Inventories of Pu, Cs, and excess Pb in sediments from freshwater and brackish lakes in Rokkasho, Japan, adjacent to a spent nuclear fuel reprocessing plant

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

Determining the Chernobyl impact on sediments of a pre-Alpine lake with a very comprehensive set of data

Man-made and natural radionuclides in Lake Wallersee were determined in the pre-Alpine environment at the northern slope of the Alps, which was heavily affected by the Chernobyl fallout in May 1986. The objective of this study was to get knowledge of location and quantity of man-made radionuclide input (especially (137)Cs) generated in the Chernobyl accident to lake sediments. Eleven sediment cores were sampled and activity depth profiles of (137)Cs and (210)Pb were determined with 5mm depth-resolution. The Chernobyl fallout produced an extreme (137)Cs peak in the sediment cores providing an excellent time marker. The chronological interpretation of deeper sediment layers was done by radiochemical analysis of (90)Sr and (239+240)Pu, which were released during atmospheric weapons' tests in the 1950s and 1960s. This allowed a complete chronological analysis of the sediment cores with a very compact set of data.     

Cs, Pu concentrations and the Pu/Pu atom ratio in a sediment core from the sub-aqueous delta of Yangtze River estuary

A sediment core collected from the sub-aqueous delta of the Yangtze River estuary was subjected to analyses of ¹³⁷Cs and plutonium (Pu) isotopes. The ¹³⁷Cs was measured using γ-spectrometry at the laboratories at the Nanjing University and Pu isotopes were determined with Accelerator Mass Spectrometry (AMS), measurements made at the Australian National University. The results show considerable structure in the depth concentration profiles of the ¹³⁷Cs and ^239+240Pu. The shape of the vertical ¹³⁷Cs distribution in the sediment core was similar to that of the Pu. The maximum ¹³⁷Cs and ^239+240Pu concentrations were 16.21 ± 0.95 mBq/g and 0.716 ± 0.030 mBq/g, respectively, and appear at same depth. The average ²⁴⁰Pu/²³⁹Pu atom ratio was 0.238 ± 0.007 in the sediment core, slightly higher than the average global fallout value. The changes in the ²⁴⁰Pu/²³⁹Pu atom ratios in the sediment core indicate the presence of at least two different Pu sources, i.e., global fallout and another source, most likely close-in fallout from the Pacific Proving Grounds (PPG) in the Marshall Islands, and suggest the possibility that Pu isotopes are useful as a geochronological tool for coastal sediment studies. The ¹³⁷Cs and ^239+240Pu inventories were estimated to be 7100 ± 1200 Bq/m² and 407 ± 27 Bq/m², respectively. Approximately 40% of the ^239+240Pu inventory originated from the PPG close-in fallout and about 50% has derived from land-origin global fallout transported to the estuary by the river. This study confirms that AMS is a useful tool to measure ²⁴⁰Pu/²³⁹Pu atom ratio and can provide valuable information on sedimentary processes in the coastal environment.     

Determining floodplain sedimentation rates using Cs in a low fallout environment dominated by channel- and cultivation-derived sediment inputs, central Queensland, Australia

Fallout ¹³⁷Cs has been widely used to determine floodplain sedimentation rates in temperate environments, particularly in the northern hemisphere. Its application in low fallout, tropical environments in the southern hemisphere has been limited. In this study we assess the utility of ¹³⁷Cs for determining rates of floodplain sedimentation in a dry-tropical catchment in central Queensland, Australia. Floodplain and reference site cores were analysed in two centimetre increments, depth profiles were produced and total ¹³⁷Cs inventories calculated from the detailed profile data. Information on the rates of ¹³⁷Cs migration through local soils was obtained from the reference site soil cores. This data was used in an advection–diffusion model to account of ¹³⁷Cs mobility in floodplain sediment cores. This allowed sedimentation rates to be determined without the first year of detection for ¹³⁷Cs being known and without having to assume that ¹³⁷Cs remains immobile following deposition. Caesium-137 depth profiles in this environment are demonstrated to be an effective way of determining floodplain sedimentation rates. The total ¹³⁷Cs inventory approach was found to be less successful, with only one of the three sites analysed being in unequivocal agreement with the depth profile results. The input of sediment from catchment sources that have little, or no, ¹³⁷Cs attached results in true depositional sites having total inventories that are not significantly different from those of undisturbed reference sites.     

210Pb as a tool for establishing sediment chronologies: examples of potentials and limitations of conventional dating models

For aquatic sediments, the use of ²¹⁰Pb originating from the decay of atmospheric ²²²Rn is a well-established methodology to estimate sediment ages and sedimentation rates. Traditionally, the measurement of ²¹⁰Pb in soils and sediments involved laborious and time-consuming radiochemical separation procedures. Due to the recent development of advanced planar (‘n-type’) semi-conductors with high efficiencies in the low-energy range which enable the gamma-spectrometric analysis of the 46.5 keV decay line of ²¹⁰Pb, sediment dating using this radionuclide has gained renewed interest.In this contribution, potentials and limitations of the ²¹⁰Pb methodology and of the models used for estimating sediment ages and sedimentation rates are discussed and illustrated by examples of freshwater and marine sediments. Comparison with the use of ¹³⁷Cs shows that the information which may be gained by these two tracers is complementary. As a consequence, both radionuclides should be used in combination for dating of recent sediments. It is shown that for various sedimentation regimes additional information from other sources (e.g. sediment lithology) may be needed to establish a reliable chronology. A strategy for sediment dating using ²¹⁰Pb is recommended.     

Recent Cs deposition in sediments of Admiralty Bay, Antarctica

Cesium-137, radium-226 and lead-210 profiles of a 25 cm sediment core give an indication of recent changes in land-ocean interactions at a polar coastal environment (Admiralty Bay, King George Island, Antarctica). The linear sedimentation accumulation rate at the study site calculated from the unsupported ²¹⁰Pb profile was 6.7 mm/year from 1965 to 2005. A 3.5-fold increase in ¹³⁷Cs concentrations was observed in the top layer of this sediment core. This sharp increase seems to indicate a recent redistribution of fallout radionuclides previously deposited on soil, vegetation and snow. These results imply enhanced land-ocean interactions at this site likely as a result of climate change. Because our results are based on a single core, additional investigations are needed to confirm our observations.     

Accumulation of Cs in puddle sediments within urban ecosystem

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

Estimating the date corresponding to the horizon of the first detection of 137Cs and 239+240Pu in sediment cores

The anthropogenic bomb fallout nuclides 137Cs and plutonium isotopes (240Pu, 239Pu) are important chronometers for the determination of recent sediment accumulation rates using sediment cores collected from various water bodies. One of the crucial time horizons used to date sediment core profiles corresponds to the date of first detection of these nuclides. Although atmospheric nuclear testing began during the mid-1940s, the year corresponding to a nuclide's first detection when measured in 2006 depends on a number of factors including fallout history, radioactive half-life, gamma/alpha detection limits, geographic latitude and the accumulated thickness of the sediment section. This paper reports estimations of the year of first detection in sediment profiles of fallout 137Cs and Pu measured by gamma and alpha spectrometry, respectively. We find that for the latitude 30-40 degrees south of the equator the year of first detection for 137Cs is 1955. The date is earlier in the northern hemisphere due to higher fallout rates. Due to better measurement sensitivity first detection of Pu is generally earlier than 137Cs by 1-2 years.     

Distribution of radionuclides in the guano sediments of Xisha Islands, South China Sea and its implication

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.     

Distribution and inventories of fallout radionuclides (239+240Pu, 137Cs) and 210Pb to study the filling velocity of salt marshes in Doñana National Park (Spain)

Within an extensive multinational and multidisciplinary project carried out in Do?ana National Park (Spain) to investigate its preservation and regeneration, the filling velocity of the salt marshes has been evaluated through the calculation of their average sediment accumulation rates. (239+240)Pu and (137)Cs from weapons testing fallout and total (210)Pb distribution profiles and inventories have been determined in some of the most characteristic zones of the park, namely, the ponds (or "lucios") and the waterjets (or "ca?os"). Plutonium inventories range from 16 to 101 Bq m(-2), (137)Cs values fluctuate between 514 and 3,758 Bq m(-2) and unsupported (210)Pb values comprise between 124 and 9398 Bq m(-2). Average sedimentation rates range from 3 to 5 mm y(-1) (1952-2002). These data are higher than those obtained by carbon dating for the period 6,500 AD-present, estimated as 1.5-2 mm y(-1), suggesting an increase in the accumulation of sediments and the alteration of the park's hydrodynamics caused by the re-channeling of the major rivers feeding the salt marshes.     

Comparative trends and seasonal variation of ⁷Be, ²¹⁰Pb and ¹³⁷Cs at two altitude sites in the central part of France

The atmospheric concentrations of ¹³⁷Cs, ²¹⁰Pb, and ⁷Be were measured over a three-year period at two research stations located less than 12 km apart and at different altitudes (puy de Dôme, 1465 m a.s.l. and Opme, 660 m a.s.l., France). Seasonal trends in all radionuclides were observed at both stations, with high concentration measured during the summer and low concentrations during the winter. The ²¹⁰Pb concentrations at both stations were similar to each other. Higher concentrations of both ⁷Be and ¹³⁷Cs were measured at puy de Dôme than at Opme. These observations can be explained by the stratospheric and upper tropospheric sources of ⁷Be and the long-range transportation of ¹³⁷Cs at high altitudes. Air mass origins during sampling periods were classified into several groups by their route to the stations (marine, marine modified, continental and mediterranean). We observed that ⁷Be concentrations were constant regardless of the air mass origins, unlike ¹³⁷Cs and ²¹⁰Pb concentrations that increased when influenced by continental air masses. Higher ⁷Be concentrations were observed when air masses were arriving from the upper troposphere than from the boundary layer, the opposite was observed for ¹³⁷Cs. The temporal trend in concentrations of ⁷Be shows good agreement with previous modelling studies suggesting that there is a good understanding of its sources and the atmospheric vertical mixing of this radionuclide. The sources and mixing of ²¹⁰Pb, however, seem to be more complex than it appeared to be in previous modelling studies.     

Pu/Cs ratios in the water column of the North Pacific: a proxy of biogeochemical processes

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.     

Time pattern of off-site plutonium deposition from rocky flats plant by lake sediment analyses

A sediment core from a lake downwind of the Rocky Flats Plant, where nuclear weapons components are produced, was used to reconstruct a time pattern of off-site plutonium deposition. Core sections were dated by analyses of ¹³⁷Cs, ^239,240Pu, ²³⁸Pu, and ²⁴¹Am fallout from nuclear testing and ²³⁸Pu fallout from a satellite failure. A peak in transuranic concentrations occurred in late 1969 which was attributable to the Plant. This was confirmed by mass isotopic analysis of plutonium isotopes in selected core segments where the global fallout and Plant contributions could be differentiated. The 18 nCi ^239,240Pu per m² from the Plant that had accumulated in the sediment is reasonable when compared to soil analyses.     

137Cs and excess 210Pb deposition patterns in estuarine and marine sediment in the central region of the Great Barrier Reef Lagoon, north-eastern Australia

This paper focuses on the distribution of 137Cs and 210Pb(xs) in 51 estuarine and marine sediment cores collected between the Upstart Bay and Rockingham Bay in the Great Barrier Reef Lagoon, north-eastern Australia. Historical records of 210Pb(xs) and 137Cs atmospheric deposition and present day terrestrial inventories in north-eastern Australia are presented. 210Pb(xs) and 137Cs fluxes measured on suspended sediments in the Burdekin River are considered to be a source of recent inputs of these nuclides to the nearshore region of this part of the Great Barrier Reef. Direct correlations between sediment nuclide inventories, maximum detectable depths, and sediment mass accumulation rates (MARs), calculated using both 137Cs and 210Pb(xs), are explored. In relation to inventories of 210Pb(xs), 60% of atmospheric fallout 137Cs appears to be missing from the sediments. The reasons for these differences in two tracers, primarily of atmospheric origin, are discussed in terms of the geochemical properties of these two nuclides. Evidence is presented to support the hypothesis that the 137Cs distribution in these cores can be a useful independent tracer which provides confirmation of MARs calculated from the decay of 210Pb(xs).     

Fukushima fallout in Northwest German environmental media

Traces of short- and long-lived fallout isotopes (¹³¹I, ¹³⁴Cs and ¹³⁷Cs) were found in environmental samples collected in Northwest Germany (rain water, river sediment, soil, grass and cow milk) from March to May 2011, following the radioactivity releases after the nuclear accident in Fukushima, Japan. The measured concentrations are consistent with reported concentrations in air, amount of rainfall and expected values applying simple radioecological models. The [¹³⁴Cs]/[¹³⁷Cs] ratio reported for air (about 1) allows for discrimination between “recent” and “old” ¹³⁷Cs. Expected ¹³⁶Cs values fell below the detection limits of the instrumentation, despite large sample masses and long counting times.     

Recent changes in Red Lake (Romania) sedimentation rate determined from depth profiles of Pb and Cs radioisotopes

This work presents a first estimation of the sedimentation rate for the Red Lake (Romania). The sediment accumulation rates were determined by two well-known methods for recent sediment dating: ²¹⁰Pb and ¹³⁷Cs methods. Both techniques implied used the gamma emission of the above-mentioned radionuclides. The ²¹⁰Pb and ¹³⁷Cs concentrations in the sediment were measured using a gamma spectrometer with a HpGe detector, Gamma-X type. Activities ranging from 41 ± 7 to 135 ± 34 Bq/kg were found for ²¹⁰Pb and from 3 ± 0.5 to 1054 ± 150 Bq/kg for ¹³⁷Cs. The sediment profile indicates acceleration in sedimentation rate in the last 18 years. Thus, the sedimentation process for the Red Lake can be divided in two periods, the last 18 years, and respectively, the period before that. Using the Constant Rate of ²¹⁰Pb Supply method values between 0.18 ± 0.04 and 1.85 ± 0.5 g/cm² year (0.32 ± 0.08 and 2.83 ± 0.7 cm/year) were obtained. Considering both periods, an average sedimentation rate of 0.87 ± 0.17 g/cm² year (1.17 cm/year) was calculated. Considering an average depth of 5.41 m for the lake and the sedimentation rate estimated for the last 18 years, it could be estimated that the lake will disappear in 195 years.     

Distribution and flux of 238Pu, 239,240Pu, 241Am, 137Cs and 210Pb to high arctic lakes in the Thule district (Greenland)

Environmental samples (soil, sediment and lake water) in the Thule area (NW Greenland) have been studied to assess the contamination of radionuclides originating from a nuclear weapons accident (the Thule accident in 1968). Four lakes were chosen at different distances from the point of impact with the Thule air base community situated in between. The sedimentation rates in the lakes varied from 0.4 mm a(-1) (5 mg cm(-2) a(-1)) to 1.6 mm a(-1) (82 mg cm(-2) a(-1)). With these sedimentation rates, it is not possible to resolve the (239,240)Pu global fallout peak from a possible (239,240)Pu "accident" peak in the sediment depth profiles. However, the (239,240)Pu/(137)Cs and the (238)Pu/(239,240)Pu ratios agreed well with global fallout ratios, indicating that plutonium originating from the accident had not reached these lakes. This also indicates that the Thule air base community has probably only been exposed to radionuclides from the accident to a very limited extent. A limited study showed that (210)Pb could not be used as a normalizing nuclide to explain the transport of transuranic elements from the catchment area to the lake, i.e. (210)Pb has a different transport mechanism from that of the transuranic elements studied in this investigation.     

Using ²¹⁰Pb measurements to estimate sedimentation rates on river floodplains

Growing interest in the dynamics of floodplain evolution and the important role of overbank sedimentation on river floodplains as a sediment sink has focused attention on the need to document contemporary and recent rates of overbank sedimentation. The potential for using the fallout radionuclides ¹³⁷Cs and excess ²¹⁰Pb to estimate medium-term (10-10² years) sedimentation rates on river floodplains has attracted increasing attention. Most studies that have successfully used fallout radionuclides for this purpose have focused on the use of ¹³⁷Cs. However, the use of excess ²¹⁰Pb potentially offers a number of advantages over ¹³⁷Cs measurements. Most existing investigations that have used excess ²¹⁰Pb measurements to document sedimentation rates have, however, focused on lakes rather than floodplains and the transfer of the approach, and particularly the models used to estimate the sedimentation rate, to river floodplains involves a number of uncertainties, which require further attention. This contribution reports the results of an investigation of overbank sedimentation rates on the floodplains of several UK rivers. Sediment cores were collected from seven floodplain sites representative of different environmental conditions and located in different areas of England and Wales. Measurements of excess ²¹⁰Pb and ¹³⁷Cs were made on these cores. The ²¹⁰Pb measurements have been used to estimate sedimentation rates and the results obtained by using different models have been compared. The ¹³⁷Cs measurements have also been used to provide an essentially independent time marker for validation purposes. In using the ²¹⁰Pb measurements, particular attention was directed to the problem of obtaining reliable estimates of the supported and excess or unsupported components of the total ²¹⁰Pb activity of sediment samples. Although there was a reasonable degree of consistency between the estimates of sedimentation rate provided by the ¹³⁷Cs and excess ²¹⁰Pb measurements, some differences existed and the various models used to interpret excess ²¹⁰Pb measurements could produce different results. By using the ¹³⁷Cs measurements to provide independent validation of the estimates of sedimentation rate provided by the different models used with the excess ²¹⁰Pb measurement it was shown that the CICCS and Composite CRS models appeared to generally provide the best results.     

Evaluation of 137Cs fallout from the Chernobyl accident in a forest soil and its impact on Alpine Lake sediments, Mercantour Massif, S.E. France

The Boréon area in the Mercantour Massif, S.E. France, was contaminated by radionuclides after the Chernobyl accident in the first days of May 1986. Sediments from a small mountain lake in this area were collected, as well as forest soils in its vicinity, in order to obtain 137Cs and 210Pb profiles. Calculated from the 210Pb inventory in a soil of a horizontal area, the flux is high in the area (0.06 Bqcm(-2)y(-1)) probably because of the great frequency of rain and uranium ores outcropping in the massif. The comparison of the 137Cs soil inventories and the unsupported 210Pb suggests that the 137Cs fallout due to the Chernobyl accident in the study site (Boréon) was at least 3.5 Bqcm(-2), more probably the double. The recent lake sediments still undergo a rather strong contamination by 137Cs and the sediment profiles show that the residence time of 137Cs in the catchment area is long. The study area is frequented by many inhabitants of the city of Nice and other cities at the Mediterranean coast during week-end and during summer and winter holidays. Thus the 137Cs external exposure impact was evaluated at 2 mSvy(-1) for 2002 in the most contaminated point.     

Lead-210 and Beryllium-7 fallout rates on the southeastern coast of Brazil

Total ²¹⁰Pb and ⁷Be fallout rates were measured on the coastal region of Niteroi, Brazil. The monthly depositional flux of ²¹⁰Pb and ⁷Be varied by a factor of 26, from 1.7 to 43.3 mBq cm⁻² year⁻¹ and ∼27, from 7.5 to 203.5 mBq cm⁻² year⁻¹, respectively. The relatively large oscillations in the depositional flux of ²¹⁰Pb at this study site were likely due to variations in air mass sources, while the ⁷Be fluctuations may be driven by a combination of weather conditions. Local geology could support the periodic high fluxes of ²¹⁰Pb from continental air masses, as shifting oceanic wind sources were affirmed by the uncorrelated ²¹⁰Pb and ⁷Be fallout activities and ⁷Be/²¹⁰Pb ratios. The ²¹⁰Pb atmospheric deposition was found to be in agreement with local sediment inventories, an important consideration in geochemical studies that estimate sedimentation processes.