Airborne concentrations and chemical considerations of radioactive ruthenium from an undeclared major nuclear release in 2017.

In October 2017, most European countries reported unique atmospheric detections of aerosol-bound radioruthenium (106Ru). The range of concentrations varied from some tenths of µBq·m-3 to more than 150 mBq·m-3 The widespread detection at such considerable (yet innocuous) levels suggested a considerable release. To compare activity reports of airborne 106Ru with different sampling periods, concentrations were reconstructed based on the most probable plume presence duration at each location. Based on airborne concentration spreading and chemical considerations, it is possible to assume that the release occurred in the Southern Urals region (Russian Federation). The 106Ru age was estimated to be about 2 years. It exhibited highly soluble and less soluble fractions in aqueous media, high radiopurity (lack of concomitant radionuclides), and volatility between 700 and 1,000 °C, thus suggesting a release at an advanced stage in the reprocessing of nuclear fuel. The amount and isotopic characteristics of the radioruthenium release may indicate a context with the production of a large 144Ce source for a neutrino experiment.

Potential Source Apportionment and Meteorological Conditions Involved in Airborne 131I Detections in January/February 2017 in Europe.

Traces of particulate radioactive iodine (131I) were detected in the European atmosphere in January/February 2017. Concentrations of this nuclear fission product were very low, ranging 0.1 to 10 µBq m-3 except at one location in western Russia where they reached up to several mBq m-3. Detections have been reported continuously over an 8-week period by about 30 monitoring stations. We examine possible emission source apportionments and rank them considering their expected contribution in terms of orders of magnitude from typical routine releases: radiopharmaceutical production units > sewage sludge incinerators > nuclear power plants > spontaneous fission of uranium in soil. Inverse modeling simulations indicate that the widespread detections of 131I resulted from the combination of multiple source releases. Among them, those from radiopharmaceutical production units remain the most likely. One of them is located in Western Russia and its estimated source term complies with authorized limits. Other existing sources related to 131I use (medical purposes or sewage sludge incineration) can explain detections on a rather local scale. As an enhancing factor, the prevailing wintertime meteorological situations marked by strong temperature inversions led to poor dispersion conditions that resulted in higher concentrations exceeding usual detection limits in use within the informal Ring of Five (Ro5) monitoring network.

Long-term radiocarbon variation studies in the air and tree rings of Slovakia.

Fifty-five years of radiocarbon variation studies are reviewed with an emphasis on a better understanding of the impacts of the Bohunice nuclear power plant and fossil fuel CO2 on the atmosphere and biosphere of Slovakia. The maximum Δ14C levels in the air up to about 1200‰ were observed during the 1970s at the Zlkovce monitoring station, which after 2005 decreased to <30‰. A relative decrease in the atmospheric Δ14C levels due to increasing levels of fossil CO2 in the atmosphere has also been significant, for example, in Bratislava down to about -330‰, but after 2005 they were only <50‰ below the Jungfraujoch European clean-air level. The tree-ring data, averaging the annual Δ14C levels for several stations in Slovakia, have been in agreement with the atmospheric data, as well as with the newly established clean-air station at Jasná in central Slovakia. Future 14C levels will depend strongly on fossil CO2 levels in the atmosphere, which will change the bomb 14C era to the fossil CO2 era. New investigations of 14C variations in the atmosphere-biosphere-hydrosphere compartments represent a great challenge for radiocarbon science, important for better understanding of environmental processes, climate change, and impacts of human activities on the total environment. This new era of radiocarbon research will also need new developments in radiocarbon analytical technologies, as further progress in accuracy and precision of results (<1‰) will be needed to meet the new radiocarbon challenges.

Tritium and radiocarbon in the water column of the Red Sea.

Despite being the busiest transient sea in the world due to the Suez Canal, radionuclide distribution studies in seawater and sediment of the Red Sea remain rare. A sampling expedition in the Red Sea was conducted from June 9 to July 6, 2021, visiting a transect of several deep sampling stations located along the central axis of the basin from the Gulf of Aqaba to the southern Red Sea (near Farasan Island, Saudi Arabia). The collected seawater profile samples were analyzed for tritium, radiocarbon and oxygen-18. The observed tritium levels in surface waters of the Red Sea peaked at 0.3-0.4 TU, similar to the values observed in the western Arabian Sea (decay corrected). The values observed at waters below 150 m were around 0.2 TU, however, at depths of 450 and 750 m, tritium minima (<0.2 TU) were observed, which could be associated with a partial return flow of bottom waters from the southern to the northern Red Sea. At two stations at the depth of about 550 m, deep Δ14C minima were observed as well (-4‰ and -10‰), documenting ongoing transport of carbon in the water column, important for sink of anthropogenic carbon.

Determination of ultra-trace levels of uranium and thorium in electrolytic copper using radiochemical neutron activation analysis.

Uranium and thorium as natural radioactive elements are present everywhere in the environment. Their trace levels are also present in various materials, such as copper, used as a shielding material in gamma-ray spectrometry, usually located very close to the detector. Ultra-low levels of uranium and thorium in electrolytic copper were determined in this study using radiochemical neutron activation analysis (RNAA) via their induced nuclides U-239/Np-239 and Pa-233, respectively. After irradiation of copper together with uranium and thorium standards, various techniques were used for their separation from the matrix. To isolate of short-lived U-239, solvent extraction in a combination of tributyl phosphate (TBP) in toluene was used. To separate Np-239 and Pa-233, extraction chromatography using TEVA and TK-400 resins was applied. Special attention was paid to the estimation of radiochemical recovery, which was determined in each sample aliquot using U-235, Np-238 and Pa-231 tracers. For quantification of induced nuclides and tracers used in the experiment, gamma-ray spectrometry was used. Obtained results showed that electrolytic copper samples contained impurities of uranium and thorium in ultra-trace levels: up to 45 pg/g (550 nBq/g) for uranium and up to 80 pg/g (330 nBq/g) for thorium. The electrolytic copper also contained impurities of Ag, As, Au, Sb, Se and Zn as observed using the k0-INAA technique.

The neutron component of background of an HPGe detector operating in a surface laboratory.

Investigation of neutron-induced background was carried out by studying interactions of cosmic-ray neutrons with an HPGe detector inside its shield placed on a ground floor of a 3-storey building. The study was conducted experimentally and by Monte Carlo simulations using GEANT4 simulation tool. Detailed analysis of measured background γ-ray spectra showed that many γ-lines visible in the spectra were induced by neutrons. The majority of detected γ-rays originated in germanium, copper, lead and tin. Iron and aluminium components were less important background sources. Inelastic scattering and neutron capture were the most often occurring processes of neutron interactions with the detector and its shielding. The contamination by natural radionuclides, specifically of 40K, 214Pb, 214Bi and 208Tl, was also present in the background spectra. Nevertheless, approximately 35% of 208Tl peak at the energy of 2614.51 keV was produced by inelastic scattering of neutrons on 208Pb nuclei. The experimental background was compared with GEANT4 simulations, which were carried out without and with the shielding layer of the building. The final integral counting rates for measured spectrum in the energy range from 50 keV to 2875 keV was 1.26 ± 0.07 s-1 and for simulated one 1.25 ± 0.13 s-1, indicating very good agreement with the experiment.

Natural radionuclides as background sources in the Modane underground laboratory.

The Modane underground laboratory (LSM) is the deepest operating underground laboratory in Europe. It is located under the Fréjus peak in Savoie Alps in France, with average overburden of 4800 m w. e. (water equivalent), providing low-background environment for experiments in nuclear and particle physics, astrophysics and environmental physics. It is crucial to understand individual sources of background such as residual cosmic-ray flux of high-energy muons, muon-induced neutrons and contributions from radionuclides present in the environment. The identified dominant sources of background are radioactive contamination of construction materials of detectors and laboratory walls, radon contamination of the laboratory air, and neutrons produced in the laboratory. The largest neutron contribution has been identified from (α, n) reactions in low Z materials (10-7-10-4 n s-1 Bq-1) and from spontaneous fission of 238U (1.1× 10-6 n s-1 Bq-1).

Impact of Saharan dust events on radionuclides in the atmosphere, seawater, and sediments of the northwest Mediterranean Sea.

In February 2004, anthropogenic radionuclides (137Cs, 236U, 239Pu and 240Pu), transported from the Sahara Desert, were observed in the Monaco air, and later in water and sediment samples collected at the DYFAMED site in the northwest (NW) Mediterranean Sea. While 236U and 137Cs in Saharan dust particles showed a high solubility in seawater, Pu isotopes were particle reactive in the water column and in the sediment. The impact of the Saharan deposition was found at 0-1.0 cm of the sediment core for 236U and 137Cs, and between 1.0 and 1.5 cm for Pu isotopes. The excess of 236U was observed more in the water column than in the sediment, whereas the 239+240Pu total inventories were comparable in the water column and the sediment. This single-day particle event represented 72% of annual atmospheric deposition in Monaco. At the DYFAMED site, it accounted for 10% (137Cs) and 15% (239+240Pu) activities of sinking particles during the period of the highest mass flux collected at the 200 and 1000 m water depths, and for a significant proportion of the total annual atmospheric input to the NW Mediterranean Sea (28-37% for 137Cs and 34-45% for 239+240Pu). Contributions to the total 137Cs and 239+240Pu sediment inventories were estimated to be 14% and 8%, respectively. The Saharan dust deposition phenomenon (atmospheric input, water column and sediment) offered a unique case to study origin and accumulation rates of radionuclides in the NW Mediterranean Sea.

Forty years of atmospheric radiocarbon monitoring around Bohunice nuclear power plant, Slovakia.

Radiocarbon variations in the atmospheric CO(2) with attenuating amplitudes and decreasing mean values with typical maxima in summer and minima in winter have been observed since 1967 in two localities of Slovakia, in Bratislava and Zlkovce, situated about 60 km NE from Bratislava, only 5 km from the Bohunice Nuclear Power Plant (NPP). The (14)C record in Bratislava has been influenced mainly by fossil CO(2) emissions, in contrast to the Zlkovce record which has been more variable, as it has clearly been affected by operation of the Bohunice NPP. However, during specific meteorological conditions with NE transport of air masses to Bratislava, the effect of the Bohunice NPP has been visible in Bratislava as well. Maximum (14)C concentrations (up to 120% above a natural background) were observed around A1 NPP which used CO(2) with admixture of air as a cooling agent. The (14)C concentrations around four pressurized light water reactors were up to 30% above the background. The Delta(14)C values in the heavily polluted atmosphere of Bratislava were up to 10% and at Zlkovce up to 5% lower than the European clean air represented by the Jungfraujoch Delta(14)C data. Later the Delta(14)C values were similar at both sites, and from 2003 they were close to the European clean air levels. The observed Delta(14)C behaviour in the atmosphere provides a unique evidence of decreased fossil fuel CO(2) emissions in the region, as well as the long-term effect of the Bohunice NPP on the Bratislava and Zlkovce stations. The estimated annual radiation doses to the local public due to digestion of radiocarbon contaminated food have been estimated to be around 3 microSv.

Ultra-low-level determination of (236)U in IAEA marine reference materials by ICPMS and AMS.

The development of analytical procedures for the measurement of ultra-low levels of (236)U in marine samples using high-resolution inductively coupled plasma mass spectrometry (HR-ICPMS) and accelerator mass spectrometry (AMS) techniques are discussed and results are presented for IAEA reference materials-marine sediments (IAEA-135, 306, 384 and 385), marine biota (IAEA-134 and 414) and seawater (IAEA-381), collected in areas affected by nuclear reprocessing plants and nuclear weapons tests. The obtained minimum detection limit of the (236)U/(238)U atom ratio was 1x10(-8) for AMS and 1x10(-6) for HR-ICPMS.

IAEA programme on the quality of marine radioactivity data.

Society's growing interest in environmental issues requires the production of reliable information for policy-makers, stakeholders and society in general. This information must be based on accurate data produced by qualified laboratories and data need to be comparable between numerous laboratories for joint assessments, e.g. in International Conventions. The Marine Environment Laboratories of the International Atomic Energy Agency has been providing Quality Assurance services to laboratories involved in marine radioactivity studies for the past 30 years. This has included training, organization of laboratory intercomparison exercises, production of Reference Materials (RMs) and more recently, production of Certified Reference Materials (CRMs) that comply with relevant ISO standards. Here, the overall process of Certification of Reference Materials is reviewed, past work summarized and future needs of marine radioactivity laboratories briefly discussed.

Impact of the Bohunice Nuclear Power Plant on atmospheric radiocarbon.

Radiocarbon variations in the atmospheric CO(2) have been observed at two localities in Slovakia (Bratislava and Zlkovce). Zlkovce is situated about 60 km NE from Bratislava, and only 5 km from the Bohunice Nuclear Power Plant (NPP). The observed Delta(14)C levels provide a unique evidence of the long-term impact of the Bohunice NPP on the Bratislava region, as well as on the decreased fossil fuel CO(2) emissions. The radiation doses estimated to the local public have been around 3 microSv/year, 20% of the dose from global fallout (14)C present in the environment.

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

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

Isotope tracing of submarine groundwater discharge offshore Ubatuba, Brazil: results of the IAEA-UNESCO SGD project.

Results of groundwater and seawater analyses for radioactive (3H, 222Rn, 223Ra, 224Ra, 226Ra, and 228Ra) and stable (D and 18O) isotopes are presented together with in situ spatial mapping and time series 222Rn measurements in seawater, direct seepage measurements using manual and automated seepage meters, pore water investigations using different tracers and piezometric techniques, and geoelectric surveys probing the coast. This study represents first time that such a new complex arsenal of radioactive and non-radioactive tracer techniques and geophysical methods have been used for simultaneous submarine groundwater discharge (SGD) investigations. Large fluctuations of SGD fluxes were observed at sites situated only a few meters apart (from 0 cm d(-1) to 360 cm d(-1); the unit represents cm3/cm2/day), as well as during a few hours (from 0 cm d(-1) to 110 cm d(-1)), strongly depending on the tidal fluctuations. The average SGD flux estimated from continuous 222Rn measurements is 17+/-10 cm d(-1). Integrated coastal SGD flux estimated for the Ubatuba coast using radium isotopes is about 7x10(3) m3 d(-1) per km of the coast. The isotopic composition (deltaD and delta18O) of submarine waters was characterised by significant variability and heavy isotope enrichment, indicating that the contribution of groundwater in submarine waters varied from a small percentage to 20%. However, this contribution with increasing offshore distance became negligible. Automated seepage meters and time series measurements of 222Rn activity concentration showed a negative correlation between the SGD rates and tidal stage. This is likely caused by sea level changes as tidal effects induce variations of hydraulic gradients. The geoelectric probing and piezometric measurements contributed to better understanding of the spatial distribution of different water masses present along the coast. The radium isotope data showed scattered distributions with offshore distance, which imply that seawater in a complex coast with many small bays and islands was influenced by local currents and groundwater/seawater mixing. This has also been confirmed by a relatively short residence time of 1-2 weeks for water within 25 km offshore, as obtained by short-lived radium isotopes. The irregular distribution of SGD seen at Ubatuba is a characteristic of fractured rock aquifers, fed by coastal groundwater and recirculated seawater with small admixtures of groundwater, which is of potential environmental concern and has implications on the management of freshwater resources in the region.

A new Certified Reference Material for radionuclides in Irish sea sediment (IAEA-385).

A new Certified Reference Material (CRM) for radionuclides in sediment (IAEA-385) is described and the results of the certification process are presented. Eleven radionuclides ((40)K, (137)Cs, (226)Ra, (228)Ra, (230)Th, (232)Th, (234)U, (238)U, (238)Pu, (239+240)Pu and (241)Am) have been certified and information mass activities with 95% confidence intervals are given for seven other radionuclides ((90)Sr, (210)Pb((210)Po), (235)U, (239)Pu, (240)Pu and (241)Pu). Results for less frequently reported radionuclides ((60)Co, (99)Tc, (134)Cs, (155)Eu, (224)Ra and (239)Np) and information on some activity and mass ratios are also reported. The CRM can be used for quality assurance/quality control of the analysis of radionuclides in sediment samples, for the development and validation of analytical methods and for training purposes.

Anthropogenic 137Cs on atmospheric aerosols in Bratislava and around nuclear power plants in Slovakia.

Nuclear power plants (NPPs) have been one of the sources of anthropogenic radionuclides in the environment. This work combines the results from monitoring stations around NPPs in Slovakia (Mochovce and Jaslovské Bohunice) and academic measurements at the Comenius University campus in Bratislava. Most of the atmospheric 137Cs in this region come from the resuspension of the Chernobyl-derived 137Cs, as well as caesium produced during nuclear weapons testing. By comparison of the obtained results at NPPs with Bratislava data, radiation impacts of the NPPs on the local environments have been estimated to be negligible.

Environmental radionuclides as contaminants of HPGe gamma-ray spectrometers: Monte Carlo simulations for Modane underground laboratory.

The main limitation in the high-sensitive HPGe gamma-ray spectrometry has been the detector background, even for detectors placed deep underground. Environmental radionuclides such as 40K and decay products in the 238U and 232Th chains have been identified as the most important radioactive contaminants of construction parts of HPGe gamma-ray spectrometers. Monte Carlo simulations have shown that the massive inner and outer lead shields have been the main contributors to the HPGe-detector background, followed by aluminum cryostat, copper cold finger, detector holder and the lead ring with FET. The Monte Carlo simulated cosmic-ray background gamma-ray spectrum has been by about three orders of magnitude lower than the experimental spectrum measured in the Modane underground laboratory (4800 m w.e.), underlying the importance of using radiopure materials for the construction of ultra-low-level HPGe gamma-ray spectrometers.

Plutonium and 137Cs in surface water of the South Pacific Ocean.

The present plutonium and 137Cs concentrations in South Pacific Ocean surface waters were determined. The water samples were collected in the South Pacific mid-latitude region (32.5 degrees S) during the BEAGLE expedition conducted in 2003-04 by JAMSTEC. 239,240Pu concentrations in surface seawater of the South Pacific were in the range of 0.5 to 4.1 mBq m(-3), whereas 137Cs concentrations ranged from 0.07 to 1.7 Bq m(-3). The observed 239,240Pu and 137Cs concentrations in the South Pacific were almost of the same level as those in the North Pacific subtropical gyre. The surface 239,240Pu in the South Pacific subtropical gyre showed larger spatial variations than 137Cs, as it may be affected by physical and biogeochemical processes. The 239,240Pu/137Cs activity ratios, which reflect biogeochemical processes in seawater, were generally smaller than that observed in global fallout, except for the most eastern station. The 239,240Pu/137Cs ratios in the South Pacific tend to be higher than that in the North Pacific. The relationships between anthropogenic radionuclides and oceanographic parameters such as salinity and nutrients were examined. The 137Cs concentrations in the western South Pacific (the Tasman Sea) and the eastern South Pacific were negatively correlated with the phosphate concentration, whereas there is no correlation between the 137Cs and nutrients concentrations in the South Pacific subtropical gyre. The mutual relationships between anthropogenic radionuclides and oceanographic parameters are important for better understanding of transport processes of anthropogenic radionuclides and their fate in the South Pacific.

Monte Carlo simulation of background characteristics of a HPGe detector operating underground in the Gran Sasso National Laboratory.

Monte Carlo (MC) simulation of background components of an ultra-low background high purity germanium (HPGe) detector operating in a deep underground laboratory was carried out. The results show that the background of the HPGe detector is about two orders of magnitude higher than the MC prediction when accounting only for cosmic-ray induced background. The difference is due to natural radioactivity in the parts surrounding the Ge detector. To get reasonable agreement between MC simulations and the experiment, a contamination in the parts surrounding the Ge crystal from 40K, 208Tl and 214Bi of 0.1mBqkg-1 was required to include in the simulations.

The valley system of the Jihlava river and Mohelno reservoir with enhanced tritium activities.

The Dukovany nuclear power plant (NPP Dukovany) releases liquid effluents, including HTO, to the Mohelno reservoir, located in a deep valley. Significantly enhanced tritium activities were observed in the form of non-exchangeable organically bound tritium in the surrounding biota which lacks direct contact with the water body. This indicates a tritium uptake by plants from air moisture and haze, which is, besides the uptake by roots from soil, one of the most important mechanisms of tritium transfer from environment to plants. Results of a pilot study based on four sampling campaigns in 2011-2015 are presented and discussed, with the aim to provide new information on tritium transport in the Mohelno reservoir - Jihlava River - plants ecosystems.