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JAEA Reports

Analysis of risk reduction effect of supposed steam condenser implementation as accident measure for accident of evaporation to dryness by boiling of reprocessed high level liquid waste

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.

JAEA Reports

Analysis of behavior of Ru with nitrogen oxide chemical behavior in accident of evaporation to dryness by boiling of reprocessed high level liquid waste

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.

JAEA Reports

SCHERN-V2: Technical guide of computer program for chemical behavior in accident of evaporation to dryness by boiling of reprocessed high level liquid waste in Fuel Reprocessing Facilities

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$$_{rm x}$$) 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$$_{rm x}$$ 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.

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:0 Percentile:0.01(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.

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

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.

JAEA Reports

Development of analytical model for condensation of vapor mixture of nitric acid and water affected volatilized ruthenium behavior in accident of evaporation to dryness by boiling of reprocessed high level liquid waste at fuel reprocessing facilities

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.

JAEA Reports

Solvent extraction and release behavior of ruthenium and europium in fire accident conditions in reprocessing plants (Contract research)

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.

Journal Articles

Release of radioactive materials from high active liquid waste in small-scale hot test for boiling accident in reprocessing plant

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:3 Percentile:36.52(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, $$^{99}$$Tc, Cs, Sr, Nd, Y, Mo, Rh and actinides such as $$^{242}$$Cm, $$^{241}$$Am. As a result, the release ratio was 0.20 for Ru and 1$$times$$$$10^{-4}$$ 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$$^{circ}$$C. Size distribution of the mist and other particle was measured.

JAEA Reports

Investigation of release behavior of volatile ruthenium species from thermal decomposition of ruthenium nitrosylnitrate

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.

Journal Articles

Research committee on Ruthenium and Technetium Chemistry in PUREX System, Organized by the Atomic Energy Society of Japan

Matsumoto, Shiro*; Uchiyama, Gunzo; Ozawa, Masaki*; Kobayashi, Y.*; Shirato, K.*

Radiochemistry, 45(3), p.219 - 224, 2003/05

no abstracts in English

Journal Articles

Characterization of technetium-ruthenium alloys for transmutation of technetium metal

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

Journal Articles

ZrC-coated particle fuel for high temperature gas-cooled reactors

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

Journal Articles

Properties of technetium and technetium-ruthenium alloys for transmutation of technetium

Minato, Kazuo; Shirasu, Yoshiro

Proceedings of 2nd Japanese-Russian Seminar on Technetium, p.77 - 78, 1999/00

no abstracts in English

Journal Articles

Preparation and characterisation of technetium metal and technetium-ruthenium alloys

Minato, Kazuo; Shirasu, Yoshiro

Proc. of 5th Int. Information Exchange Meeting on Actinide and Fission Product Partitioning, p.223 - 230, 1998/00

no abstracts in English

Journal Articles

Fission product release from ZrC-coated fuel particles during post-irradiation heating at 1800 and 2000$$^{circ}$$C

Minato, Kazuo; Ogawa, Toru; Fukuda, Kosaku; Sekino, Hajime; Kitagawa, Isamu; Mita, Naoaki

Journal of Nuclear Materials, 249(2-3), p.142 - 149, 1997/00

 Times Cited Count:57 Percentile:95.97(Materials Science, Multidisciplinary)

no abstracts in English

Journal Articles

Fission product release from ZrC-coated fuel particles during postirradiation heating at 1600$$^{circ}$$C

Minato, Kazuo; Ogawa, Toru; Fukuda, Kosaku; H.Nabielek*; Sekino, Hajime; ;

Journal of Nuclear Materials, 224, p.85 - 92, 1995/00

 Times Cited Count:50 Percentile:96.89(Materials Science, Multidisciplinary)

no abstracts in English

JAEA Reports

Combustion behavior of spent solvent in a submerged combustion process

Uchiyama, Gunzo; Maeda, Mitsuru; Fujine, Sachio; *; *

JAERI-M 93-191, 58 Pages, 1993/10

JAERI-M-93-191.pdf:2.23MB

no abstracts in English

Journal Articles

Volatilization behaviour of ruthenium from boiling solutions

Sato, Tadashi

Journal of Radioanalytical and Nuclear Chemistry, 139(1), p.25 - 29, 1990/00

 Times Cited Count:11 Percentile:73.06(Chemistry, Analytical)

no abstracts in English

Journal Articles

Instability of some nitrosylruthenium compounds in nitric acid

Sato, Tadashi

Radiochimica Acta, 46, p.213 - 221, 1989/00

no abstracts in English

28 (Records 1-20 displayed on this page)