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

https://doi.org/10.1299/mej.19-00537

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.

Boron chemistry during transportation in the high temperature region of a boiling water reactor under severe accident conditions

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

https://doi.org/10.1080/00223131.2019.1671913

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.

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.

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.

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, , 

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.

A Study of cesium chemisorption onto surface of stainless steel

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

no journal, , 

An experimental study has been conducted in order to construct a Cs chemisorption model. The model is reflected to an improvement of Cs distribution evaluation by severe accident analysis codes. Influencing factors on the chemisorption behaviors were investigated experimentally. It was found that temperature, atmosphere and Si contents in the stainless steel (SS) were the main influencing factors. Of note is the implication of revaporization of Cs chemisorbed compounds from the SS surface. It can be said from this result that the Cs chemisorption behaviors should be considered in relation to chemical properties of compounds formed.

Distribution measurement at microlevel of Cs chemisorbed compounds onto stainless steel under LWR severe accident

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.

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.

Development of long term FP behavior analysis method for TEPCO's Fukushima Daiichi Nuclear Power Plants

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.