Mechanistic insights into volatile ruthenium tetroxide formation during evaporation-to-dryness accidents of high-level liquid waste

Yoshida, Naoki; Amano, Yuki; Yoshida, Ryoichiro; Ono, Takuya; Tashiro, Shinsuke; Yamane, Yuichi

Journal of Hazardous Materials, 513, p.142332_1 - 142332_20, 2026/07

https://doi.org/10.1016/j.jhazmat.2026.142332

Volatile ruthenium tetroxide (RuO) formed during evaporation-to-dryness accidents (EDA) of high-level liquid waste (HLLW) combines high chemical toxicity with radiotoxicity from isotopes such as Ru and Ru, making it a primary hazard in nuclear-fuel reprocessing. This study experimentally elucidates the mechanisms governing RuO formation while testing the validity of the pragmatic nitrosyl-ruthenium ([RuNO]) surrogate model, an experimental model that assumes Ru in HLLW exists as [RuNO], and evaluates gaseous Ru release using nitric acid solutions of [RuNO], commonly used in RuO release assessments by comparing it with the behavior of simulated HLLW (s-HLLW). We systematically investigated potential pathways, including oxidation by liquid-phase nitric acid (HNO(l)), gas-phase nitric acid (HNO(g)), and oxygen (O2); thermal decomposition of [RuNO]; and matrix effects of coexisting nitrates. The results identify oxidation by activated HNO(l), oxidation by HNO(g) and thermal decomposition of [RuNO] as the principal routes to RuO, with HNO(g) playing a far more significant role than previously recognized. Crucially, the RuO release profile from s-HLLW differed markedly from that predicted by the [RuNO] surrogate model, demonstrating that this model fails to capture the complex matrix effects and time-dependent chemical changes of Ru species inherent to real HLLW. These findings have significant implications for improving the accuracy of hazard assessments related to RuO release during HLLW EDAs, particularly by highlighting the limitations of commonly used [RuNO] surrogate models.

Spin current generation by acousto-electric evanescent wave

Kawada, Takuya*; Yamamoto, Kei; Kono, Hiroshi*; Hayashi, Masamitsu*

Proceedings of SPIE, Vol.14081, p.140810M_1 - 140810M_6, 2026/05

https://doi.org/10.1117/12.3099294

Metallization and pressure-induced superconductivity in carrier doped excitonic insulator (TaTi)NiSe

Tsuchida, Shun*; Hirose, Yusuke; Sekikawa, Takuya; Ono, Yoshiaki*; Hirahara, Takuya*; Sano, Sumika*; Kawaguchi, Shogo*; Kobayashi, Shintaro*; Uwatoko, Yoshiya*; Settai, Rikio*

Journal of the Physical Society of Japan, 94(11), p.114703_1 - 114703_7, 2025/10

https://doi.org/10.7566/JPSJ.94.114703

We investigated the carrier doping effect on an excitonic insulator TaNiSe by means of the electrical resistivity and Hall coefficient using single crystals of (TaTi)NiSe, and band calculation. The excitonic transition temperature is continuously suppressed to 83 K at = 0.104 while preserving the crystal structure. With increasing substitution concentration , a semiconducting increment of and is strongly suppressed and a metallic behavior is observed at > 0.06. Ti substitution can realize an excitonic correlated metallic state. This metallization is explained by the hole doping effect based on the band calculations. Applying pressure to the carrier doped (TaTi)NiSe, we found superconductivity above 2.6 GPa, which is much smaller than that of TaNiSe around 8 GPa. The carrier doping induced by Ti substitution favors superconductivity in this compound.

Combustion properties of glove-box panel resins under fire accidents

Tashiro, Shinsuke; Uchiyama, Gunzo; Ono, Takuya; Amano, Yuki; Yoshida, Ryoichiro; Watanabe, Koji*; Abe, Hitoshi; Yamane, Yuichi

Nuclear Technology, 211(3), p.429 - 438, 2025/03

https://doi.org/10.1080/00295450.2024.2329832

Contributing to the confinement safety evaluation of glove-box (GB) connected with high efficiency particle air (HEPA) filters for radioactive materials under fire accidents, combustion tests of a flammable polymer, Polymethyl methacrylate (PMMA), and a flame retardant polymer, Polycarbonate (PC), as typical GB panel resins have been conducted with an engineering-scale combustion apparatus. The combustion properties such as the mass loss rate (MLR) and the heat release rate (HRR) of PMMA and PC were investigated in the combustion tests. In the tests with the same shapes, it was found the followings; MLRs and HRRs of PMMA were larger than those of PC under the same supply flow rate into the combustion cell (Fv); MLRs and HRRs of PMMA and PC were constant under different Fv. Moreover, in the tests of PMMA with different cross section areas (S), MLRs and HRRs were found to be proportional to S. Using these results, the relationships of MLR and HRR to S of PMMA and PC were deduced.

Decommissioning report for Wastewater Treatment Facility (Part 2); Chapter on contamination inspection section

Yamamoto, Keisuke; Nakagawa, Takuya; Shimojo, Hiroto; Kijima, Jun; Miura, Daiya; Onose, Yoshihiko*; Namba, Koji*; Uchida, Hiroaki*; Sakamoto, Kazuhiko*; Ono, Chika*; et al.

JAEA-Technology 2024-019, 211 Pages, 2025/02

JAEA-Technology-2024-019.pdf:35.35MB

The uranium enrichment facilities at the Nuclear Fuel Cycle Engineering Laboratories of Japan Atomic Energy Agency (JAEA) were constructed sequentially to develop uranium enrichment technology with centrifugal separation method. The developed technologies were transferred to Japan Nuclear Fuel Limited until 2001. And the original purpose has been achieved. Wastewater Treatment Facility, one of the uranium enrichment facilities, was constructed in 1976 to treat radioactive liquid waste generated at the facilities, and it finished the role in 2008. In accordance with the Medium/Long-Term Management Plan of JAEA Facilities, interior equipment installed in this facility had been dismantled and removed since November 2021 to August 2023. This report summarizes the findings obtained through the work related to the contamination inspection methods cancellation the controlled area of Wastewater Treatment Facility from September 2023 to March 2024.

Changes in molecular conformation and electronic structure of DNA under C ions based on first-principles calculations

Sekikawa, Takuya; Matsuya, Yusuke; Hwang, B.*; Ishizaka, Masato*; Kawai, Hiroyuki*; Ono, Yoshiaki*; Sato, Tatsuhiko; Kai, Takeshi

Nuclear Instruments and Methods in Physics Research B, 548, p.165231_1 - 165231_6, 2024/03

https://doi.org/10.1016/j.nimb.2023.165231

One of the main causes of radiation effects on the human body is thought to be damage to DNA, which carries genetic information. However, it is not fully understood what kind of molecular structural changes DNA undergoes upon radiation damage. Since it has been reported that various types of DNA damage are formed when DNA is irradiated, our group has investigated the relationship between DNA damage and various patterns of radiation-induced ionization induced by radiation. Although we have so far analyzed DNA damage in a simple system using a rigid body model of DNA, more detailed calculations are required to analyze the molecular structural changes in DNA, which are considered to be important in considering the effects on the human body. In this study, we attempted to clarify the molecular conformational changes of DNA using OpenMX, a first-principles calculation software that can discuss electronic states based on molecular structures. Specifically, we calculated the most stable structure, band dispersion, and wave function of DNA under the assumption that one and two electrons are ionized by various radiation. In the presentation, we will discuss the relationship between the energy dependence of each incident radiation type and the molecular conformational change of DNA. In addition, the radiation-induced changes in the basic physical properties of DNA (corresponding to the initial stage of DNA damage) will be discussed from the viewpoints of both radiation physics and solid state physics.

Clogging properties of HEPA filter induced by loading of soot from burned glove-box panel materials

Tashiro, Shinsuke; Ono, Takuya; Amano, Yuki; Yoshida, Ryoichiro; Watanabe, Koji*; Abe, Hitoshi

Nuclear Technology, 208(10), p.1553 - 1561, 2022/10

https://doi.org/10.1080/00295450.2022.2045179

To contribute to the confinement safety evaluation of the radioactive materials in the Glove box (GB) fire accident, combustion tests with the Polymethyl methacrylate (PMMA) and the Polycarbonate (PC) as typical panel materials for the GB have been conducted with a relatively large scale apparatus. As the important data for evaluating confinement safety, the release ratio and the particle size distribution of the soot generated from the burned materials were obtained. Furthermore, the rise of the differential pressure (P) of the high efficiency particle air (HEPA) filter by the soot loading was also investigated. As results, the release ratio of the soot from the PC was about seven times as large as the PMMA. In addition, it was found that the behavior of the rise of the P with soot loading could be represented uniformly regardless of kinds of combustion materials by considering effect of the loading volume of the soot particle in the relatively low loading region.

Effect of nitrous acid on migration behavior of gaseous ruthenium tetroxide into liquid phase

Yoshida, Naoki; Ono, Takuya; Yoshida, Ryoichiro; Amano, Yuki; Abe, Hitoshi

JAEA-Research 2021-011, 12 Pages, 2022/01

JAEA-Research-2021-011.pdf:1.49MB

In boiling and drying accidents involving high-level liquid waste in fuel reprocessing plants, emphasis is placed on the behavior of ruthenium (Ru). Ru would form volatile species, such as ruthenium tetroxide (RuO), and could be released to the environment with coexisting gases, including nitric acid, water, or nitrogen oxides. In this study, to contribute toward safety evaluations of these types of accidents, the migration behavior of gaseous Ru into the liquid phase has been experimentally measured by simulating the condensate during an accident. The gas absorption of RuO was enhanced by increasing the nitrous acid (HNO) concentration in the liquid phase, indicating the occurrence of chemical absorption. In control experiments without HNO, the lower the temperature, the greater was the Ru recovery ratio in the liquid phase. Conversely, in experiments with HNO, the higher the temperature, the higher the recovery ratio, suggesting that the reaction involved in chemical absorption was activated at higher temperatures.

Effect of nitrogen oxides on decomposition behavior of gaseous ruthenium tetroxide

Yoshida, Naoki; Amano, Yuki; Ono, Takuya; Yoshida, Ryoichiro; Abe, Hitoshi

JAEA-Research 2020-014, 33 Pages, 2020/12

JAEA-Research-2020-014.pdf:3.66MB

Considering the boiling and drying accident of high-level liquid waste in fuel reprocessing plant, Ruthenium (Ru) is an important element. It is because Ru would form volatile compounds such as ruthenium tetroxide (RuO) and could be released into the environment with other coexisting gasses such as nitric oxides (NOx) such as nitric oxide (NO) and nitrogen dioxide (NO). To contribute to the safety evaluation of this accident, we experimentally evaluated the effect of NOx on the decomposition and chemical change behavior of the gaseous RuO (RuO(g)). As a result, the RuO(g) decomposed over time under the atmospheric gasses with NO or NO, however, the decomposition rate was slower than the results of experiments without NOx. These results showed that the NOx stabilized RuO(g).

Competing spin modulations in the magnetically frustrated semimetal EuCuSb

Takahashi, Hidefumi*; Aono, Kai*; Nambu, Yusuke*; Kiyanagi, Ryoji; Nomoto, Takuya*; Sakano, Masato*; Ishizaka, Kyoko*; Arita, Ryotaro*; Ishiwata, Shintaro*

Physical Review B, 102(17), p.174425_1 - 174425_6, 2020/11

https://doi.org/10.1103/PhysRevB.102.174425

The competing magnetic ground states of the itinerant magnet EuCuSb, which has a hexagonal layered structure, were studied via magnetization, resistivity, and neutron-diffraction measurements on single-crystal samples. EuCuSb has a three-dimensional semimetallic band structure as confirmed by band calculation and angle-resolved photoelectron spectroscopy, consistent with the nearly isotropic metallic conductivity in the paramagnetic state. However, below the antiferromagnetic transition temperature of (8.5 K), the resistivity, especially along the hexagonal axis, increases significantly. This implies the emergence of anisotropic magnetic ordering coupled to the conducting electrons. Neutron-diffraction measurements show that the Eu spins, which order ferromagnetically within each layer, are collinearly modulated (up-up-down-down) along the hexagonal axis below , followed by the partial emergence of helical spin modulation below (6 K). Based on the observation of anomalous magnetoresistance with hysteretic behavior, we discuss the competing nature of the ground state inherent in a frustrated Heisenberg-like spin system with a centrosymmetric structure.