Rizaal, M.; Miwa, Shuhei; Suzuki, Eriko; Imoto, Jumpei; Osaka, Masahiko; Goullo, M.*
ACS Omega (Internet), 6(48), p.32695 - 32708, 2021/12
Imoto, Jumpei; Nakajima, Kunihisa; Osaka, Masahiko
Nihon Genshiryoku Gakkai Wabun Rombunshi, 20(4), p.179 - 187, 2021/12
Some of the Cs inside the Fukushima Daiichi Nuclear Power Station would be deposited in chemical forms such as CsI and CsMoO. Since Cs compounds are generally water-soluble, it is predicted that the migration of Cs through the aqueous phase occurs in the long term. Knowledge of the solubility in water is required as basic data for such migration behavior evaluation. Therefore, this study was conducted to investigate the dissolution properties of CsI and CsMoO in water at 20C and 25C. The solubilities of CsI at 25C calculated using thermodynamic data and the Pitzer ion interaction model were in good agreement with the literature value. It was found that the literature value of CsI at around room temperature is highly reliable. The experimental value of CsI at 20C obtained by the OECD test guideline 105 flask method (test guideline) was also in good agreement with the literature value. The measured solubility of CsMoO was 256.8 6.2 (g/100 g HO) at 20C using the test guideline. This measured solubility of CsMoO was found to be comparable to those of other alkaline molybdates and considered to be more reliable than the literature value.
Koyama, Shinichi; Nakagiri, Toshio; Osaka, Masahiko; Yoshida, Hiroyuki; Kurata, Masaki; Ikeuchi, Hirotomo; Maeda, Koji; Sasaki, Shinji; Onishi, Takashi; Takano, Masahide; et al.
Hairo, Osensui Taisaku jigyo jimukyoku Homu Peji (Internet), 144 Pages, 2021/08
JAEA performed the subsidy program for the "Project of Decommissioning and Contaminated Water Management (Development of Analysis and Estimation Technology for Characterization of Fuel Debris (Development of Technologies for Enhanced Analysis Accuracy and Thermal Behavior Estimation of Fuel Debris))" in 2020JFY. This presentation summarized briefly the results of the project, which will be available shortly on the website of Management Office for the Project of Decommissioning and Contaminated Water Management.
Uchida, Shunsuke; Karasawa, Hidetoshi; Kino, Chiaki*; Pellegrini, M.*; Naito, Masanori*; Osaka, Masahiko
Nuclear Engineering and Design, 380, p.111256_1 - 111256_19, 2021/08
It is essential to grasp the long-term distributions of FP as well as fuel debris all over the Fukushima Daiichi Nuclear Power Plant (1F) for safe completion of its decommissioning projects. The fuel debris is going to be removed from the plant under the severe conditions of FP being scattered during major decommissioning work, and then, the decommissioning projects are going to be terminated by storing safely the removed debris as recovered fertile materials or as materials for final radioactive disposal. In order to determine the FP distribution in the plant for the long period from the accident occurrence to the termination of the plant decommissioning, procedures for analyzing multi-term FP behaviors were proposed. The proposed procedures should be improved by applying the FP data measured in the plant and validated based on the feedback data. Then, the accuracy-improved procedures should be applied to estimate FP distribution during each period of the decommissioning projects.
Liu, J.; Miwa, Shuhei; Nakajima, Kunihisa; Osaka, Masahiko
Nuclear Materials and Energy (Internet), 26, p.100916_1 - 100916_6, 2021/03
Miyahara, Naoya; Miwa, Shuhei; Goullo, M.*; Imoto, Jumpei; Horiguchi, Naoki; Sato, Isamu*; Osaka, Masahiko
Journal of Nuclear Science and Technology, 57(12), p.1287 - 1296, 2020/12
In order to clarify the cesium iodide (CsI) transport behavior with a focus on the mechanisms of gaseous iodine formation in the reactor coolant system of LWR under a severe accident condition, a reproductive experiment of CsI transport behavior was conducted using a facility equipped with a thermal gradient tube. Various analyses on deposits and airborne materials during transportation could elucidate two mechanisms for the gaseous iodine formation. One was the gaseous phase chemical reaction in Cs-I-O-H system at relatively high-temperature region, which led to gaseous iodine transport to the lower temperature region without any further changes in gas species due to the kinetics limitation effects. The other one was the chemical reactions related to condensed phase of CsI, namely those of CsI deposits on walls with surface of stainless steel to form CsCrO compound and CsI aerosol particles with steam, which were newly found in this study.
Rizaal, M.; Nakajima, Kunihisa; Saito, Takumi*; Osaka, Masahiko; Okamoto, Koji*
Journal of Nuclear Science and Technology, 57(9), p.1062 - 1073, 2020/09
The interaction of cesium hydroxide and a calcium silicate insulation material was experimentally investigated at high temperature conditions. A thermogravimetry equipped with differential thermal analysis was used to analyze thermal events in the samples of mixed calcium silicate and cesium hydroxide under Ar-5%H and Ar-4%H-20%H0 with maximum temperature of 1100C. Prior being mixed with cesium hydroxide, a part of calcium silicate was pretreated at high temperature to evaluate the effect of possible structural changes of this material due to a preceding thermal history and also the sake of thermodynamic evaluation to those available ones. Based upon the initial condition (preliminary heat treatment) of calcium silicate, it was found that if the original material consisted of xonotlite (CaSi0(0H)), the endothermic reaction with cesium hydroxide occurred over the temperature range 575-730C meanwhile if the crystal phase of original material was changed to wollastonite (CaSi0), the interaction occurred over temperature range 700-1100C. Furthermore, the X-ray diffraction analyses have indicated on both type of pretreated calsils that regardless of Ar-5%H and Ar-4%H-20%H0 atmosphere, cesium aluminum silicate, CsAlSi0 was formed with aluminum in the samples as an impurity or adduct.
Machida, Masahiko; Yamada, Susumu; Iwata, Ayako; Otosaka, Shigeyoshi; Kobayashi, Takuya; Watanabe, Masahisa; Funasaka, Hideyuki; Morita, Takami*
Journal of Nuclear Science and Technology, 57(8), p.939 - 950, 2020/08
After direct discharges of highly contaminated water of the Fukushima Daiichi Nuclear Power Plant (1F) from April to May 2011, Kanda suggested that relatively small amounts of run-off of radionuclides from the 1F port into the Fukushima coastal region subsequently continued by his estimation method. However, the estimation period was limited to up to September 2012. Therefore, this paper estimates the discharge inventory up to June 2018. In the missing period, the Japanese government and Tokyo Electric Power Company Holdings have continued efforts to stop the discharge, and consequently, the radionuclide concentration in seawater inside the 1F port has gradually diminished. We show the monthly discharge inventory of Cs up to June 2018 by two methods, i.e., Kanda method partially improved by the authors and a more sophisticated method using Voronoi tessellation reflecting the increase in the number of monitoring points inside the 1 F port. The results show that the former always yields overestimated results compared with the latter, but the ratio of the former to the latter is less than one order of magnitude. Using these results, we evaluate the impact of the discharge inventory from the 1F port into the coastal area and radiation dose upon fish ingestion.
Suzuki, Eriko; Nakajima, Kunihisa; Osaka, Masahiko; Oishi, Yuji*; Muta, Hiroaki*; Kurosaki, Ken*
Journal of Nuclear Science and Technology, 57(7), p.852 - 857, 2020/07
The low temperature heat capacity of CsSiO, which is one of the cesium chemisorbed compounds onto stainless steel during severe accident of the light water nuclear reactor, was experimentally determined for the first time in the temperature range of 1.9 - 302 K. The experimentally determined heat capacity, (298.15K), and the standard entropy, (298.15K), were 249.4 1.1 J K mol and 322.1 1.3 J K mol, respectively. The standard Gibbs energy of formation of CsSiO at high temperatures, (), were reevaluated by using the presently obtained (298.15K) and the previously reported experimental results of the standard enthalpy of formation, (298.15K), and the standard enthalpy increments at high temperatures, ()- (298.15K).
Rizaal, M.; Saito, Takumi*; Okamoto, Koji*; Erkan, N.*; Nakajima, Kunihisa; Osaka, Masahiko
Mechanical Engineering Journal (Internet), 7(3), p.19-00563_1 - 19-00563_10, 2020/06
The adsorption of cesium (Cs) on calcium silicate insulation of primary piping system is postulated to contribute in high dose rate of surrounding pedestal area in Fukushima Daiichi NPP unit 2. In this study, room-temperature experiment of Cs adsorption on calcium silicate has been studied as an initial approach of Cs adsorption behavior toward higher temperature condition. As the result of analyzing of Cs adsorption kinetics, it was expected that the underlying adsorption mechanism is chemisorption. Furthermore, analysis of adsorption isotherm suggested unrestricted monolayer formation followed by multilayer formation.
Miwa, Shuhei; Nakajima, Kunihisa; Miyahara, Naoya; Nishioka, Shunichiro; Suzuki, Eriko; Horiguchi, Naoki; Liu, J.; Miradji, F.; Imoto, Jumpei; Afiqa, B. M.; et al.
Mechanical Engineering Journal (Internet), 7(3), p.19-00537_1 - 19-00537_11, 2020/06
We constructed the fission product (FP) chemistry database named ECUME for LWR severe accident. This version of ECUME is equipped with dataset of the chemical reactions and their kinetics constants for the reactions of cesium(Cs)-iodine(I)-boron(B)-molybdenum(Mo)-oxygen(O)-hydrogen(H) system in gas phase, the elemental model for the high temperature chemical reaction of Cs with stainless steel applied as the structural material in a reactor, and thermodynamic data for CsBO vapor species and solids of CsSiO and CsFeSiO for these chemical reactions. The ECUME will provide estimation of Cs distribution due to the evaluation of effects of interaction with BWR control material B and stainless steel on Cs behavior in the Fukushima Daiichi Nuclear Power Station.
Nakajima, Kunihisa; Nishioka, Shunichiro*; Suzuki, Eriko; Osaka, Masahiko
Mechanical Engineering Journal (Internet), 7(3), p.19-00564_1 - 19-00564_14, 2020/06
A large amount of cesium (Cs) chemisorbed onto stainless steel is predicted to be present especially in the upper region of reactor pressure vessel (RPV) during light water reactor severe accident (LWR SA) and a chemisorption model was developed for estimation of such amounts of Cs for stainless steel type 304 (SS304). However, this existing chemisorption model cannot accurately reproduce experimental results. Therefore, in this study, a modified Cs chemisorption model which accounts for silicon content in SS304 and concentration of cesium hydroxide (CsOH) in gaseous phases was constructed by combining penetration theory for gas-liquid mass transfer with chemical reaction and mass action law for CsOH decomposition at interface between gaseous and solid phases. As a result, it was found that the modified model was able to reproduce the experimental data more accurately than the existing model.
Yamaguchi, Yoshihito; Katsuyama, Jinya; Kaji, Yoshiyuki; Osaka, Masahiko; Li, Y.
Mechanical Engineering Journal (Internet), 7(3), p.19-00560_1 - 19-00560_12, 2020/06
Since the Fukushima Daiichi Nuclear Power Plant accident, we have been developing a failure evaluation method that considers creep damage mechanisms using detailed three-dimensional finite element analysis model of lower head including penetration, stub tubes, and weld parts, etc., for the early completion of the decommissioning of the nuclear power plants in Fukushima Daiichi. For the finite element analysis, we have been obtaining material properties for which no data are provided in existing databases or in the literature. In particular, creep data corresponding to the high temperature region near the melting point of materials is important in evaluating creep deformation under severe accident conditions. In this study, we obtained the uniaxial tensile and creep properties for low-alloy steel, stainless steel, and Ni-based alloy. In particular, creep test data with long rupture times at high temperatures are expanded using a tensile test machine that can measure the elongation of test specimens in a noncontact measurement system. The parameters related to the failure evaluation were improved on the basis of the expanded creep database.
Miwa, Shuhei; Takase, Gaku; Imoto, Jumpei; Nishioka, Shunichiro; Miyahara, Naoya; Osaka, Masahiko
Journal of Nuclear Science and Technology, 57(3), p.291 - 300, 2020/03
For the evaluation of transport behavior of control material boron in a severe accident of BWR from the viewpoint of chemical effects on cesium and iodine behavior, boron chemistry during transportation in the high temperature region above 400 K was experimentally investigated. The heating tests of boron oxide specimen were conducted using the dedicated experimental apparatus reproducing fission product release and transport in steam atmosphere. Released boron oxide vapor was deposited above 1,000 K by the condensation onto stainless steel. The boron deposits and/or vapors significantly reacted with stainless steel above 1,000 K and formed the stable iron-boron mixed oxide (FeO)BO. These results indicate that released boron from degraded BWR control blade in a severe accident could remain in the high temperature region such as a Reactor Pressure Vessel. Based on these results, it can be said that the existence of boron deposits in the high temperature region would decrease the amount of transported cesium vapors from a Reactor Pressure Vessel due to possible formation of low volatile cesium borate compounds by the reaction of boron deposits with cesium vapors.
Miradji, F.; Suzuki, Chikashi; Nakajima, Kunihisa; Osaka, Masahiko
Journal of Physics and Chemistry of Solids, 136, p.109168_1 - 109168_9, 2020/01
Kurata, Masaki; Osaka, Masahiko; Jacquemain, D.*; Barrachin, M.*; Haste, T.*
Advances in Nuclear Fuel Chemistry, p.555 - 625, 2020/00
The importance of fuel chemistry has been revivaled since Fukushima-Daiichi Nuclear Power Station (FDNPS) accident. The inspection and analysis of damaged three units, which had been operated in March 11, 2011, showed large differences in the accident progression sequence for these units, because operators attempted to prevent or mitigate the accident progression of each unit by all means possible. Characteristics of fuel debris are considered to be largely influenced by the difference in the sequence and, hence, deviated from those predicted from prototypic accident scenarios, which had been mainly identified from the analysis of Three Mile Island-2 (TMI-2) accident and the following sim-tests. For the proper improvement of our knowledge on severe accident (SA), including non-prototypic conditions, one has to start improving the phenomenology of fuel/core degradation and fission product (FP) behavior. Advances in the chemistry is the most essential approach. The present review attempts to focus on the recent updates and remaining concerns after the FDNPS accident.
Liu, J.; Miyahara, Naoya; Miwa, Shuhei; Takano, Masahide; Hidaka, Akihide; Osaka, Masahiko
Journal of Nuclear Materials, 527, p.151819_1 - 151819_7, 2019/12
To evaluate the effect of each constituent element on the evaporation rate of ruthenium (Ru) from fission-produced alloy precipitates, the oxidation and evaporation behaviors of metallic Ru, molybdenum (Mo), palladium (Pd), rhodium (Rh) and Mo-Ru-Pd-Rh alloy powders were investigated by thermogravimetric analysis under oxidizing atmospheres from 1473 to 1723 K. The findings led to the following conclusions: (1) The quick oxidation of Mo into condensed Mo oxides can effectively suppress the oxidation and evaporation of Ru in alloy powders; (2) After the complete evaporation of Mo, the evaporation loss rate of Ru would be directly influenced by the Ru activity in the Ru-Pd-Rh alloys, which is determined by the composition of alloys.
Machida, Masahiko; Yamada, Susumu; Iwata, Ayako; Otosaka, Shigeyoshi; Kobayashi, Takuya; Watanabe, Masahisa; Funasaka, Hideyuki; Morita, Takami*
Nihon Genshiryoku Gakkai Wabun Rombunshi, 18(4), p.226 - 236, 2019/12
After direct discharges of highly-contaminated water from Unit 2 and 3 in Fukushima Daiichi Nuclear Power Plant (1F) in April to May 2011, Kanda suggested that relatively small run-off of radionuclides from 1F port into Fukushima coastal region has subsequently continued by using his estimation scheme. However, the estimation period was limited until September 2012, and there has been no report on the issue since the work. Therefore, this paper focuses on discharge inventory from 1F port until June 2018. In the missing period, the central government and Tokyo Electric Power Company Holdings have done continuous efforts to stop the discharge, and consequently sea water concentration inside 1F port has diminished gradually. We show monthly discharge inventory of Cs-137 until June 2018 by two schemes, i.e., Kanda's scheme partially improved by authors and more sophisticated one using Voronoi tessellation reflecting the increment of the number of monitoring points inside 1F port. The results show that the former always presents overestimated results compared to the latter but the ratio of former to latter is less than one order. Based on these results, we evaluate impact of discharge inventory from 1F port into the coastal area and radiation does via fish digestion.
Nishioka, Shunichiro; Nakajima, Kunihisa; Suzuki, Eriko; Osaka, Masahiko
Journal of Nuclear Science and Technology, 56(11), p.988 - 995, 2019/11
In order to contribute to improvement of Cs chemisorption model used in severe accident analysis codes, the influence of chemical factors (temperature, atmosphere, concentration of affecting chemical elements etc.) on the Cs chemisorption behaviour onto stainless steel was investigated experimentally. It was found that the surface reaction rate constant used in the current Cs-chemisorption model was influenced by not only temperature, as already known, but also atmosphere, cesium hydroxide (CsOH) concentration in the gas phase and silicon content in SS304. Such chemical factors should be considered for the construction of the improved Cs-chemisorption model. Another important finding is that the chemisorption behavior at lower temperatures, around 873 K, could differ from those above 1073 K. Namely, Cs-Fe-O compounds would form as the main Cs-chemisorbed compounds at 873 K while Cs-Si-Fe-O compounds at more than 1073 K.
Miwa, Shuhei; Miyahara, Naoya; Nakajima, Kunihisa; Nishioka, Shunichiro; Suzuki, Eriko; Horiguchi, Naoki; Liu, J.; Miradji, F.; Imoto, Jumpei; Afiqa, B. M.; et al.
Proceedings of 27th International Conference on Nuclear Engineering (ICONE-27) (Internet), 8 Pages, 2019/05
We constructed the first version of fission product (FP) chemistry database named ECUME for LWR severe accident. The first version of ECUME is equipped with dataset of the chemical reactions and their kinetics constants for the reactions of cesium(Cs)-iodine(I)-boron(B)-molybdenum(Mo)-oxygen(O)-hydrogen(H) system in gas phase, the elemental model for the high temperature chemical reaction of Cs with stainless steel, and thermodynamic data for CsBO vapor species and solids of CsSiO and CsFeSiO. The ECUME will provide more accurate estimation of Cs distribution due to the evaluation of effects of interaction with BWR control material B and stainless steel on Cs behavior in the Fukushima Daiichi Nuclear Power Station.