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Journal Articles

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

 Times Cited Count:0 Percentile:100(Nuclear Science & Technology)

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)$$_{2}$$BO$$_{3}$$. 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.

Journal Articles

Cesium chemisorbed species onto stainless steel surfaces; An Atomistic scale study

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

Journal of Physics and Chemistry of Solids, 136, p.109168_1 - 109168_9, 2020/01

 Times Cited Count:0 Percentile:100(Chemistry, Multidisciplinary)

Journal Articles

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

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.

Journal Articles

An Experimental investigation of influencing chemical factors on Cs-chemisorption behavior onto stainless steel

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

Journal of Nuclear Science and Technology, 56(11), p.988 - 995, 2019/11

 Times Cited Count:1 Percentile:34.57(Nuclear Science & Technology)

In order to contribute to improvement of Cs chemisorption model used in severe accident analysis codes, the influence of chemical factors (temperature, atmosphere, concentration of affecting chemical elements etc.) on the Cs chemisorption behaviour onto stainless steel was investigated experimentally. It was found that the surface reaction rate constant used in the current Cs-chemisorption model was influenced by not only temperature, as already known, but also atmosphere, cesium hydroxide (CsOH) concentration in the gas phase and silicon content in SS304. Such chemical factors should be considered for the construction of the improved Cs-chemisorption model. Another important finding is that the chemisorption behavior at lower temperatures, around 873 K, could differ from those above 1073 K. Namely, Cs-Fe-O compounds would form as the main Cs-chemisorbed compounds at 873 K while Cs-Si-Fe-O compounds at more than 1073 K.

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

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 $$mu$$m as expected in terms of the particle movement equation.

Journal Articles

Expansion of high temperature creep test data for failure evaluation of BWR lower head in a severe accident

Yamaguchi, Yoshihito; Katsuyama, Jinya; Kaji, Yoshiyuki; Osaka, Masahiko; Li, Y.

Proceedings of 27th International Conference on Nuclear Engineering (ICONE-27) (Internet), 7 Pages, 2019/05

After the Fukushima Daiichi (1F) Nuclear Power Plant accident, we have been developing a prediction method for rupture time and location considering creep damage mechanisms using finite element analysis for early completion of the decommissioning of nuclear power plants in 1F. We have also been obtaining material properties at high temperature near the melting point which are not provided in existing database or literature for the finite element analysis. In this study, we performed uni-axial tensile and creep tests for low alloy steel, Ni-based alloy steel and stainless steels and expanded existing database of material properties. Especially, creep data with longer rupture time at high temperature were obtained by a creep test equipment with a noncontact measurement system. To improve the accuracy of failure evaluation under severe accident conditions, we determined parameters of creep constitutive law based on the expanded database.

Journal Articles

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

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

Experimental investigation on boron oxidative vaporization processes from zirconium-boron and iron-boron alloys in a high temperature steam atmosphere

Imoto, Jumpei; Miwa, Shuhei; Osaka, Masahiko

Proceedings of International Topical Workshop on Fukushima Decommissioning Research (FDR 2019) (Internet), 4 Pages, 2019/05

Boron (B) oxidative vaporization processes from the representative alloys of Fe-B and Zr-B formed in the mixed melt of BWR control material boron carbide, stainless steel and Zircaloy were experimentally investigated toward the construction of B release model under severe accident. The results show that B oxidative vaporization from ZrB$$_{2}$$ would proceed in the formation of ZrO$$_{2}$$ and B$$_{2}$$O$$_{3}$$ due to the oxidation of ZrB$$_{2}$$, followed by the formation of volatile H-B-O vapor species by the reaction of B$$_{2}$$O$$_{3}$$ with steam. On the other hand, for Fe$$_{2}$$B and FeB, the B oxidative vaporization processes would proceed in the same manner. Complex Fe-B-O compounds formation in addition to amorphous B$$_{2}$$O$$_{3}$$ were observed by the oxidation of Fe$$_{2}$$B and FeB. Then the B vaporization would occur by the formation of volatile H-B-O compound by the reaction of B$$_{2}$$O$$_{3}$$, which were derived from both oxidation of Fe$$_{2}$$B and decomposition of Fe-B-O compounds.

Journal Articles

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

 Times Cited Count:1 Percentile:100(Chemistry, Multidisciplinary)

A combined method of NEXAFS measurement and DFT-calculation was employed for Cs evaluation in clay minerals. The Cs M$$_{4,5}$$ NEXAFS spectra of Cs halides were analyzed using the DFT-calculations, and were well reproduced by incorporating the core-hole strength. The Cs M$$_{4,5}$$ 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.

Journal Articles

Modelling of cesium chemisorption under nuclear power plant severe accident conditions

Miradji, F.; Suzuki, Chikashi; Nishioka, Shunichiro; Suzuki, Eriko; Nakajima, Kunihisa; Osaka, Masahiko; Barrachin, M.*; Do, T. M. D.*; Murakami, Kenta*; Suzuki, Masahide*

Proceedings of 9th Conference on Severe Accident Research (ERMSAR 2019) (Internet), 21 Pages, 2019/03

Journal Articles

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

 Times Cited Count:2 Percentile:14.12(Nuclear Science & Technology)

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.

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:4 Percentile:17.31(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

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

 Times Cited Count:0 Percentile:100(Nuclear Science & Technology)

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.

330 (Records 1-20 displayed on this page)