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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：100(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 1100
C. 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 (Ca
Si0
(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
Times Cited Count：0 Percentile：100(Nuclear Science & Technology)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.
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：100(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; Mohamad, B. A.; 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
Times Cited Count：0 Percentile：100(Nuclear Science & Technology)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
Times Cited Count：1 Percentile：27.81(Chemistry, Multidisciplinary)Machida, Masahiko; Yamada, Susumu; Iwata, Ayako; Otosaka, Shigeyoshi; Kobayashi, Takuya; Watanabe, Masahisa; Funasaka, Hideyuki; Morita, Takami*
Nippon 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
Times Cited Count：4 Percentile：9.78(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; Mohamad, B. A.; 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.
Horiguchi, Naoki; Miyahara, Naoya; Uesawa, Shinichiro; Yoshida, Hiroyuki; Osaka, Masahiko
Proceedings of 27th International Conference on Nuclear Engineering (ICONE-27) (Internet), 8 Pages, 2019/05
For source term evaluation from reactor buildings (RBs) in LWR severe accidents, we have launched to develop an evaluation method of FP aerosol particle deposition onto surfaces of internal structures in an RB based on computational fluid dynamics (CFD). This paper describes development of a CFD simulation tool as the base part of the evaluation method. A preliminary simulation for a representative RB under a representative flow condition was conducted to confirm the tool performance by roughly grasping the deposition behaviors of FP aerosol particle and decontamination factor (DF) in the RB. Calculation results showed that most of aerosol particles were deposited along with gas flow formed by the internal structures in the RB, demonstrating the advantageous feature of the present CFD tool. The DFs from 4 to 14 were obtained with increase of the particle diameters from 0.1 to 10 
m as expected in terms of the particle movement equation.
Yamaguchi, Yoshihito; Katsuyama, Jinya; Kaji, Yoshiyuki; Osaka, Masahiko; Li, Y.
Proceedings of 27th International Conference on Nuclear Engineering (ICONE-27) (Internet), 7 Pages, 2019/05
After the Fukushima Daiichi (1F) Nuclear Power Plant accident, we have been developing a prediction method for rupture time and location considering creep damage mechanisms using finite element analysis for early completion of the decommissioning of nuclear power plants in 1F. We have also been obtaining material properties at high temperature near the melting point which are not provided in existing database or literature for the finite element analysis. In this study, we performed uni-axial tensile and creep tests for low alloy steel, Ni-based alloy steel and stainless steels and expanded existing database of material properties. Especially, creep data with longer rupture time at high temperature were obtained by a creep test equipment with a noncontact measurement system. To improve the accuracy of failure evaluation under severe accident conditions, we determined parameters of creep constitutive law based on the expanded database.
Uesawa, Shinichiro; Miyahara, Naoya; Horiguchi, Naoki; Yoshida, Hiroyuki; Osaka, Masahiko
Proceedings of 27th International Conference on Nuclear Engineering (ICONE-27) (Internet), 5 Pages, 2019/05
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.
Imoto, Jumpei; Miwa, Shuhei; Osaka, Masahiko
Proceedings of International Topical Workshop on Fukushima Decommissioning Research (FDR 2019) (Internet), 4 Pages, 2019/05
Boron (B) oxidative vaporization processes from the representative alloys of Fe-B and Zr-B formed in the mixed melt of BWR control material boron carbide, stainless steel and Zircaloy were experimentally investigated toward the construction of B release model under severe accident. The results show that B oxidative vaporization from ZrB would proceed in the formation of ZrO and BO due to the oxidation of ZrB, followed by the formation of volatile H-B-O vapor species by the reaction of BO with steam. On the other hand, for FeB and FeB, the B oxidative vaporization processes would proceed in the same manner. Complex Fe-B-O compounds formation in addition to amorphous BO were observed by the oxidation of FeB and FeB. Then the B vaporization would occur by the formation of volatile H-B-O compound by the reaction of BO, which were derived from both oxidation of FeB and decomposition of Fe-B-O compounds.
Suzuki, Chikashi; Yaita, Tsuyoshi; Suzuki, Shinichi; Pacold, J.*; Altman, A. B.*; Minasian, S. G.*; Tyliszczak, T.*; Shuk, D. K.*; Yoshida, Hiroyuki; Osaka, Masahiko
Journal of Physics and Chemistry of Solids, 127, p.169 - 177, 2019/04
Times Cited Count：1 Percentile：73.27(Chemistry, Multidisciplinary)A combined method of NEXAFS measurement and DFT-calculation was employed for Cs evaluation in clay minerals. The Cs M
NEXAFS spectra of Cs halides were analyzed using the DFT-calculations, and were well reproduced by incorporating the core-hole strength. The Cs M NEXAFS spectrum of clay minerals was well-reproduced by the DFT-calculations including the major transitions and tail structures with the established method. The further evaluation of this spectrum by charge density suggests that these major transitions and the tail structures likely reflect bonding states and local environments around the Cs atoms. Comparison of electronic states of Cs in the clay mineral with those in the Cs halides by DFT-calculations has shown that the interaction between Cs and the nearest-neighbor atom is largest in the clay mineral, because the energy level of Cs-5s and 5p is closer to that of O-2s and 2p than the s and p orbitals of other alkali metal and alkali earth metal elements.
