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JAEA Reports

Improvement of model for cesium chemisorption onto stainless steel in severe accident analysis code SAMPSON (Joint research)

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:1.41MB
JAEA-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$$_{2}$$ at 873 K to 973 K with higher water-solubility, CsFeSiO$$_{4}$$ at 973 K to 1273 K and Cs$$_{2}$$Si$$_{4}$$O$$_{9}$$ 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.

Journal Articles

Revaporization behavior of cesium and iodine compounds from their deposits in the steam-boron atmosphere

Rizaal, M.; Miwa, Shuhei; Suzuki, Eriko; Imoto, Jumpei; Osaka, Masahiko; Gou$"e$llo, M.*

ACS Omega (Internet), 6(48), p.32695 - 32708, 2021/12

 Times Cited Count:1 Percentile:7.13(Chemistry, Multidisciplinary)

Journal Articles

Interaction between caesium iodide particles and gaseous boric acid in a flowing system through a thermal gradient tube (1030 K-450 K) and analysis with ASTEC/SOPHAEROS

Gou$"e$llo, M.*; Hokkinen, M.*; Suzuki, Eriko; Horiguchi, Naoki; Barrachin, M.*; Cousin, F.*

Progress in Nuclear Energy, 138, p.103818_1 - 103818_10, 2021/08

 Times Cited Count:3 Percentile:58.27(Nuclear Science & Technology)

The present work aimed to study the transport of caesium iodide particles through a Thermal Gradient Tube (TGT) from 1023 K to 453 K. Retention inside the tube was evaluated for laminar flowrates composed of argon and steam. Higher retention of particles was highlighted for the experiments using higher steam content and lower flowrate. The second phase of the experiment aimed at identifying the possible revaporization or/and resuspension processes after the deposition. Three atmosphere compositions (Ar/H$$_{2}$$O, Ar/H$$_{2}$$ and Ar/Air) were investigated. The particles removed from what was deposited on the surface walls during the sampling phase exhibited a similar GMD in Ar/H$$_{2}$$O and Ar/H$$_{2}$$ and a bigger diameter in Ar/Air. The experimental results were then analysed with the SOPHAEROS module of the ASTEC code. Overall, the results obtained during the first phase were in agreement with the measured experimental results and during second phase led to no resuspension process.

Journal Articles

Low temperature heat capacity of Cs$$_{2}$$Si$$_{4}$$O$$_{9}$$

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:3 Percentile:46.37(Nuclear Science & Technology)

The low temperature heat capacity of Cs$$_{2}$$Si$$_{4}$$O$$_{9}$$, 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, $$C_{p}$$$$^{o}$$ (298.15K), and the standard entropy, $$S^{o}$$ (298.15K), were 249.4 $$pm$$ 1.1 J K$$^{-1}$$ mol$$^{-1}$$ and 322.1 $$pm$$ 1.3 J K$$^{-1}$$ mol$$^{-1}$$, respectively. The standard Gibbs energy of formation of Cs$$_{2}$$Si$$_{4}$$O$$_{9}$$ at high temperatures, $$Delta$$$$_{f}$$$$G^{o}$$($$T$$), were reevaluated by using the presently obtained $$S^{o}$$ (298.15K) and the previously reported experimental results of the standard enthalpy of formation, $$Delta$$$$_{f}$$$$H^{o}$$ (298.15K), and the standard enthalpy increments at high temperatures, $$H^{o}$$($$T$$)-$$H^{o}$$ (298.15K).

Journal Articles

Development of fission product chemistry database ECUME for the LWR severe accident

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$$_{2}$$ vapor species and solids of Cs$$_{2}$$Si$$_{4}$$O$$_{9}$$ and CsFeSiO$$_{4}$$ 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.

Journal Articles

Study on chemisorption model of cesium hydroxide onto stainless steel type 304

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.

Journal Articles

An Experimental investigation of influencing chemical factors on Cs-chemisorption behavior onto stainless steel

Nishioka, Shunichiro; Nakajima, Kunihisa; Suzuki, Eriko; Osaka, Masahiko

Journal of Nuclear Science and Technology, 56(11), p.988 - 995, 2019/11

 Times Cited Count:11 Percentile:78.07(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.

Journal Articles

Development of fission product chemistry database ECUME for the LWR severe accident

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$$_{2}$$ vapor species and solids of Cs$$_{2}$$Si$$_{4}$$O$$_{9}$$ and CsFeSiO$$_{4}$$. 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.

Journal Articles

Study on chemisorption model of cesium hydroxide onto stainless steel type 304

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.

Journal Articles

Experimental study on Cs chemisorption behaviour onto stainless steel at around 873 K

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.

Journal Articles

Chemical trapping of Sr vapor species by Zircaloy cladding under a specific chemical condition

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$$_{2}$$ 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.

Journal Articles

Modelling of cesium chemisorption under nuclear power plant severe accident conditions

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

Journal Articles

Synthesis and characterization of CeO$$_{2}$$-based simulated fuel containing CsI

Takamatsu, 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$$_{2}$$) based simulated fuels containing Cesium iodide (CsI) are performed by using spark plasma sintering (SPS) method. The sintered CeO$$_{2}$$ pellets with homogeneous distribution of several micro meter of CsI spherical precipitates were successfully obtained by optimizing SPS conditions.

Journal Articles

Effect of atmosphere on the vaporization behavior of CsFeSiO$$_{4}$$

Suzuki, Eriko; Nakajima, Kunihisa; Osaka, Masahiko

Progress in Nuclear Science and Technology (Internet), 5, p.165 - 167, 2018/11

In severe accident condition, CsFeSiO$$_{4}$$ 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$$_{4}$$ at high temperature was investigated by thermal gravimetric-differential thermal analyzer (TG-DTA) experiments. As a result, it was found that vaporization of CsFeSiO$$_{4}$$ in reducing atmosphere (Ar-5%H$$_{2}$$) started at relatively low temperature, about 800$$^{circ}$$C, compared with in atmosphere containing H$$_{2}$$O (Ar-5%H$$_{2}$$-5%H$$_{2}$$O). It was inferred that a possible chemical reaction for the weight loss at around 800$$^{circ}$$C would occurred by the decomposition of CsFeSiO$$_{4}$$ into volatile Cs vapor species under H$$_{2}$$.

Journal Articles

An Experimental investigation for atmospheric effects on Cs chemisorption onto stainless steel

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.

Journal Articles

Chemical form analysis of reaction products in Cs-adsorption on stainless steel by means of HAXPES and SEM/EDX

Kobata, Masaaki; Okane, Tetsuo; Nakajima, Kunihisa; Suzuki, Eriko; Owada, Kenji; Kobayashi, Keisuke*; Yamagami, Hiroshi; Osaka, Masahiko

Journal of Nuclear Materials, 498, p.387 - 394, 2018/01

 Times Cited Count:16 Percentile:85.51(Materials Science, Multidisciplinary)

In this study, for the understandings of Cesium (Cs) adsorption behavior on structure materials in severe accidents at a light water nuclear reactor, the chemical state of Cs and its distribution on the surface of SUS304 stainless steel (SS) with different Si concentration were investigated by hard X-ray photoelectron spectroscopy (HAXPES) and scanning electron microscope / energy dispersive X-ray spectroscopy (SEM/EDX). As a result, it was found that Cs is selectively adsorbed at the site where Si distributes with high concentration. CsFeSiO$$_{4}$$ is a dominant Cs products in the case of low Si content, mainly formed, while Cs$$_{2}$$Si$$_{2}$$O$$_{5}$$ and Cs$$_{2}$$Si$$_{4}$$O$$_{9}$$ are formed in addition to CsFeSiO$$_{4}$$ in the case of high Si content. The chemical forms of the Cs compounds produced in the adsorption process on the SS surface has a close correlation with the concentration and chemical states of Si originally included in SS.

Journal Articles

Results and progress of fundamental research on FP chemistry

Osaka, Masahiko; Nakajima, Kunihisa; Miwa, Shuhei; Di Lemma, F. G.*; Miyahara, Naoya; Suzuki, Chikashi; Suzuki, Eriko; Okane, Tetsuo; Kobata, Masaaki

Proceedings of 8th European Review Meeting on Severe Accident Research (ERMSAR 2017) (Internet), 11 Pages, 2017/05

Fundamental research on fission product (FP) chemistry is underway at Japan Atomic Energy Agency. The purpose is to establish a FP chemistry database in each region of a LWR under severe accident conditions. Improvement of FP chemical models based on this database is also an important task of the research. Research outputs are reflected to the research and development of decommissioning of Fukushima Daiichi Nuclear Power Station (1F) and the enhancement of LWR safety. Four research items have thus been established considering the specific issues of 1F and the priority in the source term research area, as follows: - Effects of boron (B) release kinetics and thermal-hydraulic conditions on FP behavior, - Cesium (Cs) chemisorption and reactions with structural materials, - Establishment of a thermodynamic and thermophysical properties database for FP compounds, - Development of experimental and analytical techniques for the reproduction of FP behavior. In this paper, results and progress of the research are presented.

JAEA Reports

Results and progress of fundamental research on fission product chemistry; Progress report in 2015

Osaka, Masahiko; Miwa, Shuhei; Nakajima, Kunihisa; Di Lemma, F. G.*; Suzuki, Chikashi; Miyahara, Naoya; Kobata, Masaaki; Okane, Tetsuo; Suzuki, Eriko

JAEA-Review 2016-026, 32 Pages, 2016/12

JAEA-Review-2016-026.pdf:6.18MB

A fundamental research program on fission product (FP) chemistry has started since 2012 for the purpose of establishment of a FP chemistry database in each region of LWR under severe accident and improvement of FP chemical models based on the database. Research outputs are reflected as fundamental knowledge to both the research and development of decommissioning of Fukushima Daiichi Nuclear Power Station (1F) and enhancement of LWR safety. Four research items have thus been established considering the specific issues of 1F and the priority in the source term research area, as follows: effects of boron (B) release kinetics and thermal-hydraulic conditions on FP behavior, cesium (Cs) chemisorption and reactions with structural materials, enlargement of a thermodynamic and thermophysical properties database for FP compounds and development of experimental and analytical techniques for the reproduction of FP behavior and for direct measurement methods of chemical form of FP compounds. In this report, the research results and progress for the year 2015 are described. The main accomplishment was the installation of a reproductive test facility for FP release and transport behavior. Moreover, basic knowledge about the Cs chemisorption behavior was also obtained. In addition to the four research items, a further research item is being considered for deeper interpretation of FP behavior by the analysis of samples outside of the 1F units.

Journal Articles

Development of completely Solenoidless tokamak operation in JT-60U

Ushigome, Masahiro*; Ide, Shunsuke; Ito, Satoshi*; Jotaki, Eriko*; Mitarai, Osamu*; Shiraiwa, Shunichi*; Suzuki, Takahiro; Takase, Yuichi*; Tanaka, Shigetoshi*; Fujita, Takaaki; et al.

Nuclear Fusion, 46(2), p.207 - 213, 2006/02

 Times Cited Count:11 Percentile:37.02(Physics, Fluids & Plasmas)

This papaer studies on tokamak plasma start-up completely without central solenoid (CS). On the JT-60 tokamak it is demonstrated that a completely CS-less Ip start-up to 100 kA was achieved even without any null-point by Electron cyclotron range of frequencies (ECRF) and outer PF coil current swing only. Necessary conditions (the EC power, the toroidal field etc.) were clarified. Moreover, it was succeded to maintain Ip = 260kA for 1 sec without CS by NB only. In addition Ip ramp-up by EC and NB only (without LHCD) from 215 to 310kA was achieved. In a high confinement reversed shear discharge, a result suggesting bootstrap over drive was obtained.

Journal Articles

Formation of advanced tokamak plasmas without the use of an ohmic-heating solenoid

Shiraiwa, Shunichi*; Ide, Shunsuke; Ito, Satoshi*; Mitarai, Osamu*; Naito, Osamu; Ozeki, Takahisa; Sakamoto, Yoshiteru; Suzuki, Takahiro; Takase, Yuichi*; Tanaka, Shigetoshi*; et al.

Physical Review Letters, 92(3), p.035001_1 - 035001_4, 2004/01

 Times Cited Count:46 Percentile:82.99(Physics, Multidisciplinary)

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