Distribution of Np and Pu in Swedish lichen samples (Cladonia stellaris) contaminated by atmospheric fallout

The activity concentrations of (237)Np and the two Pu isotopes, (239)Pu and (240)Pu, were determined in lichen samples (Cladonia stellaris) contaminated by fallout from atmospheric nuclear test explosions and the Chernobyl accident. The samples were collected at 18 locations in Sweden, from north to south, between 1986 and 1988 and analysed with high-resolution inductively coupled plasma mass spectrometry (HR-ICP-MS) and alpha spectrometry. Data on the activity ratios (238)Pu/(239+240)Pu and (134)Cs/(137)Cs measured previously were also included in this study for comparison. The (237)Np activity concentration ranged from 0.08 +/- 0.01 to 2.08 +/- 0.17 MBq kg(-1), depending on the location of the sampling site and time of collection. The (239+240)Pu activity concentration ranged from 0.09 +/- 0.01 to 4.09 +/- 0.15 Bq kg(-1), with the (240)Pu/(239)Pu atomic ratio ranging between 0.16 +/- 0.01 and 0.44 +/- 0.03, the higher ratios indicating a combination of weapons test fallout and Chernobyl fallout. The (237)Np/(239)Pu atomic ratios ranged between 0.06 +/- 0.01 and 0.42 +/- 0.04, the lower ratios indicating combination of weapons test fallout and Chernobyl fallout. At a well-defined sampling site at Lake Rogen (62.32 degrees N, 12.38 degrees E), additional lichen samples were collected between 1987 and 1998 to study the distribution of Np and Pu in different layers. The concentrations of the two elements follow each other quite well in the profile.     

Use of AMS in the marine environment

In recent years, the field of AMS has expanded into many areas of science. This paper reviews a variety of applications of AMS in the marine environment, focusing particularly on recent developments and applications. Following a brief summary of the three main isotope techniques used in environmental studies: dating, tracing and source identification, a number of applications are considered. Traditional (14)C-dating is no longer the dominant application of AMS measurements, and together with measurements of (10)Be, (26)Al and (36)Cl, much of the research is now directed towards an understanding of global climate change via studies of oceanic circulation, atmospheric processes and past climates by cosmic ray exposure dating. Profiles of long-lived cosmogenic radionuclides in sediments and ice cores, as a function of depth and, thus, age, provide key information on past solar variability, production rate changes and atmospheric transport and deposition mechanisms. Useful paleoclimatic information may be derived from these archives both because deposition is influenced by climate and because solar activity (which influences production) and solar radiance (which influences climate) are correlated. In recent years, emphasis has been put on the development and application of AMS techniques for the measurement of heavier long-lived isotopes, including (99)Tc, (129)I, (236)U and other actinide isotopes. AMS combines ultra low detection limits and the possibility to analyse isotope ratios that can be difficult with traditional instruments and has been used in a number of applications on the consequences and uses of releases from nuclear energy. Finally, the use AMS in environmental sciences is expected to expand further in the foreseeable future with long-lived cosmogenic radionuclides contributing to a large body of knowledge on processes involving atmosphere, oceans, ice sheets, biosphere, soils and sediments.     

Technetium-99 in the Irish marine environment

Technetium-99 activity concentrations in seawater and biota from Irish coastal waters are presented. Time series measurements of 99Tc in seawater and Fucus vesiculosus from the western Irish Sea show that activity concentrations have increased in line with the increase in discharges of 99Tc from Sellafield. The peak in activity concentrations in both seawater and Fucus vesiculosus occurred in 1997 approximately two years after the peak in 99Tc discharges. The highest activity concentration recorded in Fucus vesiculosus showed a 29-fold increase over the mean concentration for the period 1988-1993. Technetium-99 activity concentrations were measured in fish, lobsters, prawns, mussels and oysters landed at major fishing ports on the east and northeast coasts of Ireland between 1996 and 1998. Concentration factors for 99Tc in the brown seaweed Fucus vesiculosus and certain species of fish, crustaceans and molluscs from the Irish Sea were estimated. In general, these concentration factors were higher than those in the literature which were derived from laboratory studies, but agreed well with values which were based on field studies. The mean committed effective doses to Irish typical and heavy seafood consumers due to 99Tc in the period 1996-1998 were 0.061 and 0.24 microSv, respectively.     

240Pu/239Pu atom ratios in seawater from Sagami Bay, western Northwest Pacific Ocean: sources and scavenging

Seawater samples were collected in Sagami Bay, western Northwest Pacific Ocean, and their (239+240)Pu activities and (240)Pu/(239)Pu atom ratios were determined by alpha-spectrometry and sector field high-resolution ICP-MS. A few samples also were analyzed for (137)Cs activities. The (239+240)Pu inventory of 41.1 Bq m(-2) was equivalent to the expected cumulative deposition density of atmospheric global fallout at the same latitude and this inventory was considerably lower than inventories in the underlying sediment columns. This result indicated that a significant amount of (239+240)Pu has been removed into the underlying sediments through enhanced scavenging from the water column by the high fluxes of particles in this region. The atom ratio of (240)Pu/(239)Pu showed no notable variation from the surface to the bottom; the average value was 0.234+/-0.004. This atom ratio was significantly higher than the mean global fallout ratio of 0.18, proving the existence of close-in fallout plutonium originating from the Pacific Proving Grounds (PPG). The relative contributions of the global stratospheric fallout and the PPG close-in fallout were evaluated by using the two end-member mixing model. The contribution of the PPG close-in fallout was estimated to be 15.2 Bq m(-2), which corresponded to 37% of the (239+240)Pu inventory in the water column. Thus (239)Pu and (240)Pu from the two sources of global fallout and close-in fallout have been homogenized in the water masses in the western Northwest Pacific margin during the past three decades.     

The concentration of Cs in the surface of the Greek marine environment

The radiological status of the Greek marine environment, prior to the Chernobyl accident, was characterized mainly by the fallout from nuclear weapon tests. However, the release of radioactivity into the environment from the accident in the Chernobyl Nuclear Power Plant and its deposition in the Greek marine environment resulted in an increase of the ¹³⁷Cs activity concentration by approximately one order of magnitude. In addition, the direct transport of radiocaesium into the North Aegean Sea has been further influenced by the late impact of the Chernobyl accident on the Greek marine environment, related to the transfer of ¹³⁷Cs, mainly through the Dnieper but also the Danube rivers, to the Black Sea and further to the North Aegean Sea through the Straits of Dardanelles. The aim of this work is to provide a present day picture of the geographic variation of the concentration of ¹³⁷Cs in the surface layer of the Greek marine environment and hence, to evaluate the annual committed effective dose delivered to humans through the ingestion pathway from marine sources.     

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.     

Radiocesium in North San Francisco Bay and Baja California coastal surface waters

Radiocesium, 137Cs, and rare earth elements (REEs) were determined in suspended material and dissolved fractions of waters across the salinity gradient in North San Francisco Bay (estuary). We describe the variation of this conservative isotope tracer with salinity and sediment load. REE data are used to differentiate marine and terrigenous source terrains for suspended material and dissolved fractions. We estimate that about 1-4 x 10(10) Bq of 137Cs migrates annually on suspended material through the North Bay. In addition, 137Cs concentrations were measured in surface waters off Baja California. Combined in situ water density (sigma(t)) and 137Cs data distinguish between California Current and Gulf of California water, and delineate areas of upwelling, where nutrient-rich, deep Pacific Intermediate water, with little or no 137Cs, is brought to the surface off promontories along Baja California.     

Polybrominated diphenyl ether flame retardants in the North American environment

North America consumes over half of the world's production of polybrominated diphenyl ether (PBDE) flame retardants. About 98% of global demand for the Penta-BDE mixture, the constituents of which are the most bioaccumulative and environmentally widespread, resides here. However, research on the environmental distribution of PBDEs in North America has lagged behind that in Northern Europe. Examination of available governmentally maintained release data suggests that Deca-BDE use in the US substantially exceeds that in Canada. Penta-BDE use probably follows a similar pattern. PBDE demand in Mexico is uncertain, but is assumed to be comparatively modest. Recent research examining air, water, sediment, sewage sludge and aquatic biota suggests that Penta-BDE constituents are present in geographically disparate locations in the US and Canada. The less brominated congeners have been observed in areas distant from their known use or production, e.g. the Arctic. PBDEs have been detected in low concentrations in North American air, water and sediment, but much higher levels in aquatic biota. Increased burdens as a function of position in the food web have been noted. PBDE concentrations in US and Canadian sewage sludges appear to be at least 10-fold greater than European levels and may be a useful barometer of release. In general, PBDE concentrations in environmental media reported in North America are comparable or exceed those observed elsewhere in the world. In contrast to Europe, environmental burdens are increasing over time here, consistent with the greater consumption of the commercial mixtures. However, data remain relatively scarce. Deca-BDE in the North American environment appears largely restricted to points of release, e.g. urban areas and those where PBDE-containing sewage sludges have been applied. This lack of redistribution is likely due to its extremely low volatility and water solubility. Penta-BDE and Deca-BDE products are used in different applications and this may also be a factor controlling their environmental release.     

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.     

Sources and distributions of Cs, Pu, Pu radionuclides in the north-western Barents Sea

Sediment deposits are the ultimate sink for anthropogenic radionuclides entering the marine environment. The major sources of anthropogenic radionuclides to the Barents Sea are fallout from nuclear weapons tests, long range transport from other seas, and river and non-point freshwater supplies. In this study we investigated activity concentrations, ratios, and inventories of the anthropogenic radionuclides, ¹³⁷Cs, ²³⁸Pu, ^239,240Pu in dated sediment cores collected along a north-south transect in the northwestern Barents Sea. The data were used to evaluate the influence of different sources on the derived spatial and temporal patterns of anthropogenic radionuclides in seafloor sediment deposits. Activity concentrations of ¹³⁷Cs ranged from <0.1 Bq/kg to 10.5 Bq/kg while ^239,240Pu ranged from <0.01 Bq/kg to 2.74 Bq/kg and ²³⁸Pu activity concentrations ranged from <0.01 Bq/kg to 0.22 Bq/kg. Total inventories of ¹³⁷Cs ranged from 29.5 ± 1.5 Bq/m² to 152.7 ± 5.6 Bq/m² and for ^239,240Pu inventories (6 sediment layers only) ranged from 9.5 ± 0.3 Bq/m² to 29.7 ± 0.4 Bq/m². Source contributions varied among stations and between the investigated radionuclides. The ²³⁸Pu/^239,240Pu ratios up to 0.18 indicate discharges from nuclear fuel reprocessing plants as a main contributor of plutonium. Based on ²³⁸Pu/^239,240Pu ratio, it was calculated that up to 19-27% of plutonium is supplied from sources other than atmospheric global fallout. Taking into account Atlantic current flow trajectories and that both activity concentrations and inventories of plutonium negatively correlate with latitude, Sellafield is a major source for the Barents Sea. Concentrations and inventories of ¹³⁷Cs correlate positively with latitude and negatively with distance from the Svalbard archipelago. The ¹³⁷Cs concentrations are highest in an area of intensive melting of sea ice formed along the Siberian coast. Thus, sea ice and supplies from Svalbard may be important source of ¹³⁷Cs to the Barents Sea seafloor.     

POSEIDON/RODOS models for radiological assessment of marine environment after accidental releases: application to coastal areas of the Baltic, Black and North Seas

In the framework of the developments of the European system RODOS (Real-time On-line DecisiOn support System) for emergency response to nuclear accident, the computer code POSEIDON, that was developed to assess the radiological consequences of radioactive releases into marine environment, was adapted to cope with emergency conditions, in situations of radioactive discharges into the oceans from direct deposition from the atmosphere, sunken ships and containers, from discharges of rivers and estuaries and from coastal run-off. Based on the box model developed within the 'Marina' project, POSEIDON can calculate the dose effects from radionuclide releases in the coastal waters of Europe integrated over long time periods. A dynamic food chain model was implemented to deal with the short-term dynamical uptake of radioactivity by specific marine plants and organisms. POSEIDON has been installed on a UNIX platform to be fully compatible with RODOS input/output databases and on a Windows platform with an interface based on web technology. The 3D hydrodynamic model THREETOX is a part of the POSEIDON/RODOS system. It has been applied to coastal areas of the Baltic Sea, the Black Sea, and the North Sea. to derive the parameters for a flexible system of well-defined model compartments to be adapted to emergency conditions. The activity concentrations in water and in the marine food web were calculated by means of POSEIDON for radioactive fallout resulting from bomb testing, from the Chernobyl accident, and from routine discharges from nuclear facilities. POSEIDON's model results were compared with measurement data, and with calculation results from THREETOX. The model results agreed with the measurement data sufficiently.     

Long-term study of 99Tc in the marine environment on the Swedish west coast

The activity concentration of (99)Tc in brown seaweed (Fucus vesiculosus and Fucus serratus) and seawater were analysed in samples collected in 1991, 1995 and 2001 at several stations along the Swedish west coast. In addition to these locations, a well-defined site (S?rdal, 56.76 degrees N, 12.63 degrees E) was included with (99)Tc activity concentration data in seaweed from 1967 to 2000. Over the years, the major source of (99)Tc in the coastal waters of western Sweden has been the radioactive liquid discharge from the nuclear fuel reprocessing plant in Sellafield (UK) transported via ocean currents in the North Sea. The (99)Tc activity concentration in seaweed at the S?rdal site increased from approximately 30 Bq kg(-1) up to 230 Bq kg(-1) (dry weight) between 1997 and 2000 due to the Sellafield EARP (Enhanced Actinide Removal Plant) discharges in 1995-1996, yielding an approximate transport time of 4-5 years between the Irish Sea and the Kattegat. Due to the very sharp gradient in (99)Tc concentration between the Baltic Sea and the North Sea, (99)Tc is presently one of the best transit tracers for the recent ventilation events in the Baltic Sea.     

Comparison of Pu and (137)Cs as tracers of soil and sediment transport in a terrestrial environment

Following atmospheric nuclear weapons testing in the 1950s and 1960s significant quantities of (137)Cs and (239+240)Pu were deposited worldwide. In recent decades, (137)Cs has been commonly used as a tracer of soil erosion and sedimentation, particularly in the Northern Hemisphere where atomic deposition was three times as great as in the Southern Hemisphere. The relatively short 30-year half-life of this isotope means that its sensitivity as a tracer is rapidly decreasing. In contrast, with half-lives of 24,110 and 6561 years, the sensitivity of the two plutonium isotopes remains essentially the same as when it was deposited. Here we use the technique of Accelerator Mass Spectrometry to demonstrate the potential of anthropogenic Pu as an alternative to (137)Cs as a tracer of soil transport in Australia. We measure an average (137)Cs/(239+240)Pu activity ratio of 27.3+/-1.5 and an average (240)Pu/(239)Pu atom ratio of 0.149+/-0.003, both slightly lower than the global average.     

Distribution and fate of persistent organochlorine pesticides in coastal marine environment of Mumbai

Multi-compartment monitoring of residue levels of OCPs in coastal marine environment of Mumbai has been studied. The concentration of total HCHs in seawater varied from 0.16 to 15.92 ng/L and concentrations of total DDT varied from 3.01 to 33.21 ng/L. The total HCH concentration in the sediment samples was in the range of 3.8 to 16.2 ng/g. Gamma-HCH contributed almost 55% to the total HCH. In sediment samples the DDT has higher mean concentration in comparison to its metabolite DDE and DDD. The concentration of total HCHs in different marine species varied from 0.87 to 33.73 ng/g and concentrations of total DDT varied from 0.38 to 34.1 ng/g. The variation in the beta-HCH in different compartments is not significant and this could be due to the high persistence and metabolically inactive nature of this isomer. The alpha-HCH is found to be more dominant in fish samples whereas the gamma-HCH is major contributor in the sediment samples.     

Optimisation of sampling for the temporal monitoring of technetium-99 in the Arctic marine environment

Monitoring of the marine environment for radioactivity, for both radiological protection and oceanographic purposes, remains an expensive and labour intensive activity due to the large sample volumes needed and the complex and lengthy analytical procedures required to measure low levels of contamination. Because of this, some consideration must be given to the design of sampling plans to ensure effective and efficient sampling that can be defended on the basis of scientific rationale. This article tests the hypothesis that geostatistical techniques may prove of use in the optimisation and design of sampling regimes for the monitoring of temporal fluctuations in the levels of technetium at a location in the Norwegian Arctic marine environment. The level of temporal correlation exhibited by two relevant time series was investigated and the information used to observe the effect of sampling frequency on the production of monthly estimates of activity of technetium in both seawater and seaweed. The results indicate that reduced sampling frequency allows production of estimates that acceptably replicate the actual data and that use of geostatistical procedures may offer advantages in the planning of monitoring systems for marine radioactivity. The use of an oceanographic model was also investigated as a means of assessing the temporal correlation prior to actual sampling, an approach that may offer significant advantages by reducing the need to have lengthy time series prior to designing sampling regimes.     

Transport of plutonium in surface and sub-surface waters from the Arctic shelf to the North Pole via the Lomonosov Ridge

New data on the levels and long-range transport of plutonium in the Arctic Ocean, recorded in the course of two expeditions to this zone in 1994 and 1996, are discussed in this paper. Specifically, approximately 100 plutonium measurements in surface and sub-surface water sampled at 58 separate stations throughout the Kara, Laptev and East Siberian Seas, as well as along latitudinal transects across the Lomonosov Ridge, are reported and interpreted in terms of the circulation pathways responsible for the transport of this element from the North Atlantic to the Arctic Shelf and into the Arctic interior. In addition, the behaviour of plutonium in its transit through the vast Arctic shelf seas to open waters under extreme environmental conditions is discussed in terms of the partitioning of plutonium between filtered (<0.45 microm) seawater and suspended particulate, and its association with colloidal matter. Finally, limited evidence of the presence of a colloidal plutonium component in Arctic waters subject to direct riverine input is adduced.     

210Po in the marine environment with emphasis on its behaviour within the biosphere

The distribution and behaviour of the natural-series alpha-emitter polonium-210 in the marine environment has been under study for many years primarily due to its enhanced bioaccumulation, its strong affinity for binding with certain internal tissues, and its importance as a contributor to the natural radiation dose received by marine biota as well as humans consuming seafoods. Results from studies spanning nearly 5 decades show that ²¹⁰Po concentrations in organisms vary widely among the different phylogenic groups as well as between the different tissues of a given species. Such variation results in ²¹⁰Po concentration factors ranging from approximately 10³ to over 10⁶ depending upon the organism or tissue considered. ²¹⁰Po/²¹⁰Pb ratios in marine species are generally greater than unity and tend to increase up the food chain indicating that ²¹⁰Po is preferentially taken up by organisms compared to its progenitor ²¹⁰Pb. The effective transfer of ²¹⁰Po up the food chain is primarily due to the high degree of assimilation of the radionuclide from ingested food and its subsequent strong retention in the organisms. In some cases this mechanism may lead to an apparent biomagnification of ²¹⁰Po at the higher trophic level. Various pelagic species release ²¹⁰Po and ²¹⁰Pb packaged in organic biodetrital particles that sink and remove these radionuclides from the upper water column, a biogeochemical process which, coupled with scavenging rates of this radionuclide pair, is being examined as a possible proxy for estimating downward organic carbon fluxes in the sea. Data related to preferential bioaccumulation in various organisms, their tissues, resultant radiation doses to these species, and the processes by which ²¹⁰Po is transferred and recycled through the food web are discussed. In addition, the main gaps in our present knowledge and proposed areas for future studies on the biogeochemical behaviour of ²¹⁰Po and its use as a tracer of oceanographic processes are highlighted in this review.     

Customisation of the decision support system MOIRA-PLUS for applications to the marine environment

The present short communication describes a technique to customise the decision system MOIRA-PLUS for applications to the marine environment. MOIRA-PLUS was originally designed to predict the behaviour of ¹³⁷Cs and ⁹⁰Sr in fresh water ecosystems and to evaluate the environmental, social and economic impacts of selected countermeasures aimed at restoring the polluted environment and at reducing the doses to man. An example of application for predicting the concentration of radiocaesium of Chernobyl origin in the Mediterranean Sea is described and discussed. The technique allows the user to easily integrate existing state-of-the-art box models of sea water circulation into the MOIRA-PLUS decision system.