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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; 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$$_{2}$$ 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

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*

Nippon 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:1 Percentile:38.14(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

ScPd$$_2$$Al$$_3$$; New polymorphic phase in Al-Pd-Sc system

Pospisil, J.; Haga, Yoshinori; Nakajima, Kunihisa; Ishikawa, Norito; C$'i$sa$v{r}$ov$'a$, I.*; Tateiwa, Naoyuki; Yamamoto, Etsuji; Yamamura, Tomoo*

Solid State Communications, 268, p.12 - 14, 2017/12

 Percentile:100(Physics, Condensed Matter)

Journal Articles

Prediction of chemical effects of Mo and B on the Cs chemisorption onto stainless steel

Di Lemma, F. G.; Yamashita, Shinichiro; Miwa, Shuhei; Nakajima, Kunihisa; Osaka, Masahiko

Energy Procedia, 127, p.29 - 34, 2017/09

 Percentile:100

Chemical effects of molybdenum (Mo) and boron (B), which were considered to form compounds with Cs, on the Cs chemisorption were predicted using a chemical equilibrium calculation. It is seen that Cs$$_{2}$$MoO$$_{4}$$ were formed in the chemisorbed compounds. On the other hand, little effects were observed for B. The results suggest that the effects of Mo should be considered for further experimental investigation.

Journal Articles

Development of experimental and analytical technologies for fission product chemistry under LWR severe accident condition

Miyahara, Naoya; Miwa, Shuhei; Nakajima, Kunihisa; Osaka, Masahiko

Proceedings of 2017 Water Reactor Fuel Performance Meeting (WRFPM 2017) (USB Flash Drive), 9 Pages, 2017/09

This paper presents the development of a reproductive experimental setup for FP release and transport and an analysis tool considering chemical reaction kinetics for the construction of the FP chemistry database. The performance test of the reproductive experimental setup TeRRa using CsI compounds show that TeRRa can reproduce well a FP chemistry-related behavior such as aerosol formation, growth and deposition behavior. An analytical tool has been developed based on the commercial ANSYS-FLUENT code. Some additional models was added to evaluate detailed FP chemistry during release and transport in this study. A test analysis simulating the CsI heating test in steam atmosphere was carried out to demonstrate the performance of the improved code. The result shows the appropriateness of the additional models.

Journal Articles

Thermodynamic study of gaseous CsBO$$_{2}$$ by Knudsen effusion mass spectrometry

Nakajima, Kunihisa; Takai, Toshihide; Furukawa, Tomohiro; Osaka, Masahiko

Journal of Nuclear Materials, 491, p.183 - 189, 2017/08

 Times Cited Count:1 Percentile:64.68(Materials Science, Multidisciplinary)

One of the main chemical forms of cesium in the gas phase during severe accidents of light water reactor is expected to be cesium metaborate, CsBO$$_{2}$$, by thermodynamic equilibrium calculation considering reaction with boron. But accuracy of the thermodynamic data of gaseous metaborate, CsBO$$_{2}$$(g), has been judged as poor quality. Thus, Knudsen effusion mass spectrometric measurement of CsBO$$_{2}$$ was carried out to obtain reliable thermodynamic data. The evaluated values of standard enthalpy of formation of CsBO$$_{2}$$(g), $$Delta$$$$_{f}$$H$$^{circ}$$$$_{298}$$(CsBO$$_{2}$$,g), by the 2nd and 3rd law treatments are -700.7$$pm$$10.7 kJ/mol and -697.0$$pm$$10.6 kJ/mol, respectively, and agree with each other within the errors, which suggests our data are reliable. Further, it was found that the existing data of the Gibbs energy function and the standard enthalpy of formation agreed well with the values evaluated in this study, which indicates the existing thermodynamic data are also reliable.

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.

Journal Articles

Experimental investigation of the influence of Mo contained in stainless steel on Cs chemisorption behavior

Di Lemma, F. G.; Nakajima, Kunihisa; Yamashita, Shinichiro; Osaka, Masahiko

Journal of Nuclear Materials, 484, p.174 - 182, 2017/02

 Times Cited Count:4 Percentile:18.09(Materials Science, Multidisciplinary)

Chemisorption phenomena can affect fission products retention in the nuclear reactor vessel during a Severe Accident (SA). This paper will describe the influence of molybdenum contained in type 316 stainless steel (SS) on Cs chemisorption. Our experiments showed the formation of Cs-Mo compounds in addition to CsFeSiO$$_{4}$$, observed previously on SS304. The results of high temperature stability tests on the deposits are also presented. These tests aimed at simulating the revaporization of FP from structural materials during a SA. From our results, it can be inferred that Cs-Mo deposits may revaporize, contributing as a delayed source to the radioactive release.

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

Determination of optimal vapor pressure data by the second and third law methods

Nakajima, Kunihisa

Mass Spectrometry (Internet), 5(2), p.S0055_1 - S0055_6, 2016/12

Though equilibrium vapor pressures are utilized to determine thermodynamic properties of not only gaseous species but also condensed phases, the obtained data often disagree by a factor of 100 and more. A new data analysis method is proposed using the so-called second and third law procedures to improve accuracy of vapor pressure measurements. It was found from examination of vapor pressures of cesium metaborate and silver that the analysis of the difference between the second and third law values can result in determination of an optimal data set. Since the new thermodynamic method does not require special techniques and or experiences in dealing with measured data, it is reliable and versatile to improve the accuracy of vapor pressure evaluation.

Journal Articles

Boron effects on fission product behavior under severe accident conditions

Miwa, Shuhei; Di Lemma, F. G.; Nakajima, Kunihisa; Osaka, Masahiko

Proceedings of Annual Topical Meeting on LWR Fuels with Enhanced Safety and Performance (TopFuel 2016) (USB Flash Drive), p.861 - 868, 2016/09

The basic studies have been performed for the evaluation of boron (B) release from the degraded BWR control rod material and its effect on cesium (Cs) and iodine (I) chemistry during a severe accident. The B effect on Cs and I chemistry was evaluated by thermal equilibrium calculation considering the change in B release behavior under the degradation of BWR control rod material. Results shows that The generation of gaseous iodine as well as CsBO$$_{2}$$ could be suppressed under a steam-starvation atmosphere because of a lower B release fraction owing to the possible formation of stable iron Fe-B alloys. In response to this prediction result, the basic experiments and analyses are underway. The B release behavior from the boron carbide/stainless steel/Zircaloy reaction products, the thermochemical properties and phase states of complex Cs-B-O compounds are being studied. For the validation of all these evaluation results, reproductive test for FP release and transport will be performed.

Journal Articles

Surface analyses of cesium hydroxide chemisorbed onto type 304 stainless steel

Di Lemma, F. G.; Nakajima, Kunihisa; Yamashita, Shinichiro; Osaka, Masahiko

Nuclear Engineering and Design, 305, p.411 - 420, 2016/08

 Times Cited Count:7 Percentile:13.96(Nuclear Science & Technology)

Chemisorption is of main importance during a Severe Accident (SA) at a light water reactor, as it can influence fission products retention in the reactor vessel. Information on the distribution, composition and properties of such deposits can influence the decommissioning practice after a SA. Moreover such information can enhance the description of the chemisorption models applied in SA codes, consequently improving the source term assessment. This paper will present the results obtained from CsOH chemisorption experiments onto type 304 stainless steel samples, used as simulants of reactor structural materials. The samples post-analyses showed that CsOH will absorb onto the surface, reacting preferentially with Si impurities and forming a newly detected compound, CsFeSiO$$_{4}$$. From our results, it can be inferred that Si content in structural materials can determine the amount of radioactive Cs deposited onto the reactor vessel after a SA.

Journal Articles

Thermal conductivity of U-20 wt.%Pu-2 wt.%Am-10 wt.%Zr alloy

Nishi, Tsuyoshi; Nakajima, Kunihisa; Takano, Masahide; Kurata, Masaki; Arita, Yuji*

Journal of Nuclear Materials, 464, p.270 - 274, 2015/09

 Percentile:100(Materials Science, Multidisciplinary)

no abstracts in English

JAEA Reports

Development of measurement technique of the equilibrium vapor pressure of simulated fission products

Takai, Toshihide; Nakajima, Kunihisa; Furukawa, Tomohiro

JAEA-Technology 2015-002, 20 Pages, 2015/03

JAEA-Technology-2015-002.pdf:3.46MB

To improve the evaluation technique of source term, the measurement technique of the equilibrium vapor pressure using a high temperature mass spectrometer is required to expand the thermodynamic database of the simulated FPs. Existing test apparatus was adapted for this purpose. A mass spectrometer capable of measuring a wide mass number range and glove box for handling simulated FPs were installed for analyzing heavy FPs and preventing deterioration of simulated FPs in an air atmosphere, respectively. Function verification using standard sample and precision investigation using simulated FP sample were carried out. The oxygen dissociation pressure and standard enthalpy of formation of RuO$$_{2}$$(s) were evaluated, and it was confirmed these evaluated values were agreed with the calculated value from existing thermodynamic data and evaluation value written in the literature. Consequently, it was proven that high precision thermodynamic data was able to obtain by using this apparatus.

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