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.

An episode of Ru-106 in air over Europe, September-October 2017 - Geographical distribution of inhalation dose over Europe.

Between the end of September and early October 2017, 106Ru was recorded by air monitoring stations across parts of Europe. In the environment, this purely anthropogenic radionuclide can be detected very rarely only. As far as known, 106Ru is only used in radiotherapy and possibly in radiothermal generators. Therefore, the episode drew considerable interest in the monitoring community, although the activity concentrations and resulting exposure were far below radiological concern. Health consequences can be practically excluded except possibly near the source. 106Ru in aerosols could be detected for several weeks and in some regions of Central and Eastern Europe tens, up to over 100 mBq/m³ were measured as one-day means. Discussions about a possible source continue until today (early 2019). Atmospheric back-modelling led to trajectories likely originating in the Southern to Northern Ural region of Russia and possibly Northern Kazakhstan. Suspiciously, no other anthropogenic radionuclides have been observed alongside, except minute concentrations of comparatively short-lived 103Ru (half life 39 d vs. 376 d for 106Ru). Due to the absence of other anthropogenic radionuclides, a reactor accident can be excluded, although both Ru isotopes are fission products generated in nuclear reactors. The exposure resulting from 106Ru activity concentration in air exceeded 200 mBq × d/m³ in some parts of Central and Eastern Europe. This leads to inhalation doses of up to about 0.3 µSv regionally, assuming the radiologically most efficient speciation, lacking better information, and inhalation dose conversion factors from ICRP 119. We show an interpolated map of the dose distribution over parts of Europe where sufficient measurements are available to us. Overlaying population density, we give an estimate of collective dose. The opportunity is also used to give a short review of origin, properties and use of 106Ru, as well as of accidents which involved release of this radionuclide.

238Pu/(239+240)Pu activity ratio as an indicator of Pu originating from the FDNPP accident in the terrestrial environment of Fukushima Prefecture.

The Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident has caused significant radionuclide contamination. Pu isotopes at the level of GBq were released from the damaged reactors to terrestrial and marine ecosystems. In this work, 35 samples were collected at different locations of Fukushima. Samples consisted of three types, soil, forest litter and alluvial dust (road dust, sludges from drainage systems and below gutter pipe outflows). The obtained activity ratios of 238Pu/(239+240)Pu ranged from 0.030 to 1.86. 14 of our samples contained trace amounts of Pu originating from the damaged reactors (2SM verification). Our study identified a few previously unknown "hot spots" of 238Pu/(239+240)Pu activity ratio localized in an area between 15 and 30 km in the northwest direction from the FDNPP. Additionally, results obtained in this study combined with previously published data allowed us to prepare a map of spatial distribution of the Pu isotope fingerprints (238Pu/(239+240)Pu) in Fukushima Prefecture.

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.

Variations in Pu isotopic composition in soils from the Spitsbergen (Norway): Three potential pollution sources of the Arctic region.

Although the polar regions have not been industrialised, numerous contaminants originating from human activity are detectable in the Arctic environment. This study reports evidence of 240Pu/239Pu atomic ratios in the tundra and initial soils from different parts of west and central Spitsbergen and recognizes possible environmental inputs of non-global fallout Pu. The average atomic ratio of 240Pu/239Pu equal to 0.179 (ranging between 0.129 and 0.201) in tundra soils are comparable to the characteristic ratio for global fallout (0.180). However, the 240Pu/239Pu atomic ratios in the initial soils from proglacial zone of glaciers change within wide range between 0.1281 and 0.234 with the mean value of 0.169. By combining alpha and mass spectrometry, the three-sources model was used to identify the Pu sources in initial soils. Our study indicated that the main source of Pu is nuclear tests and that a second source with lower Pu ratio may come from weapons grade Pu (unexploded weapons grade Pu ie. material from bomb which didn't undergo nuclear explosions for example for security tests). Additionally, we found samples with high 238Pu/239+240Pu activity ratios and with typical global fallout 240Pu/239Pu atomic ratios, which are associated with separate sources of pure 238Pu from the SNAP-9A satellite burn up in the atmosphere.

NATURAL RADIOACTIVITY LEVEL AND ELEMENTAL COMPOSITION OF SOIL SAMPLES FROM A HIGH BACKGROUND RADIATION AREA ON EASTERN COAST OF INDIA (ODISHA).

A comprehensive study was carried out to determine the radioactivity concentration of soil samples from different sites of a high background radiation area in the eastern coast of India, Odisha state. The dose rate measured in situ varied from 0.25 to 1.2 µSv h-1 The gamma spectrometry measurements indicated Th series elements as the main contributors to the enhanced level of radiation and allowed the authors to find the mean level of the activity concentration (±SD) for 226Ra, 228Th and 40K as 130±97, 1110±890 and 360±140 Bq kg-1, respectively. Human exposure from radionuclides occurring outdoor was estimated based on the effective dose rate, which ranged from 0.14±0.02 to 2.15±0.26 mSv and was higher than the UNSCEAR annual worldwide average value 0.07 mSv. Additionally, X-ray fluorescence analysis provided information about the content of major elements in samples and indicated the significant amount of Ti (7.4±4.9 %) in soils.

Variation of counting efficiency in determination of 131I activity in the thyroid gland as a result of its position relative to the detector.

The appropriate determination of the 131I which was absorbed into the human body, especially by thyroid, depends not only on individual features of each measurement subjects but also on reproducibility of their position or the thyroid's position in the human neck. Possible uncertainties caused by changes of the thyroid position relative to detector were studied in a series of measurements. The research has shown that the dispersion of the results can reach up even to the level of 50 %.

Tracking of airborne radionuclides from the damaged Fukushima Dai-ichi nuclear reactors by European networks.

Radioactive emissions into the atmosphere from the damaged reactors of the Fukushima Dai-ichi nuclear power plant (NPP) started on March 12th, 2011. Among the various radionuclides released, iodine-131 ((131)I) and cesium isotopes ((137)Cs and (134)Cs) were transported across the Pacific toward the North American continent and reached Europe despite dispersion and washout along the route of the contaminated air masses. In Europe, the first signs of the releases were detected 7 days later while the first peak of activity level was observed between March 28th and March 30th. Time variations over a 20-day period and spatial variations across more than 150 sampling locations in Europe made it possible to characterize the contaminated air masses. After the Chernobyl accident, only a few measurements of the gaseous (131)I fraction were conducted compared to the number of measurements for the particulate fraction. Several studies had already pointed out the importance of the gaseous (131)I and the large underestimation of the total (131)I airborne activity level, and subsequent calculations of inhalation dose, if neglected. The measurements made across Europe following the releases from the Fukushima NPP reactors have provided a significant amount of new data on the ratio of the gaseous (131)I fraction to total (131)I, both on a spatial scale and its temporal variation. It can be pointed out that during the Fukushima event, the (134)Cs to (137)Cs ratio proved to be different from that observed after the Chernobyl accident. The data set provided in this paper is the most comprehensive survey of the main relevant airborne radionuclides from the Fukushima reactors, measured across Europe. A rough estimate of the total (131)I inventory that has passed over Europe during this period was <1% of the released amount. According to the measurements, airborne activity levels remain of no concern for public health in Europe.