Natural radioactivity and element characterization in pit lakes in Northern Sweden.

Northern Sweden has been the object of intense metal mining in the last decades producing several water-filled open-pits, or pit lakes. Most of these pit lakes have been limed to maintain a good water quality and to prevent generation of acidic water that could leach the exposed rocks and release metals into water. The aim of this work was to examine the concentration of stable elements and naturally occurring radionuclides in water and sediment samples from pit lakes originating from non-uranium mining activities in Northern Sweden. Surface water and surface sediments were collected from 27 pit lakes in Northern Sweden. Water quality parameters, concentration of stable elements and radionuclides were measured by a water probe, ICP-MS and XRF, and alpha and gamma spectrometry, respectively. Furthermore, a multivariate statistical analysis (PCA) was performed on the water samples and sediments. In general, the quality of the surface water was good, but some lakes had low pH values (2.5-5.7), and high concentrations of Fe (up to 200 mg/L) and other metals (e.g. Zn, Cu). When relating the metal concentrations in sediments in pit lakes with the concentration found in natural lakes, some sites had relatively high levels of Cu, As, Cr and Pb. The activity concentration of 210Po, and U and Th isotopes in water and sediment samples were at environmental levels, as was the ambient dose equivalent rate at these sites (range 0.08-0.14 µSv/h).

The study of Canadian Arctic freshwater system toward radioactive contamination - status in 1999.

This work provides a novel data set on accumulations of both anthropogenic (137Cs, 238Pu, 239+240Pu, 241Am) and natural (210Pb, 226Ra, 232Th) radionuclides and an element (K). Sampling of soils and lake sediments was accomplished in 1999 during Tundra Northwest (TNW-99) international expedition to a remote region of the Canadian Arctic. The sediment ages and sedimentation rates were determined. The obtained results overall indicated a high geographical diversity of contamination levels and trends. Accumulation rates were also differential, and a sediment focusing contribution was distinctly visible. Radioactive pollution was found to be lower relative to temperate counterparts. The activity ratios of anthropogenic radionuclides corresponded to global fallout as a prevailing source in the entire examined area. The post-Chernobyl radiocaesium was observed for the westernmost lake only. The elevated level of 137Cs and 239+240Pu in the topmost sediment at the northern and eastern Arctic Archipelago was attributed to recent resuspension and subsequent redistribution of radionuclides.

Radiometrical and physico-chemical characterisation of contaminated glass waste from a glass dump in Sweden.

Around former glass factories in south eastern Sweden, there are dozens of dumps whose radioactivity and physico-chemical properties were not investigated previously. Thus, radiometric and physico-chemical characteristics of waste at Madesjö glass dump were studied to evaluate pre-recycling storage requirements and potential radiological and environmental risks. The material was sieved, hand-sorted, leached and scanned with X-Ray Fluorescence (XRF). External dose rates and activity concentrations of Naturally Occurring Radioactive Materials from 238U, 232Th series and 40K were also measured coupled with a radiological risk assessment. Results showed that the waste was 95% glass and dominated by fine fractions (<11.3 mm) at 43.6%. The fine fraction had pH 7.8, 2.6% moisture content, 123 mg kg-1 Total Dissolved Solids, 37.2 mg kg-1 Dissolved Organic Carbon and 10.5 mg kg-1 fluorides. Compared with Swedish EPA guidelines, the elements As, Cd, Pb and Zn were in hazardous concentrations while Pb leached more than the limits for inert and non-hazardous wastes. With 40K activity concentration up to 3000 Bq kg-1, enhanced external dose rates of 40K were established (0.20 µSv h-1) although no radiological risk was found since both External Hazard Index (Hex) and Gamma Index (Iγ) were <1. The glass dump needs remediation and storage of the waste materials under a safe hazardous waste class 'Bank Account' storage cell as a secondary resource for potential future recycling.

Journal of Environmental Radioactivity special issue: II International Conference on Radioecological Concentration Processes. (50 years later).

An international conference on Radioecological Concentration Processes was held in Seville, Spain, 6-9 November 2016 at the Centro Nacional de Aceleradores. It was attended by 160 participants from 35 different countries. This was the 2nd conference on this item since 1966, 50 years ago. The conference covered aspects of radiological important radionuclides on terrestrial, marine and freshwater environments and has allowed obtaining a clear picture of the status of the Radioecology as a consolidated discipline in the 21st century.

Radioecological modelling of Polonium-210 and Caesium-137 in lichen-reindeer-man and top predators.

This work deals with analysis and modelling of the radionuclides 210Pb and210Po in the food-chain lichen-reindeer-man in addition to 210Po and 137Cs in top predators. By using the methods of Partial Least Square Regression (PLSR) the atmospheric deposition of 210Pb and 210Po is predicted at the sample locations. Dynamic modelling of the activity concentration with differential equations is fitted to the sample data. Reindeer lichen consumption, gastrointestinal absorption, organ distribution and elimination is derived from information in the literature. Dynamic modelling of transfer of 210Pb and 210Po to reindeer meat, liver and bone from lichen consumption, fitted well with data from Sweden and Finland from 1966 to 1971. The activity concentration of 210Pb in the skeleton in man is modelled by using the results of studying the kinetics of lead in skeleton and blood in lead-workers after end of occupational exposure. The result of modelling 210Pb and 210Po activity in skeleton matched well with concentrations of 210Pb and 210Po in teeth from reindeer-breeders and autopsy bone samples in Finland. The results of 210Po and 137Cs in different tissues of wolf, wolverine and lynx previously published, are analysed with multivariate data processing methods such as Principal Component Analysis PCA, and modelled with the method of Projection to Latent Structures, PLS, or Partial Least Square Regression PLSR.

Radioactivity levels in the marine environment along the Exclusive Economic Zone (EEZ) of Qatar.

A study on (137)Cs, (40)K, (226)Ra, (228)Ra, and (238)U was carried out along the EEZ of Qatar. Results serve as the first ever baseline data. The level of (137)Cs (mean value 1.6 ± 0.4 Bq m(-3)) in water filters was found to be in the same order of magnitude as reported by others in worldwide marine radioactivity studies. Results are also in agreement with values reported from other Gulf regions. The computed values of sediment-water distribution coefficients Kd, are lower than the values given by IAEA. Measurements were carried out for bottom sediments, biota samples like fish, oyster, sponge, seashell, mangrove, crab, shrimp, starfish, dugong and algae. The 'concentration factors' reported for biota samples are below the levels published by IAEA and cause no significant impact on human health for seafood consumers in Qatar.

Polonium-210 and Caesium-137 in lynx (Lynx lynx), wolverine (Gulo gulo) and wolves (Canis lupus).

Wolves, lynx and wolverines are on the top of the food-chain in northern Scandinavia and Finland. (210)Po and (137)Cs have been analysed in samples of liver, kidney and muscle from 28 wolves from Sweden. In addition blood samples were taken from 27 wolves. In 9 of the wolves, samples of muscle, liver and blood were analysed for (210)Po. Samples of liver and muscle were collected from 16 lynx and 16 wolverines from Norway. The liver samples were analysed for (210)Po and (137)Cs. Only (137)Cs analyses were carried out for the muscle samples. The wolves were collected during the winter 2010 and 2011, while the samples for lynx and wolverines were all from 2011. The activity concentrations of (210)Po in wolves were higher for liver (range 20-523 Bq kg(-1) d.w.) and kidney (range 24-942 Bq kg(-1) d.w.) than muscle (range 1-43 Bq kg(-1) d.w.) and blood (range 2-54 Bq kg(-1) d.w.). Activity ratios, (210)Po/(210)Pb, in wolf samples of muscle, liver and blood were in the ranges 2-77, 9-56 and 2-54. Using a wet weight ratio of 3.8 the maximal absorbed dose from (210)Po to wolf liver was estimated to 3500 µGy per year. Compared to wolf, the ranges of (210)Po in liver samples were lower in lynx (range 22-211 Bq kg(-1) d.w.) and wolverine (range16-160 Bq kg(-1) d.w.). Concentration of (137)Cs in wolf samples of muscle, liver, kidney and blood were in the ranges 70-8410 Bq kg(-1) d.w., 36-4050 Bq kg(-1) d.w., 31-3453 Bq kg(-1) d.w. and 4-959 Bq kg(-1) d.w., respectively. (137)Cs in lynx muscle and liver samples were in the ranges 44-13393 Bq kg(-1) d.w. and 125-10260 Bq kg(-1) d.w. The corresponding values for (137)Cs in wolverine were 22-3405 Bq kg(-1) d.w. for liver and 53-4780 Bq kg(-1) d.w. for muscle. The maximal absorbed dose from (137)Cs to lynx was estimated to 3000 µGy per year.

(7)Be, (210)Pb, and (210)Po in the surface air from the Arctic to Antarctica.

In the present study we have investigated the activity concentrations of (210)Pb, (210)Po as well as (7)Be in surface air of the North and South Atlantic (1988-1989), the Arctic Ocean (1991), and along the coastline of Siberia (1994) during succeeding expeditions in the Swedish Polar Research program. During the cruises in the Arctic Ocean during 1991-07-28 to 1991-10-04 the average air concentrations of (7)Be was 0.6 ± 0.4 mBq/m(3), (210)Pb 40 ± 4 µBq/m(3) and (210)Po-38 ± 10 µBq/m(3). During the Swedish-Russian Tundra Ecology-94 expedition along the Siberian coastline the average air concentrations of (7)Be and (210)Pb measured during May-July were 11 ± 3, and 2.4 ± 0.4 mBq/m(3), and during July-September they were 7.2 ± 2 and 2.7 ± 1.1 mBq/m(3) respectively. The results from measurements of the activity concentration of (210)Pb in the air over the Arctic Ocean vary between 75 and 176 µBq/m(3). In the air close to land masses, however, the activity concentration of (210)Pb in the air increases to 269-2712 µBq/m(3). The activity concentration of (7)Be in the South Atlantic during the cruise down to Antarctica varied between 1.3 and 1.7 with an average of 1.5 ± 0.8 mBq/m(3). The activity concentration of (210)Pb in the South Atlantic down to Antarctica varied between 6 and 14 µBq/m(3). At the Equator the activity concentration recorded in November 1988 was 630 µBq/m(3) and in April 1989 it was 260 µBq/m(3). The average activity concentration of (210)Pb during the route Gothenburg-Montevideo in 1988 was 290 and on the return Montevideo-Gothenburg it was 230 µBq/m(3). The activity concentration of (210)Po in the South Atlantic down to Antarctica varied between 15 and 58 µBq/m(3). At the Equator the activity concentration in November 1988 was 170 and in April 1989 it was 70 µBq/m(3). The average activity concentration of (210)Po during the route Gothenburg-Montevideo in 1988 was 63 and on the return Montevideo-Gothenburg it was 60 µBq/m(3). The average of the activity concentrations in the Antarctic air of (210)Pb was 27 ± 10 µBq/m(3) and of (210)Po it was 12 ± 7 µBq/m(3). All our results were compiled together with other published data, and the global latitudinal distribution of (210)Pb was converted to total annual deposition (Bq/m(2)/a) and fitted to a 4th degree polynomial. By using the global latitudinal distribution of (210)Po/(210)Pb-activity ratio from our own results the global latitudinal distribution of (210)Po annual deposition was derived.

Distribution of artificial gamma-ray emitting radionuclide activity concentration in the top soil in the vicinity of the Ignalina Nuclear Power Plant and other regions in Lithuania.

The impact of the operating Ignalina Nuclear Power Plant (INPP) on the contamination of top soil layer with artificial radionuclides has been studied. Results of the investigation of artificial gamma-ray emitting radionuclide distribution in soil in the vicinity of the INPP and distant regions in Lithuania in 1996-2008 (INPP operational period) show that nowadays (137)Cs remains the most important artificial gamma-ray emitting radionuclide in the upper soil layer. Mean (137)Cs activity concentrations in the top soil layer in the vicinity of the INPP were found to be significantly lower compared to those in remote regions of Varena and Plunge (~300 km from INPP). In 1996 and 1998 mean (137)Cs activity concentrations were in the range of 28-45 Bq/kg in the nearest vicinity to the INPP, 103 Bq/kg in Varena and 340 Bq/kg in Plunge region. (137)Cs activity concentrations were 5-20 times lower in meadow soil (4-14 Bq/kg) compared to swamp and forest soil. (60)Co, the INPP origin radionuclide, was detected in samples only in 1996 and 2000, and the activity concentration of (60)Co was found to be in the range from 0.4 to 7.0 Bq/kg at the sampling ground nearest to the INPP. Average annual activity concentrations of the INPP origin (137)Cs and (60)Co in the air and depositions in the INPP region were modeled using Pasquill-Gifford equations. The modeling results of (137)Cs and (60)Co depositional load in the INPP vicinity agree with the experimentally obtained values. Our results provide the evidence that the operation of INPP did not cause any significant contamination in soil surface.

Polonium-210 and lead-210 in the terrestrial environment: a historical review.

The radionuclides (210)Po and (210)Pb widely present in the terrestrial environment are the final long-lived radionuclides in the decay of (238)U in the earth's crust. Their presence in the atmosphere is due to the decay of (222)Rn diffusing from the ground. The range of activity concentrations in ground level air for (210)Po is 0.03-0.3 Bq m(-3) and for (210)Pb 0.2-1.5 Bq m(-3). In drinking water from private wells the activity concentration of (210)Po is in the order of 7-48 mBq l(-1) and for (210)Pb around 11-40 mBq l(-1). From water works, however, the activity concentration for both (210)Po and (210)Pb is only in the order of 3 mBq l(-1). Mosses, lichens and peat have a high efficiency in capturing (210)Po and (210)Pb from atmospheric fallout and exhibit an inventory of both (210)Po and (210)Pb in the order of 0.5-5 kBq m(-2) in mosses and in lichens around 0.6 kBq m(-2). The activity concentrations in lichens lies around 250 Bq kg(-1), dry mass. Reindeer and caribou graze lichen which results in an activity concentration of (210)Po and (210)Pb of about 1-15 Bq kg(-1) in meat from these animals. The food chain lichen-reindeer or caribou, and Man constitutes a unique model for studying the uptake and retention of (210)Po and (210)Pb in humans. The effective annual dose due to (210)Po and (210)Pb in people with high consumption of reindeer/caribou meat is estimated to be around 260 and 132 µSv a(-1) respectively. In soils, (210)Po is adsorbed to clay and organic colloids and the activity concentration varies with soil type and also correlates with the amount of atmospheric precipitation. The average activity concentration levels of (210)Po in various soils are in the range of 20-240 Bq kg(-1). Plants become contaminated with radioactive nuclides both by absorption from the soil (supported Po) and by deposition of radioactive fallout on the plants directly (unsupported Po). In fresh leafy plants the level of (210)Po is particularly high as the result of the direct deposition of (222)Rn daughters from atmospheric deposition. Tobacco is a terrestrial product with high activity concentrations of (210)Po and (210)Pb. The overall average activity concentration of (210)Po is 13 ± 2 Bq kg(-1). It is rather constant over time and by geographical origin. The average median daily dietary intakes of (210)Po and (210)Pb for the adult world population was estimated to 160 mBq day(-1) and 110 mBq day(-1), corresponding to annual effective doses of 70 µSv a(-1) and 28 µSv a(-1), respectively. The dietary intakes of (210)Po and (210)Pb from vegetarian food was estimated to only 70 mBq day(-1) and 40 mBq day(-1) corresponding to annual effective doses of 30.6 µSv a(-1) and 10 µSv a(-1), respectively. Since the activity concentration of (210)Po and (210)Pb in seafood is significantly higher than in vegetarian food the effective dose to populations consuming a lot of seafood might be 5-15 fold higher.

Journal of Environmental Radioactivity special issue: international topical conference on Po and radioactive Pb isotopes.

An international conference on polonium (Po) and radioactive isotopes was held in Seville Spain, 26-28 October 2009 at the Centro Nacional de Aceleradores. It was attended by 138 participants from 38 different countries. The sessions covered all aspects on Po and lead (Pb) such as radiochemistry, terrestrial and marine radioecology, kinetics, sedimentation rates, atmospheric tracers, NORM industries and dose assessment.

U, Pu, and Am nuclear signatures of the Thule hydrogen bomb debris.

This study concerns an arctic marine environment that was contaminated by actinide elements after a nuclear accident in 1968, the so-called Thule accident In this study we have analyzed five isolated hot particles as well as sediment samples containing particles from the weapon material for the determination of the nuclear fingerprint of the accident. We report that the fissile material in the hydrogen weapons involved in the Thule accident was a mixture of highly enriched uranium and weapon-grade plutonium and that the main fissile material was 235U (about 4 times more than the mass of 239Pu). In the five hot particles examined, the measured uranium atomic ratio was 235U/238U = 1.02 +/- 0.16 and the Pu-isotopic ratios were as follows: 24Pu/239Pu = 0.0551 +/- 0.0008 (atom ratio), 238Pu/239+240Pu = 0.0161 +/- 0.0005 (activity ratio), 241Pu/239+240Pu = 0.87 +/- 0.12 (activity ratio), and 241Am/ 239+240Pu = 0.169 +/- 0.005 (activity ratio) (reference date 2001-10-01). From the activity ratios of 241Pu/241Am, we estimated the time of production of this weapon material to be from the late 1950s to the early 1960s. The results from reanalyzed bulk sediment samples showed the presence of more than one Pu source involved in the accident, confirming earlier studies. The 238Pu/239+240PU activity ratio and the 240Pu/ 239Pu atomic ratio were divided into at least two Pu-isotopic ratio groups. For both Pu-isotopic ratios, one ratio group had identical ratios as the five hot particles described above and for the other groups the Pu isotopic ratios were lower (238Pu/ 239+240PU activity ratio approximately 0.01 and the 240Pu/P239Pu atomic ratio 0.03). On the studied particles we observed that the U/Pu ratio decreased as a function of the time these particles were present in the sediment. We hypothesis that the decrease in the ratio is due to a preferential leaching of U relative to Pu from the particle matrix.

Studies of Np and Pu in the marine environment of Swedish-Danish waters and the North Atlantic Ocean.

The long-lived anthropogenic radionuclides (237)Np, (239)Pu and (240)Pu were determined in marine environmental samples (seaweed and seawater) collected from Swedish-Danish waters and the North Atlantic Ocean at various locations on different occasions during the period 1991-2001. The measurements were performed with sector field Inductively Coupled Plasma Mass Spectrometry (ICP-MS) and conventional alpha spectrometry. The (237)Np activity concentrations in Fucus vesiculosus and surface seawater from the Swedish west coast and Danish waters ranged from 0.16+/-0.02 to 1.02+/-0.09 mBq kg(-1) (dry weight) and 0.65+/-0.02 to 1.69+/-0.02 mBq m(-3), respectively, depending on the location and sampling year. Most of the (237)Np in these waters is believed to originate from the Sellafield nuclear reprocessing plant, with some contribution from global fallout. The (240)Pu/(239)Pu atomic ratios in F. vesiculosus samples are reported in this study with an overall average of 0.17+/-0.03. The (237)Np and (239)Pu activity concentrations observed in surface seawater collected in North Atlantic waters ranged from 0.16+/-0.01 to 0.62+/-0.08 mBq m(-3) and from 0.64+/-0.05 to 4.27+/-0.08 mBq m(-3), respectively, and the (237)Np/(239)Pu atomic ratios were a good indicator of conservative behaviour of Np in marine waters.

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

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

Rapid removal of Chernobyl fallout from Mediterranean surface waters by biological activity

In this report, data from a time-series sediment trap experiment and concomitant zooplankton collections showed conclusively that Chernobyl radioactivity, in particular the rate earth nuclides Ce and Ce, entering the Mediterranean as a single pulse, was rapidly removed from surface waters and transported to a depth of 200 m in a few days primarily by zooplankton grazing