New highly radioactive particles derived from Fukushima Daiichi Reactor Unit 1 : Properties and environmental impacts

A contaminated zone elongated toward Futaba Town, north-northwest of the Fukushima Daiichi Nuclear Power Plant (FDNPP), contains highly radioactive particles released from reactor Unit 1. There are uncertainties associated with the physio-chemical properties and environmental impacts of these particles. In this study, 31 radioactive particles were isolated from surface soils collected 3.9 km north-northwest of the FDNPP. Two of these particles have the highest particle-associated 134+137Cs activity ever reported for Fukushima (6.1 × 105 and 2.5 × 106 Bq per particle after decay-correction to March 2011). The new, highly-radioactive particle labeled FTB1 is an aggregate of flaky silicate nanoparticles with an amorphous structure containing ~0.8 wt% Cs, occasionally associated with SiO2 and TiO2 inclusions. FTB1 likely originates from the reactor building, which was damaged by a H2 explosion, after adsorbing volatilized Cs. The 134+137Cs activity in the other highly radioactive particle labeled FTB26 exceeded 106 Bq. FTB26 has a glassy carbon core and a surface that is embedded with numerous micro-particles: Pb–Sn alloy, fibrous Al-silicate, Ca-carbonate or hydroxide, and quartz. The isotopic signatures of the micro-particles indicate neutron capture by B, Cs volatilization, and adsorption of natural Ba. The composition of the micro-particles on FTB26 reflects the composition of airborne particles at the moment of the H2 explosion. Owing to their large size, the health effects of the highly radioactive particles are likely limited to external radiation during static contact with skin; the highly radioactive particles are thus expected to have negligible health impacts for humans. By investigating the mobility of the highly radioactive particles, we can better understand how the radiation dose transfers through environments impacted by Unit 1. The highly radioactive particles also provide insights into the atmospheric conditions at the time of the Unit 1 explosion and the physio-chemical phenomena that occurred during reactor meltdown.Peer reviewe

Particulate plutonium released from the Fukushima Daiichi meltdowns

Traces of Pu have been detected in material released from the Fukushima Daiichi Nuclear Power Plant (FDNPP) in March of 2011; however, to date the physical and chemical form of the Pu have remained unknown. Here we report the discovery of particulate Pu associated with cesium-rich microparticles (CsMPs) that formed in and were released from the reactors during the FDNPP meltdowns. The Cs-pollucite-based CsMP contained discrete U(IV)O2 nanoparticles,Peer reviewe

Occurrence of highly radioactive microparticles in the seafloor sediment from the Pacific coast 35 km northeast of the Fukushima Daiichi Nuclear Power Plant

To understand the properties and significance of highly radioactive particles in the marine environment, we have examined seafloor sediment with a radioactivity of ∼1200 Bq/kg (dry weight; after decay correction to March 2011) collected 35 km northeast of the Fukushima Daiichi Nuclear Power Plant (FDNPP). Among the 697 highly radioactive particles separated from the sediment, two particles, D1-MAX and D1-MID, had a total Cs radioactivity of ∼56 and 0.67 Bq (after decay correction to March 2011), respectively. These particles were characterized with a variety of electron microscopic techniques, including transmission electron microscopy. The 134Cs/137Cs radioactivity ratio of D1-MAX, 1.04, was comparable to that calculated for Unit 2 or 3. D1-MAX consisted mainly of a Cs-rich microparticle (CsMP) with a silica glass matrix. The data clearly suggested that D1-MAX resulted from a molten core–concrete interaction during meltdowns. In contrast, D1-MID was an aggregate of plagioclase, quartz, anatase, and Fe-oxide nanoparticles as well as clay minerals, which had adsorbed soluble Cs. D1-MID was likely a terrestrial particle that had been transported by wind and/or ocean currents to a site 35 km from the FDNPP. The radioactive fractions of D1-MAX and D1-MID were 15% and 0.36%, respectively, of the total radioactivity in the bulk sediment. These highly radioactive particles have a great impact on the movement of radioactive Cs in the marine environment by carrying condensed Cs radioactivity with various colloidal and desorption properties depending on the host phase

Dissolution of radioactive, cesium-rich microparticles released from the Fukushima Daiichi Nuclear Power Plant in simulated lung fluid, pure-water, and seawater

To understand the chemical durability of highly radioactive cesium-rich microparticles (CsMPs) released from the Fukushima Daiichi Nuclear Power Plant in March 2011, we have, for the first time, performed systematic dissolution experiments with CsMPs isolated from Fukushima soils (one sample with 108 Bq and one sample with 57.8 Bq of Cs-137) using three types of solutions: simulated lung fluid, ultrapure water, and artificial sea water, at 25 and 37 degrees C for 1-63 days. The Cs-137 was released rapidly within three days and then steady-state dissolution was achieved for each solution type. The steady-state Cs-137 release rate at 25 degrees C was determined to be 4.7 x 10(3), 1.3 x 10(3), and 1.3 x 10(3) Bq . m(-2)s(-1) for simulated lung fluid, ultrapure water, and artificial sea water, respectively. This indicates that the simulated lung fluid promotes the dissolution of CsMPs. The dissolution of CsMPs is similar to that of Si-based glass and is affected by the surface moisture conditions. In addition, the Cs release from the CsMPs is constrained by the rate-limiting dissolution of silicate matrix. Based on our results, CsMPs with similar to 2 Bq, which can be potentially inhaled and deposited in the alveolar region, are completely dissolved after >35 years. Further, CsMPs could remain in the environment for several decades; as such, CsMPs are important factors contributing to the long-term impacts of radioactive Cs in the environment. (C) 2019 Elsevier Ltd. All rights reserved.Peer reviewe

Abundance and distribution of radioactive cesium-rich microparticles released from the Fukushima Daiichi Nuclear Power Plant into the environment

International audienceThe abundance and distribution of highly radioactive cesium-rich microparticles (CsMPs) that were released from the Fukushima Daiichi Nuclear Power Plant (FDNPP) during the first stage of the nuclear disaster in March 2011 are described for 20 surface soils collected around the FDNPP. Based on the spatial distribution of the numbers (particles/g) and radioactive fraction (RF) of the CsMPs in surface soil, which is defined as the sum of the CsMP radioactivity (in Bq) divided by the total radioactivity (in Bq) of the soil sample, three regions of particular interest have been identified: i.) near-northwest (N-NW), ii.) far-northwest (F-NW), and iii.) southwest (SW). In these areas, the number and RF of CsMPs were determined to be 22.1–101 particles/g and 15.4–34.0%, 24.3–64.8 particles/g and 36.7–37.4%, and 0.869–8.00 particles/g and 27.6–80.2%, respectively. These distributions are consistent with the plume trajectories of material released from the FDNPP on March 14, 2011, in the late afternoon through to the late afternoon of March 15, 2011, indicating that the CsMPs formed only during this short period. Unit 3 is the most plausible source of the CsMPs at the beginning of the release based on an analysis of the sequence of release events. The lower RF values in the N-NW region indicate a larger influence from subsequent plumes that mainly consisted of soluble Cs species formed simultaneously with precipitation. The quantitative map of the distribution of CsMPs provides an important understanding of CsMP dispersion dynamics and can be used to assess risks in inhabited regions