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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.

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

 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

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

 Percentile:100(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:1 Percentile:38.14(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

 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.

Journal Articles

Challenges for enhancing Fukushima environmental resilience, 7; Behavior and abundance of radiocesium in the coastal area off Fukushima

Otosaka, Shigeyoshi; Kobayashi, Takuya; Machida, Masahiko

Nippon Genshiryoku Gakkai-Shi, 59(11), p.659 - 663, 2017/11

It is estimated that about 70% of radiocesium released to the environment by the Fukushima Daiichi nuclear accident was carried to the ocean. In addition to monitoring surveys by the government, oceanographic research by many institutions has revealed the distribution and behavior of the accident-derived radiocesium in the ocean. Numerical simulations are efficiently used in such oceanographic investigations, and further improvements are being made based on findings newly obtained after the accident. In this paper, we review the abundance and behavior of radiocesium in the coastal area of Fukushima, deepen the scientific understanding of the current situation of environmental restoration, and explain the issues to be addressed in the future.

Journal Articles

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

 Percentile:100

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 Cs$$_{2}$$MoO$$_{4}$$ 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.

Journal Articles

Development of experimental and analytical technologies for fission product chemistry under LWR severe accident condition

Miyahara, Naoya; Miwa, Shuhei; Nakajima, Kunihisa; Osaka, Masahiko

Proceedings of 2017 Water Reactor Fuel Performance Meeting (WRFPM 2017) (USB Flash Drive), 9 Pages, 2017/09

This paper presents the development of a reproductive experimental setup for FP release and transport and an analysis tool considering chemical reaction kinetics for the construction of the FP chemistry database. The performance test of the reproductive experimental setup TeRRa using CsI compounds show that TeRRa can reproduce well a FP chemistry-related behavior such as aerosol formation, growth and deposition behavior. An analytical tool has been developed based on the commercial ANSYS-FLUENT code. Some additional models was added to evaluate detailed FP chemistry during release and transport in this study. A test analysis simulating the CsI heating test in steam atmosphere was carried out to demonstrate the performance of the improved code. The result shows the appropriateness of the additional models.

Journal Articles

Thermodynamic study of gaseous CsBO$$_{2}$$ by Knudsen effusion mass spectrometry

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

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

 Times Cited Count:1 Percentile:64.68(Materials Science, Multidisciplinary)

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$$_{2}$$, by thermodynamic equilibrium calculation considering reaction with boron. But accuracy of the thermodynamic data of gaseous metaborate, CsBO$$_{2}$$(g), has been judged as poor quality. Thus, Knudsen effusion mass spectrometric measurement of CsBO$$_{2}$$ was carried out to obtain reliable thermodynamic data. The evaluated values of standard enthalpy of formation of CsBO$$_{2}$$(g), $$Delta$$$$_{f}$$H$$^{circ}$$$$_{298}$$(CsBO$$_{2}$$,g), by the 2nd and 3rd law treatments are -700.7$$pm$$10.7 kJ/mol and -697.0$$pm$$10.6 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.

Journal Articles

Creep damage evaluations for BWR lower head in severe accident

Katsuyama, Jinya; Yamaguchi, Yoshihito; Nemoto, Yoshiyuki; Kaji, Yoshiyuki; Osaka, Masahiko

Transactions of 24th International Conference on Structural Mechanics in Reactor Technology (SMiRT-24) (USB Flash Drive), 11 Pages, 2017/08

It is difficult to assess rupture behavior of the lower head of reactor pressure vessel in boiling-water-type nuclear power plants due to severe accident like Fukushima Daiichi because Boiling Water Reactor (BWR) lower heads have geometrically complicated structure with a lot of penetrations. Therefore, we have been developing an analysis method to predict time and location of RPV lower head rupture of BWRs considering creep damage mechanisms based on coupled analysis of three-dimensional Thermal-Hydraulics (TH) and thermal-elastic-plastic-creep analyses. In this study, we performed creep damage evaluations to investigate the effects of the debris depth and heat generation locations on failure behavior of lower head. From the analysis results, we discussed the outflow paths of the relocated molten core to the containment, and it was concluded that failure regions of BWR lower head are only the control rod guide tubes or stub tubes under simulated conditions.

312 (Records 1-20 displayed on this page)