Quantitative estimation of dust transport in the desert region of northwest China by plutonium isotopes.

Dust is an important source of atmospheric pollution, and quantitative estimation of desert dust transport is crucial for air pollution control. In this study, five typical sandy soil profiles in the Tengger Desert were collected and analyzed for 239,240Pu concentration and 240Pu/239Pu atomic ratios in order to identify the source of 239,240Pu in this area and explore the sedimentary characteristics of dust in different profiles. The results revealed that the concentrations of 239,240Pu in the soil profiles were between 0.002 and 0.443 mBq/g with an exception of the deep layer soil at one site. The measured atomic ratios of 240Pu/239Pu are at the global atmospheric fallout level with a mean of 0.184 ± 0.020, indicating that global fallout is the dominant source of plutonium in this region. The total inventories of 239,240Pu in the reference sites in this area were estimated to be 39.2-44.6 Bq/m2, this is in agreement with the value from the global fallout of atmospheric nuclear weapon tests at the similar latitude (30-40 °N: 42 Bq/m2). The estimated erosion rate in the erosion profile utilizing soil erosion intensity mode is 2491 t/km2/yr and the soil erosion depth is 9.86 cm, While, the stacking rate of the accumulation profile is 1383 t/km2/yr, and the depth of accumulation is estimated to be 5.48 cm. The difference between the erosion and accumulation profiles indicated that approximately 1107 t/km2/yr of dust was exported from the Gobi landform area of the Tengger Desert, which might be transported long distance in the downwind direction.

Level, distribution and sources of Np, Pu and Am isotopes in Peter the Great Bay of Japan sea.

Transuranium elements such as Np, Pu and Am, are considered to be the most important radioactive elements in view of their biological toxicity and environmental impact. Concentrations of 237Np, Pu isotopes and 241Am in two sediment cores collected from Peter the Great Bay of Japan Sea were determined using radiochemical separation combined with inductively coupled plasma mass spectrometry (ICP-MS) measurement. The 239,240Pu and 241Am concentrations in all sediment samples range from 0.01 Bq/kg to 2.02 Bq/kg and from 0.01 Bq/kg to 1.11 Bq/kg, respectively, which are comparable to reported values in the investigated area. The average atomic ratios of 240Pu/239Pu (0.20 ± 0.02 and 0.21 ± 0.01) and 241Am/239+240Pu activity ratios (3.32 ± 2.76 and 0.45 ± 0.17) in the two sediment cores indicated that the sources of Pu and Am in this area are global fallout and the Pacific Proving Grounds through the movement of prevailing ocean currents, and no measurable release of Np, Pu and Am from the local K-431 nuclear submarine incident was observed. The extremely low 237Np/239Pu atomic ratios ((2.0-2.5) × 10-4) in this area are mainly attributed to the discrepancy of their different chemical behaviors in the ocean due to the relatively higher solubility of 237Np compared to particle active plutonium isotopes. It was estimated using two end members model that 23% ± 6% of transuranium radionuclides originated from the Pacific Proving Grounds tests, and the rest (ca. 77%) from global fallout.

A multi-collector ICP-MS method for quantification of plutonium, uranium, and americium in hair and nails of occupationally or medically exposed individuals.

The 239Pu, 238U, and 241Am concentrations and 239Pu/240Pu, 235U/238U, and 236U/238U atom ratios were measured in the hair and nail samples using a new method utilized TEVA, UTEVA, and DGA extraction chromatography and multi-collector ICP-MS. Samples were collected from individuals who donated their bodies to the United States Transuranium and Uranium Registries. The concentration of 239Pu ranged from 0.22 to 15.8 ng/kg. The 240Pu/239Pu isotopic ratios ranged from 0.026 to 0.127 which is consistent with weapons-grade plutonium. Concentration of uranium fell between 1.84 µg/kg and 29.5 µg/kg and 235U/238U ratios ranged from 4.8 × 10-3 to 7.6 × 10-3. Elevated 236U/238U atom ratios were measured in two cases and ranged from 5.0 × 10-6 - 2.4 × 10-5 indicating exposure to spent or reprocessed uranium material. The concentration of 241Am was measured in four hair samples and ranged from 0.02 to 0.21 ng/kg.

The records of 239+240Pu and 137Cs of global fallout in Lake East Dongting Sediments and Responses to watershed environmental changes.

Plutonium-239 + 240 and 137Cs in the environment can usually be used to track the impact of nuclear activities on the environment, and have become important tools in environmental geochemical studies. In this study, nine sediment cores (E1-E9) in Lake East Dongting were collected and measured for the activity concentration of 239+240Pu, 137Cs and the atomic ratio of 240Pu/239Pu, and then their vertical distribution characteristics were analyzed. The results show that: the activity concentrations of 137Cs and 239+240Pu in Lake East Dongting ranged from 5.26 ± 0.43 to 28.6 ± 2.23 Bq kg-1 and 0.29 ± 0.02 to 1.37 ± 0.09 Bq kg-1, with an average of 7.48 ± 0.68 Bq kg-1 and 0.39 ± 0.03 Bq kg-1, respectively. The atomic ratios of 240Pu/239Pu are 0.168 ± 0.012-0.211 ± 0.015, which are basically consistent with the global atmospheric deposition. The vertical profiles of 137Cs and 239+240Pu in sediment cores show obvious single-peak distribution in E1-E6 and bimodal distribution in E7-E9. The results of sedimentation rates calculated by 137Cs and 239+240Pu method ranged from 0.59 cm y-1 to 1.99 cm y-1 with a mean of 1.18 cm y-1 and 0.61 cm y-1 to 2.18 cm y-1 with a mean of 1.26 cm y-1. The inventories of 137Cs and 239+240Pu in nine sediment cores are 5.87-10.8 kBq m-2 and 307-545 Bq m-2, which are about 8-14 and 9-15 times the inventory in the global average atmospheric deposition at the same latitude respectively. Comparing the results of the sedimentation rates and the inventories from different sampling points indicates that extreme climatic events and human activities have a significant impact on sediment environment of Lake East Dongting.

Particulate matter from water moss of a large Siberian river: Morphometric, mineral, elemental and radionuclide composition.

Particulate matter trapped by tufts of water moss Fontinalis antipyretica inhabiting fast flowing waters of the Yenisei River (Siberia, Russia) contaminated with artificial radionuclides has been studied as a potential monitor of radioactive releases to the river. Particulate matter, which was removed from wet tufts of water moss of the Yenisei by rinsing them in water, constituted at least 38% of bulk dry weight of the moss biomass sample and was similar in the contents of chemical elements, minerals, organic matter, and artificial radionuclides to bottom sediments of the Yenisei. Considerable bulk percentages of artificial radionuclides in the sample of water moss, 77% of 137Cs, 44% of 60Co, 41% of 152Eu, 55% of 154Eu, 66% of 241Am, and 34-36% of plutonium were associated with extracellular particles. The comparative study and correlation analysis suggested that 137Cs was mainly associated with mineral particles trapped by moss and that organic matter was responsible for binding plutonium in samples of water moss. Consequently, analysis of extracellular particles of water moss can provide data on contents and speciation of radionuclides transported by water current. Although a considerably high proportion of particulate matter had been washed out from tufts of water moss, some extracellular mineral particulate material and a large number of epiphytic diatoms remained attached to leaves of water moss. Our study proves that particulate matter trapped by water moss can be used as an informative monitor to trace radioactive pollutants transported by water current in running waters deficient in bottom sediments and potential biomonitors.

Spatial distribution and modelling of 239+240Pu in the sediments and seawater columns of the South China Sea and Indian Ocean.

In order to investigate the 239+240Pu potential influence in the ocean, and develop a new method for rapidly monitoring radioactive pollution, the 239+240Pu spatial distribution in the South China Sea (SCS) and the Indian Ocean (IND) sediments is analyzed by SF-ICP-MS (ELEMENT 2). The inventory-weighted mean activities of 239+240Pu were 0.413 ± 0.333 mBq/g, 0.128 ± 0.044 mBq/g, and 0.483 ± 0.606 mBq/g in the sediments of the SCS, eastern IND, and Arabian Sea, respectively. The 239+240Pu activity spatial distribution in the SCS sediments was influenced by the current, the vertical distribution of Pu in seawater, and the transport of particulate matter. The 239+240Pu activity spatial distribution in the IND sediments could be impacted by Antarctic Intermediate Water. The average of 240Pu/239Pu atomic ratios were 0.258 ± 0.034, 0.219 ± 0.031, and 0.212 ± 0.028 in the sediments of the SCS, eastern IND, and Arabian Sea, respectively. The 240Pu/239Pu atomic ratios in the SCS and IND indicate that Pu from the Pacific Proving Ground (PPG) is transported to the IND via the SCS internal current and transverse ocean currents within Indonesia. In addition, a seawater advection-dispersion equation (S-ADE) model is established based on the actual physical processes of radionuclides in the seawater column and well fitting results were obtained (R2 = 0.49 to 0.99). The 239+240Pu data and the geographic information from the sample site were used to correct the Pu distribution in the seawater. The calculated 239+240Pu mean concentrations in the surface seawater were 2.465 mBq/m3 and 2.205 mBq/m3 for the SCS and the eastern IND seawater, respectively, and the result is consistent with the previous measurements. Then, the 239+240Pu stored in the study area of SCS and eastern IND was estimated to be approximately 1.0-1.4% of the global ocean based on the model. This study provides a useful model for guiding and designing future monitoring of pollution by anthropogenic Pu and other isotopes.

Spatial distribution, source identification, and transportation paths of plutonium in the Beibu Gulf, South China Sea.

To investigate the spatial distribution and source of plutonium isotopes in the Beibu Gulf, surface sediments were collected and analyzed using sector field inductively coupled plasma mass spectrometry (SF-ICP-MS). The activities of 239+240Pu in surface sediments ranged from 0.012 to 0.451 mBq/g (mean: 0.171 ± 0.138 mBq/g, n = 36), indicating a decreasing trend in a counterclockwise direction from the southern bay mouth. The counterclockwise decreasing trend in the south of the bay mouth is similar to the current in the Beibu Gulf. The 240Pu/239Pu atom ratios in surface sediments ranged from 0.156 to 0.283 (mean: 0.236 ± 0.031, n = 36), slightly higher than that of the global fallout value of 0.18. This suggests that the Pu in the Beibu Gulf was a combination of global fallout and Pacific Proving Ground (PPG). The average contribution of the plutonium (Pu) derived from the PPG in the sediment was estimated to be 52 % ± 24 %.

Parallels between natural Oklo reaction zones and industrial reactors dynamics.

The first man-made nuclear reactor was developed by Fermi and collaborators at the University of Chicago and reached criticality in December 1942. This was the confirmation that men were able to use sustained fission reactions in order to produce energy. Following this success, nuclear reactors studies gave rise to several families of reactors corresponding to different orientations and technical choices. They are linked mainly to the choice of fuel (natural uranium, enriched uranium, plutonium, thorium), coolant (water, carbon dioxide, helium, sodium, ...) and moderator for slow neutron reactors (graphite, light water, heavy water). Out of all these choices, the pressurized water reactor (PWR) family is the closest to the Oklo natural reactors. Many intriguing similarities are observed and discussed in the present article. Our present-day understanding of the PWR operating conditions has been a great help for understanding the Oklo reactors.

Modified human respiratory tract model to describe the retention of plutonium in scar tissues.

The Human Respiratory Tract Model described in Publication 130 of the International Commission on Radiological Protection provides some mechanisms to account for retention of material that can be subject to little to no mechanical transport or absorption into the blood. One of these mechanisms is 'binding', which refers to a process by which a fraction ('bound fraction') of the dissolved material chemically binds to the tissue of the airway wall. The value of the bound fraction can have a significant impact on the radiation doses imparted to different parts of the respiratory tract. To properly evaluate-and quantify-bound fraction for an element, one would need information on long-term retention of the element in individual compartments of the respiratory tract. Such data on regional retention of plutonium in the respiratory tract of four workers-who had inhaled materials with solubility ranging from soluble nitrate to very insoluble high-fired oxides-were obtained at the United States Transuranium and Uranium Registries. An assumption of bound fraction alone was found to be inconsistent with this dataset and also with a review of the literature. Several studies show evidence of retention of a large amount of Pu activity in the scar tissues of humans and experimental animals, and accordingly, a model structure with scar-tissue compartments was proposed. The transfer rates to these compartments were determined using Markov Chain Monte Carlo analysis of the bioassay and post-mortem data, considering the uncertainties associated with deposition, dissolution and particle clearance parameters. The models predicted that a significant amount-between 20 and 100% for the cases analyzed-of plutonium retained in the respiratory tract was sequestered in the scar tissues. Unlike chemically-bound Pu that irradiates sensitive epithelial cells, Pu in scar tissues may not be dosimetrically significant because the scar tissues absorb most, if not all, of the energy from alpha emissions.

Rapid measurement of actinides in urine by mass and alpha spectrometric methods.

To provide timely information for prompting decision-making in emergency radiation therapy, we developed simple and rapid mass and alpha spectrometric methods for urinary bioassays to determine ultra-trace actinide isotopes. For the mass spectrometric method, after organic matter decomposition, LaF3/CaF2 co-precipitation and chromatographic purification using 2 ml of AG MP-1 M anion exchange resin, U and Pu isotopes were measured in a 20-ml urine sample by inductively coupled plasma-mass spectrometry. In the alpha spectrometric method, after organic matter decomposition, iron hydroxide co-precipitation and chromatographic purification using 2 ml of TEVA and 2 ml of DGA resin cartridges, Pu, U and Am/Cm isotopes were measured in a 500-ml urine sample by alpha spectrometry. These alpha and mass spectrometric methods were then applied for participation in the 2020 intercomparison organized by the Association for the PROmotion of Quality COntrol in RADiotoxicological Analysis (PROCORAD), France, for method validations.

Comparison for the simultaneous determination of 237Np and Pu isotopes between TEVA and TK200 resin.

A reliable and stable method was developed to accurately analyze neptunium (237Np) and plutonium isotopes in environmental samples using 242Pu or 236Pu as a tracer. Key parameters, including the valence adjustment conditions and the stabilities of Pu and Np in the different resins, were investigated using TK200 and TEVA resin. It was found that Pu and Np could be efficiently extracted simultaneously using TK200 resin under the optimal loading conditions (6-12 M HNO3) with the addition of 0.01-0.12 M NaNO2 for valence adjustment. These isotopes were subsequently stripped out using a solution containing 0.1 M HCl, 0.05 M HF, and 0.01 M NH2OH·HCl. The separation efficiencies of Pu and Np were >93%, and the chemical yield ratio between Np and Pu was maintained steady at an average of 1.00 ± 0.03 (n > 50) under the optimal conditions. The analytical method was validated by analyzing environmental soil samples spiked with known amounts of 239Pu and 237Np standard solutions or certified reference materials. The measured values of 237Np, 239Pu, and 240Pu obtained by inductively coupled plasma tandem mass spectrometry were consistent with their International Atomic Energy Agency literature values within a 95% confidence interval. These results confirm the reliability and high analytical precision (<6%) of this developed method using Pu as a non-isotopic tracer for monitoring the chemical yield of 237Np. The developed method can also be used for environmental pollutant monitoring and for tracer studies of the 237Np and Pu isotopes.

Dose reconstruction for plutonium-239 intakes at the Rocky Flats Plant.

PURPOSE: The Rocky Flats (RF) Plant was a weapons manufacturing facility that operated from the early 1950s to 1989. Its primary missions were the production of plutonium (Pu) pits for thermonuclear weapons and the processing of retired weapons for Pu recovery. The purpose of this study was to estimate radiation doses to a cohort of 4499 RF workers from an intake of 239Pu, the primary plutonium isotope handled at the site. MATERIALS AND METHODS: The latest biokinetic models of the International Commission on Radiological Protection, or site-specific variations of those models, were used to estimate 239Pu intakes for each worker based on model fits to bioassay data often coupled with lung measurements. RESULTS: Urinary excretion and lung retention data for most 239Pu intakes could be fit reasonably well by a mixture of Pu dioxide and moderately soluble material. For some workers, better fits were obtained by application of other absorption types including Type S, 239Pu nitrate, or pure 239Pu dioxide, or by assuming intake via a wound. The lungs typically received the highest tissue doses, with fifty-year committed equivalent doses in the range of 0.5-1 Sv for 275 workers, 1-5 Sv for 115 workers, and greater than 5 Sv for 12 workers. CONCLUSIONS: RF was a unique site regarding a large number of lung measurements available for determining the appropriate absorption types for inhaled material. This provided higher confidence in reconstructed 239Pu doses than is generally gained from urinary data alone.

New data on mobility of transuranium elements in sediments of the Yenisei River.

The inflow of transuranium elements to the Yenisei River was previously associated with the production of weapons-grade plutonium at the Mining-and-Chemical Combine (MCC, Zheleznogorsk, Russia), but the source of transuranium elements in the River today is fabrication of MOX fuel that started recently at the MCC. The current study presents results of sequential chemical extraction of radionuclides from sediment samples collected in 2014 and 2020 in two areas near the MCC discharge site and compares these results with the data obtained previously by sequential extraction of sediments collected during 1999-2007. Over the study period, the strength of binding of 137Cs and 60Co in the Yenisei River sediments was high (up to 100%) and remained so, while the percentages of 241Am and 152Eu in residual solids after sequential extraction increased considerably and the percentage of 239,240Pu in residual solids decreased in samples from all study areas. In samples collected at the position located close to the MCC discharge site, the percentages of the strongly bound 241Am and 152Eu as well as 239,240Pu were lower than in the samples from the other positions. The study demonstrated an enormous increase in 239,240Pu activity concentration in the top sediment layers collected at all positions in 2020 relative to 2014. In the same period, as literature data suggest, 239,240Pu activity concentrations also increased in aquatic organisms of the Yenisei River, which can be indicative of the growing potential bioavailability of plutonium in the aquatic ecosystem, which could be caused by the presence of the mobile form of plutonium in the routine discharges from the MCC.

Plutonium in sediments of the Eastern Guangdong coast-its sources and their contribution.

The 239+240Pu activities and 240Pu/239Pu atom ratios of surface sediments from the Eastern Guangdong coast (EGDC) were determined by sector field ICP-MS in order to examine the sources of plutonium (Pu) and quantify their contributions. The 239+240Pu activities in the EGDC ranged from 0.113 to 0.451 Bq kg-1, with an average of 0.225 ± 0.090 Bq kg-1 (n = 17). Consistently high 240Pu/239Pu atom ratios, ranging from 0.218 to 0.274 (average = 0.254 ± 0.014, n = 17), indicate a non-global fallout Pu source in the EGDC. The horizontal distribution of the 240Pu/239Pu atom ratios in the EGDC sediment suggests the non-global fallout Pu is sourced from close-in fallout from the Pacific Proving Grounds (PPG). Using a simple two end-member mixing model, we calculated the relative proportions of Pu from the PPG and global fallout in the EGDC to be 57 ± 9 % and 43 ± 9 %, respectively. Moreover, from the well-defined relationship between 239+240Pu activity and total organic carbon content in sediments and a two end-member mixing model using δ13C, we further calculated the Terr-global fallout (riverine input) and Mar-global fallout (direct atmospheric deposition) to be 11 ± 2 % and 32 ± 6 %, respectively. Finally, from the activity levels and atom ratios of Pu isotopes in the EGDC, we established a baseline for future use in environmental risk assessment related to nuclear power plant operations.

No long-term variation of 240Pu/239Pu atom ratio in liver of Japanese common squid (Todarodes pacificus) collected from seven sea areas around Japan during 2003-2018.

The 239+240Pu concentrations and 240Pu/239Pu atom ratios were determined to trace the temporal variability in concentration and atom ratio in liver of the Japanese common squid during 2003-2018. The differences in their concentrations and atom ratios and the dependency on the collection areas and migratory history were compared. The organ affinity of Pu in mantle, limb, liver, and internal organs except liver was also investigated. The average 239+240Pu concentrations were the highest in liver followed in order by internal organs except liver, limb, and mantle. The Pu accumulation in liver could be explained by a mechanism for foreign substance processing. A significant difference in the average 239+240Pu concentrations in liver was found among the sea areas for specimen collection during 2003-2018. In spite of a noticeable difference in the average 239+240Pu concentrations, the 240Pu/239Pu atom ratios showed no significant temporal variability around Japan; thus, they were continuously uniform during 2003-2018.

Sources, seasonal cycling, and fate of plutonium in a seasonally stratified and radiologically contaminated pond.

Unlike short-term laboratory experiments, studies at sites historically contaminated with radionuclides can provide insight into contaminant migration behavior at environmentally-relevant decadal timescales. One such site is Pond B, a seasonally stratified reservoir within Savannah River Site (SC, USA) has low levels (µBq L-1) of plutonium in the water column. Here, we evaluate the origin of plutonium using high-precision isotope measurements, investigate the impact of water column geochemistry on plutonium cycling during different stratification periods, and re-evaluate long-term mass balance of plutonium in the pond. New isotopic data confirm that reactor-derived plutonium overwhelms input from Northern Hemisphere fallout at this site. Two suggested mechanisms for observed plutonium cycling in the water column include: (1) reductive dissolution of sediment-derived Fe(III)-(oxyhydr)oxides during seasonal stratification and (2) plutonium stabilization complexed strongly to Fe(III)-particulate organic matter (POM) complexes. While plutonium may be mobilized to a limited extent by stratification and reductive dissolution, peak plutonium concentrations are in shallow waters and associated with Fe(III)-POM at the inception of stratification. This suggests that plutonium release from sediments during stratification is not the dominant mechanism driving plutonium cycling in the pond. Importantly, our analysis suggests that the majority is retained in shallow sediments and may become increasingly recalcitrant.

Assessment of soil-soil solution distribution coefficients of global fallout 237Np and 239Pu in Japanese upland soils.

Neptunium-237 and 239Pu are important radionuclides in the safety assessment related to geological disposal of radioactive waste because of the possibility of long-term exposure to humans. Mobilities of these radionuclides in the environment are of particular importance for their radiation dose evaluation; therefore, in this study, we have made the assessment of the soil-soil solution distribution coefficient (Kd, L/kg) using global fallout 237Np and 239Pu in Japanese upland soils. The Kd values were determined by extracting these radionuclides from 24 soil samples using a laboratory batch method. The desorption Kd values of 237Np ranged from 3.3 × 102 to 1.0 × 104 L/kg, and their geometric mean (GM) and arithmetic mean (AM) were 1.7 × 103 L/kg and 2.6 × 103 L/kg, respectively. The desorption Kd values of 239Pu were found to vary from 9.4 × 103 to 7.1 × 104 L/kg, and their GM and AM were 3.3 × 104 L/kg and 4.0 × 104 L/kg, respectively. In Japanese upland soils, the Kd value of 239Pu was one order of magnitude higher than that of 237Np.

Health risks from radioactive particles on Cumbrian beaches near the Sellafield nuclear site.

A monitoring programme, in place since 2006, continues to recover radioactive particles (<2 mm diameter) and larger objects from the beaches of West Cumbria. The potential risks to members of the public using the beaches are mainly related to prolonged skin contact with or the inadvertent ingestion of small particles. Most particles are classified as either 'beta-rich' or 'alpha-rich' and are detected as a result of their caesium-137 or americium-241 content. Beta-rich particles generally also contain strontium-90, with90Sr:137Cs ratios of up to about 1:1, but typically <0.1:1. Alpha-rich particles contain plutonium isotopes, with Pu:241Amαratios usually around 0.5-0.6:1. 'Beta-rich' particles have the greatest potential to cause localised skin damage if held in stationary contact with the skin for prolonged periods. However, it is concluded that only particles of >106Bq of137Cs, with high90Sr:137Cs ratios, would pose a significant risk of causing acute skin ulceration. No particles of this level of activity have been found. Inadvertent ingestion of a particle will result in the absorption to blood of a small proportion of the radionuclide content of the particle. The subsequent retention of radionuclides in body organs and tissues presents a potential risk of the development of cancer. For 'beta-rich' particles with typical activities (mean 2 × 104Bq137Cs, Sr:Cs ratio of 0.1:1), the estimated committed effective doses are about 30µSv for adults and about 40µSv for 1 year old infants, with lower values for 'alpha-rich' particles of typical activities. The corresponding estimates of lifetime cancer incidence following ingestion for both particle types are of the order of 10-6for adults and up to 10-5for infants. These estimates are subject to substantial uncertainties but provide an indication of the low risks to members of the public.

137Cs and isotopic ratios of Pu and U in lichens and mosses from Russian Arctic areas.

Knowledge of past anthropogenic sources of radionuclide contamination in Russian Arctic areas is important to assess the radioecological situation of these less-studied regions. Therefore, we investigated the sources of radionuclide contamination in Russian Arctic in the 1990s. Lichen and moss samples were collected from 1993 to 1996 in Kola Peninsula, Franz Josef Land, and few other locations. The activity concentration of 137Cs was determined from the archived samples by gamma spectrometry in 2020. After radiochemical separation of Pu and U isotopes from the lichens and mosses, mass ratios 240Pu/239Pu, 234U/238U, 235U/238U, and 236U/238U were determined by mass spectrometry. 137Cs activity concentrations at the sampling date were found to vary from 3.1 ± 1.4 (Inari, Finnish-Russian border) to 303 ± 7 (Kola Peninsula) Bq/kg. The ranges of isotopic ratios were 0.0592 ± 0.0007 to 0.253 ± 0.082 for 240Pu/239Pu, (4.89 ± 3.91) × 10-5 to (6.86 ± 0.04) × 10-5 for 234U/238U, 0.0072104(21) to 0.007376(41) for 235U/238U, and from below 1 × 10-7 to (2.65 ± 0.19) × 10-6 for 236U/238U, respectively. Based on the measured isotopic ratios and characteristic isotopic ratios of known contamination sources, the main Pu and U sources in the sampled lichens and mosses are global fallout, the Chernobyl accident, and possibly local nuclear activities. These results contribute to further understanding of past nuclear events and resulting nuclear contamination in Russian Arctic terrestrial areas.

Plutonium isotopes in the ground air layer in southern Poland (2010-2016): Source terms, seasonal variability and correlations with meteorological conditions.

In this study, the results of the analysis of Pu-238 and Pu-239 + 240 activity concentrations on aerosol filters collected from 2010 to 2016 in Krakow (Southern Poland) are presented and discussed. For the first time, the temporal variation of Pu-239 + 240 activity concentration in surface air in Poland was studied using Fourier analysis. The analysis clearly showed that the Pu-239 + 240 content in the near-ground air layer is subject to seasonal variations and demonstrates annual periodicity. Pu analyses were performed using alpha spectrometry. The measured values ranged from 1.93∙10-10 Bq/m3 to 1.31∙10-8 Bq/m3 with an average of 2.07∙10-9 Bq/m3 for Pu-239 + 240 and from 9.07∙10-11 Bq/m3 to 1.27∙10-9 Bq/m3 with the average 1.52∙10-10 Bq/m3 for Pu-238. The analysis of the potential sources of plutonium isotopes in the air aerosols samples indicated that only two samples are uniquely characterized by the ratio corresponding to spent nuclear fuel: February 2012 (0.59 ± 0.18) and February 2015 (0.68 ± 0.19). The remaining samples showed mixed origins, with global radioactive fallout appearing to contribute more than spent nuclear fuel. To study the relationship between Pu-239 + 240 and meteorological conditions, Pearson's correlation and circulation pattern analyses were performed. The analyses showed that the Pu-239 + 240 activity concentration depends on air temperature (R = 0.51), the sum of ice and snowfall (R = -0.45), relative humidity (R = -0.54) and mean total cloud cover (R = -0.56). High concentrations of Pu-239 + 240 were positively correlated with air advection from the southern and eastern sectors, whereas low concentrations were observed during dynamic weather conditions with intense circulation from the western sector. In case of Pu-238 no significant correlation was observed.