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 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.

Development of evaluation method for aerosol particle deposition in a reactor building based on CFD

Horiguchi, Naoki; Miyahara, Naoya; Uesawa, Shinichiro; Yoshida, Hiroyuki; Osaka, Masahiko

Proceedings of 27th International Conference on Nuclear Engineering (ICONE-27) (Internet), 8 Pages, 2019/05

For source term evaluation from reactor buildings (RBs) in LWR severe accidents, we have launched to develop an evaluation method of FP aerosol particle deposition onto surfaces of internal structures in an RB based on computational fluid dynamics (CFD). This paper describes development of a CFD simulation tool as the base part of the evaluation method. A preliminary simulation for a representative RB under a representative flow condition was conducted to confirm the tool performance by roughly grasping the deposition behaviors of FP aerosol particle and decontamination factor (DF) in the RB. Calculation results showed that most of aerosol particles were deposited along with gas flow formed by the internal structures in the RB, demonstrating the advantageous feature of the present CFD tool. The DFs from 4 to 14 were obtained with increase of the particle diameters from 0.1 to 10 m as expected in terms of the particle movement equation.

Observation of aerosol particle behavior near gas-liquid interface

Uesawa, Shinichiro; Miyahara, Naoya; Horiguchi, Naoki; Yoshida, Hiroyuki; Osaka, Masahiko

Proceedings of 27th International Conference on Nuclear Engineering (ICONE-27) (Internet), 5 Pages, 2019/05

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 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.

Evaluation of electronic state of Cs-adsorbed clay minerals by NEXAFS analysis using DFT calculations

Suzuki, Chikashi; Yaita, Tsuyoshi; Suzuki, Shinichi; Pacold, J.*; Altman, A. B.*; Minasian, S. G.*; Tyliszczak, T.*; Shuk, D. K.*; Yoshida, Hiroyuki; Osaka, Masahiko

Journal of Physics and Chemistry of Solids, 127, p.169 - 177, 2019/04

https://doi.org/10.1016/j.jpcs.2018.11.011

A combined method of NEXAFS measurement and DFT-calculation was employed for Cs evaluation in clay minerals. The Cs M NEXAFS spectra of Cs halides were analyzed using the DFT-calculations, and were well reproduced by incorporating the core-hole strength. The Cs M NEXAFS spectrum of clay minerals was well-reproduced by the DFT-calculations including the major transitions and tail structures with the established method. The further evaluation of this spectrum by charge density suggests that these major transitions and the tail structures likely reflect bonding states and local environments around the Cs atoms. Comparison of electronic states of Cs in the clay mineral with those in the Cs halides by DFT-calculations has shown that the interaction between Cs and the nearest-neighbor atom is largest in the clay mineral, because the energy level of Cs-5s and 5p is closer to that of O-2s and 2p than the s and p orbitals of other alkali metal and alkali earth metal elements.

Synthesis and characterization of CeO-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

https://doi.org/10.3327/taesj.J17.025

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

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

https://doi.org/10.15669/pnst.5.168

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.

Release and transport behaviors of non-gamma-emitting fission products and actinides in steam and hydrogen atmospheres

Miwa, Shuhei; Ducros, G.*; Hanus, E.*; Bottomley, P. D. W.*; Van Winckel, S.*; Osaka, Masahiko

Nuclear Engineering and Design, 326, p.143 - 149, 2018/01

https://doi.org/10.1016/j.nucengdes.2017.11.017

The release and transport behaviors of 13 non-gamma-emitting fission products (FPs) and actinides in steam and hydrogen atmospheres were investigated based on the chemical analysis of their deposits on the components of VERCORS test loops. The new findings were obtained; strontium release was significantly enhanced in hydrogen atmosphere and a part of released strontium was transported towards the lower temperature region, uranium release was enhanced in steam atmosphere but most of released uranium deposited at high temperature region.

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

https://doi.org/10.1016/j.egypro.2017.08.092

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 CsMoO 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.

Thermodynamic study of gaseous CsBO by Knudsen effusion mass spectrometry

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

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

https://doi.org/10.1016/j.jnucmat.2017.05.001

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, by thermodynamic equilibrium calculation considering reaction with boron. But accuracy of the thermodynamic data of gaseous metaborate, CsBO(g), has been judged as poor quality. Thus, Knudsen effusion mass spectrometric measurement of CsBO was carried out to obtain reliable thermodynamic data. The evaluated values of standard enthalpy of formation of CsBO(g), H(CsBO,g), by the 2nd and 3rd law treatments are -700.710.7 kJ/mol and -697.010.6 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.