Present background levels of surface 137Cs and (239,240)Pu concentrations in the Pacific

The present levels of anthropogenic radionuclides, 137Cs and (239,240)Pu, in surface waters of the Pacific are estimated using the HAM database, which is a comprehensive data set of 137Cs, (239,240)Pu and other anthropogenic radionuclides. The time-series data of surface 137Cs and (239,240)Pu suggests that surface 137Cs and (239,240)Pu concentrations in the Pacific since 1971 decrease exponentially in each sea area, although the temporal changes of surface 137Cs and (239,240)Pu differed between sea areas of the Pacific. The calculated 137Cs concentrations in the Pacific surface waters in 2000 are homogeneous in the Pacific, comparing with that in the 1960s and 1970s, although they are still high in the North Pacific and low in the South Pacific. The biogeochemical and physical processes are significant factors to control present levels of surface (239,240)Pu concentrations, which are high in the Subarctic and equatorial Pacific and low in the mid-latitude region of the eastern North Pacific.     

Suspended particle adhesion on aquatic plant surfaces: implications for 137Cs and 133Cs uptake rates and water-to-plant concentration ratios

Suspended particle adhesion on aquatic biota can significantly increase the apparent concentration of radionuclides above their endogenous value, leading to an overestimation of the uptake rate and concentration ratios. This study is an attempt to assess quantitatively the importance of suspended particle adhesion on periphyton samples (biological material coating submerged surfaces). The concentrations of 137Cs and stable Cs (133Cs) in periphyton, suspended particles and filtered water were measured to determine the net water-to-periphyton concentration ratios for 137Cs and stable Cs. The net amount of 133Cs (or 137Cs) taken up by periphyton was calculated by subtracting from the total amount of 133Cs (or 137Cs) on the collected material (periphyton + inorganic particles), the 133Cs (or 137Cs) due to the inorganic particles adhering to periphyton. The mass of suspended particles adhering to the periphyton surface was calculated using scandium as an indicator of the mineral fraction of the suspended particles. The relationship between the concentration ratios for 137Cs and stable Cs and suspended particle adhesion on periphyton external surfaces is discussed.     

(137)Cs concentrations in Atlantic and western Antarctic surface waters: results of the 7th Ukrainian Antarctic Expedition, 2002

The latitudinal distribution of (137)Cs in the Atlantic--western Antarctic surface waters was studied during the 7th Ukrainian Antarctic Expedition in January--May 2002. The (137)Cs concentrations have also been measured in the upper ice of the coastal glacier Woozle Hill located near the Ukrainian Antarctic station "Akademik Vernadsky" (western Antarctica, 65 degrees 15' S-64 degrees 16' W). Comparison of these data with results of previous same-route expeditions SWEDARP (Swedish Antarctic Research Expedition, 1988/1989) and the French R/V "Jeanne d'Arc" (1992/1993), has shown practically parallel changes of (137)Cs surface concentrations between 40 degrees N and 20 degrees S, pointing to decrease of (137)Cs radioactivity at these latitudes with an apparent half-life of 10--15 years (12.5+/-2.1 years on average). This suggests that decrease of (137)Cs surface concentration within this latitude band is controlled, besides the radioactive decay of (137)Cs (half-life=30 years), by vertical mixing of the upper water masses. South of 20 degrees S, the (137)Cs concentrations in surface water have decreased more rapidly because of the influence of the less contaminated Antarctic waters. At 50--60 degrees S and near the Antarctic coast, the (137)Cs activity in 2002 was similar to those measured during the SWEDARP and "Jeanne d'Arc" expeditions, suggesting an additional input of (137)Cs to these waters from the melted ice from the adjacent glaciers.     

90Sr, 137Cs and (239,240)Pu concentration surface water time series in the Pacific and Indian Oceans--WOMARS results

Under an IAEA's Co-ordinated Research Project "Worldwide Marine Radioactivity Studies (WOMARS)" 90Sr, 137Cs and (239,240)Pu concentration surface water time series in the Pacific and Indian Oceans have been investigated. The Pacific and Indian Oceans were divided into 17 latitudinal boxes according to ocean circulation, global fallout patterns and the location of nuclear weapons test sites. The present levels and time trends in radionuclide concentrations in surface water for each box were studied and the corresponding effective half-lives were estimated. For the year 2000, the estimated average 90Sr, 137Cs and (239,240)Pu concentrations in surface waters of the Pacific and Indian Oceans varied from 0.1 to 1.5 mBq/L, 0.1 to 2.8 mBq/L, and 0.1 to 5.2 microBq/L, respectively. The mean effective half-lives for 90Sr and 137Cs in surface water were 12+/-1 years for the North, 20+/-1 years for the South and 21+/-2 years for the Equatorial Pacific. For (239,240)Pu the corresponding mean effective half-lives were 7+/-1 years for the North, 12+/-4 years for the South and 10+/-2 years for the Equatorial Pacific. For the Indian Ocean the mean effective half-lives of 137Cs and (239,240)Pu were 21+/-2 years and 9+/-1 years, respectively. There is evidence that fallout removal rates before 1970 were faster than those observed during recent decades. The estimated surface water concentrations of 90Sr, 137Cs and (239,240)Pu in latitudinal belts of the Pacific and Indian Oceans for the year 2000 may be used as the average levels so that any new contribution from nuclear facilities, nuclear weapons test sites, radioactive waste dumping sites and from possible nuclear accidents can be identified.     

A process-based model for the partitioning of soluble, suspended particulate and bed sediment fractions of plutonium and caesium in the eastern Irish Sea

A dynamic model of plutonium behaviour in the marine environment has been developed, representing the oxidation state distribution and partitioning of plutonium between the soluble, colloidal, suspended particulate and seabed sediment fractions. With simple re-parameterisation, this model can also be applied to (137)Cs. The model, which is calibrated and validated against field data, has been used to predict concentrations of Pu(alpha) and (137)Cs in both water and seabed sediments from the vicinity of the Sellafield Ltd. reprocessing plant in Cumbria, UK. The model predicts that sediment reworking and transport are the key environmental processes as the Sellafield Pu(alpha) and (137)Cs discharge continues to decline. Inventory calculations generated by the model are consistent with previous estimations. For a hypothetical post-discharge scenario, the concentrations of these radionuclides in both seawater and surface sediments are predicted to decrease sharply, concurrent with a downward vertical migration of the activity retained in sediments.     

Discharge of 137Cs and 90Sr by Finnish rivers to the Baltic Sea in 1986-1996

The total amounts of 137Cs and 90Sr transported from Finland by rivers into the Gulf of Finland, Gulf of Bothnia and Archipelago Sea since 1986 were estimated. The estimates were based on long-term monitoring of 137Cs and 90Sr in river and other surface waters and on the statistics of water discharges from Finnish rivers to the above sub-areas of the Baltic Sea. The total amounts of 137Cs and 90Sr removed from Finland into the Baltic Sea during 1986-1996 were estimated to be 65 and 10 TBq, respectively. The results show that, although the deposition of 137Cs was much higher than that of 90Sr after the Chernobyl accident, the amount of 137Cs removed from Finland is only six times as high as that of 90Sr. This emphasizes the importance of 90Sr while considering radiation doses from surface waters and 137Cs while estimating doses via pathways from catchment soil, lake sediments and biota after a fallout situation.     

Estimating sediment and caesium-137 fluxes in the Ribble Estuary through time-series airborne remote sensing

High spatial and temporal resolution airborne imagery were acquired for the Ribble Estuary, North West England in 1997 and 2003, to assess the application of time-series airborne remote sensing to quantify total suspended sediment and radionuclide fluxes during a flood and ebb tide sequence. Concomitant measurements of suspended particulate matter (SPM) and water column turbidity were obtained during the time-series image acquisition for the flood and ebb tide sequence on the 17th July 2003 to verify the assumption of a vertically well mixed estuary and thus justifying the vertical extrapolation of spatially integrated estimate of surface SPM. The ¹³⁷Cs activity concentrations were calculated from a relatively stable relationship between SPM and ¹³⁷Cs for the Ribble Estuary. Total estuary wide budgets of sediment and ¹³⁷Cs were obtained by combining the image-derived estimates of surface SPM and ¹³⁷Cs with estimates of water volume from a two-dimensional hydrodynamic model (VERSE) developed for the Ribble Estuary. These indicate that around 10,000 tonnes of sediment and 2.72 GBq of ¹³⁷Cs were deposited over the tidal sequence monitored in July 2003. This compared favourably with bed height elevation change estimated from field work. An uncertainty analysis on the total sediment and ¹³⁷Cs flux yielded a total budget of the order of 40% on the final estimate. The results represent a novel approach to providing a spatially integrated estimate of the total net sediment and radionuclide flux in an intertidal environment over a flood and ebb tide sequence.     

Vertical distributions of (99)Tc and the (99)Tc/(137)Cs activity ratio in the coastal water off Aomori, Japan

Using a sector-field ICP-MS the vertical distributions of the ⁹⁹Tc concentration and ⁹⁹Tc/¹³⁷Cs activity ratio were measured in the coastal waters off Aomori Prefecture, Japan, where a spent-nuclear-fuel reprocessing plant has begun test operation. The ⁹⁹Tc concentrations in surface water ranged from 1.8 to 2.4 mBq/m³, no greater than the estimated background level. Relatively high ⁹⁹Tc/¹³⁷Cs activity ratios (10-12 × 10⁻⁴) would be caused by the inflow of the high-⁹⁹Tc/¹³⁷Cs water mass from the Japan Sea. There is no observable contamination from the reprocessing plant in the investigated area. The ⁹⁹Tc concentration and the ⁹⁹Tc/¹³⁷Cs activity ratio in water column showed gradual decreases with depth. Our results implied that ⁹⁹Tc behaves in a more conservative manner than ¹³⁷Cs in marine environments.     

Radionuclide tracing of water masses and processes in the water column and sediment in the Algerian Basin

Caesium-137 and (239,240)PU were analysed in the water column along the Algerian coast. The (137)Cs activity concentration in surface water increased from the west to the east from 1.6 to 3.3 mBq L(-1), documenting a presence of Modified Atlantic Water (MAW) in the region. Higher concentrations observed in deep waters may be due to an intrusion of Levantine Intermediate Water (LIW), which has been carrying higher levels of (137)Cs from Chernobyl accident. The (239,240)Pu sub-surface concentration peaked at about 250 m water depth as a result of biogeochemical processes in the water column. The observed (239,240)Pu/(137)Cs activity ratio at the surface (0.003) was significantly lower than that in global fallout (0.04). This decrease exceeds that expected from radioactive decay of (137)Cs, and confirms that Pu due to its adsorption on sinking particles is more effectively removed from surface layers than is (137)Cs. An increase of the (239,240)Pu/(137)Cs activity ratio with depth suggests that (239,240)Pu, similarly as (137)Cs, should be also transported by advection to maintain the observed ratios in deep waters. An intrusion of LIW may enhance therefore both the (137)Cs and (239,240)Pu concentrations in deep waters. The average (238)Pu/(239+240)Pu activity ratio in seawater was 0.03+/-0.02, confirming a global fallout origin of Pu in the Algerian Basin. Caesium-137 and (239,240)Pu inventories in the water column were estimated to be from 2.7+/-0.5 kBq m(-2) to 3.8+/-0.7 kBq m(-2), and from 13.8+/-2.6 Bq m(-2) to 41+/-7B qm(-2), respectively. The (137)Cs massic activities in surface sediment were almost constant, the average activity was 9.0+/-0.8 Bq kg(-1). Sedimentation rates obtained using the (210)Pb method were from 0.1 to 0.7 cm y(-1), and resulting penetration depths of (137)Cs in the sediment cores were from 15 to over 40 cm. The (137)Cs peaks found in the sediment cores were associated with the Chernobyl accident (1986) and global fallout (1964). The (137)Cs inventories in the sediment were increasing from the west (180 Bq m(-2)) to the east (350 Bq m(-2)).     

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.     

An elemental rationing technique for assessing concentration data from a complex water system

Water samples have been collected at the surface and bottom layers at 51 locations throughout Chesapeake Bay. The suspended particulate and dissolved fractions of these samples have been analyzed for Cd, Ce, Co, Cu, Fe, Mn, Mo, Ni, Pb, Sc, Sn, Th, U, and Zn using neutron activation analysis and atomic absorption spectrometry. Special chemical procedures were used to preconcentrate the elements of interest in the dissolved samples and separate them from the salt water matrix. The elemental concentrations observed in the dissolved samples were evaluated by direct comparison to those found in coastal seawater; however, the elemental concentrations in the particulate samples (mass per volume of water) were strongly influenced by the total amount of particulate material suspended in the water at time of collection. A double normalization procedure was used to calculate crustal enrichment factors for each sample, and these enrichment factors provided both a means to observe sample-to-sample variations, and also allowed a crude comparison with the natural levels occurring in the earth's crust.     

Concentration and specific activity of fallout 137Cs in extracted and particle-size fractions of cultivated soils

Fallout (137)Cs and stable Cs in soils were separated with two extractants (1M CH(3)COONH(4) solution and 0.8M CH(3)COONH(4) in 5% HNO(3) solution after H(2)O(2) oxidization). The residue remaining after removal of the oxidizable organic-bound fraction was separated into the particle-size fractions including clay, silt, fine sand and coarse sand with a sieving and sedimentation method. Then, the concentrations of (137)Cs and stable Cs in the extracted fractions and the particle-size fractions were determined. The (137)Cs contents in the exchangeable and organic-bound fractions in the soil were approximately 10 and 20%, respectively. The (137)Cs content in the strongly bound fraction was about 70%, and the concentration of (137)Cs in the clay was the richest among the particle-size fractions. The specific activity of (137)Cs (concentration ratio of fallout (137)Cs/stable Cs) decreased in the order exchangeable, organic-bound and strongly bound fractions. The data suggest that equilibrium between (137)Cs and stable Cs was not reached among those fractions, even though most of the (137)Cs that had been deposited on the soil was derived from fallout weapons tests that occurred several decades ago. The concentration of (137)Cs among the particle-size fractions in each soil was different, whereas the specific activity of (137)Cs in the particle-size fractions had a relatively similar value.     

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).     

Contamination of the southern Baltic Sea with 137Cs and 90Sr over the period 2000-2004

Changes of the (137)Cs activity concentrations in the southern Baltic Sea waters were investigated over the period 2000-2004 and distribution of the (90)Sr concentrations was determined in 2004. In the discriminated period further decrease of (137)Cs concentrations was observed. The average activity concentration of (137)Cs declined from 59.4Bq/m(3) in 2000 to 45.1Bq/m(3) in 2004. The greatest changes of (137)Cs activities occurred in 2003 as a consequence of the medium-size inflow of a saline waters from the North Sea. This inflow affected (137)Cs activities as well as its distribution in the Baltic Sea. Changes in (90)Sr activity concentrations proceeded at much slower rate. The average activity concentration of (90)Sr was equal to 8.7Bq/m(3) in 2004. The annual fluvial (137)Cs fluxes from the Vistula river were also estimated. In 2000, the (137)Cs load from Vistula was of an order of 0.15TBq/year, and in 2004 0.05TBq/year.     

Numerical simulation of 137Cs and (239,240)Pu concentrations by an ocean general circulation model

We simulated the spatial distributions and the temporal variations of 137Cs and (239,240)Pu concentrations in the ocean by using the ocean general circulation model which was developed by National Center of Atmospheric Research. These nuclides are introduced into seawaters from global fallout due to atmospheric nuclear weapons tests. The distribution of radioactive deposition on the world ocean is estimated from global precipitation data and observed values of annual deposition of radionuclides at the Meteorological Research Institute in Japan and several observed points in New Zealand. Radionuclides from global fallout have been transported by advection, diffusion and scavenging, and this concentration reduces by radioactive decay in the ocean. We verified the results of the model calculations by comparing simulated values of 137Cs and (239,240)Pu in seawater with the observed values included in the Historical Artificial Radionuclides in the HAM database, which has been constructed by the Meteorological Research Institute. The vertical distributions of the calculated 137Cs concentrations were in good agreement and are in good agreement with the observed profiles in the 1960s up to 250 m, in the 1970s up to 500 m, in the 1980s up to 750 m and in the 1990s up to 750 m. However, the calculated 137Cs concentrations were underestimated compared with the observed 137Cs at the deeper layer. This may suggest other transport processes of 137Cs to deep waters. The horizontal distributions of 137Cs concentrations in surface water could be simulated. A numerical tracer release experiment was performed to explain the horizontal distribution pattern. A maximum (239,240)Pu concentration layer occurs at an intermediate depth for both observed and calculated values, which is formed by particle scavenging. The horizontal distributions of the calculated (239,240)Pu concentrations in surface water could be simulated by considering the scavenging effect.     

Temporal variation of 137Cs water column inventory in the North Pacific since the 1960s

The temporal variation of water column inventories of 137Cs in the North Pacific since the 1960s was examined based on the analysis of the 137Cs profiles in HAM database. 137Cs in seawater in the North Pacific have originated mainly from global fallout from atmospheric nuclear weapons tests, which occurred in the early 1960s. In the 1960s, both the meridional distribution of 137Cs inventory in the North Pacific and that of fallout on land stations showed mid-latitude maximum. The region with higher deposition at land stations, however, was more northern than the latitudes where the 137Cs inventory in the North Pacific showed a maximum. The difference of the latitude where maximum 137Cs deposition/inventory was observed reflects the difference of the geographical distribution of the precipitation amount in the Pacific and Atlantic Oceans followed by the different warm current systems in each ocean. A good positive relation between 137Cs inventory and annual precipitation amount was discovered in the ocean stations at the middle latitude in the North Pacific. The horizontal distribution of 137Cs inventories at the middle latitudes in the North Pacific is characterized as west-high and east-low in the early 1960s, which was basically controlled by the distribution of annual precipitation amount. Eastward advection, then, modified it to be less difference in 1966-1967 after the highest deposition periods in 1963-1965. In the 1970s and 1980s, increases of the 137Cs inventory at the lower latitude of 10-20 deg. N are found. Surface and subsurface southward transports are considered as the source of this increasing 137Cs inventory.     

A modelling study on 137Cs and 239,240Pu behaviour in the Alborán Sea, western Mediterranean

A model for simulating the dispersion processes of 137Cs and 239,240Pu in the Alborán Sea is described. The model consists of two hydrodynamic models: a 2D depth-averaged model and a two-layer model which provide tidal and geostrophic currents, respectively; a sediment transport model which provides suspended particle concentrations and sedimentation rates over the domain; and the radionuclide dispersion model including interactions of dissolved radionuclides with suspended particles and bed sediments. These processes are formulated using kinetic transfer coefficients. The hydrodynamic and sediment models are run and validated in advance, and their results are then used to simulate the dispersion of 137Cs and 239,240Pu, which are introduced from atmospheric fallout. Radionuclide concentrations in the water column and distributions in bed sediments have been compared with measurements in the sea. Both set of data are, in general, in agreement. The model has also been applied to calculate radionuclide fluxes through the Strait of Gibraltar. These computed fluxes have been compared with previous estimations as well.     

Importance of colloids in the transport within the dissolved phase (<450 nm) of artificial radionuclides from the Rhône river towards the Gulf of Lions (Mediterranean Sea)

The significance of colloidal fractions regarding the transport of artificial radionuclides in natural water systems is underlined by using sequential ultrafiltration both in the Rh?ne freshwater and the marine area under and outside the influence of the river outflow. Indeed, the Rhodanian aquatic system represents an interesting test site as various artificial radionuclides are released into the Rh?ne river by several nuclear installations. We focused our study on (137)Cs, (106)Ru, (60)Co, (238)Pu and (239+240)Pu. Our results show that Fe, Al and Organic carbon (OC) are the main components of colloidal matter. Colloids represent about 15% of dissolved (<450 nm) OC and 25% of dissolved Fe and Al exported towards the sea. Within the dissolved (< 450 nm) phase, these colloidal compounds are shown to account for the transport of 40% for both Co and Ru, 60% for (238)Pu and (239+240)Pu and have no significance on (137)Cs flux.     

(137)Cs concentration in zooplankton and its relation to taxonomic composition in the western North Pacific Ocean

To study the role of zooplankton in the transport of (137)Cs in the ocean, zooplankton samples were collected in October 2005 and June 2006 in the western North Pacific Ocean. The peak zooplankton biomass was observed in the surface layer, and gelatinous plankton was more abundant in October 2005 than in June 2006 reflecting exchange of water masses. The concentrations of (137)Cs in zooplankton varied from 11 to 24 mBq kg wet(-1) and were higher in October 2005 than in June 2006. The elevated abundance of gelatinous zooplankton probably led to higher concentration of (137)Cs in zooplankton in October 2005. Annual export fluxes of (137)Cs by ontogenetic vertical migrant copepods were estimated to be 0.8 and 0.6 mBq m(-2) year(-1) at 200 and 1000 m depths, respectively; this suggested that transport of (137)Cs by zooplankton may be no trivial pathway.     

长江口南北支水沙特性观测研究

利用2009和2010年洪枯季、大小潮长江口南北支长时间序列的水沙盐观测资料,系统分析了近期南北支的水沙盐时空分布特征及南北支之间的关系,探讨了北支水沙盐倒灌,特别是泥沙倒灌对南支水域悬沙浓度的影响。分析结果表明:北支盐度和悬沙浓度年际、季节性及大小潮差异明显,一般大潮大于小潮,枯季大于洪季,平水年大于丰水年;南支受径流影响大,悬沙浓度均值在0.2kg/m3左右,盐度在0.25‰左右,南支悬沙浓度和盐度的大小均较北支小一个量级,其变化较北支复杂,尤其是在落潮时段盐度和悬沙浓度短时间内明显增加。北支作为河口唯一受潮汐控制的分支,水沙盐倒灌南支,倒灌期间南支悬沙浓度增加,洪季大潮有微弱沙量倒灌,悬沙浓度有0.05kg/m3的增幅,枯季大潮泥沙倒灌尤甚,南支悬沙浓度长时间维持在0.25kg/m3左右,最高可达0.62kg/m3。如上游径流量减小显著,则北支泥沙和盐水倒灌对南支的影响会增大。