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1.
Pu isotopes and (137)Cs were analyzed using sector field ICP-MS and γ spectrometry, respectively, in surface sediment and core sediment samples from the Yangtze River estuary. (239+240)Pu activity and (240)Pu/(239)Pu atom ratios (>0.18) shows a generally increasing trend from land to sea and from north to south in the estuary. This spatial distribution pattern indicates that the Pacific Proving Grounds (PPG) source Pu transported by ocean currents was intensively scavenged into the suspended sediment under favorable conditions, and mixed with riverine sediment as the water circulated in the estuary. This process is the main control for the distribution of Pu in the estuary. Moreover, Pu is also an important indicator for monitoring the changes of environmental radioactivity in the estuary as the river basin is currently the site of extensive human activities and the sea level is rising because of global climate changes. For core sediment samples the maximum peak of (239+240)Pu activity was observed at a depth of 172 cm. The sedimentation rate was estimated on the basis of the Pu maximum deposition peak in 1963-1964 to be 4.1 cm/a. The contributions of the PPG close-in fallout Pu (44%) and the riverine Pu (45%) in Yangtze River estuary sediments are equally important for the total Pu deposition in the estuary, which challenges the current hypothesis that the riverine Pu input was the major source of Pu budget in this area.  相似文献   

2.
Following 50 years of nuclear production at Mayak PA, sediments in storage reservoirs are significantly contaminated. Dam failure or flooding could potentially transport large amounts of sediments, via rivers, to the Ob estuary and Kara Sea. The objectives of this work were to investigate fresh and seawater remobilization of 137Cs, 50Co, 99Tc, and 90Sr from contaminated Reservoir 10 sediments. Sediments were extracted sequentially using synthetic Techa freshwater, seawater, and chemical reagents with increasing dissolution powers. 137Cs and 90Sr freshwater distribution coefficients (apparent Kd) agreed quite well with published values; values for 99Tc were higher and values for 60Co were lower than expected. In seawater, mean apparent Kd values decreased by 94, 77, 48, and 73% (137Cs, 60Co, 99Tc, and 90Sr, respectively), indicating increased radionuclide mobility. Remobilization in seawater was 5, 15, 1, and 23% of total activities (i.e., releases of 165, 11, 0.3, and 170 kBq kg(-1) d.w.) for 137Cs, 60Co, 99Tc, and 90Sr, respectively. 137Cs and 99Tc were strongly bound to sediments (60% and 80%, respectively). 60Co and 90Sr were more mobile (70% reversibly bound). In conclusion, Mayak Reservoir sediments could potentially contaminate the Ob estuary due to remobilization of sediment-held radionuclides upon contact with seawater.  相似文献   

3.
Concentrations of chlordane, a banned termiticide and pesticide, were examined in recently collected surficial sediment (10 sites) and sediment cores (4 sites) in Long Island Sound (LIS). The highest chlordane concentrations were observed in western LIS, near highly urbanized areas. Chlordane concentrations did not decrease significantly in the past decade when compared to the data collected in 1996, consistent with the observation of near-constant chlordane levels in blue mussel tissues collected during the same time period. Chlordane concentrations in many of the sites exceeded levels above which harmful effects on sediment-dwelling organisms are expected to frequently occur. Chlordane concentrations in two of the four sediment cores showed a peak below the sediment surface, suggesting reduced chlordane inputs in recent years. The lack of a chlordane concentration maximum below the sediment surface in the other two cores, coupled with the lack of a well-defined 137Cs peak, indicated significant sediment mixing. Simulations of 137Cs and 210Pb profiles in sediment cores with a simple sediment-mixing model were used to constrain both the deposition rate and the bioturbation rate of the sediment. Simulations of the chlordane profiles indicated continued chlordane input to LIS long after chlordane was phased out in the U.S. Continued chlordane input and significant sediment mixing may have contributed to the persistent chlordane concentrations in surficial sediment, which poses long-term threats to benthic organisms in LIS.  相似文献   

4.
Vertical distributions of As, Fe, and organic C were determined in dated (210Pb and 137Cs) sediment cores obtained from two adjacent basins (one perennially oxic and the other seasonally anoxic) of an oligotrophic headwater lake where atmospheric deposition is the only input of anthropogenic As. Despite similar sources in the two basins, the As profiles in the sediments differed markedly. Differences include the following: (i) As concentrations increased sharply upward close to the sediment surface in the perennially oxic basin due to scavenging of upward diffusing As by Fe oxyhydroxides, whereas they decreased in the seasonally anoxic basin where As scavenging by Fe oxyhydroxides did not occur, and (ii) the magnitude and position of major subsurface As maxima differed between the two basins. We applied a one-dimensional transport-reaction equation to porewater As concentration profiles obtained at the two sites to estimate sedimentary As concentrations at the time of deposition as well as subsequent addition or removal of As at various sediment depths. By multiplying As concentrations at the time of deposition by sediment mass accumulation rates, we were able to estimate variations in As fluxes at the sediment surface over the last two centuries. These fluxes were then transformed into atmospheric As deposition fluxes by applying a correction for basin-specific processes using the ratio of expected from atmospheric deposition to measured unsupported 210Pb inventories at the sampling sites. The resulting chronological profiles of atmospheric fluxes of As deposition are similar in both basins, and are consistent with both the history of specific markers for coal combustion and direct historical measurements of As in dry and wet atmospheric deposition in rural areas of North America. We conclude that the history of As inputs can be reconstructed from As sedimentary records using appropriate corrections for diagenesis and basin-specific processes.  相似文献   

5.
An analytical method was developed for the trace analysis of 98 semivolatile organic compounds (SOCs) in remote, high-elevation lake sediment. Sediment cores from Lone Pine Lake (west of the Continental Divide) and Mills Lake (east of the Continental Divide) in Rocky Mountain National Park, CO, were dated using 210Pb and 137Cs and analyzed for polybrominated diphenyl ethers (PBDEs), organochlorine pesticides, phosphorothioate pesticides, thiocarbamate pesticides, amide herbicides, triazine herbicides, polychlorinated biphenyls (PCBs), and polycyclic aromatic hydrocarbons (PAHs) using this method. SOC deposition profiles were reconstructed, and deposition half-lives and doubling times were calculated, for U.S. historic-use pesticides (HUPs) and current-use pesticides (CUPs) as well as PBDEs, PCBs, and PAHs. Sediment records indicate that the deposition of CUPs has increased in recent years, while the deposition of HUPs has decreased since U.S. restriction, but has not been eliminated. This is likely due to the revolatilization of HUPs from regional soils, atmospheric transport, and deposition. Differences in the magnitude of SOC sediment fluxes, flux profiles, time trends within those profiles, and isomeric ratios suggest that SOC deposition in high-elevation ecosystems is dependent on regional upslope wind directions and site location with respect to regional sources and topographic barriers.  相似文献   

6.
Over the past five decades, authorized low-level discharges from coastal nuclear facilities have released significant quantities of artificial radionuclides into the marine environment. In northwest Europe, the majority of the total discharge has derived from nuclear reprocessing activities at Sellafield in the United Kingdom and COGEMA-La Hague in France. At the Sellafield site, a significant amount of the discharges has been trapped in offshore fine sediment deposits, and notably in local coastal and estuarine sediments, and much research has been focused on understanding the distribution, accumulation, and reworking of long-lived radionuclides in these deposits. In contrast, there are few high-resolution published data on the vertical distribution of radionuclides in fine-grained estuarine sediments near, and downstream of, COGEMA-La Hague. This paper therefore examines the vertical distribution of a range of anthropogenic radionuclides in dated salt marsh cores from two estuaries, one adjacent to, and the other downstream of, the COGEMA-La Hague discharge point (the Havre de Carteret at Barneville-Carteret and the Baie de Somme, respectively). The radionuclides examined show a vertical distribution which predominantly reflects variations in input from COGEMA-La Hague (albeit much more clearly at Barneville-Carteret than at the Baie de Somme site), and Pu isotopic ratios are consistent with a La Hague, rather than weapons' fallout, source. Because of sediment mixing, the marshes apparently retain an integrated record of the La Hague discharges, rather than an exact reproduction of the discharge history. Sorption of radionuclides increases in the order 90Sr < 137Cs < 60Co < 239,240Pu, which is consistent with Kd values reported in the literature. In general, the radionuclide activities observed at the sites studied are low (particularly in comparison with salt marsh sediments near the Sellafield facility), but are similar to those found in areas of fine sedimentation in the central Channel. These marshes are not major sinks for discharged reprocessing wastes.  相似文献   

7.
The specific activity of 137Cs and 90Sr from the global fallout, as well as from the fallout after the reactor accident at Chernobyl, was determined in flour, bran and straw from wheat, rye, barley and oats as well in the corresponding soils (Cambisol). The results show that the activity of 137Cs, but not of 90Sr, in the plant material was considerably higher in 1986, and still to some extent in 1987, compared to 1982. For 137Cs an 90Sr, as well as for most cereal samples, the activity in the bran and straw was significantly higher than in the flour. Determination of stable potassium and calcium in all samples revealed that this enrichment is, to a large extent, the result of a comparable enrichment of these elements in brans and straw. The plant/soil concentration ratios, averaged over all cereals, were for 137Cs (1982 and 1987): flour 0.026 +/- 0.018; bran 0.079 +/- 0.042; straw 0.055 +/- 0.027. For 90Sr (1982, 1986, and 1987): flour 0.19 +/- 0.095; bran 0.70 +/- 0.23; straw 2.35 +/- 0.82.  相似文献   

8.
A survey on long-lived artificial radionuclides 137Cs and 90Sr in vegetables produced in Finland was carried out in 2009–2010. The mean 137Cs concentrations of all the outdoor vegetables were well below 0.5 Bq kg?1, ranging from <0.01 to 8.15 Bq kg–1 (fresh weight). The highest 137Cs contents were found in potato and root vegetables. The uneven distribution of the 137Cs deposition after the Chernobyl accident in 1986 was still seen in the 137Cs contents of outdoor vegetables. The 137Cs contents of greenhouse vegetables varied from <0.01 to 9.3 Bq kg?1, and the highest concentrations were found in organic lettuce grown in peat pots. The concentrations of 90Sr in the vegetables varied from 0.0087 to 0.17 Bq kg?1 fresh weight. The mean effective dose resulting from 137Cs and 90Sr in vegetables in 2009–2010 was <0.3 µSv a?1 and poses no health risk to the consumers.  相似文献   

9.
Radioactive 137Cs has leaked from underground waste tanks into the vadose zone at the Hanford Reservation in south-central Washington State. There is concern that 137Cs, currently located in the vadose zone, can reach the groundwater. In this study, we investigated whether, and to what extent, colloidal particles can facilitate the transport of 137Cs at Hanford. We used colloidal materials isolated from Hanford sediments. Transport experiments were conducted under variably saturated, steady-state flow conditions in repacked, 20 cm long Hanford sediment columns, with effective water saturations ranging from 0.2 to 1.0. Cesium, pre-associated with colloids, was stripped off during transport through the sediments. The higher the flow rates, the less Cs was stripped off, indicating in part that Cs desorption from carrying colloids was a residence-time-dependent process. Depending on the flow rate, up to 70% of the initially sorbed Cs desorbed from colloidal carriers and was captured in the stationary sediments. Less Cs was stripped off colloids under unsaturated than under saturated flow conditions at similar flow rates. This phenomenon was likely due to the reduced availability of sorption sites for Cs on the sediments as the water content decreased and water flow was divided between mobile and immobile regions.  相似文献   

10.
Using the infrastructure of the National Atmospheric Deposition Program (NADP), numerous measurements of radionuclide wet deposition over North America were made for 167 NADP sites before and after the Fukushima Dai-ichi Nuclear Power Station incident of March 12, 2011. For the period from March 8 through April 5, 2011, wet-only precipitation samples were collected by NADP and analyzed for fission-product isotopes within whole-water and filterable solid samples by the United States Geological Survey using gamma spectrometry. Variable amounts of (131)I, (134)Cs, or (137)Cs were measured at approximately 21% of sampled NADP sites distributed widely across the contiguous United States and Alaska. Calculated 1- to 2-week individual radionuclide deposition fluxes ranged from 0.47 to 5100 Becquerels per square meter during the sampling period. Wet deposition activity was small compared to measured activity already present in U.S. soil. NADP networks responded to this complex disaster, and provided scientifically valid measurements that are comparable and complementary to other networks in North America and Europe.  相似文献   

11.
To date, areas contaminated by radionuclides discharged from the Fukushima Dai-ichi nuclear power plant accident have been mapped in detail. However, size of the radionuclides and their mixing state with other aerosol components, which are critical in their removal from the atmosphere, have not yet been revealed. We measured activity size distributions of (134)Cs and (137)Cs in aerosols collected 47 days after the accident at Tsukuba, Japan, and found that the activity median aerodynamic diameters of (134)Cs and (137)Cs in the first sample (April 28-May 12) were 0.54 and 0.53 μm, respectively, and those in the second sample (May 12-26) were both 0.63 μm. The activity size distributions of these radiocesium were within the accumulation mode size range and almost overlapped with the mass size distribution of non-sea-salt sulfate aerosol. From the analysis of other aerosol components, we found that sulfate was the potential transport medium for these radionuclides, and resuspended soil particles that attached radionuclides were not the major airborne radioactive substances at the time of measurement. This explains the relatively similar activity sizes of radiocesium measured at various sites during the Chernobyl accident. Our results can serve as basic data for modeling the transport/deposition of radionuclides.  相似文献   

12.
In a field investigation (1983-1985) comprising eight places of the most important viticultural regions in the Federal Republic of Germany, the contents of the radionuclides tritium (3H), carbon-14 (14C), strontium-90 (90Sr), and cesium-137 (137Cs) in air, soils, leaves of the vine, grapes and wine were measured and site-specific transfer factors were calculated. Data concerning soil parameters, climatic conditions, cultivation and vinification were collected. The tritium content of all samples was 10 Bq/l water of combustion, independent of location and year. The specific activity of 14C in the atmosphere and in biological material was 0.22 Bq/g carbon, independent of site and year. 90Sr contents of soils fluctuated between 0.7 and 3.5 Bq/kg dry matter. The mean content of leaves was 2 Bq/kg fresh material, of grapes 0.035 Bq/kg and of wine 0.008 Bq/l. 137Cs content of soils fluctuated between 1.3 and 7.9 Bq/kg dry matter. The mean content of leaves was 0.098 Bq/kg fresh material, of grapes 0.021 Bq/kg and of wine 0.0085 Bq/l. A relation between transfer of radionuclides and soil parameters and between the contents of grapes and wine was not recognizable. While cultivar-specific differences were not observed in grapes, red wines contained somewhat more 137Cs than white wines. Transfer factors soil grapes were 0.027 for 90Sr and 0.0057 for 137Cs. Site-specific influences such as soil parameters, climate, cultivation, vinification and differences between years led to a relatively small fluctuation of values. An influence of the nuclear power station Neckarwestheim has not been found in any of the radionuclides.  相似文献   

13.
Quadrupole inductively coupled plasma mass spectrometry has been used to rapidly establish the chronology of recent aquatic sediments via measurements of the activities of 239Pu, 240Pu, and the atom ratio 240Pu/239Pu. Following addition of 0.007 Bq of a 242Pu spike isotope, Pu is leached from 3-20 g aliquots of dry-ashed sediments with HNO3. A selective anion exchanger is used to preconcentrate Pu into approximately 2 mL aliquots, which are directly analyzed using a pneumatic nebulizer and double-pass spraychamber operating at 60 microL/min solution uptake rate. The ICPMS data collection is performed for 10 min per sample. The U concentrations were 0.01-0.05 microg/L in the analyzed solutions, and the interference of 238U1H+ upon 239Pu+ was negligible. The method has been applied to determining Pu activities, inventory, and 240Pu/239Pu in a complete sediment core from Old Woman Creek (Huron, OH). The Pu activity profiles, obtained in approximately 6 h of instrumental measurement time, are in agreement with a y spectrometric 137Cs profile. Peak 239+240Pu and 137Cs activities in the core were 1.60 +/- 0.02 and 47.8 +/- 0.8 Bq/kg, respectively; inventories were 108 +/- 2 Bq/m2 239+240Pu and 2710 +/- 40 Bq/m2 137Cs. Detection limits, based upon the analysis of 20 g samples, were 0.004 Bq/kg 239Pu, 0.012 Bq/kg 240Pu, and 0.012 Bq/kg 239+240Pu. 240Pu/239Pu atom ratios of 0.16-0.19 were obtained for all core intervals containing detectable Pu, which indicates that global fallout is the source of these radionuclides.  相似文献   

14.
137Cesium and other contaminants have leaked from single-shell storage tanks (SSTs) into coarse-textured, relatively unweathered unconsolidated sediments. Contaminated sediments were retrieved from beneath a leaky SST to investigate the distribution of adsorbed 137Cs+ across different sediment size fractions. All fractions contained mica (biotite, muscovite, vermiculatized biotite), quartz, and plagioclase along with smectite and kaolinite in the clay-size fraction. A phosphor-plate autoradiograph method was used to identify particular sediment particles responsible for retaining 137Cs+. The Cs-bearing particles were found to be individual mica flakes or agglomerated smectite, mica, quartz, and plagioclase. Of these, only the micaceous component was capable of sorbing Cs+ strongly. Sorbed 137Cs+ could not be significantly removed from sediments by leaching with dithionite citrate buffer or KOH, but a fraction of the sorbed 137Cs+ (5-22%) was desorbable with solutions containing an excess of Rb+. The small amount of 137Cs+ that might be mobilized by migrating fluids in the future would likely sorb to nearby micaceous clasts in downgradient sediments.  相似文献   

15.
Concentrations of anthropogenic radionuclides were measured in the muscle of marine mammals collected from various locations all over the world, and the global distribution of 137Cs in marine mammals was investigated. 40K was detected in all the specimens of marine mammals with no apparent difference between regions. An anthropogenic radionuclide, 137Cs, was detected in most of the species of marine mammals. With regard to the worldwide distribution of 137Cs, the highest concentration was noticed in the U.K. coast, followed by Lake Baikal, and decreases toward the southern sampling points. A strong positive correlation was observed between 137Cs levels in the muscle of marine mammals and the ambient seawater. Marine mammals feeding on fishes showed a higher concentration factor (CF) for 137Cs than those feeding on cephalopods. To our knowledge, this is the first report on the global distribution of 137Cs and the effect of feeding habits on the CF values of 137Cs in marine mammals.  相似文献   

16.
The macrotidal Severn Estuary (southwestern UK) has received a broad range of industrial discharges since the beginning of the Industrial Revolution. A more recent anthropogenic input to the estuary has been technogenic tritium (specifically organically bound tritium, OBT). This was derived from a specialized industrial laboratory producing custom radiolabeled compounds for life science research and diagnostic testing from 1980 until 2008. While it was generally acknowledged that the radiological impact of the tritium discharges into the Estuary was small, public concern motivated the company and regulatory agencies to commission several research studies from 1998 to 2005 to better understand their environmental impact. This study examined OBT interaction with estuarine sediment by acquiring a broad range of geochemical and sedimentological data from a suite of sediment cores collected from the northern side of the Estuary. Two important observations are that the OBT compounds are strongly bound to the clay/silt fraction of sediment and that the down-core OBT profiles in intertidal and subtidal sediments are broadly similar to the discharge record. Geochemical and chronometric methods (Cu, Pb and Zn elemental profiles, (210)Pb, (137)Cs) provide important corroboration of the OBT record. A key additional piece of evidence that firmly authenticated the established chronology was the discovery of a previously unreported sedimentary marker layer that was generated by a major storm surge that occurred on December 13, 1981. Although this study has provided clear evidence of systematic accumulation of OBT in sedimentary sinks of the region, an estimation of its depositional inventory shows it represents only a small fraction of the total discharge. This modest retention in the principal sedimentary sinks of the Severn Estuary system reflects the particular dynamics of this highly macrotidal sediment starved estuary.  相似文献   

17.
ABSTRACT

Samples of the edible mushroom Boletus edulis Bull. were studied to assess the risk for human health related to their content of the artificial radionuclide 137Cs. Fresh B. edulis carpophores were collected in four undeveloped microhabitats of Lucca province (Tuscany, North-Central Italy). Dried non-cultivated samples coming from this same district and 11 other Italian provinces or European countries were instead purchased fromcommercial sources. Contents of 137Cs, reported as Bq kg?1 dry weight (dw), were measured by γ-spectrometry. The radionuclide concentration varied depending on the gathering site in fresh samples, with 41.8 ± 5.2 Bq kg?1 dw at site 1 (Tosco-Emiliani Apennine) and four-fold less, 12.8 ± 1.3 Bq kg?1 dw, at site 2 (Apuan Alps). Moreover, fresh or dried carpophores from Lucca province displayed among the lowest 137Cs contents in Europe. Average 137Cs levels in all analysed samples were substantially below the legal threshold for edible mushrooms, 600 Bq kg?1 dw. Conclusively, we report that 137Cs amounts in B. edulis depend on both the distance from the Chernobyl accident and multifactorial features of collection sites. We also show that the consumption of European B. edulis does not represent a major health risk with respect to 137Cs radio contamination.  相似文献   

18.
We investigated the impacts of the Deepwater Horizon (DWH) oil spill on two dominant coastal saltmarsh plants, Spartina alterniflora and Juncus roemerianus, in the northern Gulf of Mexico and the processes controlling differential species-effects and recovery. Seven months after the Macondo MC 252 oil made landfall along the shoreline salt marshes of northern Barataria Bay, Louisiana, concentrations of total petroleum hydrocarbons in the surface 2 cm of heavily oiled marsh soils were as high as 510 mg g(-1). Heavy oiling caused almost complete mortality of both species. However, moderate oiling impacted Spartina less severely than Juncus and, relative to the reference marshes, had no significant effect on Spartina while significantly lowering live aboveground biomass and stem density of Juncus. A greenhouse mesocosm study supported field results and indicated that S. alterniflora was much more tolerant to shoot oil coverage than J. roemerianus. Spartina recovered from as much as 100% oil coverage of shoots in 7 months; however, Juncus recovered to a much lesser extent. Soil-oiling significantly affected both species. Severe impacts of the Macondo oil to coastal marsh vegetation most likely resulted from oil exposure of the shoots and oil contact on/in the marsh soil, as well as repeated oiling events.  相似文献   

19.
The transport and deposition (adhesion) kinetics of viable Cryptosporidium parvum oocysts onto ultrapure quartz surfaces in a radial stagnation point flow system were investigated. Utilizing an optical microscope and an image-capturing device enabled real time observation of oocyst deposition behavior onto the quartz surface in solutions containing either monovalent (KCl) or divalent (CaCl2) salts. Results showed a significantly lower oocyst deposition rate in the presence of a monovalent salt compared to a divalent salt. With a monovalent salt, oocyst deposition rates and corresponding attachment efficiencies were relatively low, even at high KCl concentrations where Derjaguin-Landau-Verwey-Overbeek (DLVO) theory predicts the absence of an electrostatic energy barrier. On the other hand, in the presence of a divalent salt, oocyst deposition rates increased continuously as the salt concentration was increased over the entire range of ionic strengths investigated. The unusually low deposition rate in a monovalent salt solution is attributed to "electrosteric" repulsion between the Cryptosporidium oocyst and the quartz surface, most likely due to proteins on the oocyst surface that extend into the solution. It is further proposed that specific binding of calcium ions to the oocyst surface functional groups results in charge neutralization and conformational changes of surface proteins that significantly reduce electrosteric repulsion.  相似文献   

20.
Short-term (approximately monthly) sediment deposition and resuspension rates of surficial bed sediments in two PCB-laden impoundments on the Fox River, WI, were determined in the summer and fall of 1998 using 7Be, a naturally occurring radioisotope produced in the atmosphere. Decay-corrected activities and inventories of 7Be were measured in bed sediment and in suspended particles. Beryllium-7 activities generally decreased with depth in the top 5-10 cm of sediments and ranged from undetectable to approximately 0.9 pCi cm(-3). Inventories of 7Be, calculated from the sum of activities from all depths, ranged from 0.87 to 3.74 pCi cm(-2), and the values covaried between sites likely reflecting a common atmospheric input signal. Activities of 7Be did not correlate directly with rainfall. Partitioning the 7Be flux into "new" and "residual" components indicated that net deposition was occurring most of the time during the summer. Net erosion, however, was observed at the upstream site from the final collection in the fall. This erosion event was estimated to have removed 0.10 g (cm of sediment)(-2), corresponding to approximately 0.5 cm of sediment depth, and approximately 6-10 kg of polychlorinated biphenyls (PCBs) over the whole deposit. Short-term accumulation rates were up to approximately 130 times higher than the long-term rates calculated from 137Cs profiles, suggesting an extremely dynamic sediment transport environment, even within an impounded river system.  相似文献   

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