Structure, stability, and actinide leaching of simulated nuclear fuel debris synthesized from UO, Zr, and stainless-steel

Kirishima, Akira*; Akiyama, Daisuke*; Kumagai, Yuta; Kusaka, Ryoji; Nakada, Masami; Watanabe, Masayuki; Sasaki, Takayuki*; Sato, Nobuaki*

Journal of Nuclear Materials, 567, p.153842_1 - 153842_15, 2022/08

https://doi.org/10.1016/j.jnucmat.2022.153842

To understand the chemical structure and stability of nuclear fuel debris consisting of UO, Zr, and Stainless Steel (SUS) generated by the Fukushima Daiichi Nuclear Power Plant accident in Japan in 2011, simulated debris of the UO-SUS-Zr system and other fundamental component systems were synthesized and characterized. The simulated debris were synthesized by heat treatment for 1 to 12 h at 1600C, in inert (Ar) or oxidative (Ar + 2% O) atmospheres. Np and Am tracers were doped for the leaching tests of these elements and U from the simulated debris. The characterization of the simulated debris was conducted by XRD, SEM-EDX, Raman spectroscopy, and Mssbauer spectroscopy, which provided the major uranium phase of the UO -SUS-Zr debris was the solid solution of UO (s.s.) with Zr(IV) and Fe(II) regardless of the treatment atmosphere. The long-term immersion test of the simulated debris in pure water and that in seawater revealed the macro scale crystal structure of the simulated debris was chemically very stable in the wet condition for a year or more. Furthermore, the leaching test results showed that the actinide leaching ratios of U, Np, Am from the UO-SUS-Zr debris were very limited and less than 0.08 % for all the experiments in this study.

Basic research on the stability of fuel debris including alloy phase (Contract research); FY2020 Nuclear Energy Science & Technology and Human Resource Development Project

Collaborative Laboratories for Advanced Decommissioning Science; Tohoku University*

JAEA-Review 2022-009, 73 Pages, 2022/06

JAEA-Review-2022-009.pdf:2.08MB

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 FY2020. 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 from FY2018 to FY2021 (this contract was extended to FY2021). Since the final year of this proposal was FY2021, the results for four fiscal years were summarized. The present study 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-SUS system and UO-Zr(ZrO)-SUS system by high-temperature heat treatment, and measure their chemical property and dissolution behavior in water. Also, we will conduct

Study on degradation of fuel debris by combined effects of radiological, chemical, and biological functions (Contract research); FY2020 Nuclear Energy Science & Technology and Human Resource Development Project

Collaborative Laboratories for Advanced Decommissioning Science; Tokyo Institute of Technology*

JAEA-Review 2022-005, 93 Pages, 2022/06

JAEA-Review-2022-005.pdf:6.95MB

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 FY2020. 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 FY2019, this report summarizes the research results of the "Study on degradation of fuel debris by combined effects of radiological, chemical, and biological functions" conducted in FY2020. In the project, radiochemists, nuclear chemists, nuclear physicists, material scientists, and environmental biologists are teamed to elucidate the mechanism of the degradation of fuel debris by combined effects of radiological, chemical, and biological functions. In fiscal year 2020, the members of the project team have conducted on the degradation of He ions irradiated simulated fuel debris, complex formation of tetravalent elements, uranium (VI) detection in microchannel, sorption of trivalent elements by iron bearing materials, and microbial degradation by model microorganisms and

Irradiation growth behavior and effect of hydrogen absorption of Zr-based cladding alloys for PWR

Kakiuchi, Kazuo; Amaya, Masaki; Udagawa, Yutaka

Annals of Nuclear Energy, 171, p.109004_1 - 109004_9, 2022/06

https://doi.org/10.1016/j.anucene.2022.109004

Development of an continuous air monitor for the measurement of highly radioactive alpha-emitting particulates (-aerosols) under high humidity environment

Tsubota, Yoichi; Honda, Fumiya; Tokonami, Shinji*; Tamakuma, Yuki*; Nakagawa, Takahiro; Ikeda, Atsushi

Nuclear Instruments and Methods in Physics Research A, 1030, p.166475_1 - 166475_7, 2022/05

https://doi.org/10.1016/j.nima.2022.166475

In the long-lasting decommissioning of the Fukushima Daiichi Nuclear Power Station (1F), the dismantling of nuclear fuel debris (NFD) remaining in the damaged reactors is an unavoidable but significant issue with many technical difficulties. The dismantling is presumed to involve mechanical cutting, generating significant concentrations of particulates containing -radionuclides (-aerosols) that pose significant health risk upon inhalation. In order to minimize the radiation exposure of workers with -aerosols during the dismantling/decommissioning process at 1F, it is essential to monitor the concentration of -aerosols at the point of initial generation, i.e. inside the primary containment vessels (PCV) of the damaged reactors. Toward this end, an monitoring system for -aerosols ( alpha air monitor: IAAM) was developed and its technical performance was investigated under the conditions expected for the actual environments at 1F. IAAM was confirmed to fulfill four technical requirements: (1) steady operation under high humidity, (2) operation without using filters, (3) capability of measuring a high counting rate of -radiation, and (4) selective measurement of -radiation even under high radiation background with /-rays. IAAM is capable of selectively measuring -aerosols with a concentration of 3.3 10 Bq/cm or higher without saturation under a high humid environment (100%-relative humidity) and under high background with /-radiation (up to 100 mSv/h of -radiation). These results demonstrate promising potential of IAAM to be utilized as a reliable monitoring system for -aerosols during the dismantling of NFD, as well as the whole long-lasting decommissioning of 1F.

Reactivity estimation based on the linear equation of characteristic time profile of power in subcritical quasi-steady state

Yamane, Yuichi

Journal of Nuclear Science and Technology, 14 Pages, 2022/04

https://doi.org/10.1080/00223131.2022.2053221

The reactivity was estimated from a time profile of neutron count rate or a simulated data in a quasi-steady state after sudden change of reactivity or external neutron source strength. The estimation was based on the equation of power in subcritical quasi-steady state. The purpose of the study is to develop the method of timely reactivity estimation from complicated time profile of neutron count rate. The developed method was applied to the data simulating neutron count rate created by using one-point kinetics code, AGNES, and Poisson-distributed random noise and to the transient subcritical experiment data measured by using TRACY. The result shows that the difference of the estimated and reference value was within about 5% or less for (simeq) -1.4 and -3.1 for the experimental data. It was also shown that the possibility of the reactivity estimation several ten seconds after the status change.

Advanced reactor experiments for sodium fast reactor fuels (ARES) project; Transient irradiation experiments for metallic and MOX fuels

Jensen, C. B.*; Wachs, D. M.*; Woolstenhulme, N. E.*; Ozawa, Takayuki; Hiroka, Shun; Kato, Masato

Proceedings of International Conference on Fast Reactors and Related Fuel Cycles; Sustainable Clean Energy for the Future (FR22) (Internet), 9 Pages, 2022/04

Development of rapid and sensitive radionuclide analysis method by simultaneous analysis of , , and X-rays (Contract research); FY2020 Nuclear Energy Science & Technology and Human Resource Development Project

Collaborative Laboratories for Advanced Decommissioning Science; Japan Chemical Analysis Center*

JAEA-Review 2021-060, 105 Pages, 2022/03

JAEA-Review-2021-060.pdf:4.59MB

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 FY2020. 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 FY2020, this report summarizes the research results of the "Development of rapid and sensitive radionuclide analysis method by simultaneous analysis of , , and X-rays" conducted in FY2020. The present study aims to enable rapid analysis of radionuclides in fuel debris and waste, and develops the measurement system such as multiple -ray detection method. We develop a spectral determination method (SDM method) for integrated analysis by constructing a spectral database for nuclides including -rays and X-rays by measurement using this system and radiation simulation calculation. This method enables simultaneous quantification of multiple nuclides and reduces the chemical separation process.

Development of dispersed phase tracking method for time-series 3-dimensional interface shape data

Horiguchi, Naoki; Yoshida, Hiroyuki; Yamamura, Sota*; Fujiwara, Kota*; Kaneko, Akiko*; Abe, Yutaka*

Proceedings of 19th International Topical Meeting on Nuclear Reactor Thermal Hydraulics (NURETH-19) (Internet), 14 Pages, 2022/03

Investigation of environment induced property change and cracking behavior in fuel debris (Contract research); FY2020 Nuclear Energy Science & Technology and Human Resource Development Project

Collaborative Laboratories for Advanced Decommissioning Science; The University of Tokyo*

JAEA-Review 2021-058, 75 Pages, 2022/02

JAEA-Review-2021-058.pdf:4.82MB

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 FY2020. 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 FY2020, this report summarizes the research results of the "Investigation of environment induced property change and cracking behavior in fuel debris" conducted in FY2020. The present study aims to investigate the environment induced property change and cracking behavior in fuel debris from the viewpoints of materials science. The research objective is cracking behavior in fuel debris which is presumed to be influenced by environment during long-term fuel debris processing period. The degradation models will be established to simulate the oxidation and hydrogenation processes possibly occurred at fuel debris. The evolution of phase constitution and the corresponding property change in the simulated fuel debris under various environmental conditions will be systematically