.  相似文献   

6.
As a result of former uranium mining and milling activities at ?irovski vrh, Slovenia, 0.6 million tons of uranium mill tailings (UMT) were deposited onto a nearby waste pile Boršt. Resulting enhanced levels of natural radionuclides in UMT could pose threat for the surrounding environment. Therefore, sequential extraction protocol was performed to assess mobility and bioavailability of 238U, 234U, 230Th and 226Ra in soils from the waste pile and its surrounding. The radionuclides associated with exchangeable, organic, carbonate, Fe/Mn oxides and residual fraction, respectively, were determined. Results showed that the highest activity concentrations for the studied radionuclides were on the bottom of the waste pile. In non-contaminated locations, about 80% of all radionuclides were in the residual fraction. Considering activity concentrations in the UMT, 238U and 234U are the most mobile. Mobility of 226Ra is suppressed by high sulphate concentrations and is similar to mobility of 230Th.  相似文献   

7.
A sample of contaminated groundwater was analyzed using a combination of wet techniques to obtain geochemical information on the mobile species of 60Co, 125Sb, 137Cs and 241Am. The techniques were combined in a scheme to determine the predominant character of the radionuclides in negative or positive fractions, size separation by ultrafiltration, and their association with natural organic matter (NOM). The analyses indicated that the radionuclides of interest were predominantly in the negative fraction. Most of the 60Co and 125Sb were in the small size fraction (<5000 Da), and 137Cs and 241Am were found with the larger, colloidal-sized material. Antimony-125 and 60Co were predominantly in the hydrophilic fraction, while 137Cs and 241Am were found in hydrophobic fractions. Our analysis indicated that 137Cs is found in the same fraction as the large-sized colloidal (hydrophobic) material, suggesting an association with NOM. The results suggested that 60Co and 241Am were associated with NOM, in different size fractions, suggesting that these two nuclides are bound to different sites. Finally, the 125Sb results were inconclusive, whether this nuclide is associated with NOM, or it is inorganic.  相似文献   

8.
This study examines the chemical composition of PM10, the thoracic fraction of the atmospheric particulate matter. An eight-stage Anderson impactor is used to separate the PM10 from other fractions with different aerodynamic behaviour at three different area representative sites in Delhi from February to May 1998. PM10 particulate are subdivided into two fractions, coarse (> 2.1-10 microns) and fine (< 2.1 microns). The concentrations of major heavy metals such as Pb, Zn, Cd, Ni, and Fe are determined by atomic absorption spectrophotometer. The average concentration of coarse fraction of PM10 is found to be 68.3 +/- 17 micrograms/m3 while the fine fraction of PM10 is 71.3 +/- 15 micrograms/m3 for Delhi. Metal concentration (except Fe) in fine fraction exceeds by a factor of up to 6, as compared to that in the coarse fraction. In order to identify the major sources of fine and coarse fraction of PM10, principle component analysis (PCA) was undertaken and three major sources were identified, namely vehicular emissions, industrial emission, and soil resuspension.  相似文献   

9.
Samples of atmospheric particulate material and terrestrial plants, including lichens, were collected in New Brunswick, Canada between 1980 and 1983 and analyzed for a wide range of artificial and naturally-occuring radionuclides, including fission products (141Ce, 144Ce, 103Ru, 106Ru, 95Zr and 137Cs) derived from the 16 October 1980 Chinese nuclear test. Activity ratios of some of the short-lived fission products in air particulates and lichens are in reasonable agreement with those predicted from fission product yields for nuclear weapons tests, indicating that only minor fractionation occurred for these radionuclides during their transport through air particulate and lichen environmental phases. The 7Be inventories measured in a suite of lichen (Cladonia rangiferina) samples were used to calibrate each lichen plant for its collection efficiency for atmospheric particulates and fallout radioactivity.A lichen model has been developed to predict lichen inventories of radioactivity for different lichen growth functions and bio-elimination rates. Assuming that lichen growth results in a linear increase in surface area with time, the experimental results yield biological residence times of 1–2 years for 210Pb and Pu and 5–8 years for 137Cs. The more efficient retention of 137Cs is probably due to its physiological uptake in lichen plants as a proxy for potassium, as evidenced by an observed, inverse relationship between 137Cs and 40K activities in lichen.  相似文献   

10.
The behaviour of radionuclides discharged from nuclear facilities in the Rh?ne River depends on their distribution among the dissolved, colloidal and particulate phases. A large water sample was fractionated using sequential ultrafiltration. Size distributions of organic carbon, Fe, Al, Si, Ca, Mg, Cu, Zn, 137Cs, 60Co and 106Ru were obtained. Our results show that organic colloids account for 11% of the total organic carbon content. Approximately 20% of the dissolved (< 450 nm) Fe and Al are in colloidal classes. 137Cs is not significantly transferred by the colloidal phase while 25% of 60Co or 106Ru is associated with organic and inorganic colloids.  相似文献   

11.
Knowledge about propagation of radionuclides from nuclear power plants (NPPs) along the course of a river is of great interest in radioecological assessments. By use of a model previously applied in the cases of the Rhine and Weser Rivers, the distribution of various radionuclides released into the Moselle from the NPP Cattenom at normal operation is described with 58Co, 60Co and 110mAg as tracers. A comparison of field measurements with calculated values revealed that the radionuclide concentrations in suspended matter and nuclide loads calculated from emission rates agreed with the measured data by a factor of less than two on average.Radionuclide concentrations and loads along the river course decrease mainly due to deposition of particulate radioactive matter in high-sedimentation areas and due to dilution with uncontaminated material from tributaries and other sources. The rate constants of both processes were evaluated, and the mean range of suspended radioactive particles in the Moselle was estimated. Moreover, this study showed anew that suspended matter has to be considered as the main carrier by which the radionuclides from NPPs may be transported over long distances.  相似文献   

12.
The sorption and release kinetics of 54Mn, 58Co, 59Fe, 109Cd, 110mAg and 134Cs by freshwater suspended particles were investigated to better identify the biogeochemical processes involved and to obtain suitable data for improving models describing radionuclide migration in freshwater streams. In order to observe any seasonal variability in the interaction of radionuclides with natural particles, experiments were performed both in winter and in summer during a phytoplanktonic bloom. Two kinetic models are compared in this paper: the "one-step reversible" model, based on the hypothesis that the transfer of radionuclides between water and suspended solids is governed by a reversible reaction, and the "two-successive-step reversible" model, which assumes two distinct types of sites or reactions on the solid phase. The "one-step reversible" model is generally unable to describe properly the exchange kinetics; this result shows that at least two processes are generally involved in radionuclide exchange between water and suspended particles. On the contrary, a model involving the existence of two successive reversible reactions properly simultes both the sorption and release kinetics. The determination of the kinetic coefficients allows quantitative assessment of the relative importance and kinetics of the processes. In particular, it has been shown that, except for Cs and Cd, major fractions of the radionuclides are associated at equilibrium with particulate sites involving strong interactions. The kinetics to reach this equilibrium depend on seasonal conditions, especially for Co and Mn: the transfer of Co and Mn to particulate sites involving strong interactions is much slower in winter. The distribution of the radionuclides between water and particulate sites involving weak interactions also shows seasonal variations for Co, Mn, Fe and Ag: the capacity to associate radionuclides is much higher in summer for Co and Mn, while the inverse tendency is observed for Fe and Ag. For Cs and Cd, no significant seasonal differences were observed.  相似文献   

13.
Significantly high radiation level and radionuclide concentration along Quilon beach area of coastal Kerala have been reported by several investigators. Detailed gamma radiation level survey was carried out using a portable scintillometer. Detailed studies on radionuclides concentration in different environmental matrices of high background areas were undertaken in the coastal areas of Karunagapalli, Kayankulam, Chavara, Neendakara and Kollam to study the distribution and enrichment of the radionuclides in the region. The absorbed gamma dose rates in air in high background area are in the range 43-17,400 nGyh−1. Gamma radiation level is found to be maximum at a distance of 20 m from the sea waterline in all beaches. The soil samples collected from different locations were analysed for primordial radionuclides by gamma spectrometry. The activity of primordial radionuclides was determined for the different size fractions of soil to study the enrichment pattern. The highest activity of 232Th and 226Ra was found to be enriched in 125-63 μ size fraction. The preferential accumulation of 40K was found in <63 μ fraction. The minimum 232Th activity was 30.2 Bq kg−1, found in 1000-500 μ particle size fraction at Kollam and maximum activity of 3250.4 Bq kg−1 was observed in grains of size 125-63 μ at Neendakara. The lowest 226Ra activity observed was 33.9 Bq kg−1 at Neendakara in grains of size 1000-500 μ and the highest activity observed was 482.6 Bq kg−1 in grains of size 125-63 μ in Neendakara. The highest 40K activity found was 1923 Bq kg−1 in grains of size <63 μ for a sample collected from Neendakara. A good correlation was observed between computed dose and measured dose in air. The correlation between 232Th and 226Ra was also moderately high. The results of these investigations are presented and discussed in this paper.  相似文献   

14.
The effect of americium-241 (241Am), an alpha-emitting radionuclide of high specific activity, on luminous bacteria Photobacterium phosphoreum was studied. Traces of 241Am in nutrient media (0.16-6.67 kBq/L) suppressed the growth of bacteria, but enhanced luminescence intensity and quantum yield at room temperature. Lower temperature (4 °C) increased the time of bacterial luminescence and revealed a stage of bioluminescence inhibition after 150 h of bioluminescence registration start. The role of conditions of exposure the bacterial cells to the 241Am is discussed. The effect of 241Am on luminous bacteria was attributed to peroxide compounds generated in water solutions as secondary products of radioactive decay. Increase of peroxide concentration in 241Am solutions was demonstrated; and the similarity of 241Am and hydrogen peroxide effects on bacterial luminescence was revealed. The study provides a scientific basis for elaboration of bioluminescence-based assay to monitor radiotoxicity of alpha-emitting radionuclides in aquatic solutions.  相似文献   

15.
Most of the surface explosions in nuclear tests have released radioactivity to the environment in the form of bulk glassy materials originating from the melting of sandy soil in the neighbourhood of ground zero. In view of clarifying issues concerning the mechanism of formation and the radiological impact of these materials, we investigated incorporation and volume distribution of radionuclides in a typical fragment of trinitite, the glassy substance generated following the first nuclear test (Trinity Site, New Mexico, 1945). Specific activities were determined by γ-spectrometry for the most significant fission and activation products. In particular, 152Eu activity was used to estimate the original point of collection of the sample with respect to ground zero. After embedding in an epoxy resin, the sample was then sliced to perform cross-sectional β- and α-autoradiograph. α-spectrometry was also carried out on a fine powder obtained by surface abrasion. In the β-autoradiography, hot spots were distinguishable in the proximity of the blast side, over a 1000 times less intense background of sand activation products. Also α-contamination (from 239+240Pu and 241Am) was mostly concentrated within the superficial layer, in a fraction of only 20% of the overall volume of the sample, exhibiting a discontinuous, droplet-like distribution. This evidence would partially support a recent hypothesis on trinitite formation according to which most of the glass layer was formed not on the ground but by a rain of material injected into the fireball that melted, fell back, and collected on a bed of already fused sand.  相似文献   

16.
Particle-reactive, naturally occurring radionuclides are useful tracers of the sinking flux of organic matter from the surface to the deep ocean. Since the Joint Global Ocean Flux Study (JGOFS) began in 1987, the disequilibrium between 234Th and its parent 238U has become widely used as a technique to measure particle export fluxes from surface ocean waters. Another radionuclide pair, 210Po and 210Pb, can be used for the same purpose but has not been as widely adopted due to difficulty with accurately constraining the 210Po/210Pb radiochemical balance in the ocean and because of the more time-consuming radiochemical procedures. Direct comparison of particle flux estimated in different ocean regions using these short-lived radionuclides is important in evaluating their utility and accuracy as tracers of particle flux. In this paper, we present paired 234Th/238U and 210Po/210Pb data from oligotrophic surface waters of the subtropical Northwest Atlantic and discuss their advantages and limitations. Vertical profiles of total and particle size-fractionated 210Po and 234Th activities, together with particulate organic carbon (POC) concentrations, were measured during three seasons at the Bermuda Atlantic Time-series Study (BATS) site. Both 210Po and 234Th reasonably predict sinking POC flux caught in sediment traps, and each tracer provides unique information about the magnitude and efficiency of the ocean's biological pump.  相似文献   

17.
Distributions of anthropogenic radionuclides (90Sr, 137Cs and 239+240Pu) in seabed sediment in the Japan Sea were collected during the period 1998–2002. Concentration of 90Sr, 137Cs and 239+240Pu in seabed sediment was 0.07–1.6 Bq kg−1, 0.4–9.1 Bq kg−1 and 0.002–1.9 Bq kg−1, respectively. In the northern basin of the sea (Japan Basin), 239+240Pu/137Cs ratios in seabed sediment were higher and their variation was smaller compared to that in the southeastern regions of the sea. The higher 239+240Pu/137Cs ratios throughout the Japan Basin were considered to reflect production of Pu-enriched particles in the surface layer and substantial sinking of particulate materials in this region. In the southern regions of the Japan Sea (<38°N), both inventories and 239+240Pu/137Cs ratios in sediment were larger than those in the other regions. In the southern Japan Sea, observations suggested that supply of particulate radionuclides by the Tsushima Warm Current mainly enhanced accumulation of the radionuclides in this region.  相似文献   

18.
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   

19.
Activities of radionuclides in the 238U (230Th, 226Ra, 210Pb) and 232Th (232Th, 228Th, 228Ra) decay series were determined in sediments from an east Texas watershed and examined with isotope ratios and compared to particulate organic carbon (POC), % fines (<63 microm) and total concentrations of Al, Fe and Mn. The objective was to elucidate the presence or absence of relationships affecting the effectiveness of these radionuclides in modeling sediment transport. Strong positive correlations were observed between radionuclides and Mn (Th) and % fines (Ra and Th). Isotope ratios effectively reduce these influences, supporting the contention that isotope ratios offset extrinsic variability in terrestrial sediments. Strong associations of 210Pbxs (excess 210Pb) and 226Ra/230Th with POC agree with data from marine and terrestrial settings, indicating that the role of POC in isotope fractionation, transport and sequestration merits further investigation.  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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