Atmospheric resuspension of insoluble radioactive cesium-bearing particles found in the difficult-to-return area in Fukushima

The deposition of insoluble radiocesium-bearing microparticles (CsMPs), which were released from the Fukushima Daiichi Nuclear Power Plant (F1NPP) accident in March 2011, has resulted in the widespread contamination of eastern Japan. Obviously, these deposited insoluble CsMPs may become the secondary contamination sources by atmospheric migration or other environmental transferring process; however, the understanding of the transport mechanism remains non-elucidation, and the relevant evidence has not been directly provided. This study, for the first time, provides the direct evidence for the resuspension of these insoluble CsMPs to the atmosphere from (1) proximity of ¹³⁷Cs radioactivity and resemblance of the morphology and the elemental compositions of CsMPs in the samples of soil and aerosol derived from the same sampling site, (2) the special characteristics of the resuspended CsMPs of which the ratios of Na/Si, K/Si and/or Cs/Si were smaller than those from the initially released CsMPs collected at either long distance or near F1NPP, which can be ascribed to the slowly natural corrosion of CsMPs by the loss of the small amount of soluble contents in CsMPs, and (3) high CsMPs concentration of 10 granules/g in the surface soil of our sampling site and high resuspension frequency of CsMPs in spring when predominant suspended particles were soil dust. Specifically, 15 single CsMPs were successfully isolated from the aerosol filters collected by unmanned high-volume air samplers at a severely polluted area in Fukushima Prefecture, about 25 km away from F1NPP, from January 2015 to September 2019. The mean diameter of these CsMPs was 1.8 ± 0.5 μm, and the average ¹³⁷Cs radioactivity was 0.35 ± 0.23 Bq/granule. The contribution rate of the resuspended CsMPs to the atmospheric radiocesium was estimated from the ratio of ¹³⁷Cs radioactivity of a single CsMP to that of the aerosol filter to be of 23.9 ± 15.3%. There has been no considerable decreasing trend in the annual CsMP resuspension frequency

First determination of Pu isotopes (239Pu, 240Pu and 241Pu) in radioactive particles derived from Fukushima Daiichi Nuclear Power Plant accident

Radioactive particles were released into the environment during the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident. Many studies have been conducted to elucidate the chemical composition of released radioactive particles in order to understand their formation process. However, whether radioactive particles contain nuclear fuel radionuclides remains to be investigated. Here, we report the first determination of Pu isotopes in radioactive particles. To determine the Pu isotopes (239Pu, 240Pu and 241Pu) in radioactive particles derived from the FDNPP accident which were free from the influence of global fallout, radiochemical analysis and inductively coupled plasma-mass spectrometry measurements were conducted. Radioactive particles derived from unit 1 and unit 2 or 3 were analyzed. For the radioactive particles derived from unit 1, activities of 239+240Pu and 241Pu were (1.70-7.06)×10-5 Bq and (4.10-8.10)×10-3 Bq, respectively and atom ratios of 240Pu/239Pu and 241Pu/239Pu were 0.330-0.415 and 0.162-0.178, respectively. These ratios were consistent with the simulation results from ORIGEN code and measurements from various environmental samples. In contrast, Pu was not detected in the radioactive particles derived from unit 2 or 3. The difference in Pu contents is clear evidence towards different formation processes of radioactive particles, and detailed formation processes can be investigated from Pu analysis

Investigation of the Chemical Characteristics of Individual Radioactive Microparticles Emitted from Reactor 1 by the Fukushima Daiichi Nuclear Power Plant Accident by Using Multiple Synchrotron Radiation X-ray Analyses

Seven radioactive particles were separated from a soil sample collected at the Northwest region of the Fukushima Daiichi Nuclear Power Plant (FDNPP). It has been pointed out that the soil is contaminated by radioactive materials emitted from reactor 1 of the FDNPP by the accident that occurred in March, 2011. The physical characteristics of these radioactive particles with –100 μm in diameter and non-uniform shape are clearly different from those of spherical microparticles, known as Cesium-balls, thought to be emitted from the FDNPP reactor 2. Three kinds of synchrotron radiation-based X-ray analyses (X-ray fluorescence analysis, X-ray absorption near edge structure analysis and X-ray diffraction analysis) were nondestructively applied to radioactive particles using a micro-focused X-ray beam at the SPring-8 to investigate their detailed chemical properties. Various elements related to fission products of nuclear fuel and components of the reactor were detected from the particles emitted from the FDNPP reactor 1 with an obvious heterogeneous elemental distribution. In particular, the chemical compositional feature of these particles was characterized by several elements (Sr, Ba etc.), which were easily volatilized in a reducing atmosphere. Although a main component of the particles was identified as silicate glass similar to the Cesium-balls, some crystalline materials were also found in microscopic regions containing Fe and other metallic elements. We concluded that these radioactive particles were emitted from reactor 1 to the atmosphere during 12th to 13th March, 2011. Our results suggest the fact that the nuclear fuel and the reactor vessels around the fuel were melted together at a very early stage of the accident. In addition, it was demonstrated that chemical compositional information of individual radioactive materials can be a new indicator as an alternative to the radioactive ratio to estimate the source of emissions

Provenance of uranium particulate contained within Fukushima Daiichi Nuclear Power Plant Unit 1 ejecta material.

Here we report the results of multiple analytical techniques on sub-mm particulate material derived from Unit 1 of the Fukushima Daiichi Nuclear Power Plant to provide a better understanding of the events that occurred and the environmental legacy. Through combined x-ray fluorescence and absorption contrast micro-focused x-ray tomography, entrapped U particulate are observed to exist around the exterior circumference of the highly porous Si-based particle. Further synchrotron radiation analysis of a number of these entrapped particles shows them to exist as UO2-identical to reactor fuel, with confirmation of their nuclear origin shown via mass spectrometry analysis. While unlikely to represent an environmental or health hazard, such assertions would likely change should break-up of the Si-containing bulk particle occur. However, more important to the long-term decommissioning of the reactors at the FDNPP (and environmental clean-upon), is the knowledge that core integrity of reactor Unit 1 was compromised with nuclear material existing outside of the reactors primary containment