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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:0

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.

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:0 Percentile:100(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

Experimental evaluation of release and transport behavior of gaseous ruthenium under boiling accident in reprocessing plant

Yoshida, Naoki; Tashiro, Shinsuke; Amano, Yuki; Yoshida, Kazuo; Yamane, Yuichi; Abe, Hitoshi

NEA/CSNI/R(2017)12/ADD1 (Internet), p.293 - 305, 2018/01

The "Evaporation to Dryness due to the Loss of Cooling Functions" (EDLCF) of highly-active liquid waste (HALW) was newly defined as one of the severe accidents in Japan's nuclear safety standard for the reprocessing plant. Studies on accident scenarios and their source terms have led to an increased need for the development of accident management measures and the assessment of their effectiveness. Previous studies have shown that ruthenium was released at a greater rate than other elements because it formed volatile species such as ruthenium tetroxide (RuO4). In addition, ruthenium isotopes, 106Ru and 103Ru, have radiotoxicity. Accordingly, the accident management measures require the experimental information on the release and transport behavior of the gaseous ruthenium (Ru(g)). This paper summarizes our experimental results on the characteristics of Ru(g) in the EDLCF. This work includes the results of the experiments carried out under the agreement among JAEA, Japan Nuclear Fuel Ltd. and Japan Nuclear Energy Safety Organization.

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.

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:60.48(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

Study on release behavior of radioiodine from fuel solution under criticality accident condition

Tashiro, Shinsuke; Abe, Hitoshi

JAEA-Technology 2015-044, 20 Pages, 2016/03

JAEA-Technology-2015-044.pdf:1.26MB

In order to estimate public dose under a criticality accident in fuel solution of a fuel reprocessing plant, release behavior of radioiodine from the fuel solution to atmosphere is very important. In this report, time evolution of $$^{133}$$I concentration in gas phase of TRACY core tank was measured until the concentration in the solution decreased. Furthermore, cumulative release ratio (CRR) and release rate (RR) from the solution to the atmosphere of radioiodine were evaluated by applying previously-reported evaluation model. As a result, for the case of short transient criticality, RR of $$^{133}$$I became maximum at 1 hour later from the ending and almost constant after 8 hour later. Furthermore, relationship of each elapsed time between total fission number and release rate of $$^{133}$$I could be derived. On the other hand, for the case of long criticality excursion, such as JCO criticality accident, the CRR and RR of radioiodine increased monotonously with time.

Journal Articles

Release Characteristics of Ruthenium from Highly Active Liquid Waste in Drying Step

Tashiro, Shinsuke; Amano, Yuki; Yoshida, Kazuo; Yamane, Yuichi; Uchiyama, Gunzo; Abe, Hitoshi

Nippon Genshiryoku Gakkai Wabun Rombunshi, 14(4), p.227 - 234, 2015/12

The release characteristics of Ru from highly active liquid waste (HALW) have been investigated under the condition of accidental evaporation to dryness by boiling of HALW. Using a laboratory-scale apparatus, non-radioactive simulated HALW (s-HALW) was heated with an external heater to dryness to observe the release characteristics of Ru and gaseous nitrogen oxides. As a result, Ru was significantly released between 120 and 300 $$^{circ}$$C of the s-HALW. The cumulative release ratio of Ru was 0.088. It was also found that the partially released amount of Ru against the temperature of the s-HALW had two peaks with one maximal at about 140 $$^{circ}$$C and maximum at about 240 $$^{circ}$$C. Referring to the results of the release rate of gaseous nitrogen oxides and the volume of condensate, which was a collection of the mixed vapors of steam and nitric acid released from the s-HALW, we discussed the causes of Ru release around these peaks.

Journal Articles

Experimental study on boiling accident of high active liquid waste in reprocessing

Uchiyama, Gunzo; Tashiro, Shinsuke; Amano, Yuki; Abe, Hitoshi; Yamane, Yuichi; Yoshida, Kazuo; Ishikawa, Jun

Proceedings of 21st International Conference & Exhibition; Nuclear Fuel Cycle for a Low-Carbon Future (GLOBAL 2015) (USB Flash Drive), p.1056 - 1063, 2015/09

The experimental study for source term data of radioactive materials has been conducted at a boiling accident of high active liquid waste (HALW) in reprocessing plants. In the study, three kinds of tests have been conducted including a cold small scale test, a cold engineering scale test and a hot small scale test. The following results were obtained: Ruthenium and Technetium were released into the gas phase in the form of both mist and gas under the boiling accident conditions of a simulated HALW. Non-volatile fission products (FPs) such as Nd and Cs were released into the gas phase in the form of mist. The release ratios of non-volatile FPs from a vessel of the simulated HALW were about 10$$^{-4}$$. The release ratios of actinide nuclides such as Am were almost the same as those of non-volatile FPs.

Journal Articles

Trends of nitrogen oxide release during thermal decomposition of nitrates in highly active liquid waste

Amano, Yuki; Watanabe, Koji; Tashiro, Shinsuke; Yamane, Yuichi; Ishikawa, Jun; Yoshida, Kazuo; Uchiyama, Gunzo; Abe, Hitoshi

Nippon Genshiryoku Gakkai Wabun Rombunshi, 14(2), p.86 - 94, 2015/06

Radioactive materials could be released into air due to the accidental boiling of high active liquid waste (HALW) in reprocessing plants. Volatile radioactive nuclides, such as ruthenium, are released from the tanks into the atmosphere. Nitrogen oxides (NOx) are also released due to the thermal decomposition of metal nitrates in HALW. The released NOx transport volatile ruthenium and cause redox reactions associated with the composition or decomposition of volatile ruthenium. In this study, NOx release data were obtained by heating simulated HALW up to 600$$^{circ}$$C. As a result, the release of NOx from the simulated HALW was observed from 200$$^{circ}$$C to 600$$^{circ}$$C, and the main release of NOx was observed at about 340$$^{circ}$$C. All the lanthanide nitrates were found to decompose in the simulated HALW, and the thermal decomposition temperature of the lanthanide nitrates decreased after the addition of ruthenium dioxide to the mixed lanthanide nitrates solution.

Journal Articles

Release of radioactive materials from simulated high level liquid waste at boiling accident in reprocessing plant

Tashiro, Shinsuke; Uchiyama, Gunzo; Amano, Yuki; Abe, Hitoshi; Yamane, Yuichi; Yoshida, Kazuo

Nuclear Technology, 190(2), p.207 - 213, 2015/05

 Times Cited Count:4 Percentile:56.57(Nuclear Science & Technology)

The release behavior of radioactive materials from high active liquid waste (HALW) has been investigated under boiling accident conditions. Results of the experiment using a nonradioactive simulated HALW found Ru to be a volatile element under the accident conditions and to be released into the gas phase in the form of both mist and gas. The Ru release rate and the apparent Ru volatilization rate constant were obtained under the boiling conditions of simulated HALW. The other fission product elements such as Cs were found to be nonvolatile and to be released into the gasphase in the form of mist. The mist size distribution near the surface of the simulated HALW in the reactor vessel was found to range from 0.05 to 20 $$mu$$m with a peak diameter of $$sim$$ 2 $$mu$$m.

Journal Articles

Development of Ru transfer rate correlation to vapor phase in accident of evaporation to dryness by boiling of reprocessed high-level liquid waste

Yoshida, Kazuo; Tashiro, Shinsuke; Amano, Yuki; Yamane, Yuichi; Uchiyama, Gunzo; Abe, Hitoshi

Nippon Genshiryoku Gakkai Wabun Rombunshi, 13(4), p.155 - 166, 2014/12

An accident of evaporation to dryness by boiling of high level liquid waste (HLLW) is postulated as one of the severe accidents to occur caused by the loss of cooling function at a fuel reprocessing plant. In this case, a large amount of ruthenium (Ru) will be volatilized and transfer to the vapor phase in the tank, and could be released to the environment. Therefore, the quantitative estimation of released Ru is one of the key issues in the assessment of the accident consequence. To resolve this issue, an empirical correlation for Ru transfer rate to vapor phase with the temperature, nitric acid mol fraction and activity of HLLW has been developed based on the data obtained from the accelerated experiments using simulated HLLW. A simulation study with the developed correlation demonstrated that amount of Ru transfer to vapor phase was in a good agreement with the long term experiment using actual HLLW.

Journal Articles

Characterization and storage of radioactive zeolite waste

Yamagishi, Isao; Nagaishi, Ryuji; Kato, Chiaki; Morita, Keisuke; Terada, Atsuhiko; Kamiji, Yu; Hino, Ryutaro; Sato, Hiroyuki; Nishihara, Kenji; Tsubata, Yasuhiro; et al.

Journal of Nuclear Science and Technology, 51(7-8), p.1044 - 1053, 2014/07

 Times Cited Count:8 Percentile:36.57(Nuclear Science & Technology)

For safe storage of zeolite wastes generated by treatment of radioactive saline water at the Fukushima Daiichi Nuclear Power Station, properties of the Herschelite adsorbent were studied and its adsorption vessel was evaluated for hydrogen production and corrosion. Hydrogen production depends on its water level and dissolved species because hydrogen is oxidized by radicals in water. It is possible to evaluate hydrogen production rate in Herschelite submerged in seawater or pure water by taking into account of the depth effect of the water. The reference vessel of decay heat 504 W with or without residual pure water was evaluated for the hydrogen concentration by thermal hydraulic analysis using obtained fundamental properties. Maximum hydrogen concentration was below the lower explosive limit (4 %). The steady-state corrosion potential of a stainless steel 316L increased with absorbed dose rate but its increase was repressed by the presence of Herschelite. At 750 Gy/h and $$<$$60$$^{circ}$$C which were values evaluated at the bottom of the vessel of 504 W, the localized corrosion of SUS316L contacted with Herschelite would not immediately occur under 20,000 ppm of Cl$$^{-}$$ concentration.

Journal Articles

Release behavior of radioactive materials at a boiling accident of high active liquid waste in reprocessing plants

Uchiyama, Gunzo; Tashiro, Shinsuke; Amano, Yuki; Abe, Hitoshi; Yamane, Yuichi; Yoshida, Kazuo; Ishikawa, Jun

Proceedings of International Waste Management Symposia 2014 (WM 2014) (Internet), 9 Pages, 2014/05

The experimental study for source term data of radioactive materials has been conducted at a boiling accident of high active liquid waste (HALW) in a reprocessing plant. In the small scale cold test using a non-radioactive simulated HALW, the release behavior of FP elements from the simulated HALW were investigated under various boiling accident conditions. In the engineering scale cold test, the release behavior of FP elements at boiling accident conditions was investigated mainly as a spatial function. In the small scale hot test using a radioactive simulated HALW, the release behavior of radioactive materials (FP, alpha nuclides) were obtained under typical boiling accident conditions. In the small scale hot test, the release fractions of Ru and non-volatile FPs obtained were almost the same as those of the small scale cold test.

Journal Articles

Study on release and transport of aerial radioactive materials in reprocessing plant

Amano, Yuki; Tashiro, Shinsuke; Uchiyama, Gunzo; Abe, Hitoshi; Yamane, Yuichi; Yoshida, Kazuo

Proceedings of International Nuclear Fuel Cycle Conference; Nuclear Energy at a Crossroads (GLOBAL 2013) (CD-ROM), p.1411 - 1417, 2013/09

JAEA Reports

Experiment on evaluation of confinement capability of fuel cycle facility under combustion of combustible materials (Contract research)

Abe, Hitoshi; Tashiro, Shinsuke; Watanabe, Koji; Uchiyama, Gunzo

JAEA-Research 2012-035, 26 Pages, 2013/01

JAEA-Research-2012-035.pdf:1.94MB

To contribute on confirmation of safety of fuel cycle facilities, an evaluation method for soundness of confinement capability of the facilities under fire accident has been investigated. Organic extraction solvents, zinc stearate, which is added into MOX powder in MOX fuel preparation process, and typical lubricating oil were considered to be examination objects as the representative combustible materials in the facilities. Combustion property data, such as mass loss rate and soot release fraction, of them and clogging property data of HEPA filter with combustion of the organic extraction solvents were measured. As the results, it was found that soot release fraction from burning 30%TBP/70%dodecane was larger than that of the other materials including dodecane and very rapid rise of differential pressure of HEPA filter, which has not been reported, would be induced in the last stage of combustion of 30%TBP/70%dodecane. Furthermore, it was confirmed that zinc stearate, of which combustibility has not been considered, burned continuously in the condition which was heated from outside.

JAEA Reports

Experiment on the gaseous iodine release from irradiated cesium iodide solutions (Contract research)

Moriyama, Kiyofumi; Tashiro, Shinsuke; Chiba, Noriaki; Maruyama, Yu; Nakamura, Hideo; Watanabe, Atsushi*

JAEA-Research 2011-016, 125 Pages, 2011/06

JAEA-Research-2011-016.pdf:2.71MB

The volatile iodine production due to radiation chemical effects in the containment vessel of light water reactors (LWRs) during severe accidents was investigated by experiments in small scale and with well controlled conditions. Cesium iodide solutions, 10$$^{-4}$$M, labeled with $$^{131}$$I, at controlled pH by boric acid-sodium hydroxide buffer, were $$gamma$$-irradiated and swept with a constant gas flow rate. The gaseous iodine released from the solution was collected by species selective filters and quantified separately for I$$_2$$ and organic iodines. The influences of pH, temperature, inorganic and organic impurities, oxygen and hydrogen concentrations in the cover gas on the iodine release behavior were examined. Data including time dependent gaseous iodine release fractions, comparison of the final iodine release fractions in terms of the parameter effects, as well as the initial, boundary and interface conditions necessary for simulating the experiments by computer codes are provided.

Journal Articles

Experiment and modeling for solvent leaching from paint matrix considering equilibrium

Moriyama, Kiyofumi; Chiba, Noriaki; Tashiro, Shinsuke; Maruyama, Yu; Nakamura, Hideo; Watanabe, Atsushi*

Journal of Nuclear Science and Technology, 48(6), p.885 - 891, 2011/06

 Times Cited Count:0 Percentile:100(Nuclear Science & Technology)

The leach of remaining solvent in an epoxy paint coating when it is submerged in water was experimentally studied. A leach kinetics model considering the equilibrium of the solvent concentration in the paint matrix and in water was developed. Three model parameters, equilibrium constant $$K$$, leaching rate $$k_d$$, and initial concentration of the solvent in the paint $$C_p^0$$ were evaluated based on the experimental results, and empirical correlation equations for them were obtained. The model showed good qualitative and quantitative agreement with the observed evolution of the leached solvent mass in the present experiment. Also the model showed consistency with experimental data by Ball et al. (2003).

Journal Articles

Experiments on the release of gaseous iodine from $$gamma$$-irradiated aqueous CsI solution and influence of oxygen and Methyl Isobutyl Ketone (MIBK)

Moriyama, Kiyofumi; Tashiro, Shinsuke; Chiba, Noriaki; Hirayama, Fumio*; Maruyama, Yu; Nakamura, Hideo; Watanabe, Atsushi*

Journal of Nuclear Science and Technology, 47(3), p.229 - 237, 2010/03

 Times Cited Count:12 Percentile:31.74(Nuclear Science & Technology)

The volatile iodine production due to radiation chemistry is an important uncertainty source in the source term evaluation for LWRs. The gaseous release of molecular iodine and organic iodine from $$gamma$$-irradiated ($$sim 7$$kGy/h, 2h) cesium iodide aqueous solution (1E-4M) containing methyl-isobuthyl-ketone (MIBK) was measured. The solution was buffered at pH$$sim$$7. The concentration of MIBK (up to 1E-3M) and oxygen were changed as parameters. The total iodine release fraction and the fraction released as organic iodine were 2-47% and 0.02-1.5%, respectively, at the end of the irradiation. With the same cover gas condition, the total iodine release decreased and the organic iodine release increased when the MIBK concentration increased. This behavior can be explained by branching of the reaction path of organic degradation depending on availability of dissolved oxygen and competition between iodine and organic compounds on the consumption of radicals.

Journal Articles

Research on consequence analysis method for probabilistic safety assessment of nuclear fuel facilities, 4; Investigation of safety evaluation method for fire and explosion incidents

Abe, Hitoshi; Tashiro, Shinsuke; Ueda, Yoshinori*

Nippon Genshiryoku Gakkai Wabun Rombunshi, 9(1), p.82 - 95, 2010/03

A special committee of "Research on the analysis methods for accident consequence of nuclear fuel facilities (NFF)" was organized by the Atomic Energy Society of Japan under the entrustment of JAEA. The committee aims to research on the state-of-the-art of consequence analysis method for Probabilistic Safety Assessment (PSA) of NFF such as fuel reprocessing and fuel fabrication facilities. The objective is to obtain the useful information related to establishing quantitative performance objectives and to risk-informed regulation through qualifying issues needed to be resolved for applying PSA to NFF. The research activities of the committee were mainly focused on the analysis method of consequences for postulated accidents with potentially large consequence in NFF resulting in release of radio active material to the environment. In this technical report, the research results about basic experimental data and method for safety evaluation for fire and explosion incidents were summarized.

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