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(3-4), 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.

Seven-year temporal variation of cesium-137 discharge inventory from the port of Fukushima Dai-ichi Nuclear Power Plant; Continuous monthly estimation of cesium-137 discharge in the period from April 2011 to June 2018

Machida, Masahiko; Yamada, Susumu; Iwata, Ayako; Otosaka, Shigeyoshi; Kobayashi, Takuya; Watanabe, Masahisa; Funasaka, Hideyuki; Morita, Takami*

Nippon Genshiryoku Gakkai Wabun Rombunshi, 18(4), p.226 - 236, 2019/12

https://doi.org/10.3327/taesj.J18.030

After direct discharges of highly-contaminated water from Unit 2 and 3 in Fukushima Daiichi Nuclear Power Plant (1F) in April to May 2011, Kanda suggested that relatively small run-off of radionuclides from 1F port into Fukushima coastal region has subsequently continued by using his estimation scheme. However, the estimation period was limited until September 2012, and there has been no report on the issue since the work. Therefore, this paper focuses on discharge inventory from 1F port until June 2018. In the missing period, the central government and Tokyo Electric Power Company Holdings have done continuous efforts to stop the discharge, and consequently sea water concentration inside 1F port has diminished gradually. We show monthly discharge inventory of Cs-137 until June 2018 by two schemes, i.e., Kanda's scheme partially improved by authors and more sophisticated one using Voronoi tessellation reflecting the increment of the number of monitoring points inside 1F port. The results show that the former always presents overestimated results compared to the latter but the ratio of former to latter is less than one order. Based on these results, we evaluate impact of discharge inventory from 1F port into the coastal area and radiation does via fish digestion.

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

https://doi.org/10.1299/jsmeicone.2019.27.1993

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.

Chemical reaction kinetics dataset of Cs-I-B-Mo-O-H system for evaluation of fission product chemistry under LWR severe accident conditions

Miyahara, Naoya; Miwa, Shuhei; Horiguchi, Naoki; Sato, Isamu*; Osaka, Masahiko

Journal of Nuclear Science and Technology, 56(2), p.228 - 240, 2019/02

https://doi.org/10.1080/00223131.2018.1544939

In order to improve LWR source term under severe accident conditions, the first version of a fission product (FP) chemistry database named "ECUME" was developed. The ECUME is intended to include major chemical reactions and their effective kinetic constants for representative SA sequences. It is expected that the ECUME can serve as a fundamental basis from which FP chemical models in the SA analysis codes can be elaborated. The implemented chemical reactions in the first version were those for representative gas species in Cs-I-B-Mo-O-H system. The chemical reaction kinetic constants were evaluated from either literature data or calculated values using ab-initio calculations. The sample chemical reaction calculation using the presently constructed dataset showed meaningful kinetics effects at 1000 K. Comparison of the chemical equilibrium compositions by using the dataset with those by chemical equilibrium calculations has shown rather good consistency for the representative Cs-I-B-Mo-O-H species. From these results, it was concluded that the present dataset should be useful to evaluate FP chemistry in Cs-I-B-Mo-O-H system under LWA SA conditions.

Effect of atmosphere on the vaporization behavior of CsFeSiO

Suzuki, Eriko; Nakajima, Kunihisa; Osaka, Masahiko

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

https://doi.org/10.15669/pnst.5.165

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

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

https://doi.org/10.1016/j.jnucmat.2017.10.035

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 is a dominant Cs products in the case of low Si content, mainly formed, while CsSiO and CsSiO are formed in addition to CsFeSiO 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.