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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.

Oral presentation

Results and progress of fundamental research on FP chemistry

Osaka, Masahiko; Nakajima, Kunihisa; Miwa, Shuhei; Miyahara, Naoya; Suzuki, Eriko; Suzuki, Chikashi; Horiguchi, Naoki; Imoto, Jumpei; Liu, J.; Nishioka, Shunichiro; et al.

no journal, , 

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.

Oral presentation

Investigation of in-reactor cesium chemical behavior in TEPCO's Fukushima Daiichi Nuclear Power Station accident, 3; Analysis of Cs chemisorption behavior onto stainless steel by mass transfer model

Nishioka, Shunichiro; Nakajima, Kunihisa; Miradji, F.; Suzuki, Eriko; Osaka, Masahiko

no journal, , 

The temperature dependency of surface reaction rate of Cs onto stainless steel, which is obtained by experimental test was analyzed by using mass transfer model. It was found that Cs concentration in gas phase influenced on the surface reaction rate.

Oral presentation

Quantum modelling of Cs substances in the case of LWR severe accident

Miradji, F.; Suzuki, Chikashi; Nakajima, Kunihisa; Osaka, Masahiko

no journal, , 

Oral presentation

Modelling of Cs chemisorption behaviour under LWR severe accident

Nishioka, Shunichiro; Nakajima, Kunihisa; Suzuki, Eriko; Miradji, F.; Osaka, Masahiko

no journal, , 

In order to contribute to Cs distribution analysis in Fukushima Daiichi Nuclear Power Station reactors by using severe accident analysis code, the influence of chemical factors (temperature, atmosphere etc.) on the Cs chemisorption behaviour onto stainless steel was investigated experimentally. An improved Cs chemisorption model was then established considering the effect of chemical factors obtained by the experiment. The accuracy of the present model is greatly improved by 1 order of magnitude compared with that incorporated in the existing SA codes.

Oral presentation

Structural and thermal properties of Cs-Fe-Si-O systems under LWR severe accident by DFT calculations

Miradji, F.; Suzuki, Chikashi; Nakajima, Kunihisa; Osaka, Masahiko

no journal, , 

Oral presentation

Fundamental research on FP chemistry; Boron effects on cesium and iodine chemistry

Miwa, Shuhei; Nakajima, Kunihisa; Miyahara, Naoya; Nishioka, Shunichiro; Suzuki, Chikashi; Suzuki, Eriko; Horiguchi, Naoki; Imoto, Jumpei; Liu, J.; Miradji, F.; et al.

no journal, , 

We have been conducting the fundamental study on fission product (FP) chemistry under severe accident (SA) conditions. The objective is to construct the FP chemistry database and to improve FP chemistry model for the improvement of source term evaluation technology. We have established the technical basis, such as experimental set-up and analysis tool, for the evaluation of FP chemistry in SA conditions. Fundamental knowledges on the effects of boron on the cesium and iodine chemistry were also obtained.

Oral presentation

Cesium chemisorption behavior onto stainless steel at temperatures higher than 1073 K

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.

Oral presentation

Comparative study of Cs silicates properties between DFT calculation and experimental data

Miradji, F.; Suzuki, Eriko; Nishioka, Shunichiro; Suzuki, Chikashi; Nakajima, Kunihisa; Oishi, Yuji*; Muta, Hiroaki*; Kurosaki, Ken*; Do, Thi Mai Dung*; Osaka, Masahiko

no journal, , 

Oral presentation

Development of Ru chemistry database under severe accident conditions of nuclear facilities

Miyahara, Naoya; Miwa, Shuhei; Miradji, F.; Liu, J.; Horiguchi, Naoki; Osaka, Masahiko

no journal, , 

In order to contribute to the improvement of source term under severe accidents of nuclear facilities, a database of gaseous phase chemical reaction rate constants in the Ru-N-O-H system was developed. The data implemented in the database were prepared by either literature review or, if the literature data was not available, ab-initio based calculation. It was confirmed by preliminary analyses that there is no lack of reaction path in the database and the changes of Ru chemical forms were successfully calculated. These results indicated that the developed database would be useful to evaluate Ru chemical forms considering the chemical reaction kinetics.

Oral presentation

Reaction products in Cs-adsorption on concrete in the 600$$sim$$150$$^{circ}$$C temperature range

Do, 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 Cs$$_{2}$$MoO$$_{4}$$ with concrete within the temperature range of 600$$sim$$150$$^{circ}$$C in Ar gas is studied. It seems that there is no reaction between Cs$$_{2}$$MoO$$_{4}$$ aerosol particles with concrete at these temperatures. However, because of the hygroscopic property, Cs$$_{2}$$MoO$$_{4}$$ aerosol particles change to the liquid phase and quickly diffused inside the concrete bulk.

Oral presentation

Fission product chemistry database ECUME

Imoto, Jumpei; Miwa, Shuhei; Miyahara, Naoya; Nakajima, Kunihisa; Nishioka, Shunichiro; Suzuki, Eriko; Horiguchi, Naoki; Liu, J.; Miradji, F.; Mohamad, A.; et al.

no journal, , 

Fission product (FP) chemistry database ECUME (Effective Chemistry database of fission products Under Multiphase rEaction) consists of three kinds of datasets: CRK (dataset for Chemical Reaction Kinetics), EM (Elemental Model set) and TD (ThermoDynamic dataset). The present ECUME is equipped with the CRK for the reaction of Cs-I-B-Mo-O-H system in gas phase, the EM for the Cs chemical reaction with stainless steel (SS) (Cs chemisorption onto SS) and the TD for CsBO$$_{2}$$ vapor species and solid Cs$$_{2}$$Si$$_{4}$$O$$_{9}$$ and CsFeSiO$$_{4}$$. The Cs chemisorption behavior model has successfully reproduced the effects of CsOH vapor concentration in gas phase and Si content in SS on the Cs chemisorption behavior which were not able to be considered by the existing model. The ECUME are expected to contribute to more accurate evaluation of FP distribution in Fukushima Daiichi Nuclear Power Station.

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