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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：0Suzuki, Chikashi; Nakajima, Kunihisa; Osaka, Masahiko
Journal of Nuclear Science and Technology, 59(3), p.345 - 356, 2022/03
Times Cited Count：0During 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 CsSi
FeO 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
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 20
C 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.
Liu, J.; Miwa, Shuhei; Nakajima, Kunihisa; Osaka, Masahiko
Nuclear Materials and Energy (Internet), 26, p.100916_1 - 100916_6, 2021/03
Times Cited Count：0 Percentile：0.01(Nuclear Science & Technology)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：0 Percentile：0.01(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.
SiO
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
Times Cited Count：0 Percentile：0.01(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).
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.
Miradji, F.; Suzuki, Chikashi; Nakajima, Kunihisa; Osaka, Masahiko
Journal of Physics and Chemistry of Solids, 136, p.109168_1 - 109168_9, 2020/01
Times Cited Count：1 Percentile：23.44(Chemistry, Multidisciplinary)Nishioka, Shunichiro; Nakajima, Kunihisa; Suzuki, Eriko; Osaka, Masahiko
Journal of Nuclear Science and Technology, 56(11), p.988 - 995, 2019/11
Times Cited Count：6 Percentile：75.46(Nuclear Science & Technology)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.
Nakajima, Kunihisa; Nishioka, Shunichiro; Suzuki, Eriko; Osaka, Masahiko
Proceedings of 27th International Conference on Nuclear Engineering (ICONE-27) (Internet), 8 Pages, 2019/05
Cesium chemisorption models were developed for estimation of amount of cesium chemisorbed onto stainless steel type 304 (SS304) during light water reactor severe accident. However, existing chemisorption models cannot accurately reproduce experimental results. In this study, a modified cesium chemisorption model was constructed based on a penetration theory for gas-liquid mass transfer with chemical reaction and was able to adequately describe effects on concentration of cesium hydroxide in gaseous phase and silicon content in SS304. It was found that the modified model can more accurately reproduce the experimental data than the existing model.
Suzuki, Eriko; Takase, Gaku; Nakajima, Kunihisa; Nishioka, Shunichiro; Hashimoto, Naoyuki*; Isobe, Shigehito*; Osaka, Masahiko
Proceedings of International Topical Workshop on Fukushima Decommissioning Research (FDR 2019) (Internet), 4 Pages, 2019/05
In order to acquire the knowledge of the Cs chemisorption behaviour in the lower temperature region, the Cs chemisorbed compounds and the surface reaction rates were investigated by conducting the Cs chemisorption tests onto stainless steel at 873 and 973 K. As a result, The cesium ferrate compounds were revealed to be formed at this temperatures. It was seen that the dependences of surface reaction rate constant on this temperature were different from that at the higher temperature region. This behaviour leads to the conclusion that the Cs chemisorption model in the low temperature region should be newly constructed.
Mohamad, A.*; Nakajima, Kunihisa; Suzuki, Eriko; Miwa, Shuhei; Osaka, Masahiko; Oishi, Yuji*; Muta, Hiroaki*; Kurosaki, Ken*
Proceedings of International Topical Workshop on Fukushima Decommissioning Research (FDR 2019) (Internet), 4 Pages, 2019/05
In the accident of Fukushima Daiichi Nuclear Power Station, formation of a volatile SrCl could have occurred by the sea-water injection into the core. This can cause the release of non-volatile group Sr from the fuel to induce chemical reactions with reactor structural materials, such as stainless steel and Zircaloy (Zry) cladding. Such reactions could cause the changes in distribution of Sr in the reactor. Chemical reactions between Sr species and Zry were therefore investigated experimentally. As the result, it can be said that Sr vapor species were chemically trapped right after the release from fuel. This trapping effect of Sr by Zry-cladding implies a possibility of preferable Sr retention in the oxide phase of debris.
Miradji, F.; Suzuki, Chikashi; Nishioka, Shunichiro; Suzuki, Eriko; Nakajima, Kunihisa; Osaka, Masahiko; Barrachin, M.*; Do, T. M. D.*; Murakami, Kenta*; Suzuki, Masahide*
Proceedings of 9th Conference on Severe Accident Research (ERMSAR 2019) (Internet), 21 Pages, 2019/03
-based simulated fuel containing CsITakamatsu, Yuki*; Ishii, Hiroto*; Oishi, Yuji*; Muta, Hiroaki*; Yamanaka, Shinsuke*; Suzuki, Eriko; Nakajima, Kunihisa; Miwa, Shuhei; Osaka, Masahiko; Kurosaki, Ken*
Nihon Genshiryoku Gakkai Wabun Rombunshi, 17(3/4), p.106 - 110, 2018/12
In order to establish the synthesis method of simulated fuel contacting Cesium (Cs) which is required for the evaluation of physical/chemical characteristics in fuel and release behavior of Cs, sintering tests of the cerium dioxide (CeO) based simulated fuels containing Cesium iodide (CsI) are performed by using spark plasma sintering (SPS) method. The sintered CeO pellets with homogeneous distribution of several micro meter of CsI spherical precipitates were successfully obtained by optimizing SPS conditions.
Suzuki, Eriko; Nakajima, Kunihisa; Osaka, Masahiko
Progress in Nuclear Science and Technology (Internet), 5, p.165 - 167, 2018/11
In severe accident condition, CsFeSiO could be formed by Cesium (Cs) chemisorption onto reactor structural materials. For evaluation of re-vaporization behavior, effect of atmosphere on the vaporization behavior of CsFeSiO at high temperature was investigated by thermal gravimetric-differential thermal analyzer (TG-DTA) experiments. As a result, it was found that vaporization of CsFeSiO in reducing atmosphere (Ar-5%H) started at relatively low temperature, about 800C, compared with in atmosphere containing HO (Ar-5%H-5%HO). It was inferred that a possible chemical reaction for the weight loss at around 800C would occurred by the decomposition of CsFeSiO into volatile Cs vapor species under H.
Nakajima, Kunihisa; Suzuki, Eriko; Miyahara, Naoya; Osaka, Masahiko
Progress in Nuclear Science and Technology (Internet), 5, p.168 - 170, 2018/11
Chemical interaction between cesium (Cs) vapor and stainless steel (SS) surface known as chemisorption can cause a significant amount of Cs retention on the inner surfaces within the reactor pressure vessel during a light water reactor severe accident (SA). Although the chemisorption is known to be influenced with temperature and atmosphere, their dependancies are not yet fully understood. Therefore, the Cs chemisorption behaviours under mixed gases of steam and hydrogen were experimentally examined to contribute to a better understanding of the chemisorption behaviours under various atmospheres experienced during the SA at the Fukushima Daiichi Nuclear Power Station. As a result, it was found that the deposited amounts of Cs onto the SS in the steam-containing atmosphere were much higher than those in the no steam atmosphere. It was considered that Cs revaporization from a chemisorbed product was one of the reasons why the deposited amounts under the reducing atmosphere decreased.
