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.
Nanoparticle‐based voluminous 3D networks with low densities are a unique class of materials and are commonly known as aerogels. Due to the high surface‐to‐volume ratio, aerogels and xerogels might be suitable materials for applications in different fields, e.g. photocatalysis, catalysis, or sensing. One major difficulty in the handling of nanoparticle‐based aerogels and xerogels is the defined patterning of these structures on different substrates and surfaces. The automated manufacturing of nanoparticle‐based aerogel‐ or xerogel‐coated electrodes can easily be realized via inkjet printing. The main focus of this work is the implementation of the standard nanoparticle‐based gelation process in a commercial inkjet printing system. By simultaneously printing semiconductor nanoparticles and a destabilization agent, a 3D network on a conducting and transparent surface is obtained. First spectro‐electrochemical measurements are recorded to investigate the charge–carrier mobility within these 3D semiconductor‐based xerogel networks.
A contamination with
the ubiquitous radioactive fission product 137Cs cannot
be assigned per se to its source.
We used environmental samples with varying contamination levels from
various parts of the world to establish their characteristic 135Cs/137Cs isotope ratios and thereby allow their
distinction. The samples included biological materials from Chernobyl
and Fukushima, historic ashed human lung tissue from the 1960s from
Austria, and trinitite from the Trinity Test Site, USA. After chemical
separation and gas reaction shifts inside a triple quadrupole ICP
mass spectrometer, characteristic 135Cs/137Cs
isotope signatures (all as per March 11, 2011) were obtained for Fukushima-
(∼0.35) and Chernobyl-derived (∼0.50) contaminations,
in agreement with the literature for these contamination sources.
Both signatures clearly distinguish from the characteristic high ratio
(1.9 ± 0.2) for nuclear-weapon-produced radiocesium found in
human lung tissue. Trinitite samples exhibited an unexpected, anomalous
pattern by displaying a low (<0.4) and nonuniform 135Cs/137Cs ratio. This exemplifies a 137Cs-rich
fractionation of the plume in a nuclear explosion, where 137Cs is a predominant species in the fireball. The onset of 135Cs was delayed because of the longer half-life of its parent nuclide 135Xe, causing a spatial separation of gaseous 135Xe from condensed 137Cs, which is the reason for the atypical 135Cs/137Cs fractionation in the fallout at the
test site.
Understanding the circumstances of the undeclared 2017 nuclear release of ruthenium that led to widespread detections of the radioisotope 106 Ru in the Eurasian region, and whether it derives from a civilian or military source, is of major importance for society and future improvements in nuclear safety. Until now, the released nuclear material has merely been studied by analyzing short-lived radioisotopes. Here, we report precise measurements of the stable isotopic composition of ruthenium captured in air filters before, during, and after the nuclear release, and find that the ruthenium collected during the period of the 2017 nuclear release has a non-natural isotopic composition. By comparing our results with ruthenium isotopic compositions of spent nuclear fuels, we show that the release is consistent with the isotopic fingerprints of a civilian Russian water-water energetic reactor (VVER) fuel at the end of its lifetime, and is not related to the production of plutonium for nuclear weapons.
The undeclared release and subsequent detection of ruthenium-106 (106Ru) across Europe from late September to early October of 2017 prompted an international effort to ascertain the circumstances of the event. While dispersion modeling, corroborated by ground deposition measurements, has narrowed possible locations of origin, there has been a lack of direct empirical evidence to address the nature of the release. This is due to the absence of radiological and chemical signatures in the sample matrices, considering that such signatures encode the history and circumstances of the radioactive contaminant. In limiting cases such as this, we herein introduce the use of selected chemical transformations to elucidate the chemical nature of a radioactive contaminant as part of a nuclear forensic investigation. Using established ruthenium polypyridyl chemistry, we have shown that a small percentage (1.2 ± 0.4%) of the radioactive106Ru contaminant exists in a polychlorinated Ru(III) form, partly or entirely as β-106RuCl3, while 20% is both insoluble and chemically inert, consistent with the occurrence of RuO2, the thermodynamic endpoint of the volatile RuO4. Together, these findings present a clear signature for nuclear fuel reprocessing activity, specifically the reductive trapping of the volatile and highly reactive RuO4, as the origin of the release. Considering that the previously established103Ru:106Ru ratio indicates that the spent fuel was unusually young with respect to typical reprocessing protocol, it is likely that this exothermic trapping process proved to be a tipping point for an already turbulent mixture, leading to an abrupt and uncontrolled release.
Related to the recent nuclear release of radioactive ruthenium isotopes in fall 2017, we analyzed air filters from Vienna for irregularities in the (stable) elemental composition of particulate matter from this period. Methods were SEM/EDXS and INAA. For comparison, a reference filter from 2007 and blank filters were used. The chemical fingerprint encompassed 28 elements. The results show no indication for a considerable change in the elemental composition of the suspended matter. For example, no anomalies in the abundance of platinum group elements were found. The results suggest that the release of 106Ru had not been accompanied by a release of detectable amounts of (activatable) stable elements.
In article number 1902186, Nadja C. Bigall and co‐workers manufacture semiconductor nanoparticle‐based aerogel‐coated electrodes automatically via inkjet printing. By simultaneously printing a destabilization agent and semiconductor nanoparticles, a 3D aerogel‐type network on a conducting and transparent surface is obtained. Furthermore, the charge‐carrier mobility within the 3D aerogel‐type network is investigated via spectro‐electrochemical measurements.
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