Anthropogenic Radionuclides in the Caspian Sea

Analysis and interpretation of the distribution of anthropogenic radionuclides ⁹⁰Sr, ¹³⁷Cs, and ^239,240Pu in the Caspian Sea water are presented. These radionuclides are shown to be of environmental importance and to be useful for studying water mass dynamics.     

Distribution of 137Cs in the Lena River estuary-Laptev Sea system.

Surface sediment samples in the Laptev Sea have average 137Cs content of 7.1 Bq kg(-1), a value intermediate between that of the western Kara Sea (23 Bq kg(-1) and the East Siberian Sea (4.2 Bq kg-'). Both surface sediment content and sediment inventory of 137Cs in the Laptev Sea sediments show significant variability, and the influence of a variety of environmental factors.137Cs concentrations in the Laptev Sea surface sediments range from 0.8 to 16 Bq kg(-1). There is a marked increase in 137Cs content of surface sediment samples collected near the Lena River delta, and a local enrichment in the 137Cs inventories at these sites is also evident. Fine-grained mixed-layer illite/ smectite rich sediments in the estuary provide effective adsorption sites to fix 137Cs, in spite of desorption processes associated with low salinities in estuarine mixing. The Lena River-Laptev Sea mixing zone is a major site of sea-ice production. River and shelf sediments are incorporated into sea-ice formed in this region (Holmes and Creager, 1974). The irregular 137Cs activity profiles of the Lena River estuary cores indicate disturbance or removal of 137Cs-laden sediments via sea-ice related processes. Lena River and Estuary sediments may have served as a secondary source (i.e. other than direct fallout) of 137Cs in sea-ice. North-east of the Lena River estuary, sediment contains a thin layer of 137Cs-bearing material over an erosion surface. The 137Cs-laden surface layer may be the result of transient deposition of estuarine sediments being delivered by sea-ice or spring floods.     

Rating Water Quality in Sevastopol Bay by the Fluxes of Pollutant Deposition in Bottom Sediments

Sevastopol Bay is used as an example for the development of criteria for rating anthropogenic impact by elimination fluxes from the water area of post-Chernobyl (⁹⁰Sr, ¹³⁷Cs, ^239,240Pu) and natural (²¹⁰Pо) radionuclides, as well as mercury and organochlorine compounds. The differentiation of the bay water area into zones with different biogeochemical conditions and the balance approach to interpreting field observation data were used to assess the conditioning capacity of Sevastopol Bay ecosystem for conservative radioactive and chemical substances by elimination fluxes of pollutants into aqueous depot, which is the open part of the Black Sea and into the geological depot, i.e., its bottom sediment stratum.     

Organic carbon flow in the Ob, Yenisey Rivers and Kara Sea of the Arctic region

Stable carbon isotope and elemental C/N ratios of the organic fraction of a set of samples along a transect in the Ob and Yenisey Rivers into the Kara Sea in the Arctic were measured. Previously, the concentrations of 239,240Pu and 137Cs in these same samples had been determined. The coupled measurements were carried out to assess possible connectivity between organic carbon flow into the Kara Sea and transport of radioactive nuclides in this marine environment. Organic carbon flow into the Kara Sea is influenced significantly by terrigenous sources carried by the Ob and Yenisey Rivers. The carbon isotope-organic carbon relationship provides evidence that a rich source of terrigenous carbon exists in the riverine system. A weak, but significant relationship between stable carbon isotope ratio and 137Cs suggests that most of the 137Cs is derived from riverine particles, as compared to Pu which is also derived from in situ scavenging within the water column.     

Accumulation,solid partitioning and remobilisation of 99Tc in subtidal and intertidal sediments in the Irish Sea

Recent studies have shown that accumulation of ⁹⁹Tc in seabed sediments labelled by authorised radioactive liquid discharges into the NE Irish Sea from the Sellafield reprocessing complex is greater than previously thought. In this paper, new data on ⁹⁹Tc concentration profiles in subtidal and intertidal sediments from the eastern and western Irish Sea are provided with a view to elucidating the processes responsible for the incorporation and retention of ⁹⁹Tc in the seabed. The data show that substantial amounts of ⁹⁹Tc have accumulated in the fine-grained subtidal sediments off the Cumbrian coast, particularly after increased releases from Sellafield following the commissioning of the Enhanced Actinide Removal Plant (EARP) in 1994. In all the cores taken in this area, ⁹⁹Tc has been found to be present to depths in excess of 30 cm. Analysis of ¹³⁷Cs and ²⁴¹Am profiles, together with other supporting geochemical data, show a high degree of homogenisation of the sediments down to these depths as a result of physical and biological processes, and confirm that incorporation of ⁹⁹Tc into the sediment compartment is actually the result of mixing and reworking, rather than active sediment accumulation. In contrast, active deposition of material transported from this mixed pool of sediment appears to be the dominant mechanism controlling ⁹⁹Tc profiles in intertidal areas close to the Sellafield discharge outfall.Data obtained from the analysis of subtidal sediment cores from the western Irish Sea mud basin suggest that similar mixing processes to those occurring in the subtidal sediments of the eastern Irish Sea are also active in this area. Time-series data on ⁹⁹Tc concentrations in surficial sediments from this basin, gathered in the period 1988–2004, inclusive, show a clear increase in concentrations, by a factor of ～2, between samples collected pre-EARP and post-EARP. The constancy of ⁹⁹Tc concentrations in surface sediments throughout the 1980s and the early-1990s suggests that little redissolution and export of ⁹⁹Tc occurred over this extended period. A similar observation applies to the post-EARP period, when concentrations remained relatively constant despite the reported steady decrease in ⁹⁹Tc concentrations in the overlying waters.This apparent lack of remobilisation is consistent with data from sequential extraction analyses, which indicate that the bulk of the ⁹⁹Tc is strongly bound to non-labile geochemical phases, with only a small proportion associated with exchangeable and acido-soluble phases. Further, these analyses show that ⁹⁹Tc is not associated with oxygen-sensitive and highly-reactive acid-volatile sulphides (AVS) to any significant extent.     

Radionuclide adsorption to sediments from nuclear waste dumping sites in the Kara Sea

Environmental parameters (salinity, sediment concentration, equilibration time) affecting radionuclide partitioning between sediment and seawater were experimentally investigated for Kara Sea sediments collected from nuclear waste dumping sites in Abrosimov and Stepovogo Bays off Novaya Zemlya. Adsorption kinetics were examined and the influence of salinity and sediment concentration were evaluated over the range of concentrations expected in the bays for the following radionuclides: ^{110 m}Ag; ²⁴¹Am; ¹⁰⁹Cd; ⁶⁰Co; ⁵⁷Co-cobalamine; ¹³⁴Cs; ¹⁵²Eu; ⁵⁴Mn; ¹³³Ba; ¹⁰⁶Ru; and ⁸⁵Sr. The major findings of this investigation are that 1. radionuclide distribution coefficients (K_ds) were most sensitive to variations in sediment character (²⁴¹Am, ⁶⁰Co, ¹⁰⁹Cd) and concentration (⁵⁷Co-cobalamine, ⁸⁵Sr, and ¹³³Ba), 2. distribution coefficients generally decreased with increasing sediment concentration and 3. fast adsorption kinetics (near equilibrium ≈1 day) were observed only for ¹³⁷Cs and ^{110 m}Ag. The observed differences in K_ds for sediments from the two dumpsites exemplifies the importance of undertaking site-specific determinations of K_ds. For purposes of confining radioactive wastes to the dumpsites in Stepovogo and Abrosimov Bays, the findings of this study indicate that based on sediment character alone, Stepovogo Bay will be more effective at retaining radionuclides than Abrosimov Bay. This is unfortunate since less radioactive waste resides in Stepovogo Bay (0.6 PBq) than in Abrosimov Bay (1.4 PBq).     

Modelling temporal trends of 137Cs and 99Tc concentrations in Fucus vesiculosus from the eastern Irish coastline

Time series of ¹³⁷Cs and ⁹⁹Tc activity concentrations in the brown seaweed Fucus vesiculosus and seawater, gathered at three locations on the eastern Irish coastline during the period 1988-2008, have been modelled using a novel approach incorporating a variable uptake rate in the seaweed. Seasonal variations in the time series, identified using spectral analysis, were incorporated into the model which was used to determine transfer kinetic parameters and to predict ¹³⁷Cs and ⁹⁹Tc concentrations in seaweed, as influenced by levels in ambient seawater. An optimisation method combining evolutionary and grid search minimisation techniques was adopted to determine the best values for the model parameters, from which concentration factors (CF) and biological half-lives (tb_1/2) for ¹³⁷Cs and ⁹⁹Tc in F. vesiculosus were calculated. CF values of 170-179 and 1.1 × 105 l kg⁻¹ (dry weight) were obtained for ¹³⁷Cs and ⁹⁹Tc, respectively, while the corresponding tb_1/2 values were 39-47 and 32 days, respectively.     

Geochronological reconstruction of Cs transport from the Coruh river to the SE Black Sea: comparative assessment of radionuclide retention in the mountainous catchment area

The deposition record of ¹³⁷Cs was traced in the SE Black Sea sediments adjacent to the Coruh river mouth in comparison with the earlier studied chronology of ¹³⁷Cs deposition in front of the Danube delta (NW Black Sea). In both cases, the ¹³⁷Cs profiles showed two subsurface peaks attributable to maximum fallout of ‘bomb’ and Chernobyl radionuclides. The Coruh profile revealed a larger contribution of ‘bomb’ ¹³⁷Cs in comparison with the Chernobyl input, suggesting different coverage of NW and SE Black Sea regions with the Chernobyl fallout. The ¹³⁷Cs-derived dating showed that maximum deposition of particulate bound ¹³⁷Cs in sediments adjacent to the Coruh river mouth was delayed for 14 yr relative to date of Chernobyl accident, reflecting a buffer effect of the watershed soils. This transit time is 3 times longer than in the Danube catchment area, indicating a difference in retention processes in these mountainous (Coruh) and lowland (Danube) river basins. The ¹³⁷Cs profile in Coruh sediments showed penetration of ¹³⁷Cs to much greater depth than would be expected from ¹³⁷Cs fallout chronology, suggesting the sediment mixing rate of 1.3 cm² yr⁻¹. This value was used to evaluate deposition chronology of ¹³⁷Cs, applying the model developed for pulse fallout case. Comparing the measured and modelled data has allowed differentiation of the flood-induced discharge of the ¹³⁷Cs-containing suspended matter and the slower transit of eroded soil particles from the contaminated catchment areas. The obtained results may be used for the prediction of period when the pollutants, deposited over the river basins, can reach the Black Sea.     

Modern (<100 years) sedimentation in the Taiwan Strait: Rates and source-to-sink pathways elucidated from radionuclides and particle size distribution

A large number of sediment cores collected during 2005-2010 from the Taiwan Strait were analyzed for radionuclides (²¹⁰Pb, ¹³⁷Cs and ⁷Be) to elucidate sedimentation dynamics in this all-important gateway linking two largest marginal seas in the western Pacific (namely, the South China Sea and the East China Sea). Apparent sediment accumulation rates derived from ²¹⁰Pb and ¹³⁷Cs profiles vary from <0.1 to >2 cm/yr, averaging ∼0.4 cm/yr and showing a spatial pattern closely related to hydrodynamics and sediment source-to-sink pathways. Spatial-temporal variation of ⁷Be activity in surface sediments off Taiwan’s west coast indicates episodic deposition of flood layers and their mobility from river estuaries toward the north. In conjunction with particle size distribution in surface sediments and the structure of sediment strata revealed by sub-bottom echo images; the radionuclide data can be used to outline three different sediment source-to-sink dispersal systems. Based on sediment loads of surrounding rivers and the distribution of sediment accumulation rates, lateral transport is required to account for the budget and size distribution of sediments in the strait.     

Plutonium,radiocesium and radiocobalt in sediments of the Hudson River estuary

Anthropogenic radionuclides have reached the Hudson estuary as global fallout from nuclear weapons testing and through local releases from commercial nuclear reactors. Significant activities of²³⁸Pu and^239,240Pu (fallout-derived),¹³⁴Cs and⁶⁰Co (reactor-released), and¹³⁷Cs (derived from both sources), have accumulated in the sediments throughout the estuary, with the primary zone of accumulation near the downstream end of the system in New York harbor. The estuary appears to have trapped nearly all of the^239,240Pu delivered as fallout, and consequently, ocean dumping of dredged harbor sediment is currently the primary means for the net transport of these nuclides to coastal waters. In contrast, only 10–30% of the¹³⁷Cs,¹³⁴Cs and⁶⁰Co delivered to the estuary have been retained on the fine particles which accumulate at a rapid rate in the harbor.The primary factors which have governed the distribution of anthropogenic radionuclides in Hudson sediments are: (1) spread of fine particles labeled with both fallout and reactor nuclides throughout the axis of the estuary, (2) differences in timing of the peak fallout years (1962–1964) and years of maximum reactor releases (1971–1972), (3) large variations in sediment accumulation rates, ranging from a few millimeters per year or less to many tens of centimeters per year, (4) appreciable desorption of¹³⁷Cs and¹³⁴Cs from particles at higher salinities, and (5) possible enhanced desorption of⁶⁰Co at higher salinities (relative to¹³⁴Cs and¹³⁷Cs) which may be associated with the release of reduced manganese from the harbor sediments.     

(235)U, (238)U, (232)Th, (40)K and (137)Cs activity concentrations in marine sediments along the northern coast of Oman Sea using high-resolution gamma-ray spectrometry

The natural radioactivity levels in sediment samples of the northern coast of Oman Sea, covering the coastal strip from Hormoz canyon to Goatr seaport, as the first time has been determined. The results of measurements will serve as background reference level for Oman Sea coastlines. Sediments from 36 coastal and near shore locations were collected for analysis. Analysis on the collected samples were carried out to determine (235)U, (238)U, (232)Th, (40)K and (137)Cs using two high purity germanium detectors with 38.5% and 55% relative efficiencies. The concentration of (235)U, (238)U, (232)Th, (40)K and (137)Cs in sediment samples ranged between 1.01 and 2.87Bq/kg, 11.83 and 22.68Bq/kg, 10.7 and 25.02Bq/kg, 222.89 and 535.07Bq/kg and 0.14 and 2.8Bq/kg, respectively. The radium equivalent activity was well below the defined limit of 370Bq/kg. The external hazard indices were found to be less than 1, indicating a low dose.     

Summary of IAEA-MEL's investigation of Kara Sea radioactivity and radiological assessment

IAEA-MEL participated in five expeditions to the Kara Sea with the aim of assessing the radiological consequences of dumped radioactive wastes in the Novaya Zemlya Bays and Trough. The programme included sampling, in-situ underwater investigations, laboratory analyses of water, sediment and biota samples, the development of a marine radioactivity database, modelling and radiological assessment, the organization of intercomparison exercises and the evaluation of distribution coefficients. Radiometric investigations have shown that no radiologically significant environmental contamination has occurred. Leakages which have led to locally increased levels of radionuclides in sediment have only been observed in Stepovoy and Abrosimov Bays. Computer modelling results suggest that only radiological effects on local and regional scales may be of importance. The global radiological impact of the disposals in the Arctic Seas will be negligible.     

Floodplain sedimentation rates in an alpine watershed determined by radionuclide techniques

Vertical profiles of the activities of ¹³⁷Cs and ²¹⁰Pb were measured on floodplain sediment cores and upland soil cores along the Soda Butte Creek and the Yellowstone River to determine floodplain sedimentation rates. The position of mine tailings from a 1950 impoundment failure was used as a stratigraphic marker to estimate the sedimentation rates and to make comparisons with rates provided by radionuclide‐based methods. Mass accumulation (sedimentation) rates calculated from the position of the mine tailings ranged from 0·00 to 0·17 g cm^?2 yr^?1 and were in good agreement with sedimentation rates calculated from the inventories of ¹³⁷Cs and ²¹⁰Pb. Sedimentation rates calculated from the position of the ¹³⁷Cs peak generally overestimated the sedimentation rates, probably because of increased downward migration of ¹³⁷Cs caused by the low pH of water moving through the mine tailings or the high permeability of floodplain sediments relative to upland reference soils. This study demonstrates that the ¹³⁷Cs and ²¹⁰Pb inventory methods for determining sedimentation rates can be applied to an alpine floodplain where sedimentation events are episodic and where orographic effects on precipitation generate strong downstream gradients in the delivery of atmospheric radionuclides. Copyright © 2007 John Wiley & Sons, Ltd.     

Concentrations of 137Cs, 90Sr, 108m Ag, 239+240 Pu and atom ratio of 240Pu/239Pu in tanner crabs, Chionoecetes japonicus and Chionoecetes opilio collected around Japan

The anthropogenic radionuclides, ¹³⁷Cs, ⁹⁰Sr, ^108mAg, ^239+240Pu, were measured in two Chionoecetes species, red queen crab (Chionoecetes japonicus) and snow crab (Chionoecetes opilio) collected around Japan during 1996–2007. There was no increase in the concentrations of these radionuclides and no large variation of the atom ratio of ²⁴⁰Pu/²³⁹Pu during this research period. These results indicated that the source of the radionuclides was not the radioactive wastes dumped by the former USSR and Russia and originated from past nuclear weapon tests. The higher atom ratio in the crab species than that from global fallout would be contributed by the Pacific Proving Grounds close-in fallout. The variability of the concentration of radionuclides in the crab species would result from the variability of the composition and quantity in the diet. However, the decrease in the concentration of radionuclides with sampling depth would depend on the concentration in the seawater and diet.     

Radionuclide ratios in wet and dry deposition samples from June 1976 through December 1977

²³⁸Pu,²³⁹Pu and¹³⁷Cs in rain and dry fallout and⁹⁰Sr in rain samples were measured at Woods Hole, Massachusetts, from June 1976 through December 1977. The dry fallout was estimated to be about 7.8% of the total deposition of²³⁹Pu and¹³⁷Cs.²³⁹Pu/¹³⁷Cs ratios, almost constant at about 0.011 in rain or dry fallout, February through December 1977, suggested that fractionation between the refractory and volatile radionuclides is insignificant in stratospheric fallout. This supports the idea of regional homogeneity of radionuclide ratios in fallout.     

Radiocesium reaction with illite and organic matter in marine sediment

The mineralogical effect on the (137)Cs reaction with marine sediment has not been systematically studied yet, even though illite has been known to adsorb Cs preferentially on its frayed edge sites in a low Cs concentration. Ninety-three marine sediment samples were collected near Yangnam, Korea for quantitative X-ray-diffraction (XRD), gamma-ray, and total organic carbon (TOC) analysis. Illite content was in the range of 0-23 wt.% and those of (137)Cs and TOC were minimum detectable activity (MDA) approximately 7.19 Bq/kg-dry and approximately 3.32%, respectively. The illite content in the marine sediment showed a good relationship with the (137)Cs content (R(2)=0.69), but with an increase in the illite content, the relationship became less linear. This trend can be clearly shown in two groups of samples with different size fractions (< and >5Mdvarphi). For the samples of larger particle sizes (low contents of illite), the relationship is linear, but for the samples of the smaller particle sizes (high illite content) it is less linear with a decreased slope, indicating that increase in illite content does not significantly contribute to the fixation of (137)Cs in marine sediment. Rather, the TOC has a more linear relationship with (137)Cs content with no slope change in all particle size ranges. This may indicate that humic materials in marine sediment block the access of (137)Cs to the frayed edge site and reduces the adsorption of (137)Cs on illite and that the organic materials in marine sediment play more important roles in adsorbing Cs than illite.     

Altitude-dependent distribution of ~(137)Cs in the environment:a case study of Aragats massif,Armenia

This paper considers the distribution of technogenic 137Cs and naturally occurring radionuclides:238 U,232 Th and40 R concentrations in soils and 137Cs in atmospheric dry depositions by altitudinal belts of the Aragats mountain massif,Republic of Armenia.Undisturbed soil samples were collected at altitudes from 1000 to 3200 m.For the determination of geochemical variability,two soil sampling campaigns were undertaken.Atmospheric dry depositions were sampled from five stations at1100-3200 m collected onto organic fiber filters between June and December 2016.137Cs activity was measured using a high-purity Germanium detector coupled to a multichannel analyzer(Canberra).Results indicated that specific activity of 137Cs in soils at 1000 m is495-528 Bq m^-2,andat3200 mis10,500-11,470 Bq m^-2.No correlation observed for 137Cs versus naturally occurring radionuclides,which varies in distribution by altitude.Specific activities of 137Cs in dry atmospheric depositions varies from 1.06 at 846 m to2.37 Bq m^-2 per quarter at 3200 m and increases as the altitude increases.Activities of 137Cs in soil and dry atmospheric deposition correlated significantly,and 137Cs activity in soils and atmospheric dry depositions decrease as the absolute altitude decreases.The 50-year effective dose from exposure to 137Cs fallout varies with altitude from 0.007 to 1.42 m Sv.     

Can channel banks be the dominant source of fine sediment in a UK river?: an example using 137Cs to interpret sediment yield and sediment source

Cultivated fields have been shown to be the dominant sources of sediment in almost all investigated UK catchments, typically contributing 85 to 95% of sediment inputs. As a result, most catchment management strategies are directed towards mitigating these sediment inputs. However, in many regions of the UK such as the Nene basin there is a paucity of sediment provenance data. This study used the caesium‐137 (¹³⁷Cs) inventories of lake and floodplain cores as well as the ¹³⁷Cs activities of present day sediment to determine sediment provenance. Sediment yields were also reconstructed in a small lake catchment. Low ¹³⁷Cs inventories were present in the lake and floodplain cores in comparison to the reference inventory and inventories in cores from other UK catchments. Caesium‐137 activities in the present day sediments were low; falling close to those found in the channel bank catchment samples. It was estimated that 60 to 100% of the sediment in the Nene originated from channel banks. Pre‐1963 sediment yields were approximately 11.2 t km^?2 yr^?1 and post‐1963 was approximately 11.9 t km^?2 yr^?1. The lack of increased sediment yield post‐1963 and low sediment yield is unusual for a UK catchment (where a yield of 28 to 51 t km^?2 yr^?1 is typical for a lowland agricultural catchment), but is explained by the low predicted contribution of sediment from agricultural topsoils. The high channel bank contribution is likely caused by the river being starved of sediment from topsoils, increasing its capacity to entrain bank material. The good agreement between the results derived using cores and recently transported sediments, highlight the reliability of ¹³⁷Cs when tracing sediment sources. However, care should be taken to assess the potential impacts of sediment particle size, sediment focusing in lakes and the possible remobilization of ¹³⁷Cs from sedimentary deposits. Copyright © 2016 John Wiley & Sons, Ltd.     

The accumulation of radiocesium in coarse marine sediment: effects of mineralogy and organic matter

The controlling factors affecting the accumulation of (137)Cs in marine sediment have not been investigated in detail, especially in coarse grained sediment. Eighty eight coarse marine sediment samples near Wuljin, Korea, were characterized by quantitative X-ray-diffraction (XRD), gamma-ray, and total organic carbon (TOC) analysis. Those factors were then compared. The grain size was in the range of -0.48 to 3.6Mdphi corresponding to sand grains. TOC content was in the range of 0.06-1.75%, and the concentration of (137)Cs was 相似文献   

Distribution of radioactive pollution of 238U, 232Th, 40K and 137Cs in northwestern coasts of Persian Gulf, Iran

A reconnaissance study has been made of the distribution of 238U, 232Th, 40K and 137Cs and geochemical features in soils and sediments samples at various locations in the northwestern coast of Persian Gulf. Activity concentration levels due to radionuclides were measured in 30 soil and sediment samples collected from this region. From the measured spectra, activity concentrations were determined for 40K (range from 146 to 500 Bq kg(-1)), 137Cs (from 5 to 20 Bq kg(-1)), 238U (from 21 to 65 Bq kg(-1)) and 232Th (from 15 to 45 Bq kg(-1)) with lowest limit detection (LLD) of 68, 3.2, 4.3 and 4.3 Bq kg(-1), respectively. The dose rate from ambient air at the soil ranges was between 19 and 58 nGy h(-1) with an average of 37.41+/-9.66 nGy h(-1).