Fukushima Daiichi Nuclear Power Plant Accident; Understanding Formation Mechanism of Radioactive Particles through Sr and Pu Quantities

Igarashi, Junya*; Ninomiya, Kazuhiko*; Zheng, J.*; Zhang, Z. J.*; Fukuda, Miho*; Aono, Tatsuo*; Minowa, Haruka*; Yoshikawa, Hideki*; Sueki, Keisuke*; Satou, Yukihiko; et al.

Environmental Science & Technology, 58(33), p.14823 - 14830, 2024/08

https://doi.org/10.1021/acs.est.4c03428

Behavior of radiocesium in sediments in Fukushima coastal waters; Verification of desorption potential through pore water

Otosaka, Shigeyoshi*; Kambayashi, Shota*; Fukuda, Miho*; Tsuruta, Tadahiko; Misono, Toshiharu; Suzuki, Takashi; Aono, Tatsuo*

Environmental Science & Technology, 54(21), p.13778 - 13785, 2020/11

https://doi.org/10.1021/acs.est.0c05450

Concentrations of Cs in seawater, seabed sediment, and pore water collected from the area around Fukushima were investigated from 2015 to 2018, and the potential of coastal sediments to supply radiocesium to the bottom environment was evaluated. The Cs concentration in the pore water ranged from 33 to 1934 mBq L and was 10-40 times higher than that in the overlying water (seawater overlying within 30 cm on the seabed). At most stations, the Cs concentrations in the overlying water and the pore water were approximately proportional to those in the sediment. The conditional partition coefficient between pore water and sediment was 0.9-1410 L kg, independent of the year of sampling. These results indicated that an equilibrium of Cs between pore water and sediment has established in a relatively short period, and Cs in the pore water is gradually exported to seawater near the seabed. A simple box model estimation based on these results showed that the Cs in the sediment was decreased by about 6% per year by desorption/diffusion of Cs from the seabed.

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

Igarashi, Junya*; Zheng, J.*; Zhang, Z.*; Ninomiya, Kazuhiko*; Satou, Yukihiko; Fukuda, Miho*; Ni, Y.*; Aono, Tatsuo*; Shinohara, Atsushi*

Scientific Reports (Internet), 9(1), p.11807_1 - 11807_10, 2019/08

https://doi.org/10.1038/s41598-019-48210-4

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 (Pu, Pu and Pu) 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 Pu and Pu were (1.70-7.06)10 Bq and (4.10-8.10)10 Bq, respectively and atom ratios of Pu/Pu and Pu/Pu 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.

Dissolved radiocaesium in seawater off the coast of Fukushima during 2013-2015

Fukuda, Miho*; Aono, Tatsuo*; Yamazaki, Shinnosuke*; Nishikawa, Jun*; Otosaka, Shigeyoshi; Ishimaru, Takashi*; Kanda, Jota*

Journal of Radioanalytical and Nuclear Chemistry, 311(2), p.1479 - 1484, 2017/02

https://doi.org/10.1007/s10967-016-5009-9

In order to investigate processes affecting distribution of radiocaesium in seawater in the adjacent region of Fukushima Daiichi Nuclear Power Plant (FDNPP), relationships between Cs activity in seawater and physical properties of seawater (salinity, temperature, and potential density) were observed in seven stations within 10 km radius from the FDNPP. As a whole, Cs concentrations in seawater were higher in the vicinity of the FDNPP, and were negatively correlated with potential density. From these results, it can be considered that river water discharge or export of seawater from the FDNPP's harbor has affected the higher activity levels of Cs in seawater. It was also observed that the Cs-elevated seawater can be advected to the 2050 m depths.

Radiocaesium dynamics in forested watersheds in Fukushima Prefecture

Taniguchi, Keisuke*; Takeuchi, Yukio*; Fujita, Kazuki*; Dohi, Terumi; Hayashi, Seiji*; Kuramoto, Takayuki*; Nomura, Naoki*; Aono, Tatsuo*

no journal, , 

In Fukushima Prefecture, although decontamination has been completed except for difficult-to-return areas, most of the forest has not been decontaminated yet. From the forest, radiocaesium may enter rivers and affect downstream areas. A survey was conducted in three forested watersheds of the Nanokazawa, Saruta, Nuno rivers located in Fukushima Prefecture to understand the amount and characteristics of radiocaesium flowing out. In each watershed, suspended solids (SS) were collected by a suspended sand sampler, water was collected every few months, and the water level and flow rate were measured. After freeze-drying the SS sample, the concentration of suspended Cs-137 was measured by a germanium semiconductor detector. The water sample was filtered through a membrane filter with a pore size of 0.45 m, then the dissolved Cs-137 was collected by the solid-phase extraction disk method or AMP coprecipitation method, and the dissolved Cs-137 concentration was measured by a germanium semiconductor detector. The ranges of dissolved Cs-137 concentration in FY2019 were 69-190 mBq/L in the Saruta River, 9.7-16 mBq/L in the Nanokazawa river, and ND-3.2 mBq/L in the Nuno River. In the poster, we will also present the results of SS measurements and flow observations.

Validation of exposure dose simulation considering life patterns

Sato, Rina; Yoshimura, Kazuya; Sanada, Yukihisa; Yajima, Kazuaki*; Aono, Tatsuo*

no journal, , 

no abstracts in English

Variation of radiocesium concentration in seawater and sediments at FDNPS

Aono, Tatsuo*; Fukuda, Miho*; Sakurada, Masanobu*; Takahashi, Hiroyuki*; Yamazaki, Shinnosuke*; Kambayashi, Shota*; Misono, Toshiharu; Nakanishi, Takahiro; Miura, Hikaru*; Nishikawa, Jun*; et al.

no journal, , 

From 2016 to 2020, R/V Shinsei-maru of JAMSTEC conducted four research cruises on the dynamics and bioavailability of radionuclides around off Fukushima. Seawater, sediments and organisms were collected mainly around off the Fukushima Daiichi Nuclear Power Plant (FDNPS). The purpose of those cruises is to observe the flux of radionuclides released into the ocean by the FDNPS accident and to understand the bioavailability of radionuclides. In order to understand the contaminated levels of the marine environment, the concentration of radiocaesium (Cs) in seawater and sediments around off Fukushima was investigated.

Behavior of radiocesium at sediment-water interface off Fukushima

Otosaka, Shigeyoshi; Fukuda, Miho*; Aono, Tatsuo*

no journal, , 

Behavior of dissolved radiocesium near the seafloor is discussed from the distributions of Cs in overlying water (seawater collected from 30 cm above the seabed) at 14 stations and in pore water at 3 stations off Fukushima (170 km from Fukushima Daiichi Nuclear Power Plant). The Cs concentrations in overlying water, collected during 2015 and 2016, ranged between 5 and 283 mBq/L. The Cs concentrations in overlying water were 23 times higher than those in seawater collected from intermediate (5 m above the bottom) layers. The Cs concentrations in pore water were 1030 times higher than those in overlying water. We can consider that radiocesium is dissolved in the overlying water and has been diffused from the seabed through the porewater. Nevertheless, it was estimated that the amount of Cs transferred from porewater to benthic organisms does not lead to Cs activities exceeding the regulation limits at most stations.

Exchange of radiocesium between sediment and pore water in the coastal seabed off Fukushima

Otosaka, Shigeyoshi; Fukuda, Miho*; Aono, Tatsuo*

no journal, , 

Behavior of dissolved radiocesium near the seafloor is discussed from the distributions of Cs in seawater, seabed sediment and pore water collected from the area around Fukushima. The Cs concentrations in the pore water, collected from 2015 to 2017, ranged between 33 and 1186 mBq/L, and were 1040 times higher than those in seawater on the sediment surface. The Cs concentration in the overlying water did not show clear differences regardless of the pore size of the filter used for filtration. From these results, it was confirmed that radiocesium in the seabed sediment was dissolved in pore water and diffused to the benthic layer. The apparent distribution coefficient between pore water and sediment was [0.94.2]10 L/kg, with no difference depending on the year of sampling. These results indicated that an equilibrium of Cs between pore water and sediment has established during the observation period.

Identification of plutonium isotopes in insoluble particles released by the accident of Fukushima Daiichi Nuclear Power Plant

Igarashi, Junya*; Zheng, J.*; Zhang, Z.*; Ninomiya, Kazuhiko*; Satou, Yukihiko; Fukuda, Miho*; Ni, Y.*; Aono, Tatsuo*; Shinohara, Atsushi*

no journal, , 

Plutonium is one of the most notable radionuclides in the nuclear accident. The amounts of Pu released by the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident were investigated so far. However, the existence of Pu isotopes from the global fallout makes it difficult to accurately assessment of Pu contamination by the FDNPP accident. To avoid this problem, identification of Pu contamination source from the Pu isotopic ratios is important. However, various ratios have been reported by the researches due to the contamination from global fallout. In this work, we focused on the insoluble radioactive Cs particles made of mainly SiO (insoluble particles) released from the FDNPP to determine accurate Pu isotopic ratios. Due to its insolubility, the particles retained the original property at the time of emission from the reactor. Therefore, the insoluble particles are considered to be free from the contamination of global fallout. In addition, the amounts of Pu in the insoluble particles provide the information about their formation process in the reactor. In this study, we identified Pu isotopes in insoluble particles by radioactive analysis and ICP-MS measurement. The isotopic ratios of Pu/Pu and Pu/Pu were determined as 0.330-0.415 and 0.162-0.178, respectively and activity ratio of Pu/Cs was about 10 in each particle.