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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

Thermal-hydraulics to risk assessment; Roles of thermal-hydraulics simulation to risk assessment

Maruyama, Yu; Yoshida, Kazuo

Nihon Genshiryoku Gakkai-Shi ATOMO$$Sigma$$, 63(7), p.517 - 522, 2021/07

no abstracts in English

Journal Articles

Iodine-129 in the Tokai Reprocessing Plant and the environment

Nakano, Masanao

Hoken Butsuri (Internet), 56(1), p.17 - 25, 2021/03

The Tokai Reprocessing Plant is the first reprocessing plant in Japan which started hot test in 1977, and had reprocessed 1140 tons of spent nuclear fuel by May 2007. The gaseous and liquid radioactive wastes has been discharged to the environment. Since iodine-129 ($$^{129}$$I) is one of the most important nuclides for environmental impact assessment. Therefore, $$^{129}$$I in the exhaust and effluent has been controlled, and a precise analysis method of $$^{129}$$I in the environmental samples was developed, and the concentration of 129I in the environment was investigated. This report presents an overview of these activities. Not limited to $$^{129}$$I on reprocessing facilities, it is essential for nuclear operators to reduce the amount released to the environment in the spirit of ALARA, and to continuously develop the further upgrading environmental monitoring methods and evaluation methods in order to foster a sense of safety and security among residents living in the vicinity of the facilities.

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.

Journal Articles

Vertical distributions of Iodine-129 and iodide in the Chukchi Sea and Bering Sea

Miwa, Kazuji; Obata, Hajime*; Suzuki, Takashi

Journal of Nuclear Science and Technology, 57(5), p.537 - 545, 2020/05

 Times Cited Count:1 Percentile:24.18(Nuclear Science & Technology)

This study investigated the vertical distribution of Iodine-129 ($$^{129}$$I) which is mainly produced by European nuclear reprocessing plants in the Chukchi Sea and Bering Sea. $$^{129}$$I was found to be distributed almost uniformly in fallout level, and an increasing in $$^{129}$$I concentration levels caused by high $$^{129}$$I water inflow from the Atlantic Ocean was not observed. Additionally, we revealed the vertical distribution of iodide, one chemical form of iodine, from the Bering Shelf area to the Chukchi Sea for the first time. The increasing tendency of iodide near sea bottom was observed.

Journal Articles

Improvement in flow-sheet of extraction chromatography for trivalent minor actinides recovery

Watanabe, So; Senzaki, Tatsuya; Shibata, Atsuhiro; Nomura, Kazunori; Takeuchi, Masayuki; Nakatani, Kiyoharu*; Matsuura, Haruaki*; Horiuchi, Yusuke*; Arai, Tsuyoshi*

Journal of Radioanalytical and Nuclear Chemistry, 322(3), p.1273 - 1277, 2019/12

 Times Cited Count:0 Percentile:0.01(Chemistry, Analytical)

JAEA Reports

SCHERN: Analysis program for chemical behavior of nitrogen oxide in accident of evaporation to dryness by boiling of reprocessed high level liquid waste in Fuel Reprocessing Facilities

Hiyama, Mina*; Tamaki, Hitoshi; Yoshida, Kazuo

JAEA-Data/Code 2019-006, 17 Pages, 2019/07

JAEA-Data-Code-2019-006.pdf:1.84MB

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 (NOx) 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 strongly to the transport behavior of Ru at the anticipated atmosphere condition in cells and/or compartments of the facility building. Chemical reactions of NOx with water and nitric acid are also recognized as the complex phenomena to undergo simultaneously in the vapor and liquid phases. An analysis program has been developed to simulate chemical reaction coupled with the thermo-hydraulic condition in the flow paths in the facility building.

Journal Articles

Treatment technology of highly radioactive solid waste generated by experimental tests and sample analysis in reprocessing facilities

Goto, Yuichi; Inada, Satoshi; Kuno, Takehiko; Mori, Eito*

Nihon Hozen Gakkai Dai-16-Kai Gakujutsu Koenkai Yoshishu, p.221 - 224, 2019/07

Test equipment, containers, and analytical wastes, generated by experiments using spent fuel pieces in hot cell of Operation Testing Laboratory and by analysis of highly active liquid wastes in hot analytical cell line of Tokai Reprocessing Plant, are treated as highly radioactive solid wastes. These wastes are stored in specific shielded containers called waste cask and then transport to the storage facility. The treatment of these highly radioactive solid wastes have been carried out for 40 years with upgrading waste taking out system and transportation device. As a results, automation of several procedures have been achieved utilizing conventional equipment, and work efficiency and safety have been improved.

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.

Journal Articles

Introduction and implementation of physical protection measures including trustworthiness program at Tokai Reprocessing Facilities

Nakamura, Hironobu; Kimura, Takashi; Yamazaki, Katsuyuki; Kitao, Takahiko; Tasaki, Takashi; Iida, Toru

Proceedings of International Conference on Physical Protection of Nuclear Material and Nuclear Facilities (Internet), 9 Pages, 2018/09

After the accident of Fukushima Daiichi Nuclear Power Station, to develop effective security measures based on the lesson learned from such crisis and to meet the IAEA Nuclear Security Recommendations (INFCIRC/225/Rev.5), NRA in Japan made a partial amendment of the regulations concerning the reprocessing activity in 2012. The Tokai reprocessing facility implemented all of those security measures by the end of March 2014. Those new measures help us to keep high degree of security level and contributed to our planned operations to reduce the potential risk of the plant. On the other hand, the trustworthiness program was newly introduced in 2016, based on the trustworthiness policy determined by NRA. The implementing entity of the program is JAEA for the Tokai Reprocessing Facility and is required for both the persons afford unescorted access to Category I and II, CAS/SAS, and the persons afford access to the sensitive information. Those who are involved this program will be judged before engaging the work whether they might act as insider to cause or assist radiological sabotage or unauthorized removal of nuclear material, or leak sensitive information. The program is expected as a measure against insider at reprocessing facilities, and is expected to be enforced around the autumn of 2017. As well as the establishment of security measures, the promoting nuclear security culture for all employees was a big challenge. The Tokai reprocessing facility have introduced several security culture activities, such as case study education of security events done by a small group and putting up the security culture poster and so on. This paper presents introduction and implementation with effectiveness of security measures in the Tokai reprocessing facilities and the future security measures applied to the reprocessing facilities are discussed.

Journal Articles

Demonstration of $$gamma$$-ray pipe-monitoring capabilities for real-time process monitoring safeguards applications in reprocessing facilities

Rodriguez, D.; Tanigawa, Masafumi; Nishimura, Kazuaki; Mukai, Yasunobu; Nakamura, Hironobu; Kurita, Tsutomu; Takamine, Jun; Suzuki, Satoshi*; Sekine, Megumi; Rossi, F.; et al.

Journal of Nuclear Science and Technology, 55(7), p.792 - 804, 2018/07

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

Nuclear material in reprocessing facilities is safeguarded by random sample verification with additional continuous monitoring applied to solution masses and volume in important tanks to maintain continuity-of-knowledge of process operation. Measuring the unique $$gamma$$ rays of each solution as the material flows through pipes connecting all tanks and process apparatuses could potentially improve process monitoring by verifying the compositions in real time. We tested this $$gamma$$ ray pipe-monitoring method using plutonium-nitrate solution transferred between tanks at the PCDF-TRP. The $$gamma$$ rays were measured using a lanthanum-bromide detector with a list-mode data acquisition system to obtain both time and energy of $$gamma$$-ray. The analysis and results of this measurement demonstrate an ability to determine isotopic composition, process timing, flow rate, and volume of solution flowing through pipes, introducing a viable capability for process monitoring safeguards verification.

JAEA Reports

Development of correlation of gaseous ruthenium transfer rate to condensed water in accident of evaporation to dryness by boiling of reprocessed high level liquid waste in Fuel Reprocessing Facilities

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

JAEA-Research 2017-015, 18 Pages, 2018/01

JAEA-Research-2017-015.pdf:3.08MB

An accident of evaporation to dryness by boiling of high level liquid waste is postulated as one of the severe accidents at a fuel reprocessing facility. It was observed at the experiments that a large amount of ruthenium (Ru) is volatilized and transfer to the vapor phase in the tank. The nitric acid and water mixed vapor released from the tank is condensed. Volatilized Ru is expected to transfer into the condensed water at the compartments in the building. Quantitative estimation of the amount of Ru transferred condensed water is key issues to evaluate the reduction the amount of Ru through leak path in the facility building. This report presents that a correlation has been developed for Ru transfer rate to condensed water with vapor condensing rate based on the experimental results and additional thermal-hydraulic simulation of the experiments. Applicability of the correlation has been also demonstrated with the accident simulation of typical facilities in full-scale.

Journal Articles

Effect of chloride ion on corrosion behavior of SUS316L-grade stainless steel in nitric acid solutions containing seawater components under $$gamma$$-ray irradiation

Sano, Yuichi; Ambai, Hiromu; Takeuchi, Masayuki; Iijima, Shizuka; Uchida, Naoki

Journal of Nuclear Materials, 493, p.200 - 206, 2017/09

 Times Cited Count:5 Percentile:59.32(Materials Science, Multidisciplinary)

Concerning the Fukushima Daiichi Nuclear Power Plant accident, we investigated the effect of chloride ion on the corrosion behavior of SUS316L stainless steel, which is a typical material for the equipment used in reprocessing, in HNO$$_{3}$$ solution containing seawater components, including under the $$gamma$$-ray irradiation condition. Electrochemical and immersion tests were carried out using a mixture of HNO$$_{3}$$ and artificial seawater (ASW). In the HNO$$_{3}$$ solution containing high amounts of ASW, the cathodic current densities increased and uniform corrosion progressed. This might be caused by strong oxidants, such as Cl$$_{2}$$ and NOCl, generated in the reaction between HNO$$_{3}$$ and Cl$$^{-}$$ ions. The corrosion rate decreased with the immersion time at low concentrations of HNO$$_{3}$$, while it increased at high concentrations. Under the $$gamma$$-ray irradiation condition, the corrosion rate decreased due to the suppression of the cathodic reactions by the reaction between the above oxidants and HNO$$_{2}$$ generated by radiolysis.

Journal Articles

HEPA filter clogging and volatile material release under solvent fire accident in fuel reprocessing facility

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

Proceedings of 25th International Conference on Nuclear Engineering (ICONE-25) (CD-ROM), 7 Pages, 2017/07

After the Fukushima-Daiichi accident, countermeasures against the severe accident are newly required as regulatory items for nuclear facilities. Organic solvent fire in cell was defined as one of the accidents in the fuel reprocessing plant. When the solvent burns, aerosols including soot are released. The substances clog HEPA filters in the ventilation system and their breakthrough may happen because of differential pressure rising. Moreover, the fire can also release volatile radioactive gaseous species, which can pass through HEPA filters. These phenomena are important for evaluation of confinement capability of the facility and public exposure. We have investigated, in relating to the clogging behavior, release behavior of aerosols as well as of volatile materials from burnt solvent. In the presentation, we will report experimental data and evaluation results obtained from recent research.

Journal Articles

Hydrogen absorption behavior on zirconium under $$gamma$$-radiolysis of nitric acid solution

Ishijima, Yasuhiro; Ueno, Fumiyoshi; Abe, Hitoshi

Nihon Genshiryoku Gakkai Wabun Rombunshi, 16(2), p.100 - 106, 2017/05

Zirconium (Zr) has been used as a structural material at the spent nuclear fuel reprocessing plant in Japan because of its excellent corrosion resistance against nitric acid solution. And the radiolytic hydrogen is known to be generated in the spent nuclear fuel solution. Zr is known to be highly susceptible to hydrogen embrittlement. Therefore, evaluating the radiolytic hydrogen absorption behavior of Zr in nitric acid solution (HNO$$_{3}$$) is essential. In this study, immersion tests were conducted on Zr in nitric acid solutions under $$gamma$$-ray irradiation to evaluate its radiolytic hydrogen absorption behavior. Results showed that hydrogen concentration on Zr increased both in 1-3 mol/L HNO$$_{3}$$ and pure water at 5 and 7 kGy/h after immersion. The amount of hydrogen absorption on Zr under $$gamma$$-ray irradiation had a direct correlation with the radiolytic hydrogen generation value in HNO$$_{3}$$. The results of glow discharge optical emission spectrometry, thermal desorption spectroscopy, and X-ray diffraction result shows that the absorbed radiolytic hydrogen generated a hydride on the surface of Zr.

Journal Articles

Development of metal corrosion testing method simulating equipment of reprocessing of spent nuclear fuels

Matsueda, Makoto; Irisawa, Eriko; Kato, Chiaki; Matsui, Hiroki

Proceedings of 54th Annual Meeting of Hot Laboratories and Remote Handling (HOTLAB 2017) (Internet), 4 Pages, 2017/00

In the PUREX method, spent fuels are dissolved with nitric acid media. The reprocessing solution containing Fission Products derived from spent fuels is very corrosive to metal materials, the corrosion problem often appears on the surface stainless steel devices. The oxidizing metal ions such as Ruthenium (Ru) and Neptunium (Np) in the process solution is the key reason for severe corrosion of stainless steel. In order to obtain the corrosion rate of stainless steel, we installed the corrosion test apparatus inside an airtight concrete cell in a hot laboratory (the WAste Safety TEsting Facility (WASTEF) of the Japan Atomic Energy Agency), and performed the corrosion tests of stainless steel in the heated nitric acid solution containing Np. The corrosion tests were performed in the temperature range from room temperature to boiling point for 500 hours per batch. The results show that the presence of Np accelerate the stainless steel corrosion in the nitric acid solution.

Journal Articles

Characterization of the insoluble sludge from the dissolution of irradiated fast breeder reactor fuel

Aihara, Haruka; Arai, Yoichi; Shibata, Atsuhiro; Nomura, Kazunori; Takeuchi, Masayuki

Procedia Chemistry, 21, p.279 - 284, 2016/12

BB2015-3214.pdf:0.31MB

 Times Cited Count:3 Percentile:92.31

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

Accident analysis of evaporation to dryness by boiling of reprocessed high level liquid waste at fuel reprocessing facilities with considering severe accident measures

Yoshida, Kazuo

JAEA-Research 2016-004, 15 Pages, 2016/06

JAEA-Research-2016-004.pdf:2.22MB

An accident of evaporation to dryness by boiling of high level liquid waste is postulated as one of the severe accidents caused by the loss of cooling function at a fuel reprocessing plant. In this case, some amount of fission products (FPs) will be transferred to the vapor phase in the tank, and could be released to the environment. Two mitigative accident measures have been proposed by the licensee. One of them is injecting cold water to waste tanks to prevent dryness and another is leading generated vapor through temporary duct to huge spaces in the facility to condense to liquid. Thermal-hydraulics and aerosol transport behaviors in compartments of a typical facility building have been analyzed based on the scenario with these accident measures. The effects of measures are discussed form a view point of the reduction of radioactive material release to environment.

157 (Records 1-20 displayed on this page)