Depth profile of ²³⁶U/²³⁸U in soil samples in La Palma, Canary Islands

The vertical distribution of the ²³⁶U/²³⁸U isotopic ratio was investigated in soil samples from three different locations on La Palma (one of the seven Canary Islands, Spain). Additionally the ²⁴⁰Pu/²³⁹Pu atomic ratio, as it is a well establish tool for the source identification, was determined. The radiochemical procedure consisted of a U separation step by extraction chromatography using UTEVA^® Resin (Eichrom Technologies, Inc.). Afterwards Pu was separated from Th and Np by anion exchange using Dowex 1x2 (Dow Chemical Co.). Furthermore a new chemical procedure with tandem columns to separate Pu and U from the matrix was tested. For the determination of the uranium and plutonium isotopes by alpha spectrometry thin sources were prepared by microprecipitation techniques. Additionally these fractions separated from the soil samples were measured by Accelerator Mass Spectrometry (AMS) to get information on the isotopic ratios ²³⁶U/²³⁸U, ²⁴⁰Pu/²³⁹Pu and ²³⁶U/²³⁹Pu, respectively. The ²³⁶U concentrations [atoms/g] in each surface layer (∼2 cm) were surprisingly high compared to deeper layers where values around two orders of magnitude smaller were found. Since the isotopic ratio ²⁴⁰Pu/²³⁹Pu indicated a global fallout signature we assume the same origin as the probable source for ²³⁶U. Our measured ²³⁶U/²³⁹Pu value of around 0.2 is within the expected range for this contamination source.     

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.     

Concentration and characterization of plutonium in soils of Hubei in central China

To study the Pu concentration and isotope ratio distributions present in China, the ^239+240Pu total activities and ²⁴⁰Pu/²³⁹Pu atom ratios in core soil samples from Hubei Province in central China were investigated using Accelerator Mass Spectrometry (AMS). The activities ranged from 0.019 to 0.502 mBq g⁻¹ and the ^239+240Pu inventories of 45 and ∼55 Bq m⁻² agree well with that expected from global fallout. The ²⁴⁰Pu/²³⁹Pu atom ratios in the soil ranged from 0.172 to 0.220. The ratios are similar to typical global fallout values. Hence, any close-in fallout contribution from the Chinese nuclear weapons tests, mainly conducted in the 1970s, must have either been negligible or had a similar ²⁴⁰Pu/²³⁹Pu ratio to that of global fallout. The top 10 cm layer of the soil contributes ∼90% of the total inventory and the maximum concentrations appeared in the 2-4 cm or 4-6 cm layers. It is suggested that climatic conditions and organic content are the two main factors that affect the vertical migration of plutonium in soil.     

Plutonium bioaccumulation in seabirds

The aim of the paper was plutonium (²³⁸Pu and ^239+240Pu) determination in seabirds, permanently or temporarily living in northern Poland at the Baltic Sea coast. Together 11 marine birds species were examined: 3 species permanently residing in the southern Baltic, 4 species of wintering birds and 3 species of migrating birds. The obtained results indicated plutonium is non-uniformly distributed in organs and tissues of analyzed seabirds. The highest plutonium content was found in the digestion organs and feathers, the smallest in skin and muscles. The plutonium concentration was lower in analyzed species which feed on fish and much higher in herbivorous species. The main source of plutonium in analyzed marine birds was global atmospheric fallout.     

The inflow of (238)Pu and (239+240)Pu from the Vistula River catchment area to the Baltic Sea

The aim of the work was to estimate plutonium inflow from the Vistula River’s catchments area to the Baltic Sea. There were differences in plutonium activities depending on season and sampling site. The highest activities of ²³⁸Pu and ^239+240Pu were transported from the Vistula River watershed to the Baltic Sea in spring and the lowest in summer. Annually, the southern Baltic Sea is enriched via the Vistula River with 10.3 MBq of ²³⁸Pu and 89.0 MBq of ^239+240Pu. The enhanced concentration of plutonium in water from the Vistula River is the result of its runoff from the Vistula drainage area, mostly from snowmelt, enhanced rainfalls and leached materials from river bed.     

Intake of ²³⁸U and ²³²Th through the consumption of foodstuffs by tribal populations practicing slash and burn agriculture in an extremely high rainfall area

The concentration of naturally occurring radionuclides ²³²Th, ²³⁸U was determined using Instrumental Neutron Activation Analysis (INAA) in different food groups namely cereals, vegetables, leafy vegetables, roots and tubers cultivated and consumed by tribal population residing around the proposed uranium mine. The study area is a part of rural area K. P. Mawthabah (Domiasiat) in the west Khasi Hills District of Meghalaya, India located in the tropical region of high rainfall that remains steeped in tribal tradition without much outside influence. Agriculture by Jhum (slash and burn) cultivation and animal husbandry are the main occupation of the tribal populations. A total of 89 samples from locally grown food products were analyzed. The concentration of ²³⁸U and ²³²Th in the soil of the study area was found to vary 1.6-15.5 and 2.0-5.0 times respectively to the average mean value observed in India. The estimated daily dietary intake of ²³⁸U and ²³²Th were 2.0 μg d⁻¹ (25 mBq d⁻¹) and 3.4 μg d⁻¹ (14 mBq d⁻¹) is comparable with reported range 0.5-5.0 μg d⁻¹ and 0.15-3.5 μg d⁻¹ respectively for the Asian population.     

Uranium isotopes in groundwater from the continental intercalaire aquifer in Algerian Tunisian Sahara (Northern Africa)

The disequilibrium between ²³⁴U and ²³⁸U is commonly used as a tracer of groundwater flow. This paper aims to identify uranium contents and uranium isotopic disequilibria variation in groundwater sampled from deep Continental Intercalaire aquifer (southern Algeria and Tunisia). Large variations in both U contents (0.006–3.39 ppb) and ²³⁴U/²³⁸U activity ratios (0.4–15.38) are observed. We conduct a first assessment in order to verify whether the results of our investigation support and complete previous hydrogeological and isotopic studies. The dissolved U content and ²³⁴U/²³⁸U activity ratio data were plotted on a two-dimensional diagram that was successfully utilized on sharing the CI aquifer into different compartments submitted to different oxidising/reducing conditions and leads also to distinguished two preferential flow paths in the Nefzaoua/Chott Fejej discharge area. Uranium isotopes disequilibrium indicate that ranium chemistry is mainly controlled by water–rock interaction enhanced by long residence time recognised for this aquifer.     

Plutonium isotopes in surface air of Prague in 1986–2006

Monitoring of ^239,240Pu in surface air of Prague started in 1986 in connection with the Chernobyl accident. Measurable activities of 10–28 μBq m⁻³ were found from 29 April 1986 to 5 May 1986. In the most of the monitoring periods of 1987–1996, activities of ^239,240Pu in air were not measurable. Positive values for ^239,240Pu and ²³⁸Pu in air could be obtained after installation of an aerosol sampler with higher flow-rate in 1997. Activity concentrations of ^239,240Pu and ²³⁸Pu in Prague air in the most of quarters of 1997–2006 were in the range 0.53–5.06 and <0.16–1.10 nBq m⁻³, respectively. Seasonal fluctuations can be found in content of ^239,240Pu in air. Activity ratios of ²³⁸Pu/^239,240Pu in air are higher than those in top soil, so it can be supposed that ²³⁸Pu is coming to air of Prague also from other sources than resuspension of fallout from atmospheric nuclear tests.     

Uranium isotopes in Tunisian bottled mineral waters

²³⁴U and ²³⁸U activity concentrations and their relative effective doses have been determined in 10 bottled mineral waters in Tunisia. Alpha spectrometry was used as technique to measure uranium isotopes. The obtained isotopic ratio ²³⁴U/²³⁸U varies between 1.1 and 3 which means that the two isotopes are not in radioactive equilibrium. Measured activity concentration varies between 3.2 and 40 mBq/l for ²³⁴U and between 1.5 and 26.3 mBq/l for ²³⁸U. Effective doses (assuming 2 litres per day of water consumption) coming from this two isotopes are found to vary between 0.16 and 2.02 μSv/a which is lower than the maximum recommended dose level by the WHO.     

Characterization of plutonium in deep-sea sediments of the Sulu and South China Seas

Anthropogenic Pu isotopes are important geochemical tracers for sediment studies. Their distributions and sources in the water columns as well as the sediments of the North Pacific have been intensively studied; however, information about Pu in the Southeast Asian seas is limited. To study the isotopic composition of Pu, and thus to identify its sources, we collected sediment core samples in the South China Sea and the Sulu Sea during the KH-96-5 Cruise of the R/V Hakuho Maru. We analysed the activities of ^239+240Pu and the atom ratios of ²⁴⁰Pu/²³⁹Pu using isotope dilution sector-field inductively coupled plasma mass spectrometry (SF-ICP-MS). The ²⁴⁰Pu/²³⁹Pu atom ratios in the sediments of both areas (inventory weighted mean: 0.251 for the South China Sea and 0.280 for the Sulu Sea) were higher than the global fallout value (0.178 ± 0.019), suggesting the existence of Pu from the Pacific Proving Grounds in the North Pacific. Low inventories of ^239+240Pu in sediments were observed in the South China Sea (3.75 Bq/m²) and the Sulu Sea (1.38 Bq/m²). Most of the Pu input is still present in the water column. Scavenging and benthic mixing processes were considered to be the main processes controlling the distribution of Pu in the deep-sea sediments of both study areas.     

Radioactivity measurements in moss (Hypnum cupressiforme) and lichen (Cladonia rangiformis) samples collected from Marmara region of Turkey

The present study was conducted to compare the ¹³⁷Cs, ⁴⁰K, ²³²Th, and ²³⁸U activity concentrations in epigeic moss (Hypnum cupressiforme) and lichen (Cladonia rangiformis). The activity levels in 37 moss and 38 lichen samples collected from the Marmara region of Turkey were measured using a gamma spectrometer equipped with a high purity germanium (HPGe) detector. The activity concentrations of ¹³⁷Cs, ⁴⁰K, ²³²Th, and ²³⁸U in the moss samples were found to be in the range of 0.36-8.13, 17.1-181.1, 1.51-6.17, and 0.87-6.70 Bq kg⁻¹ respectively, while these values were below detection limit (BDL)-4.32, 16.6-240.0, 1.32-6.47, and BDL-3.57 Bq kg⁻¹ respectively in lichen. The average moss/lichen activity ratios of ¹³⁷Cs, ⁴⁰K, ²³²Th, and ²³⁸U were found to be 1.32 ± 0.57, 2.79 ± 1.67, 2.11 ± 0.82, and 2.19 ± 1.02, respectively. Very low ¹³⁷Cs concentrations were observed in moss and lichen samples compared to soil samples collected from the same locations in a previous study. Seasonal variations of the measured radionuclide activities were also examined in the three sampling stations.     

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.     

Plutonium isotopes concentration in seawater and bottom sediment off the Pacific coast of Aomori sea area during 1991-2005

A radioactivity survey was launched in 1991 to determine the background levels of ^239+240Pu in the marine environment off a commercial spent nuclear fuel reprocessing plant before full operation of the facility. Particular attention was focused on the ²⁴⁰Pu/²³⁹Pu atom ratio in seawater and bottom sediment to identify the origins of Pu isotopes. The concentration of ^239+240Pu was almost uniform in surface water, decreasing slowly over time. Conversely, the ^239+240Pu concentration varied markedly in the bottom water and was dependent upon the sampling point, with higher concentrations of ^239+240Pu observed in the bottom water sample at sampling points having greater depth. The ²⁴⁰Pu/²³⁹Pu atom ratio in the seawater and sediment samples was higher than that of global fallout Pu, and comparable with the data in the other sea area around Japan which has likely been affected by close-in fallout Pu originating from the Pacific Proving Grounds. The ²⁴⁰Pu/²³⁹Pu atom ratio in bottom sediment samples decreased with sea depth. The land-originated Pu is not considered as the reason of the increasing ^239+240Pu concentration and also decreasing the ²⁴⁰Pu/²³⁹Pu atom ratio with sea depth, and further study is required to clarify it.     

Concentrations of U,U, U,Th, Th,Th, Ra,Ra, Ra,Po, Pb and Pb in drinking water in Italy: reconciling safety standards based on measurements of gross α and β

Some important naturally occurring α- and β-radionuclides in drinking water samples collected in Italy were determined and the radiological quality evaluated. The mean activity concentrations (mBq L⁻¹) of the radionuclides in the water samples were almost in the order: 26 ± 36 (²³⁴U) > 21 ± 30 (²³⁸U) > 8.9 ± 15 (²²⁶Ra) > 4.8 ± 6.3 (²²⁸Ra) > 4.0 ± 4.1 (²¹⁰Pb) > 3.2 ± 3.7 (²¹⁰Po) > 2.7 ± 1.2 (²¹²Pb) > 1.4 ± 1.8 (²²⁴Ra) > 1.1 ± 1.3 (²³⁵U) > 0.26 ± 0.39 (²²⁸Th) > 0.0023 ± 0.0009 (²³⁰Th) > 0.0013 ± 0.0006 (²³²Th). The mean estimated dose (μSv yr⁻¹) to an adult from the water intake was in this order: 2.8 ± 3.3 (²¹⁰Po) > 2.4 ± 3.2 (²²⁸Ra) > 2.1 ± 2.1 (²¹⁰Pb) > 1.8 ± 3.1 (²²⁶Ra) > 0.94 ± 1.30 (²³⁴U) > 0.70 ± 0.98 (²³⁸U) > 0.069 ± 0.087 (²²⁴Ra) > 0.036 ± 0.044 (²³⁵U) > 0.014 ± 0.021 (²²⁸Th) > 0.012 ± 0.005 (²¹²Pb) > 0.00035 ± 0.00029 (²³⁰Th) > 0.00022 ± 0.00009 (²³²Th). It is obvious that ²¹⁰Po, ²²⁸Ra, ²¹⁰Pb and ²²⁶Ra are the most important dose contributors in the drinking water intake. As far as the seventeen brands of analysed drinking water were concerned, the committed effective doses were in the range of 2.81–38.5 μSv yr⁻¹, all well below the reference level of the committed effective dose (100 μSv yr⁻¹) recommended by the WHO. These data throw some light on the scale of the radiological impact on the public from some naturally occurring radionuclides in drinking water, and can also serve as a comparison for the dose contribution from artificial radionuclides released to the environment as a result of human practices. Based on the radionuclide composition in the analysed waters, comment was made on the new screening level for gross α activity in guidelines for drinking-water quality recommended by the WHO, 2004.     

Artificial radionuclides in the atmosphere over Lithuania

Measurements of airborne radioactive aerosol concentration were carried out on the basis of 1-3 days samples after the Chernobyl disaster and during the period of 1992-2003. Transport of "hot" particles of different composition resulted in the high activity concentrations of (137)Cs, (238)Pu, (239,240)Pu and (241)Am in the atmosphere in Vilnius at the end of April 1986. The (240)Pu/(239)Pu atom ratio showed clear evidence of non-global plutonium originating from the Chernobyl accident in the atmosphere over Lithuania. The (240)Pu/(239)Pu atom ratio ranged from 0.14 to 0.40 in monthly samples in Vilnius in 1995-2003. An increase in activity concentration of (137)Cs by a factor of 100 (up to 300 microBq/m(3)) was found following forest fires in the Ukraine and Belarus. However, no transport of the Chernobyl plutonium was observed and the (240)Pu/(239)Pu atom ratio in samples collected during the forest fires was found to be 0.229 and 0.185, respectively. The exponential decrease in the (240)Pu/(239)Pu atom ratio from 0.30 to 0.19 (mean values) was observed in 1995-2003.     

Plutonium, 137Cs and 90Sr in selected invertebrates from some areas around Chernobyl nuclear power plant

Results are presented for ¹³⁷Cs, ⁹⁰Sr and plutonium activity concentrations in more than 20 samples of terrestrial invertebrates, including species of beetles, ants, spiders and millipedes, collected in the highly contaminated area of the Chernobyl exclusion zone. The majority of samples were collected in Belarus, with some also collected in the Ukraine. Three other samples were collected in an area of lower contamination. Results show that seven samples exceed an activity concentration of 100 kBq/kg (ash weight - a.w.) for ¹³⁷Cs. The maximum activity concentration for this isotope was 1.52 ± 0.08 MBq/kg (a.w.) determined in ants (Formica cynerea). Seven results for ⁹⁰Sr exceeded 100 kBq/kg (a.w.), mostly for millipedes. Relatively high plutonium activity concentrations were found in some ants and earth-boring dung beetles. Analyses of activity ratios showed differences in transfer of radionuclides between species. To reveal the correlation structure of the multivariate data set, the Partial Least-Squares method (PLS) was used. Results of the PLS model suggest that high radiocesium activity concentrations in animal bodies can be expected mainly for relatively small creatures living on the litter surface. In contrast, high strontium activity concentrations can be expected for creatures which conduct their lives within litter, having mixed trophic habits and a moderate lifespan. No clear conclusions could be made for plutonium.     

Observations and modelling of thoron and its progeny in the soil-atmosphere-plant system

Samples of pasture vegetation, mainly Trifolium pratensis, were collected at the Botanic Garden of the University of Bologna during the period 1998-2000 and measured by gamma-spectrometry for determining thoron progeny. Concentrations of ²¹²Pb were between 1.5 and 20 Bq m⁻², with individual peaks up to 70 Bq m⁻². Soil samples were collected at the same location and physically characterised. Their chemical composition (particularly Th and U) was determined by X-ray fluorescence spectroscopy. Lead-212 on plants mainly originates from dry and wet deposition of this isotope generated in the lower atmosphere by the decay of its short-lived precursor ²²⁰Rn, which is produced in the upper soil layers as a member of the natural thorium decay chain and exhales into the atmosphere. Concentrations of ²²⁰Rn in the atmosphere depend on (1) the amount of Th present in soil, (2) the radon fraction which escapes from the soil minerals into the soil pore space, (3) its transport into the atmosphere, and (4) its redistribution within the atmosphere. The mobility of radon in soil pore space can vary by orders of magnitude depending on the soil water content, thus being the main factor for varying concentrations of ²²⁰Rn and ²¹²Pb in the atmosphere. We present a simple model to predict concentrations of thoron in air and its progeny deposited from the atmosphere, which takes into account varying soil moisture contents calculated by the OPUS code. Results of this model show close agreement with our observations.     

Development of an energy discriminate CR-39(®) nuclear track etch dosimeter for Radon-220 gas measurements

An energy discriminate CR-39^® nuclear track etch dosimeter for use in a ²²⁰Rn and ²²²Rn gas monitor has been developed and experimentally assessed. It utilises a thin film of Mylar^® C to attenuate the alpha particle energies to allow only the damage tracks created by the 8.785 MeV alpha particles emitted from ²¹²Po of the ²³²Th decay chain to be registered in the CR-39^® plaque, allowing for the direct measurement of ²²⁰Rn gas concentrations. The dosimeter was developed through a combination of experimental investigations and theoretical simulations using the Monte Carlo ion transport modelling program Stopping and Range of Ions in Materials (SRIM 2008). A film thickness of 54 μm has been shown to attenuate all alpha energies less then 7.7 MeV.     

Determination of total content and isotopic compositions of plutonium and uranium in environmental samples for safeguards purposes by ICP-QMS

The aim of this work was to determine the concentrations and isotopic compositions of plutonium and uranium in environmental samples for safeguards purposes. An analytical method was developed with a plutonium and uranium separation procedure based on extraction chromatography (using 2 mL TEVA and UTEVA columns) and detection with a quadrupole ICP-MS applying an ultra-sonic nebulizer coupled with a membrane desolvation system. Starting from blank swipes, the background equivalent concentration (BEC) was 8 fg for ²³⁹Pu and 1 ng ²³⁸U. The method was successfully applied to certified reference materials as well as to round robin samples obtained in the framework of the inter-laboratory exercise program, promoted by the Brazilian–Argentine Agency for Accounting and Control of Nuclear Materials (ABACC), together with the US Department of Energy (USDOE). After the introduction of an additional ion-exchange separation step, the methodology was applied to the IAEA-384 sediment reference sample with precise and accurate total plutonium and uranium, ²⁴⁰Pu/²³⁹Pu, ²⁴¹Pu/²³⁹Pu, ²³⁴U/²³⁸U and ²³⁵U/²³⁸U atomic ratio results.     

Correlations between potassium, rubidium and cesium ((133)Cs and (137)Cs) in sporocarps of Suillus variegatus in a Swedish boreal forest

An analysis of sporocarps of ectomycorrhizal fungi Suillus variegatus assessed whether cesium (¹³³Cs and ¹³⁷Cs) uptake was correlated with potassium (K) or rubidium (Rb) uptake. The question was whether intraspecific correlations of Rb, K and ¹³³Cs mass concentrations with ¹³⁷Cs activity concentrations in sporocarps were higher within, rather than among, different fungal species, and if genotypic origin of sporocarps within a population affected uptake and correlation. Sporocarps (n = 51) from a Swedish forest population affected by the fallout after the Chernobyl accident were studied. The concentrations were 31.9 ± 6.79 g kg⁻¹ for K (mean ± SD, dwt), 0.40 ± 0.09 g kg⁻¹ for Rb, 8.7 ± 4.36 mg kg⁻¹ for ¹³³Cs and 63.7 ± 24.2 kBq kg⁻¹ for ¹³⁷Cs. The mass concentrations of ¹³³Cs correlated with ¹³⁷Cs activity concentrations (r = 0.61). There was correlation between both ¹³³Cs concentrations (r = 0.75) and ¹³⁷Cs activity concentrations (r = 0.44) and Rb, but the ¹³⁷Cs/¹³³Cs isotopic ratio negatively correlated with Rb concentration. Concentrations of K and Rb were weakly correlated (r = 0.51). The ¹³³Cs mass concentrations, ¹³⁷Cs activity concentrations and ¹³⁷Cs/¹³³Cs isotopic ratios did not correlate with K concentrations. No differences between, within or, among genotypes in S. variegatus were found. This suggested the relationships between K, Rb, ¹³³Cs and ¹³⁷Cs in sporocarps of S. variegatus is similar to other fungal species.