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 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.     

Determination of U, Pu and Am isotopes in Irish Sea sediment by a combination of AMS and radiometric methods

Samples from a marine sediment core from the Irish Sea (54.416 N, 3.563 W) were analyzed for the isotopic composition of uranium, plutonium and americium by a combination of radiometric methods and AMS. The radiochemical procedure consisted of a Pu separation step by anion exchange, subsequent U separation by extraction chromatography using UTEVA^® and finally Am separation with TRU^® Resin.Additionally to radiometric determination of these isotopes by alpha spectrometry, the separated samples were also used for the determination of ²³⁶U/²³⁸U and plutonium isotope ratios by Accelerator Mass Spectrometry (AMS) at the VERA facility.     

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.     

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.     

Estimates of (239+240)Pu inventories in Gdańsk Bay and Gdańsk basin

This paper presents and discusses the results of (239+240)Pu determinations in different components of Gdańsk bay and Gdańsk basin ecosystem, as well as estimated sources and inventories of plutonium in these basins. The total plutonium (239+240)Pu activities deposited in Gdańsk bay and Gdańsk basin sediments are 1.18 TBq and 3.77 TBq, respectively. Two rivers, the Vistula and Neman rivers, and atmospheric fallout were distinguished as the main sources of plutonium in these basins. In seawater (with suspended matter included) there is about 2.33 GBq (239+240)Pu (0.2% of total activity) in Gdańsk bay and 9.92 GBq (239+240)Pu (0.3% of total activity) in Gdańsk basin. In both cases, 56% of (239+240)Pu is associated with suspended matter. Organisms contain 3.81 MBq in Gdańsk bay and 7.45 MBq (239+240)Pu in Gdańsk basin. From this value in Gdańsk bay 82.1% of plutonium is associated with zoobenthos, 13.6% with phytobenthos, 1.6% with phytoplankton, 1.5% with zooplankton and 1.2% with fish. In Gdańsk basin, 83.2% is associated with zoobenthos, 7.5% with phytobenthos, 3.6% with phytoplankton, 3.2% with zooplankton and 2.5% with fish.     

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 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.     

Plutonium as a chronomarker in Australian and New Zealand sediments: a comparison with Cs

The construction of high resolution chronologies of sediment profiles corresponding to the last 50-100 years usually entails the measurement of fallout radionuclides ²¹⁰Pb and ¹³⁷Cs. The anthropogenic radionuclide, ¹³⁷Cs, originating from atmospheric nuclear weapons testing can provide an important “first appearance” horizon of known age (1954-1955), providing much-needed validation for the sometimes uncertain interpretations associated with ²¹⁰Pb geochronology. However, while ¹³⁷Cs usually provides a strong signal in sediment in the northern hemisphere, total fallout of ¹³⁷Cs in the southern hemisphere was only 25% that of the north and the low activities of ¹³⁷Cs seen in Australian and New Zealand sediments can make its horizon of first appearance somewhat arguable. Low ¹³⁷Cs fallout also limited the size of the 1963-1964 fallout peak, a peak that is usually seen in northern hemisphere sediment profiles but is often difficult to discern south of the equator.This paper shows examples of the use of nuclear weapons fallout Pu as a chronomarker in sediment cores from Australia (3 sites) and New Zealand (1 site). The Pu profiles of five cores are examined and compared with the corresponding ¹³⁷Cs profiles and ²¹⁰Pb geochronologies. We find that Pu has significant advantages over ¹³⁷Cs, including greater measurement sensitivity using alpha spectrometry and mass spectrometric techniques compared to ¹³⁷Cs measurements by gamma spectrometry. Moreover, Pu provides additional chronomarkers associated with changes in the Pu isotopic composition of fallout during the 1950s and 1960s. In particular, the ²³⁸Pu/^239+240Pu activity ratio shows distinct shifts in the early 1950s and the mid to late 1960s, providing important known-age horizons in southern hemisphere sediments. For estuarine and near-shore sediments Pu sometimes has another significant advantage over ¹³⁷Cs due to its enrichment in bottom sediment relative to ¹³⁷Cs resulting from the more efficient scavenging of dissolved Pu in seawater by sediment particles.     

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.     

Radiological monitoring: terrestrial natural radionuclides in Kinta District,Perak, Malaysia

Natural background gamma radiation and radioactivity concentrations were investigated from 2003 to 2005 in Kinta District, Perak, Malaysia. Sample locations were distant from any ‘amang’ processing plants. The external gamma dose rates ranged from 39 to 1039 nGy h⁻¹. The mean external gamma dose rate was 222 ± 191 nGy h⁻¹. Small areas of relatively enhanced activity were located having external gamma dose rates of up to 1039 ± 104 nGy h⁻¹. The activity concentrations of ²³⁸U, ²³²Th and ⁴⁰K were analyzed by using a high-resolution co-axial HPGe detector system. The activity concentration ranges were 12–426 Bq kg⁻¹ for ²³⁸U, 19–1377 Bq kg⁻¹ for ²³²Th and <19–2204 Bq kg⁻¹ for ⁴⁰ K. Based on the radioactivity levels determined, the gamma-absorbed dose rates in air at 1 m above the ground were calculated. The calculated dose rates and measured dose rates had a good correlation coefficient, R of 0.94. To evaluate the radiological hazard of the natural radioactivity, the radium equivalent activity, the gamma-absorbed dose rate and the mean population weighted dose rate were calculated. An isodose map for the Kinta District was also produced.     

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.     

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.     

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.     

Origin and transport of U and Ra in riverine,estuarine and marine sediments of the Krka River,Croatia

Spatial distribution of ²³⁸U and ²²⁶Ra activities in sediment columns along the Krka River and estuary, were studied using gamma spectrometry. Markedly different ²³⁸U and ²²⁶Ra activities between riverine, estuarine and marine sediments were observed. Distribution of these radionuclides, as well as their anthropogenic and natural origin, was evaluated by activity measurements, taking into account sedimentation rates estimated by ¹³⁷Cs distribution in sediment columns.     

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.