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Yoshida, Naoki; Ono, Takuya; Amano, Yuki; Yoshida, Ryoichiro; Abe, Hitoshi; Yamane, Yuichi
Nuclear Technology, 210(10), p.1999 - 2007, 2024/10
Times Cited Count：0 Percentile：0.00(Nuclear Science & Technology)A malfunction of the cooling system of high-level liquid waste (HLLW) and failure of countermeasures may lead to the "evaporation to dryness due to the loss of cooling functions" (EDLCF) of HLLW. In the EDLCF, ruthenium (Ru) can be released at a greater fraction to initial amount than other elements in HLLW by forming gaseous Ru. It is important to identify the chemical form of the released gaseous Ru to achieve a comprehensive understanding of the events impacting the source term assessment of Ru in this accident, such as particle formation, gas absorption and deposition on migration pathways. In this study, we observed the ultraviolet/visible spectroscopy of the off-gas generated during the heating of an HLLW simulant. Employing a program that allows the separation and quantification of known components within the spectrum (ruthenium tetroxide (RuO
), nitrogen dioxide, and nitric acid), we attempted to analyze the composition of gaseous Ru within the generated off-gas. Our findings reveal RuO as the main component of the gaseous Ru in off-gas after comparing the total amount of released Ru and the RuO released amount obtained via spectroscopic analysis.
Yoshida, Kazuo; Hiyama, Mina*; Tamaki, Hitoshi
JAEA-Research 2024-007, 24 Pages, 2024/08
JAEA-Research-2024-007.pdf:2.1MB
An accident of evaporation to dryness by boiling of high-level radioactive liquid waste (HLLW) is postulated as one of the severe accidents caused by the loss of cooling function 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 the atmosphere. Accurate quantitative estimation of released Ru is one of the important issues for risk assessment of those facilities. It has been observed experimentally that volatility of RuO is suppressed by HNO
generated by HNO
radiolysis. The analysis of chemical reactions of NO
including HNO and HNO in the waste tank is essential to simulate of these phenomena. To resolve this issue, an analytical approach has been attempted to couple dynamically two computer codes SHAWED and SCHERN. The simulation of boiling behavior in the tank is conducted with SHAWED. SCHERN simulates chemical behaviors of HNO, HNO and NO in the tank. A programmatic coupling algorithm and a trial simulation of the accident are presented in this report.
Yoshida, Kazuo; Tamaki, Hitoshi; Hiyama, Mina*
JAEA-Research 2023-001, 26 Pages, 2023/05
JAEA-Research-2023-001.pdf:1.61MB
An accident of evaporation to dryness by boiling of high-level radioactive liquid waste (HLLW) is postulated as one of the severe accidents caused by the loss of cooling function 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 the atmosphere. Accurate quantitative estimation of released Ru is one of the important issues for risk assessment of those facilities. To resolve this issue, an analytical approach has been developed using computer simulation programs to assess the radioactive source term from those facilities. The proposed approach consists analyses with three computer programs. At first, the simulation of boiling behavior in the HLLW tank is conducted with SHAWED code. Next step, the thermal-hydraulic behavior in the facility building is simulated with MELCOR code based on the results at the first step simulation such as flowed out mixed steam flow rate, temperature and volatilized Ru from the tank. The final analysis step is carried out for estimating amount of released radioactive materials with SCHERN computer code which simulates chemical behaviors of nitric acid, nitrogen oxide and Ru based on the condition also simulated MELCOR. Series of sample simulations of the accident at a hypothetical typical facility are presented with the data transfer between those codes in this report.
Kido, Kentaro; Kaneko, Masashi
Journal of Computational Chemistry, 44(4), p.546 - 558, 2023/02
Times Cited Count：1 Percentile：7.50(Chemistry, Multidisciplinary)Yoshida, Kazuo; Tamaki, Hitoshi; Hiyama, Mina*
JAEA-Research 2021-013, 20 Pages, 2022/01
JAEA-Research-2021-013.pdf:2.35MB
An accident of evaporation to dryness by boiling of high level liquid waste (HLLW) is postulated as one of the severe accidents caused by the loss of cooling function 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. An idea has been proposed to implement a steam condenser as an accident countermeasure. This measure is expected to prevent nitric acid steam diffusing in facility building and to increase gaseous Ru trapping ratio into condensed water. A simulation study has been carried out with a hypothetical typical facility building to analyze the efficiency of steam condenser. In this study, SCHERN computer code simulates chemical behaviors of Ru in nitrogen oxide, nitric acid and water mixed vapor based on the conditions obtained from simulation with thermal-hydraulic computer code MELCOR. The effectiveness of steam condenser has been analyzed quantitively in preventing mixed vapor diffusion and gaseous Ru trapping effect. Some issues to be solved in analytical model has been also clarified in this study.
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.
(X = 1, 2)Kido, Kentaro
International Journal of Quantum Chemistry, 121(21), p.e26781_1 - e26781_15, 2021/11
Times Cited Count：1 Percentile：12.90(Chemistry, Physical)Yoshida, Kazuo; Tamaki, Hitoshi; Hiyama, Mina*
JAEA-Research 2021-005, 25 Pages, 2021/08
JAEA-Research-2021-005.pdf:2.91MB
An accident of evaporation to dryness by boiling of high level liquid waste (HLLW) is postulated as one of the severe accidents caused by the loss of cooling function 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. Accurate quantitative estimation of released Ru is one of the important issues for risk assessment of those facilities. To resolve this issue, an empirical correlation equation of Ru mass transfer coefficient across the vapor-liquid surface, which can be useful for quantitative simulation of Ru mitigating behavior, has been obtained from data analyses of small-scale experiments conducted to clarify gaseous Ru migrating behavior under steam-condensing condition. A simulation study has been also carried out with a hypothetical typical facility building successfully to demonstrate the feasibility of quantitative estimation of amount of Ru migrating in the facility using the obtained correlation equation implemented in SCHERN computer code which simulates chemical behaviors of nitrogen oxide based on the condition also simulated thermal-hydraulic computer code.
Yoshida, Kazuo; Tamaki, Hitoshi; Hiyama, Mina*
JAEA-Data/Code 2021-008, 35 Pages, 2021/08
JAEA-Data-Code-2021-008.pdf:3.68MB
An accident of evaporation to dryness by boiling of high level liquid waste (HLLW) is postulated as one of the severe accidents caused by the loss of cooling function 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 (NO
) are also released formed by the thermal decomposition of metal nitrates of fission products (FP) in HLLW. It has been observed experimentally that NOx affects to the migration behavior of Ru at the anticipated atmosphere condition in cells and/or compartments of the facility building. Chemical reactions of NO with water and nitric acid are also recognized as the complex phenomena to undergo simultaneously in the vapor and liquid phases. The analysis program, SCHERN has been under developed to simulate chemical behavior including Ru coupled with the thermo-hydraulic condition in the flow paths in the facility building. This technical guide for SCHERN-V2 presents the overview of covered accident, analytical models including newly developed models, differential equations for numerical solution, and user instructions.
Yoshida, Ryoichiro; Amano, Yuki; Yoshida, Naoki; Abe, Hitoshi
Journal of Nuclear Science and Technology, 58(2), p.145 - 150, 2021/02
Times Cited Count：2 Percentile：19.27(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.
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).
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.
Yoshida, Kazuo
JAEA-Research 2016-012, 24 Pages, 2016/08
JAEA-Research-2016-012.pdf:3.04MB
An accident of evaporation to dryness by boiling of high level liquid waste is postulated as one of the severe accidents. In this case, Ru volatilization increases in liquid waste temperature over 120 centigrade at later boiling and dry out phases. It has been observed at the experiments with actual and synthetic liquid waste that some amount of Ru volatilizes and transfers into condensed nitric acid solution at those phases. The nitric acid and water vapor from waste tank condenses at compartments of actual facilities building. The volatilized Ru could transfer into condensed liquid. It is key issues for quantifying the amount of transferred Ru through the facility building to simulate these thermodynamic and chemical behaviors. An analytical model has been proposed in this report based on the condensation mechanisms of nitric acid and water in vapor-liquid equilibria. It has been also carried out to review the thermodynamic properties of nitric acid solution.
Amano, Yuki; Watanabe, Koji; Masaki, Tomoo; Tashiro, Shinsuke; Abe, Hitoshi
JAEA-Technology 2016-012, 21 Pages, 2016/06
JAEA-Technology-2016-012.pdf:1.81MB
To contribute to safety evaluation of fire accident in fuel reprocessing plants, solvent extraction behavior of ruthenium, which could form volatile species, was investigated. Distribution ratios of ruthenium at fire accident conditions were obtained by extraction experiments with several solvent composition at different temperature as parameters. In order to investigate release behavior of ruthenium and europium at fire accident, release ratios of ruthenium and europium were also obtained by solvent combustion experiments.
Yamane, Yuichi; Amano, Yuki; Tashiro, Shinsuke; Abe, Hitoshi; Uchiyama, Gunzo; Yoshida, Kazuo; Ishikawa, Jun
Journal of Nuclear Science and Technology, 53(6), p.783 - 789, 2016/06
Times Cited Count：6 Percentile：46.39(Nuclear Science & Technology)The release behavior of radioactive materials from high active liquid waste (HALW) has been experimentally investigated under boiling accident conditions. In the experiments using HALW obtained through laboratory scale reprocessing, release ratio was measured for the FP nuclides such as Ru, 
Tc, Cs, Sr, Nd, Y, Mo, Rh and actinides such as 
Cm, 
Am. As a result, the release ratio was 0.20 for Ru and 1
for the FP and Ac nuclides. Ru was released into the gas phase in the form of both mist and gas. For its released amount, weak dependency was found to the initial concentration in the test solution. The release ratio decreased with the initial concentration. For other FP nuclides and actinides as non-volatile, released into the gas phase in the form of mist, the released amount increased with the initial concentration. The release ratio of Ru and NOx concentration increased with temperature of the test solutions. They were released almost at the same temperature between 200 and 300
C. Size distribution of the mist and other particle was measured.
Abe, Hitoshi; Masaki, Tomoo; Amano, Yuki; Uchiyama, Gunzo
JAEA-Research 2014-022, 12 Pages, 2014/11
JAEA-Research-2014-022.pdf:1.03MB
To contribute safety evaluation of boiling and drying accident of high active liquid waste (HALW) in fuel reprocessing plant, release behavior of Ru, which was considered as an important nuclide for evaluating public dose from the volatile viewpoint, has been investigated. It has been reported that release of Ru becomes conspicuously after HALW is dried up. In this work, to grasp the release behavior of Ru, release ratio of Ru with thermal decomposition of Ru nitrate, which would be in the dried HALW, was measured and release rate constant of Ru from the nitrate was estimated. It was found that the calculation result of release rate of Ru from the nitrate with rise of temperature by using the constant could well simulate the result acquired from the beaker-scale experiment.
Matsumoto, Shiro*; Uchiyama, Gunzo; Ozawa, Masaki*; Kobayashi, Y.*; Shirato, K.*
Radiochemistry, 45(3), p.219 - 224, 2003/05
no abstracts in English
Minato, Kazuo; Ogawa, Toru; Sawa, Kazuhiro; Sekino, Hajime; Koya, Toshio; Kitagawa, Isamu; Ishikawa, Akiyoshi; Tomita, Takeshi;
Proc. of the Int. Conf. on Future Nuclear Systems (GLOBAL'99)(CD-ROM), 8 Pages, 1999/00
no abstracts in English
Shirasu, Yoshiro; Minato, Kazuo
Proc. of the Int. Conf. on Future Nuclear Systems (GLOBAL'99)(CD-ROM), 7 Pages, 1999/00
no abstracts in English
Minato, Kazuo; Shirasu, Yoshiro
Proceedings of 2nd Japanese-Russian Seminar on Technetium, p.77 - 78, 1999/00
no abstracts in English
