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at temperature range 170 - 290
CLuu, V. N.; Nakajima, Kunihisa
Nuclear Engineering and Design, 426, p.113402_1 - 113402_7, 2024/09
Li, N.*; Sun, Y.*; Nakajima, Kunihisa; Kurosaki, Ken*
Journal of Nuclear Science and Technology, 61(3), p.343 - 353, 2024/03
Times Cited Count：0 Percentile：0.01(Nuclear Science & Technology)During the Fukushima Daiichi nuclear power plant (1F) accident, an overwhelming amount of the cesium remaining in the pressure vessel could have been deposited onto 304 stainless steel (SS304) steam separators and dryers, both with large surface areas. During 1F's decommissioning, the deposited cesium is a safety hazard as it can generate radioactive dust. However, the cohesive and adhesive strengths of CsOH-chemisorbed oxide scales are yet to be defined. In this study, we investigated how CsOH-chemisorption affects the cohesive and adhesive strengths between oxide scales and SS304 substrates with a scratch tester. The scratch test results revealed that the cohesive strengths of the oxide scales decreased after CsOH-chemisorption, while adhesive failure could not be reached.
CLuu, V. N.; Nakajima, Kunihisa
Mechanical Engineering Journal (Internet), 11(2), p.23-00446_1 - 23-00446_11, 2024/01
CLuu, V. N.; Nakajima, Kunihisa
Proceedings of 30th International Conference on Nuclear Engineering (ICONE30) (Internet), 9 Pages, 2023/05
Mohamad, A. B.; Nakajima, Kunihisa; Miwa, Shuhei; Osaka, Masahiko
Journal of Nuclear Science and Technology, 60(3), p.215 - 222, 2023/03
Times Cited Count：0 Percentile：0.01(Nuclear Science & Technology)Luu, V. N.; Nakajima, Kunihisa
Journal of Nuclear Science and Technology, 60(2), p.153 - 164, 2023/02
Times Cited Count：4 Percentile：74.52(Nuclear Science & Technology)Miwa, Shuhei; Karasawa, Hidetoshi; Nakajima, Kunihisa; Kino, Chiaki*; Suzuki, Eriko; Imoto, Jumpei
JAEA-Data/Code 2021-022, 32 Pages, 2023/01
JAEA-Data-Code-2021-022.pdf:1.41MBJAEA-Data-Code-2021-022(errata).pdf:0.17MB
The improved model for cesium (Cs) chemisorption onto stainless steel (SS) in the fission product (FP) chemistry database named ECUME was incorporated into the severe accident (SA) analysis code SAMPSON for the more accurate estimation of Cs distribution within nuclear reactor vessels in the TEPCO's Fukushima Daiichi Nuclear Power Station (1F). The SAMPSON with the improved model was verified based on the analysis results reproducing the experimental results which were subjected to the modeling of Cs chemisorption behavior. Then, the experiment in the facility with the temperature gradient tube to simulate SA conditions such as temperature decrease and aerosol formation was analyzed to confirm availability of the improved model to the analysis of Cs chemisorption onto SS. The SAMPSON with the improved model successfully reproduced the experimental results, which indicates that the improved model and the analytical method such as setting a method of node-junction, models of aerosol formation and the calculation method of saturated CsOH vapor pressure can be applicable to the analysis of Cs chemisorption behavior. As the information on water-solubility of Cs deposits was also prerequisite to estimate the Cs distribution in the 1F because Cs can be transported through aqueous phase after the SA, the water-solubility of chemisorbed Cs compounds was investigated. The chemisorbed compounds on SS304 have been identified to CsFeO
at 873 K to 973 K with higher water-solubility, CsFeSiO
at 973 K to 1273 K and CsSiO
at 1073 K to 1273 K with lower water-solubility. From these results, the water-solubility of chemisorbed Cs compounds can be estimated according to the SA analysis conditions such as temperature in the reactor and the CsOH concentration affecting the amount of chemisorbed Cs.
Rizaal, M.; Nakajima, Kunihisa; Saito, Takumi*; Osaka, Masahiko; Okamoto, Koji*
ACS Omega (Internet), 7(33), p.29326 - 29336, 2022/08
Times Cited Count：3 Percentile：38.23(Chemistry, Multidisciplinary)Liu, J.; Nakajima, Kunihisa; Miwa, Shuhei; Shirasu, Noriko; Osaka, Masahiko
Journal of Nuclear Science and Technology, 59(4), p.484 - 490, 2022/04
Times Cited Count：0 Percentile：0.01(Nuclear Science & Technology)Suzuki, Chikashi; Nakajima, Kunihisa; Osaka, Masahiko
Journal of Nuclear Science and Technology, 59(3), p.345 - 356, 2022/03
Times Cited Count：1 Percentile：15.09(Nuclear Science & Technology)During a severe accident (SA) such as the Fukushima Daiichi Nuclear Power Plant accident, fission products (FP) can be retained on the surface of structural materials in reactors. Cesium (Cs) is an important FP, and various Cs compounds such as Cs silicates are formed on the surface of stainless steel (SS) in a reactor during a SA. We calculated total energies of Cs-Si-O compounds for evaluation on phase stability within an adiabatic approximation. The calculations indicate that Cs
Si
O
is the most stable of the Cs-Si-O compounds. We calculated, furthermore, total energies of Cs-Si-Fe-O compounds. These calculations indicate that Cs-Si-Fe-O compounds are more stable than C-Si-O compounds and that CsSiFeO is the most stable of these C-Si-O and Cs-Si-Fe-O compounds within an adiabatic approximation. The results of our present calculations and our previous experiments lead to the conclusion that Cs-Si-Fe-O compounds can be stably formed on SS surface by Cs chemisorption.
Osaka, Masahiko; Gou
llo, M.*; Nakajima, Kunihisa
Journal of Nuclear Science and Technology, 59(3), p.292 - 305, 2022/03
Times Cited Count：4 Percentile：54.16(Nuclear Science & Technology)Research on the fission product chemistry made after the severe accident of the Fukushima Daiichi Nuclear Power Station were reviewed with focus on the Cesium chemistry in terms of two regimes, namely the accidental source term and the long-term source term via aqueous phase towards the decommissioning. For the accidental source term, Cs chemical interaction with Mo, B and Si were reviewed. Regarding the unique issue of long-term source term via aqueous phase, Cs penetration into concrete and fuel debris leaching were mentioned as the main sources of FPs. Efforts on the preparation of thermodynamic data for the Cs complex oxides were described. All these Cs chemical behaviors should be modelled and validated/verified through the analysis and evaluation of the actual samples including fuel debris that would be taken from the Fukushima Daiichi Nuclear Power Station in near future.
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.
Miwa, Shuhei; Miyahara, Naoya*; Nakajima, Kunihisa; Imoto, Jumpei; Suzuki, Eriko
Nihon Genshiryoku Gakkai-Shi ATOMO
, 63(12), p.825 - 829, 2021/12
In the BWR severe accident, it was indicated that the control material boron significantly influences chemical behavior and transition behavior of cesium, which is important from the viewpoint of exposure, and it causes great uncertainty in the prediction of environmental release and distribution in the reactor. Therefore, in order to elucidate the important chemistry to be considered in severe accident analysis, we have developed the experimental setup that enables the evaluation of chemistry during transportation in the reactor, and evaluated cesium chemistry. Based on the results, we developed the chemistry database named ECUME composed of datasets and models that are the basis of chemical reaction analysis so that chemical behavior could be evaluated by severe accident analysis code.
Liu, J.; Miwa, Shuhei; Nakajima, Kunihisa; Osaka, Masahiko
Nuclear Materials and Energy (Internet), 26, p.100916_1 - 100916_6, 2021/03
Times Cited Count：2 Percentile：29.53(Nuclear Science & Technology)Miwa, Shuhei; Nakajima, Kunihisa; Suzuki, Chikashi; Rizaal, M.; Suzuki, Eriko; Horiguchi, Naoki; Osaka, Masahiko
Proceedings of Joint International Conference on Supercomputing in Nuclear Applications + Monte Carlo 2020 (SNA + MC 2020), p.253 - 260, 2020/12
We have proceeded the fundamental study for the improvement of the evaluation of fission product (FP) chemistry and the treatment of fine space resolution which are main issues for the evaluation of FP behaviors in a severe accident (SA). We have been developing FP chemistry database named ECUME for the improvement of SA analysis codes. We prepared thermodynamic data for Cs compounds which is no experimental data available by computational approach. Regarding the space resolution issue, we have been developing analysis tool named CHASER based on 3D-CFD code with the model for FP chemistry. More accurate evaluation of FP behavior can be achieved by incorporating ECUME to the CHASER.
Rizaal, M.; Nakajima, Kunihisa; Saito, Takumi*; Osaka, Masahiko; Okamoto, Koji*
Journal of Nuclear Science and Technology, 57(9), p.1062 - 1073, 2020/09
Times Cited Count：8 Percentile：69.90(Nuclear Science & Technology)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.
SiOSuzuki, Eriko; Nakajima, Kunihisa; Osaka, Masahiko; Oishi, Yuji*; Muta, Hiroaki*; Kurosaki, Ken*
Journal of Nuclear Science and Technology, 57(7), p.852 - 857, 2020/07
Times Cited Count：4 Percentile：43.68(Nuclear Science & Technology)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).
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.
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.
