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.

Analysis of radioxenon and Krypton-85 at the BfS noble gas laboratory.

Proportional counters and a ß-γ coincidence system and their performance characteristics are described, with emphasis on internal and external quality controls. Typical limits of detection (LD) are 8mBqm-3 for 85Kr and 4mBqm-3 for 133Xe for the proportional counters, while for similar xenon volumes the LD for 133Xe in the ß-γ system is approximately 4 times lower. Results of comparative analyses agree above the limit of quantification. Xenon-133 levels in southern Germany are presently at or below the LD of the proportional counters, but above the LD of the ß-γ system, which is now routinely used for analysis of environmental samples.

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.

Trace analysis of aerosol bound particulates and noble gases at the BfS in Germany.

The Federal Office for Radiation Protection (BfS) performs trace analysis measurements in both the frameworks of the German Integrated Measuring and Information system as well as of the International Monitoring System for verification of the Comprehensive Nuclear-Test-Ban Treaty. Therefore, different kinds of measurements of aerosol bound radionuclides as well as of radioactive noble gases in the atmosphere are performed. BfS as coordinating laboratory for trace analysis is responsible for the quality control. A quality assurance programme was set up with German institutions and expanded to European laboratories. The existing quality assurance programme of the Comprehensive Nuclear-Test-Ban Treaty Organisation for measurements of aerosol bound radionuclides will be extended for noble gas measurements. Applied methods, achieved measurement results and the different kinds of quality assurance are presented and discussed.

An inter-laboratory comparison of low-level measurements in ground-level aerosol monitoring.

After the nuclear reactor accident of Chernobyl, the "Integrated Measurement and Information System (IMIS) for Monitoring the Environmental Radioactivity and Detecting Emissions from Nuclear Plants was implemented in Germany. IMIS is a nationwide comprehensive measuring system which permanently monitors the radioactivity in all important environment media in the whole federal territory. At approximately 40 sites, the activity concentration of radioactive substances is measured in air and precipitations. At least 14 of them are responsible for trace monitoring of radionuclides in the air. The legal bases of IMIS prescribe regular inter-laboratory comparison analyses in cooperation with the Physikalisch-Technische Bundesanstalt (PTB), with the use of reference materials prepared by the Federal Coordinating Laboratories. In order to fulfil this requirement in the field of trace survey measurements in ground-level air, the Federal Office for Radiation Protection ("Bundesamt für Strahlenschutz", BfS) and the PTB have conducted a comparison with real, dust-loaded reference filters in 2005. The comparison was organized within the framework of a cooperation of trace survey stations from Austria, Germany and Switzerland. The paper describes the preparation of the real, dust-loaded reference filters, the procedure for spiking the filters with the activity standard solution containing (22)Na, (88)Y, (89)Sr, (90)Sr, (125)Sb, (133)Ba, (134)Cs, and (241)Am. Some results are discussed and conclusions are given.

Three years of operational experience from Schauinsland CTBT monitoring station.

Data from three years of operation of a low-level aerosol sampler and analyzer (RASA) at Schauinsland monitoring station are reported. The system is part of the International Monitoring System (IMS) for verification of the Comprehensive Nuclear-Test-Ban Treaty (CTBT). The fully automatic system is capable to measure aerosol borne gamma emitters with high sensitivity and routinely quantifies 7Be and 212Pb. The system had a high level of data availability of 90% within the reporting period. A daily screening process rendered 66 tentative identifications of verification relevant radionuclides since the system entered IMS operation in February 2004. Two of these were real events and associated to a plausible source. The remaining 64 cases can consistently be explained by detector background and statistical phenomena. Inter-comparison with data from a weekly sampler operated at the same station shows instabilities of the calibration during the test phase and a good agreement since certification of the system.

Monitoring ground-level air for trace analysis: methods and results.

Trace analysis enables the sensitive detection of radionuclide concentrations in ground-level air in the range of microbecquerel per cubic meter (microBq m(-3)). Typical sampling intervals of less than one day up to a few days can be used in routine operation. Trace analysis measurements are performed in the framework of the German Integrated Measuring and Information system (IMIS) and the International Monitoring System (IMS) used for verification of the Comprehensive Nuclear-Test-Ban Treaty (CTBT). Within the environmental monitoring programmes of the German IMIS the Federal Office for Radiation Protection (BfS) performs measurements of aerosol-bound radionuclides and of radioactive noble gases in the atmosphere. Aerosols are collected on filters with high-volume air samplers and analysed by gamma-spectrometry, alpha-spectrometry, and integral measurements of beta-activity, with preceding radiochemical separation. Noble gas samples from 15 sites world-wide are analysed to observe the (85)Kr-release from nuclear fuel reprocessing plants and from seven sites in Germany to monitor the (133)Xe emitted from nuclear power plants. As part of the International Monitoring System (IMS) of the CTBT an automatic aerosol sampling and measuring system and an automatic noble gas sampling and measuring system will be operated by the BfS at Mount Schauinsland near Freiburg. Because of its expertise in noble gas measurements the BfS had been chosen to perform an intercomparison experiment in the BfS laboratory in Freiburg with several automatic noble gas sampling and measurement systems before their installation at IMS sites. To establish quality-assurance programmes for trace analysis performed for the German IMIS close collaboration between the involved German institutions has been established. First steps have been taken to expand cooperation to other European laboratories. Informal data exchange already occurs between trace-analysis laboratories in Europe (Ring of Five) and helps in cases of enhanced activity concentrations to get a rapid overview of the radiological situation and to identify possible sources.