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JAEA Reports

Utilization of gamma ray irradiation at the WASTEF Facility

Sano, Naruto; Yamashita, Naoki; Watanabe, Masaya; Tsukada, Manabu*; Hoshino, Kazutoyo*; Hirai, Koki; Ikegami, Yuta*; Tashiro, Shinsuke; Yoshida, Ryoichiro; Hatakeyama, Yuichi; et al.

JAEA-Technology 2023-029, 36 Pages, 2024/03

JAEA-Technology-2023-029.pdf:2.47MB

At the Waste Safety Testing Facility (WASTEF), the gamma ray irradiation device "Gamma Cell 220" was relocated from the 4th research building of the Nuclear Science Research Institute in FY2019, and the use of gamma ray irradiation has begun. Initially, Fuel Cycle Safety Research Group, Fuel Cycle Safety Research Division, Nuclear Safety Research Center, Sector of Nuclear Safety Research and Emergency Preparedness, the owner of this device, conducted the tests as the main user, but since 2022, other users, including those outside the organization, have started using it. The gamma ray irradiation device "Gamma Cell 220" is manufactured by Nordion International Inc. in Canada. Since it was purchased in 1989, the built-in 60Co radiation source has been updated once, and safety research related to nuclear fuel cycles, etc. It is still used for this purpose to this day. This report summarizes the equipment overview of the gamma ray irradiation device "Gamma Cell 220", its permits and licenses at WASTEF, usage status, maintenance and inspection, and future prospects.

Journal Articles

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

 Times Cited Count:0 Percentile:0.01(Nuclear Science & Technology)

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 ($$Delta$$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 $$Delta$$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.

Journal Articles

Differential pressure changes of a high airflow-type HEPA filter during solvent fire in reprocessing facilities

Tashiro, Shinsuke; Uchiyama, Gunzo; Ono, Takuya; Amano, Yuki; Yoshida, Ryoichiro; Abe, Hitoshi

Nuclear Technology, 208(7), p.1205 - 1213, 2022/07

 Times Cited Count:0 Percentile:0.01(Nuclear Science & Technology)

A clogging behavior of a high-efficiency particulate air (HEPA) filter at solvent fire accidents for reprocessing facilities has been studied. In this study, the burning rates of 30% tri-butyl phosphate (TBP)/dodecane (DD) mixed solvent and DD solvent and the differential pressure ($$Delta$$P) of a high airflow typed HEPA filter applied in the actual facilities in Japan were measured. It was confirmed that the mainly burned was DD at the early stage of the mixed solvent burning and the TBP at the late stage. Furthermore, it was found that the $$Delta$$P rapidly rose at the late stage of the mixed solvent burning. The increase of the release ratio of the unburned particulate composition (TBP, its degraded solvent and inorganic phosphorus (P$$_{2}$$O$$_{5}$$)) was considered to contribute to the rapid rise. The correlating formulas with the $$Delta$$P and the mass of the loading particulates, except for the region of the rapid rise of $$Delta$$P, could be induced.

JAEA Reports

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$$_{4}$$), 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$$_{4}$$ was enhanced by increasing the nitrous acid (HNO$$_{2}$$) concentration in the liquid phase, indicating the occurrence of chemical absorption. In control experiments without HNO$$_{2}$$, the lower the temperature, the greater was the Ru recovery ratio in the liquid phase. Conversely, in experiments with HNO$$_{2}$$, the higher the temperature, the higher the recovery ratio, suggesting that the reaction involved in chemical absorption was activated at higher temperatures.

Journal Articles

Restraint effect of coexisting nitrite ion in simulated high level liquid waste on releasing volatile ruthenium under boiling condition

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

Journal of Nuclear Science and Technology, 58(2), p.145 - 150, 2021/02

 Times Cited Count:1 Percentile:12.16(Nuclear Science & Technology)

In the "evaporation and dryness due to the loss of cooling functions" which is one of the severe accidents at reprocessing plants in Japan, ruthenium (Ru) is possible to be released much more than other elements to the environment. This cause is considered that the volatile Ru compound can be released from high level liquid waste (HLLW) as gaseous compound in adding to the release by entrainment. It was expected that the release of the volatile Ru compound from the HLLW may be able to be restrained by coexisting nitrite ion because of its reduction power. To confirm the effect of nitrite ion on the release behavior of the volatile Ru compound, four experiments of heating the simulated HLLW (SHLLW) with setting the concentration of nitrite ion in the SHLLW as a parameter ware carried out. As a result, the release of the volatile Ru compound was seemed to be restrained by adding nitrite sodium as a source of nitrite ion under certain boiling condition. This result may contribute to improve source term analysis in the evaporation and dryness due to the loss of cooling functions.

Journal Articles

Consistent modelling of material weight loss and gas release due to pyrolysis and conducting benchmark tests of the model; A Case for glovebox panel materials such as polymethyl methacrylate

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

PLOS ONE (Internet), 16(1), p.e0245303_1 - e0245303_16, 2021/01

 Times Cited Count:2 Percentile:11.76(Multidisciplinary Sciences)

It is necessary to consider how a glove box's confinement function will be lost when evaluating the amount of radioactive material leaking from a nuclear facility during a fire. In this study, we build a model that consistently explains the weight loss of glove box materials because of heat input from a flame and accompanying generation of the pyrolysis gas. The weight loss suggests thinning of the glove box housing, and the generation of pyrolysis gas suggests the possibility of fire spreading. The target was polymethyl methacrylate (PMMA), used as the glove box panel. Thermal gravimetric tests on PMMA determined the parameters to be substituted in the Arrhenius equation for predicting the weight loss in pyrolysis. The pyrolysis process of PMMA was divided into 3 stages with activation energies of 62 kJ/mol, 250 kJ/mol, and 265 kJ/mol. Furthermore, quantifying the gas composition revealed that the composition of the pyrolysis gas released from PMMA can be approximated as 100 percent methyl methacrylate. This result suggests that the released amount of methyl methacrylate can be estimated by the Arrhenius equation. To investigate the validity of such estimation, a sealed vessel test was performed. In this test, we observed increase of the number of gas molecules during the pyrolysis as internal pressure change of the vessel. The number of gas molecules was similar to that estimated from the Arrhenius equation, and indicated the validity of our method. Moreover, we also performed the same tests on bisphenol-A-polycarbonate (PC) for comparison. In case of PC, the number of gas molecules obtained in the vessel test was higher than the estimated value.

JAEA Reports

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$$_{4}$$) 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$$_{2}$$). 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$$_{4}$$ (RuO$$_{4}$$(g)). As a result, the RuO$$_{4}$$(g) decomposed over time under the atmospheric gasses with NO or NO$$_{2}$$, however, the decomposition rate was slower than the results of experiments without NOx. These results showed that the NOx stabilized RuO$$_{4}$$(g).

Journal Articles

Decomposition behavior of gaseous ruthenium tetroxide under atmospheric conditions assuming evaporation to dryness accident of high-level liquid waste

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

Journal of Nuclear Science and Technology, 57(11), p.1256 - 1264, 2020/11

 Times Cited Count:8 Percentile:71.58(Nuclear Science & Technology)

Emphasis has been placed on the behavior of ruthenium (Ru) in the evaporation to dryness accident due to the loss of cooling functions (EDLCF) of high-level liquid waste in fuel reprocessing plants. It is because Ru would form volatile compounds such as ruthenium tetroxide (RuO$$_{4}$$) and could be released into the environment with other coexisting gasses such as nitric acid (HNO$$_{3}$$), water (H$$_{2}$$O). To contribute to the safety evaluation of this accident, we experimentally evaluated the decomposition and chemical change behavior of the gaseous RuO$$_{4}$$ (RuO$$_{4}$$(g)) under the various atmospheric conditions: temperature and composition of coexisting gasses. As a result, the behavior of the RuO$$_{4}$$(g) was diverse depending on the atmospheric conditions. In the experiments with the dry air or H$$_{2}$$O vapor, decomposition of RuO$$_{4}$$(g) was observed. In the experiment with the mixed gas which containing HNO$$_{3}$$, almost no decomposition of the RuO$$_{4}$$(g) was observed, and chemical form of the RuO$$_{4}$$(g) was retained.

Journal Articles

Rapid clogging of high-efficiency particulate air filters during in-cell solvent fires at reprocessing facilities

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

Nuclear Technology, 206(1), p.40 - 47, 2020/01

 Times Cited Count:2 Percentile:24.28(Nuclear Science & Technology)

Recent Japanese nuclear regulations have focused on the hazards of in-cell solvent fires at reprocessing facilities. In this work, a mixture of tributyl phosphate and dodecane-based solvents was burned to generate an aerosol composed of soot and unburned solvent that was then loaded onto a high-efficiency particulate air filter simulating the ventilation system of reprocessing facilities. A radical increase of differential pressure occurred in the filters during these tests after the dodecane burned out from the solvent in a phenomenon we named as rapid clogging, likely caused by the burnout of dodecane. This relationship provides valuable insight into the establishment of new regulations for reprocessing facilities. This work indicates that clogging of ventilation filters during solvent fires may occur more rapidly than previously estimated.

Journal Articles

Estimation of hydrogen gas production at transient criticality in uranyl nitrate solution

Yoshida, Ryoichiro; Yamane, Yuichi; Abe, Hitoshi

Proceedings of International Nuclear Fuel Cycle Conference / Light Water Reactor Fuel Performance Conference (Global/Top Fuel 2019) (USB Flash Drive), p.408 - 414, 2019/09

In a criticality accident, it is known that some kinds of radiolysis gases are generated mainly due to kinetic energy of fission fragments. Hydrogen gas (H$$_{2}$$) is one of them, which is able to initiate explosion. The rate of H$$_{2}$$ generation and its total amount can be estimated from the number of fission per second if its G value is known. In this study, it was tried to estimate G value of hydrogen gas (G(H$$_{2}$$)) by using the H$$_{2}$$ concentration measured as time-series data in Transient Experiment Critical Facility (TRACY) which was carried out by Japan Atomic Energy Agency. There was time lag in the measured H$$_{2}$$ concentration from its generation. To overcome those problems, measured profile of H$$_{2}$$ concentration was reproduced based on a hypothetical model and its total amount was evaluated. Based on the model, the obtained G(H$$_{2}$$) was 1.2.

Journal Articles

Analysis of chemical behavior of nitrogen oxide formed by thermal decomposition of FP nitrates in accident of evaporation to dryness by boiling of reprocessed high-level liquid waste

Yoshida, Kazuo; Tamaki, Hitoshi; Yoshida, Naoki; Yoshida, Ryoichiro; Amano, Yuki; Abe, Hitoshi

Nihon Genshiryoku Gakkai Wabun Rombunshi, 18(2), p.69 - 80, 2019/06

An accident of evaporation to dryness by boiling of high level liquid waste (HLLW) is postulated as one of the severe accidents at a fuel reprocessing plant. In this case, volatile radioactive materials, such as ruthenium (Ru) are released from the tanks with water and nitric-acid mixed vapor into atmosphere. In addition to this, nitrogen oxides are also released formed by the thermal decomposition of metal nitrates of fission products (FP) in HLLW. It has been observed experimentally that nitrogen oxide affects strongly to the transport behavior of Ru. Chemical reactions of nitrogen oxide with water and nitric acid are also recognized as the complex phenomena to undergo simultaneously in the vapor and liquid phases. An analysis method has been developed with coupling two types of computer codes to simulate not only thermo-hydraulic behavior but also chemical reactions in the flow paths of carrier gases. A simulation study has been also carried out with a typical facility building.

Oral presentation

Evaluation of hydrogen gas production at transient criticality in uranyl nitrate solution

Yoshida, Ryoichiro; Yamane, Yuichi; Abe, Hitoshi

no journal, , 

At criticality accident on solution fuel, it is known that hydrogen gas is generated with nuclear fission. Because of the temporary decrease effect on power through density decrease and the possibility which causes secondary accident such as explosion, it is important on safety evaluation at criticality accident that to estimate relating the amount of hydrogen gas and the number of nuclear fissions. The time history data of concentration of hydrogen gas in vent gas when the transition critically used uranyl nitrate solution, which was obtained from Transient Experiment Critical Facility (TRACY), could not be explained by simple diffusion, because of peak about 500 seconds later from reactivity addition and after that long tail. Then, calculating the transition behavior of hydrogen gas in reactor core tank by combining multiple models such as Taylor dispersion, and evaluating concentration of hydrogen gas result reproducing the measured value well. The amount of hydrogen gas also evaluated 4 mol per 10$$^{18}$$ fissions.

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