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JAEA Reports

Basic research on the stability of fuel debris including alloy phase (Contract research); FY2019 Nuclear Energy Science & Technology and Human Resource Development Project

Collaborative Laboratories for Advanced Decommissioning Science; Tohoku University*

JAEA-Review 2020-032, 97 Pages, 2021/01

JAEA-Review-2020-032.pdf:4.16MB

The Collaborative Laboratories for Advanced Decommissioning Science (CLADS), Japan Atomic Energy Agency (JAEA), had been conducting the Nuclear Energy Science & Technology and Human Resource Development Project (hereafter referred to "the Project") in FY2019. The Project aims to contribute to solving problems in the nuclear energy field represented by the decommissioning of the Fukushima Daiichi Nuclear Power Station, Tokyo Electric Power Company Holdings, Inc. (TEPCO). For this purpose, intelligence was collected from all over the world, and basic research and human resource development were promoted by closely integrating/collaborating knowledge and experiences in various fields beyond the barrier of conventional organizations and research fields. The sponsor of the Project was moved from the Ministry of Education, Culture, Sports, Science and Technology to JAEA since the newly adopted proposals in FY2018. On this occasion, JAEA constructed a new research system where JAEA-academia collaboration is reinforced and medium-to-long term research/development and human resource development contributing to the decommissioning are stably and consecutively implemented. Among the adopted proposals in FY2018, this report summarizes the research results of the "Basic Research on the Stability of Fuel Debris Including Alloy Phase" conducted in FY2019. In the present study, we focus on fuel debris consisting of oxide phase and alloy phase generated by the high-temperature chemical reaction between structure materials (SUS pipes, pressure vessels, etc.) and fuels (melted fuels, claddings components, etc.). We synthesize the simulated debris of UO$$_{2}$$-SUS system and UO$$_{2}$$-Zr(ZrO$$_{2}$$)-SUS system by high-temperature heat treatment, and measure their chemical property and dissolution behavior in water. Also, we will conduct research and development to spectroscopically analyze secular changes of oxide phase and alloy phase in the simulated debris.

Journal Articles

Experimental study on transport behavior of cesium iodide in the reactor coolant system under LWR severe accident conditions

Miyahara, Naoya; Miwa, Shuhei; Gou$"e$llo, M.*; Imoto, Jumpei; Horiguchi, Naoki; Sato, Isamu*; Osaka, Masahiko

Journal of Nuclear Science and Technology, 57(12), p.1287 - 1296, 2020/12

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

In order to clarify the cesium iodide (CsI) transport behavior with a focus on the mechanisms of gaseous iodine formation in the reactor coolant system of LWR under a severe accident condition, a reproductive experiment of CsI transport behavior was conducted using a facility equipped with a thermal gradient tube. Various analyses on deposits and airborne materials during transportation could elucidate two mechanisms for the gaseous iodine formation. One was the gaseous phase chemical reaction in Cs-I-O-H system at relatively high-temperature region, which led to gaseous iodine transport to the lower temperature region without any further changes in gas species due to the kinetics limitation effects. The other one was the chemical reactions related to condensed phase of CsI, namely those of CsI deposits on walls with surface of stainless steel to form Cs$$_{2}$$CrO$$_{4}$$ compound and CsI aerosol particles with steam, which were newly found in this study.

Journal Articles

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; Mohamad, B. A.; et al.

Mechanical Engineering Journal (Internet), 7(3), p.19-00537_1 - 19-00537_11, 2020/06

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$$_{2}$$ vapor species and solids of Cs$$_{2}$$Si$$_{4}$$O$$_{9}$$ and CsFeSiO$$_{4}$$ 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.

JAEA Reports

Basic research on the stability of fuel debris including alloy phase (Contract research); FY2018 Center of World Intelligence Project for Nuclear Science/Technology and Human Resource Development

Collaborative Laboratories for Advanced Decommissioning Science; Tohoku University*

JAEA-Review 2019-035, 61 Pages, 2020/03

JAEA-Review-2019-035.pdf:2.9MB

JAEA/CLADS, had been conducting the Center of World Intelligence Project for Nuclear Science/Technology and Human Resource Development (hereafter referred to "the Project") in FY2018. The Project aims to contribute to solving problems in nuclear energy field represented by the decommissioning of the Fukushima Daiichi Nuclear Power Station, Tokyo Electric Power Company Holdings, Inc. For this purpose, intelligence was collected from all over the world, and basic research and human resource development were promoted by closely integrating/collaborating knowledge and experiences in various fields beyond the barrier of conventional organizations and research fields. The sponsor of the Project was moved from the Ministry of Education, Culture, Sports, Science and Technology to JAEA since the newly adopted proposals in FY2018. On this occasion, JAEA constructed a new research system where JAEA-academia collaboration is reinforced and medium-to-long term research/development and human resource development contributing to the decommissioning are stably and consecutively implemented. Among the adopted proposals in FY2018, this report summarizes the research results of the "Basic Research on the Stability of Fuel Debris Including Alloy Phase". In the present study, we focus on fuel debris consisting of oxide phase and alloy phase generated by the high-temperature chemical reaction between structure materials (SUS pipes, pressure vessels, etc.) and fuels (melted fuels, claddings components, etc.). We synthesize the simulated debris of UO$$_{2}$$-SUS system and UO$$_{2}$$-Zr(ZrO$$_{2}$$)-SUS system by high-temperature heat treatment, and measure their chemical property and dissolution behavior in water. Also, we will conduct research and development to spectroscopically analyze secular changes of oxide phase and alloy phase in the simulated debris.

JAEA Reports

Fission product chemistry database ECUME version 1.1

Development Group for LWR Advanced Technology

JAEA-Data/Code 2019-017, 59 Pages, 2020/03

JAEA-Data-Code-2019-017.pdf:3.26MB
JAEA-Data-Code-2019-017-appendix(CD-ROM).zip:0.09MB

ECUME ($$underline{E}$$ffective $$underline{C}$$hemistry database of fission products $$underline{U}$$nder $$underline{M}$$ultiphase r$$underline{E}$$action) is the database for the analyses of FP chemistry which strongly affects all the FP behaviors in a severe accident (SA) of nuclear facility like LWR. ECUME consists of three kinds of datasets: CRK (dataset for $$underline{C}$$hemical $$underline{R}$$eaction $$underline{K}$$inetics), EM ($$underline{E}$$lemental $$underline{M}$$odel set) and TD ($$underline{T}$$hermo$$underline{D}$$ynamic dataset). The present version of ECUME is prepared especially for the more accurate evaluation of cesium and iodine distribution in a reactor and release amount into an environment which should be of crucial importance towards the decommissioning of Fukushima Daiichi Nuclear Power Station of Tokyo Electric Power Company Holdings (1F) and the enhancement of LWR safety after the 1F SA.

Journal Articles

Advances in fuel chemistry during a severe accident; Update after Fukushima Daiichi Nuclear Power Station (FDNPS) accident

Kurata, Masaki; Osaka, Masahiko; Jacquemain, D.*; Barrachin, M.*; Haste, T.*

Advances in Nuclear Fuel Chemistry, p.555 - 625, 2020/00

The importance of fuel chemistry has been revivaled since Fukushima-Daiichi Nuclear Power Station (FDNPS) accident. The inspection and analysis of damaged three units, which had been operated in March 11, 2011, showed large differences in the accident progression sequence for these units, because operators attempted to prevent or mitigate the accident progression of each unit by all means possible. Characteristics of fuel debris are considered to be largely influenced by the difference in the sequence and, hence, deviated from those predicted from prototypic accident scenarios, which had been mainly identified from the analysis of Three Mile Island-2 (TMI-2) accident and the following sim-tests. For the proper improvement of our knowledge on severe accident (SA), including non-prototypic conditions, one has to start improving the phenomenology of fuel/core degradation and fission product (FP) behavior. Advances in the chemistry is the most essential approach. The present review attempts to focus on the recent updates and remaining concerns after the FDNPS accident.

Journal Articles

Outline of the OECD/NEA/ARC-F Project

Nakatsuka, Toru; Maeda, Toshikatsu; Sugiyama, Tomoyuki; Maruyama, Yu

Proceedings of 18th International Topical Meeting on Nuclear Reactor Thermal Hydraulics (NURETH-18) (USB Flash Drive), p.1650 - 1656, 2019/08

The OECD/NEA is launching a new project named "Analysis of Information from Reactor Buildings and Containment Vessels of Fukushima Daiichi Nuclear Power Station (ARC-F)" Project. This project will serve as the successor to the precedent NEA project, "Benchmark Study of the Accident at the Fukushima Daiichi Nuclear Power Station (BSAF) Phase II" which investigated the accident scenarios, associated fission products behavior in the damaged units and source term to the environment. The ARC-F project comprises three tasks: Task 1: Refinement of analysis for accident scenarios and associated fission product transportation and dispersion; Task 2: Compilation and management of data and information; and Task 3: Discussion for future long-term project. Japan Atomic Energy Agency is the operating agent, responsible to lead all the tasks. Duration of the project is from January 2019 to December 2021 and the final report is planned to be published in 2022.

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

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:4 Percentile:13(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

Progress of neutron-capture cross-section measurements promoted by ImPACT project at ANNRI in MLF of J-PARC

Nakamura, Shoji; Kimura, Atsushi; Hales, B. P.; Iwamoto, Osamu; Shibahara, Yuji*; Uehara, Akihiro*; Fujii, Toshiyuki*

JAEA-Conf 2018-001, p.199 - 203, 2018/12

Study on cross-section measurements has been promoted for $$^{135}$$Cs among long-lived fission products in ImPACT Project. The feasibility study on $$^{79}$$Se sample preparation also has been conducted to measure its cross sections in future. During the feasibility study, we started the neutron-capture cross-section measurements of stable Se isotopes. This paper reports research progresses on preparation of a radioactive $$^{135}$$Cs sample, neutron irradiation experiments with the Cs sample, and cross-section measurements of stable Se isotopes.

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.

JAEA Reports

Comparison between HTFP code and minory changed FORNAX-A code

Aihara, Jun; Ueta, Shohei; Goto, Minoru; Inaba, Yoshitomo; Shibata, Taiju; Ohashi, Hirofumi

JAEA-Technology 2018-002, 70 Pages, 2018/06

JAEA-Technology-2018-002.pdf:1.46MB

HTFP code is code for calculation of additional release amount of fission product (FP) from fuel rod in high temperature gas-cooled reactor (HTGR) after stop of fission. Minory changed Fornax-A code also can calculate that. Therefore, release behavior of Cs calculated with HTFP code was compared with that calculated with minory modified FORNAX-A code in this report. Release constants of Cs evaluated with minory modified FORNAX-A code are rather different from default values for HTFP code.

Journal Articles

Influence of chemical speciation in reactor cooling system on pH of suppression pool during BWR severe accident

Shiotsu, Hiroyuki; Ishikawa, Jun; Sugiyama, Tomoyuki; Maruyama, Yu

Journal of Nuclear Science and Technology, 55(4), p.363 - 373, 2018/04

 Times Cited Count:1 Percentile:75.54(Nuclear Science & Technology)

Journal Articles

Research on neutron capture cross sections at J-PARC in ImPACT Project

Nakamura, Shoji; Kimura, Atsushi; Hales, B. P.; Iwamoto, Osamu; Tsubata, Yasuhiro; Matsumura, Tatsuro; Shibahara, Yuji*; Uehara, Akihiro*; Fujii, Toshiyuki*

JAEA-Conf 2017-001, p.15 - 22, 2018/01

Neutron nuclear data of long lived fission products (LLFPs) have been required as basic data for the technology of reduce environmental impact involved in high level radioactive wastes (HLW). The innovative large project called by "Impusing Paradigm Change through Disruptive Technologies Program: ImPACT" have been started from October, 2014. In the ImPACT project, some research groups of JAEA engaged in the Project No.2 (Nuclear Reaction Data Measurements), and have started measurements of neutron capture cross-section at J-PARC/MLF/ANNRI. In our research, we selected cesium-135 ($$^{135}$$Cs) nuclide (half life: 2.3$$times$$10$$^{6}$$ yr.) among LLFPs in the HLW, and decided to measure the neutron capture cross-sections of $$^{135}$$Cs. When measurement, the $$^{135}$$Cs sample might contained cecium-137 ($$^{137}$$Cs) as impurities because it's impossible to chemically separate each other. To measure the cross-sections of $$^{135}$$Cs, there should be also needed to know the cross-sections of $$^{137}$$Cs. In this work, sample maintenance also has been examined especially for selen-79 ($$^{79}$$Se) nuclide among LLFPs having difficulty in sample preparations. In this oral session, the outline of our research project will be presented together with a research motivation, situations of past reported data, total schedules, progress, future plans, and some of high light data for neutron capture cross-section measurements.

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

Bayesian optimization analysis of containment-venting operation in a Boiling Water Reactor severe accident

Zheng, X.; Ishikawa, Jun; Sugiyama, Tomoyuki; Maruyama, Yu

Nuclear Engineering and Technology, 49(2), p.434 - 441, 2017/03

 Times Cited Count:1 Percentile:80.48(Nuclear Science & Technology)

Journal Articles

Experimental investigation of the influence of Mo contained in stainless steel on Cs chemisorption behavior

Di Lemma, F. G.; Nakajima, Kunihisa; Yamashita, Shinichiro; Osaka, Masahiko

Journal of Nuclear Materials, 484, p.174 - 182, 2017/02

 Times Cited Count:13 Percentile:6.18(Materials Science, Multidisciplinary)

Chemisorption phenomena can affect fission products retention in the nuclear reactor vessel during a Severe Accident (SA). This paper will describe the influence of molybdenum contained in type 316 stainless steel (SS) on Cs chemisorption. Our experiments showed the formation of Cs-Mo compounds in addition to CsFeSiO$$_{4}$$, observed previously on SS304. The results of high temperature stability tests on the deposits are also presented. These tests aimed at simulating the revaporization of FP from structural materials during a SA. From our results, it can be inferred that Cs-Mo deposits may revaporize, contributing as a delayed source to the radioactive release.

JAEA Reports

Results and progress of fundamental research on fission product chemistry; Progress report in 2015

Osaka, Masahiko; Miwa, Shuhei; Nakajima, Kunihisa; Di Lemma, F. G.*; Suzuki, Chikashi; Miyahara, Naoya; Kobata, Masaaki; Okane, Tetsuo; Suzuki, Eriko

JAEA-Review 2016-026, 32 Pages, 2016/12

JAEA-Review-2016-026.pdf:6.18MB

A fundamental research program on fission product (FP) chemistry has started since 2012 for the purpose of establishment of a FP chemistry database in each region of LWR under severe accident and improvement of FP chemical models based on the database. Research outputs are reflected as fundamental knowledge to both the research and development of decommissioning of Fukushima Daiichi Nuclear Power Station (1F) and 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, enlargement of a thermodynamic and thermophysical properties database for FP compounds and development of experimental and analytical techniques for the reproduction of FP behavior and for direct measurement methods of chemical form of FP compounds. In this report, the research results and progress for the year 2015 are described. The main accomplishment was the installation of a reproductive test facility for FP release and transport behavior. Moreover, basic knowledge about the Cs chemisorption behavior was also obtained. In addition to the four research items, a further research item is being considered for deeper interpretation of FP behavior by the analysis of samples outside of the 1F units.

Journal Articles

Bayesian optimization analysis of containment venting operation in a BWR severe accident

Zheng, X.; Ishikawa, Jun; Sugiyama, Tomoyuki; Maruyama, Yu

Proceedings of 13th Probabilistic Safety Assessment and Management Conference (PSAM-13) (USB Flash Drive), 10 Pages, 2016/10

JAEA Reports

Significance of international cooperative research on fission product behavior towards decommissioning of Fukushima Daiichi Nuclear Power Station; Review of the CLADS International Workshop

Research Team for Fission Product Behavior

JAEA-Review 2016-012, 17 Pages, 2016/07

JAEA-Review-2016-012.pdf:1.46MB

The severe accident (SA) of Fukushima Daiichi Nuclear Power Station (1F) has given rise to enlarged research needs for the improvement of the source term assessment. Fission Product (FP) related researches, however, have not been widely conducted in Japan for many years, thus a framework for such research is not so robust. The Collaborative Laboratories for Advanced Decommissioning Science (CLADS) workshop held in November 2015 was an important opportunity to gain the state of art knowledge on FP and to start discussion between worldwide experts on innovative solution for 1F issues. This report describes the outcomes of FP session conducted in the CLADS workshop. It was pointed out during the workshop that further analyses were needed to properly understand the phenomena that occurred in 1F. The establishment of a Japanese FP platform is here proposed to respond to 1F issues effectively as a means to coordinate the national research efforts and increase communication between worldwide stakeholders. The FPs studies conducted in this frame will provide important information for the decommissioning of 1F, and will be also of great help for the international community to progress the knowledge on FPs behavior. Finally their outcomes could contribute in establishing improved SA management measures.

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