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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 CsSi
O
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.
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：10 Percentile：63.66(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.
Nishioka, Shunichiro; Nakajima, Kunihisa; Suzuki, Eriko; Osaka, Masahiko
Journal of Nuclear Science and Technology, 56(11), p.988 - 995, 2019/11
Times Cited Count：14 Percentile：78.39(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.
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
Suzuki, Akihiro*; Ito, Kenichi*; Nishioka, Shunichiro; Osaka, Masahiko
no journal, ,
To simulate the formation of micron-size spherical Cs-bearing particles, vaporized Cs and Si were reacted under high temperature water-vapor atmosphere and solidified in the gas phase experimentally. With this simulation study, the possibility that the Cs-bearing particles (type A spherical particles) in the environment were formed by reaction-and-solidification process under the high temperature gas phase in RPV was confirmed.
Nakajima, Kunihisa; Nishioka, Shunichiro; Suzuki, Eriko; Miradji, F.; Osaka, Masahiko
no journal, ,
Radioactive cesium (Cs) localized in the upper region of reactor pressure vessel (RPV) is one of the major concerns, especially in the case of the fuel debris retrieval accessing from top of the RPV. For estimation of amount of Cs chemisorbed onto structure materials, Cs chemisorption model is developed and incorporated into present severe accident codes. However, this chemisorption model cannot accurately reproduce experimental results. Therefore, this study elucidates essential factors influencing the Cs chemisorption behavior and construct the Cs chemisorption model considering these factors. It was found that this model can more accurately reproduce not only our experimental results but also the results used to construct the existing chemisorption model.
Suzuki, Eriko; Ogawa, Hiroaki; Nakajima, Kunihisa; Nishioka, Shunichiro; Osaka, Masahiko; Yamashita, Shinichiro; Kurishiba, Ryoko*; Endo, Takashi*; Isobe, Shigehito*; Hashimoto, Naoyuki*
no journal, ,
To elucidate Cs chemisorption behaviour onto stainless steel under LWR severe accident condition, elemental distribution measurement at microlevel was performed by using XPS and TEM. As a result, it was found that Cs-(Fe)-Si-O compounds, which have different composition, could be distributed.
Miradji, F.; Suzuki, Eriko; Nishioka, Shunichiro; Suzuki, Chikashi; Nakajima, Kunihisa; Oishi, Yuji*; Muta, Hiroaki*; Kurosaki, Ken*; Do, Thi Mai Dung*; Osaka, Masahiko
no journal, ,
Nishioka, Shunichiro; Takase, Gaku; Nakajima, Kunihisa; Suzuki, Eriko; Osaka, Masahiko
no journal, ,
The chemical/physical properties of Cs-chemisorbed deposit could change along with the progression of LWR severe accident (SA). In this study, the influence of temperature change on the properties of Cs-chemisorbed deposit was investigated experimentally. It was found that Cs-Fe-O compounds, which had been formed by chemisorption at 873 K, could transform into Cs-Si-(Fe)-O compounds at 1273 K.
Nakajima, Kunihisa; Suzuki, Eriko; Nishioka, Shunichiro; Osaka, Masahiko
no journal, ,
Information on the Cs distribution inside the reactors at Fukushima Daiichi Nuclear Power Station (1F) is important to proceed the decommissioning. For contribution to analysis of the Cs distribution, Cs chemisorption behaviors and chemical characteristics of the chemisorbed products have been investigated to establish a chemisorption model considering influences of the chemical reaction and the chemical characteristics of reaction products. As a first step, reproducibility tests were carried out to validate the existing model incorporated into sever accident analysis codes such as SAMPSON. As a result, reaction rate constants under an argon and hydrogen gas atmosphere do not increase with temperature as expected by the existing model and the chemisorbed amounts at 1000
C become lower than those at 800C. On the other hand, in the case of steam-containing argon hydrogen gas atmosphere, the reaction rate constants in such a high concentration Cs gas as expected in 1F tend to become lower than those derived from the existing model. Therefore, it was found that a chemisorption model considering difference of reducing and oxidizing atmospheres and dependence of Cs concentration in gas phase was necessary.
Kino, Chiaki*; Karasawa, Hidetoshi*; Uchida, Shunsuke*; Nishioka, Shunichiro; Osaka, Masahiko
no journal, ,
Analysis of the long-term transport behavior of fission products (FP) is important for decommissioning of Fukushima-Daiichi Nuclear Power Station, "Decommissioning analysis code" which can analyze thermal-hydraulic and FP behavior for 10 years after the severe accident has been developed based on SAMPSON code. As the results of test analysis for 2 months after SA, Cs concentration in the wet-well (W/W) decreased slower than that in the case of consideration only with treatment of contaminated water. This result indicates a possible long-term contribution of accumulated Cs in W/W as the Cs contamination source.
150C temperature rangeDo, Thi-Mai-Dung*; Nhut, V. L.*; Murakami, Kenta*; Suematsu, Hisayuki*; Nakajima, Kunihisa; Nishioka, Shunichiro; Suzuki, Eriko; Miradji, F.; Osaka, Masahiko
no journal, ,
The interaction between CsMoO with concrete within the temperature range of 600150C in Ar gas is studied. It seems that there is no reaction between CsMoO aerosol particles with concrete at these temperatures. However, because of the hygroscopic property, CsMoO aerosol particles change to the liquid phase and quickly diffused inside the concrete bulk.
Kino, Chiaki*; Karasawa, Hidetoshi*; Uchida, Shunsuke*; Nishioka, Shunichiro; Osaka, Masahiko
no journal, ,
To evaluate the remigration behavior of FP through the aqueous phase in FDNPS for a long term, an analysis methodology of contaminated water was developed based on SAMPSON code. The test analysis result for cesium concentration in the contaminated water in FDNPS unit 1 for 1 year, with the consideration of cesium release from the fuel debris to the aqueous phase had a good agreement with the actual measured cesium concentration.
Suzuki, Eriko; Nakajima, Kunihisa; Nishioka, Shunichiro*; Miwa, Shuhei; Horiguchi, Naoki; Imoto, Jumpei; Liu, J.; Karasawa, Hidetoshi; Osaka, Masahiko
no journal, ,
The elemental model set (EM) of ECUME consists of improved models which can be directly incorporated into the present severe accident analysis codes. The models of EM has advantages in considering various chemical conditions. The improved model for cesium (Cs) chemisorption has successfully reproduced the effects of Cs vapor concentration in gas phase and silicon content in stainless steel on the Cs chemisorption behavior. This improved model can contribute to more accurate estimation of Cs distribution in a high temperature area.
Imoto, Jumpei; Nishioka, Shunichiro*; Nakajima, Kunihisa; Suzuki, Eriko; Osaka, Masahiko
no journal, ,
In the case of elution of chemisorbed Cs onto the reactor pressure vessel structure materials in the Fukushima Daiichi Nuclear Power Station due to wall condensation of steam, etc., this eluted Cs can be become one of the long-term source term through the aqueous phase. Therefore, in order to clarify this dissolution behavior, a dissolution test of Cs chemisorbed onto stainless steel in water at room temperature was performed up to 50 days. As a result, it was found that Cs chemisorbed on stainless steel continues to elute in trace amounts over long period of time in water. It was suggested that this can be one of the long-term source term.
Nakajima, Kunihisa; Suzuki, Eriko; Nishioka, Shunichiro*; Miwa, Shuhei; Horiguchi, Naoki; Imoto, Jumpei; Liu, J.; Karasawa, Hidetoshi; Osaka, Masahiko
no journal, ,
Thermodynamic data of cesium compounds with boron and silicon are included in the thermodynamic dataset (TM) of ECUME. Chemical forms and fractions of cesium compounds formed in high temperature regions of nuclear reactors and revaporization amount of Cs chemisorbed onto stainless steel can be more accurately estimated by using the TM of ECUME. Incorporation of ECUME into severe accident analysis codes can cope with chemical behaviors of FPs influencing their release and transport behaviors and can be expected to improve source term estimations.
