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Journal Articles

Effect of decay heat on pyrochemical reprocessing of minor actinide transmutation nitride fuels

Hayashi, Hirokazu; Tsubata, Yasuhiro; Sato, Takumi

Nihon Genshiryoku Gakkai Wabun Rombunshi (Internet), 22(3), p.97 - 107, 2023/08

The Japan Atomic Energy Agency has chosen nitride fuel as the first candidate for the transmutation of long-lived minor actinides (MA) using accelerator-driven systems (ADS). The pyrochemical method has been considered for reprocessing spent MA nitride fuels, because their decay heat should be very large for aqueous reprocessing. This study was conducted to investigate the effect of decay heat on the pyrochemical reprocessing of MA nitride fuels. On the basis of the estimated decay heats and the temperature limits of the materials that are to be handled in pyrochemical reprocessing, quantities adequate for handling in argon gas atmosphere were evaluated. From these considerations, we proposed that an electrorefiner with a diameter of 26 cm comprising 12 cadmium (Cd) cathodes with a diameter of 4 cm is suitable. On the basis of the size of the electrorefiner, the number necessary to reprocess spent MA fuels from 1 ADS in 200 days was evaluated to be 25. Furthermore, the amount of Cd-actinides (An) alloy to produce An nitrides by the nitridation-distillation combined reaction process was proposed to be about one-quarter that of Cd-An cathode material. The evaluated sizes and required numbers of equipment support the feasibility of pyrochemical reprocessing for MA nitride fuels.

Journal Articles

ORIGEN and ORIGEN-S libraries produced from JENDL-5

Konno, Chikara; Kochiyama, Mami; Hayashi, Hirokazu

Proceedings of 30th International Conference on Nuclear Engineering (ICONE30) (Internet), 9 Pages, 2023/05

JENDL-5 released in 2021 includes enough cross section data for neutron activation calculations. Thus we have produced ORIGEN and ORIGEN-S libraries from JENDL 5. We also produced the similar libraries from JENDL/AD-2017 for comparison. Analyses of the JPDR decommissioning data with these libraries demonstrated that the libraries had no problem.

Journal Articles

Formation of MPd$$_{3+x}$$ (M = Gd, Np) by the reaction of MN with Pd and chlorination of MPd$$_{3+x}$$ using cadmium chloride

Hayashi, Hirokazu; Shibata, Hiroki; Sato, Takumi; Otobe, Haruyoshi

Journal of Radioanalytical and Nuclear Chemistry, 332(2), p.503 - 510, 2023/02

 Times Cited Count:0 Percentile:0.01(Chemistry, Analytical)

The formation of MPd$$_{3+x}$$ (M = Gd, Np) by the reaction of MN with Pd at 1323 K in Ar gas flow was observed. Cubic AuCu$$_3$$-type GdPd$$_{3.3}$$ (${it a}$ = 0.4081 $$pm$$ 0.0001 nm) and NpPd$$_3$$ (${it a}$ = 0.4081 $$pm$$ 0.0001 nm) were identified, respectively. The product obtained from the reaction of NpN with Pd contained additional phases including the hexagonal TiNi$$_3$$-type NpPd$$_3$$. Chlorination of the MPd$$_{3+x}$$ (M = Gd, Np) samples was accomplished by the solid-state reaction using cadmium chloride at 673 K in a dynamic vacuum. Pd-rich solid solution phase saturated with Cd and an intermetallic compound PdCd were obtained as by-products of MCl$$_3$$ formation.

Journal Articles

Measurement of density and viscosity for molten salts

Sato, Rika*; Nishi, Tsuyoshi*; Ota, Hiromichi*; Hayashi, Hirokazu; Sugawara, Takanori; Nishihara, Kenji

Dai-43-Kai Nihon Netsu Bussei Shimpojiumu Koen Rombunshu (CD-ROM), 3 Pages, 2022/10

no abstracts in English

Journal Articles

SCALE6.2 ORIGEN library produced from JENDL/AD-2017

Konno, Chikara; Kochiyama, Mami; Hayashi, Hirokazu

JAEA-Conf 2021-001, p.132 - 137, 2022/03

A SCALE6.2 ORIGEN library was produced with the AMPX-6 code from JENDL Activation Cross Section File for Nuclear Decommissioning 2017 (JENDL/AD-2017). For validation of the libraries, JPDR activation calculation was performed with ORIGEN and the libraries, which demonstrated the library had no problem.

Journal Articles

Electrochemical recovery of Zr and Cd from molten chloride salts for reprocessing of used nitride fuels

Murakami, Tsuyoshi*; Hayashi, Hirokazu

Journal of Nuclear Materials, 558, p.153330_1 - 153330_7, 2022/01

 Times Cited Count:0 Percentile:0.01(Materials Science, Multidisciplinary)

Excess amounts of dissolution agents, CdCl$$_2$$ and ZrCl$$_4$$, are required to dissolve transuranium (TRU: Pu and minor actinides) nitrides into LiCl-KCl melts at the chemical dissolution step, which is the first step in the reprocessing of used nitride fuels. We propose an electrochemical process where the remaining Zr and Cd are recovered from the melts to be recycled as dissolution agents for the chemical dissolution step, leaving TRU in the melts. Since the initial concentration ratio of CdCl$$_2$$/ZrCl$$_4$$ remaining in the melts would depend on the condition of the chemical dissolution step and would vary during the proposed electrochemical recovery process, electrochemical behaviors of Zr and Cd were investigated in LiCl-KCl melts with various concentration ratios of CdCl$$_2$$/ZrCl$$_4$$ at 723 K to confirm the basic feasibility of the proposed process. Potentiostatic electrolysis was performed using a liquid Cd cathode at -1.05 V (vs. Ag/AgCl), which was a more positive potential than the redox potentials of TRU on the liquid Cd electrode. The obtained results showed that the current efficiency for recovering Zr and Cd from the melts was as high as 100% regardless of the CdCl$$_2$$/ZrCl$$_4$$ concentration ratio in the melts.

Journal Articles

Antimony from brake dust to the combined sewer collection system via road effluent under rainy conditions

Ozaki, Hirokazu*; Yoshimura, Kazuya; Asaoka, Yoshihiro*; Hayashi, Seiji*

Environmental Monitoring and Assessment, 193(6), p.369_1 - 369_9, 2021/06

 Times Cited Count:6 Percentile:41.49(Environmental Sciences)

JAEA Reports

Development of module for ADS nitride fuel performance analysis

Shibata, Hiroki; Saito, Hiroaki; Hayashi, Hirokazu; Takano, Masahide

JAEA-Data/Code 2019-023, 138 Pages, 2020/03

JAEA-Data-Code-2019-023.pdf:6.99MB

Transmutation of minor actinides in the form of nitride fuel by the accelerator driven system has been developed to reduce the radiotoxicity and volume in the radioactive wastes. Nitride fuel behavior under irradiation condition is necessary for its design and development. Nitride fuel performance analysis module based on light water reactor fuel performance code, FEMAXI-7, was developed by introducing fundamental properties of nitride pellet, 9Cr-1Mo ferrite cladding, and Pi-Bi coolant. As a result of test analysis with this module, we have understood that the nitride fuel shows excellent behavior under irradiation due to its high thermal conductivity. We found that, however, it may be a main concern that fuel cladding integrity is maintained during irradiation in which pellet-cladding mechanical interaction is increased by He gas release, low creep rate of nitride pellet at low temperatures, and high creep rate of cladding above 873 K.

Journal Articles

Material balance evaluation of pyroprocessing for minor actinide transmutation nitride fuel

Tateno, Haruka; Sato, Takumi; Tsubata, Yasuhiro; Hayashi, Hirokazu

Journal of Nuclear Science and Technology, 57(3), p.224 - 235, 2020/03

 Times Cited Count:6 Percentile:55.67(Nuclear Science & Technology)

Fuel cycle technology for the transmutation of long-lived minor actinides (MAs) using an accelerator-driven system has been developed using the double-strata fuel cycle concept. A mononitride solid solution of MAs and Pu diluted with ZrN is a prime fuel candidate for the accelerator-driven transmutation of MAs. Pyro-reprocessing is suitable for recycling the residual MAs in irradiated nitride fuel with high radiation doses and decay heat. Spent nitride fuel is anodically dissolved, and the actinides are recovered simultaneously into a liquid cadmium cathode via molten salt electrorefining. The process should be designed to achieve the target recovery yield of MAs and the acceptable impurity level of rare earths in the recovered material. We evaluated the material balance during the pyro-reprocessing of spent nitride fuel to gain important insight on the design process. We examined the effects of changing processing conditions on material flow and quantity of waste.

JAEA Reports

Study on the basic system of the common non-destructive radioactivity measuring equipment for disposal of radioactive wastes generated from research, industrial and medical facilities

Izumo, Sari; Hayashi, Hirokazu; Nakata, Hisakazu; Amazawa, Hiroya; Motoyama, Mitsushi*; Sakai, Akihiro

JAEA-Technology 2018-018, 39 Pages, 2019/03

JAEA-Technology-2018-018.pdf:2.8MB

JAEA has planed the near surface disposal of LLW generated from research, industrial, and medical facilities. Maximum radioactivity concentration of each waste and total radioactivity of disposed wastes are needed to be less than the permitted values in the license of disposal facility. Thus, it is important not to evaluate the radioactivity of each waste in unduly conservative ways so as to dispose of the total amount of the waste that is originally planned. Accordingly, the detection limit is required to be as low as the clearance level for the very low level radioactive waste planned to be disposed of trench-type. In this report, the feasibility of the non-destructive assay method is studied by model calculations for gamma emitters. It is confirmed that the detection limit less than the clearance level can be achieved as regards the box type metal container that is difficult to measure. This report summarizes the requirements for the non-destructive measuring equipment.

Journal Articles

Dissolution and chemical analysis of Zr-based lanthanide nitrides

Hayashi, Hirokazu; Chiba, Rikiya*

Progress in Nuclear Science and Technology (Internet), 5, p.196 - 199, 2018/11

Uranium-free nitride fuel has been chosen as the first candidate for transmutation of long-lived minor actinides (MA: Np, Am, Cm) using sub-critical accelerator-driven system (ADS) under the double strata fuel cycle concept by Japan Atomic Energy Agency (JAEA). Dissolution behavior of ZrN-based nitrides in nitric acid is examined using lanthanides as surrogate materials of TRU elements. Chemical analysis of the ZrN-based lanthanide nitrides dissolved in nitric acid is also carried out.

JAEA Reports

Study on the evaluation methodology of the radioactivity concentration in low-level radioactive wastes generated from JRR-2 & JRR-3

Hayashi, Hirokazu; Izumo, Sari; Nakata, Hisakazu; Amazawa, Hiroya; Sakai, Akihiro

JAEA-Technology 2018-001, 66 Pages, 2018/06

JAEA-Technology-2018-001.pdf:4.12MB
JAEA-Technology-2018-001(errata).pdf:0.54MB

It is necessary to establish evaluation methodology of radioactivity concentrations of each radionuclide in waste packages for operation of the Near-surface Trench disposal and Sub-surface Pit disposal facility in near future, which has been preparing for low-level radioactive wastes generated from research facilities in JAEA. The radionuclides containing in waste packages generated from both JRR-2 and JRR-3, which are H-3, C-14, Cl-36, Co-60, Ni-63, Sr-90, Nb-94, Tc-99, Ag-108m, I-129, Cs-137, Eu-152, Eu-154, U-234, U-238, Pu-239+240, Pu-238+Am-241, Cm-243+244, were evaluated their density based on radiochemical analysis data, and the Evaluation Methodology of the Radioactivity Concentration such as Scaling Factor method and mean activity concentration method was studied in this report.

JAEA Reports

Waste acceptance criteria for waste packages destined for near surface disposal containing radioactive waste from research, industrial and medical facilities; Study on a method that fills voidage in waste package with sandy soil

Nakata, Hisakazu; Hayashi, Hirokazu; Amazawa, Hiroya; Sakai, Akihiro

JAEA-Technology 2017-031, 41 Pages, 2018/01

JAEA-Technology-2017-031.pdf:5.27MB

JAEA plans to install disposal facilities for radioactive waste arising from research institutes. It must meet the technical standards specified in the relevant rule. One technical standard is that the disposal facilities shall be performance so as not to be left with the voids after the backfilling with soil. Additionally, the rule also requires this radioactive waste be enclosed in a container in which no harmful voids remain. In order to contribute to the development of a method that adapts the disposal facilities to these technical standards, JAEA adopts a waste conditioning artifice that aims for reducing a quantity of voidage in each waste container by a vibration filling method using sandy soil, providing with average void ratios inside the disposal facilities being adequately controlled. In this reports, filling property tests are conducted in the light of filling sand characteristics, types of metal waste and vibration conditions.

Journal Articles

Research and development on pyrochemical treatment of spent nitride fuels for MA transmutation in JAEA

Hayashi, Hirokazu; Sato, Takumi; Shibata, Hiroki; Tsubata, Yasuhiro

NEA/NSC/R(2017)3, p.427 - 432, 2017/11

Transmutation of long-lived radioactive nuclides including minor actinides (MA: Np, Am, Cm) has been studied in Japan Atomic Energy Agency (JAEA). Pb-Bi cooled sub-critical accelerator-driven system (ADS) is regarded as one of the powerful tools for transmutation of MA under the double strata fuel cycle concept. Uranium-free MA-Pu nitride fuel was chosen as the first candidate for MA transmutation. Reprocessing of spent ADS fuel and reusing MA recovered from the spent ADS fuels is necessary to improve the transmutation ratio. A pyrochemical process has been proposed as the first candidate for reprocessing of the spent nitride fuel for MA transmutation, because this technique has some advantages over aqueous process, such as the resistance to radiation damage, which is an important issue for the fuels containing large amounts of highly radioactive MA, and feasibility for recovering expensive N-15 in the spent fuels to be reused. This paper overviews the current status of the technology development, including our recent study. Development of the anode suitable for electro-refining of nitride fuels and that of the apparatus for renitridation of the metals recovered in Cd cathode for 100g-Cd scale cold tests are main topics. Evaluation of the batch sizes of each process, which is necessary for estimating the scale of the engineering-apparatus, with considering the decay heat of MA and FP, will also be introduced.

Journal Articles

Technology development on reactor dismantling and investigation of contamination in FUGEN

Soejima, Goro; Iwai, Hiroki; Nakamura, Yasuyuki; Hayashi, Hirokazu; Kadowaki, Haruhiko; Mizui, Hiroyuki; Sano, Kazuya

Proceedings of 25th International Conference on Nuclear Engineering (ICONE-25) (CD-ROM), 5 Pages, 2017/07

no abstracts in English

Journal Articles

Development of the reasonable confirmation methods concerning radioactive wastes from research facilities

Hayashi, Hirokazu; Okada, Shota; Izumo, Sari; Hoshino, Yuzuru; Tsuji, Tomoyuki; Nakata, Hisakazu; Sakai, Akihiro; Amazawa, Hiroya; Sakamoto, Yoshiaki

Proceedings of 2017 International Congress on Advances in Nuclear Power Plants (ICAPP 2017) (CD-ROM), 7 Pages, 2017/04

A near surface disposal for low-level radioactive waste (LLW) generated from commercial nuclear power plants (NPP) is operating in Japan. However, the disposal of LLW from other nuclear facilities and radioisotope utilization facilities has not yet been implemented. Japan Atomic Energy Agency (JAEA) plans to implement the near surface disposal. In order to be disposed of these wastes, it must be confirmed by the regulator that each waste package (radioactive waste solidified with filling materials, such as cement, in a container by a regulated method is termed a waste package) conforms to technical standards that aim for safe disposal. JAEA has studied reasonable confirmation methods to demonstrate the conformity of the waste package to the technical standard as NPP operators have studied it. This report describes the outline of our activities focused on development of the confirmation method applicable to radioactive wastes from research facilities.

JAEA Reports

Evaluation of nuclides migration for trench-type disposal by a calculation method taking leaching into consideration

Totsuka, Masayoshi; Kurosawa, Ryohei*; Sakai, Akihiro; Nakata, Hisakazu; Hayashi, Hirokazu; Amazawa, Hiroya

JAEA-Technology 2017-001, 40 Pages, 2017/03

JAEA-Technology-2017-001.pdf:2.24MB

Japan Atomic Energy Agency is planning for the near surface disposal of low level radioactive wastes generated from research, industrial and medical facilities industry in Japan. This document provides the values of radioactivity concentrations equivalent to dose criterion for trench-type disposal. These values are derived based on the safety assessment for ground water scenarios by using a model which describes the release of radionuclides from wastes to a cover soil caused by elution. These concentrations are compared with the one calculated by a model that describes the nuclide release mechanisms as solid-liquid partitioning equilibrium. Additionally, the change in the concentrations is evaluated when the amount of water percolating into a disposal facility varies.

Journal Articles

Chlorination of UO$$_{2}$$ and (U,Zr)O$$_{2}$$ solid solution using MoCl$$_{5}$$

Sato, Takumi; Shibata, Hiroki; Hayashi, Hirokazu; Takano, Masahide; Kurata, Masaki

Journal of Nuclear Science and Technology, 52(10), p.1253 - 1258, 2015/10

 Times Cited Count:6 Percentile:45.92(Nuclear Science & Technology)

In order to explore the applicability of the chlorination by MoCl$$_{5}$$ as a potential pretreatment technique for waste treatment of fuel debris by pyrochemical methods, chlorination experiments of UO$$_{2}$$ and (U$$_{0.5}$$Zr$$_{0.5}$$)O$$_{2}$$ simulated fuel debris were carried out in two steps: the first one is a chlorination reaction by homogeneous heating, the second one is a volatilization of molybdenum by-product by heating under temperature gradient condition. Most of UO$$_{2}$$ and (U$$_{0.5}$$Zr$$_{0.5}$$)O$$_{2}$$ powder were converted to UCl$$_{4}$$ or UCl$$_{4}$$ and ZrCl$$_{4}$$ mixture at 573 K, respectively. In the case of (U$$_{0.5}$$Zr$$_{0.5}$$)O$$_{2}$$sintered particle, most of sample was converted to the chlorides because the products evaporated and be separated from sample surface at 773 K, while only the surface of the sample disk was converted to the chlorides at 573 and 673 K. Most of molybdenum by-product and ZrCl$$_{4}$$ were separated from UCl$$_{4}$$ by volatilization at 573 K.

Journal Articles

Current status and future plan of research and development on partitioning and transmutation based on double-strata concept in JAEA

Tsujimoto, Kazufumi; Sasa, Toshinobu; Maekawa, Fujio; Matsumura, Tatsuro; Hayashi, Hirokazu; Kurata, Masaki; Morita, Yasuji; Oigawa, Hiroyuki

Proceedings of 21st International Conference & Exhibition; Nuclear Fuel Cycle for a Low-Carbon Future (GLOBAL 2015) (USB Flash Drive), p.657 - 663, 2015/09

To continue the utilization of the nuclear fission energy, the management of the high-level radioactive waste is one of the most important issues to be solved. Partitioning and Transmutation technology of HLW is expected to be effective to mitigate the burden of the HLW disposal by reducing the radiological toxicity and heat generation. The Japan Atomic Energy Agency (JAEA) has been conducting the research and development on accelerator-driven subcritical system (ADS) as a dedicated system for the transmutation of long-lived radioactive nuclides. This paper overviews the recent progress and future R&D plan of the study on the ADS and related fuel cycle technology in JAEA.

Journal Articles

Development of nitride fuel cycle technology for transmutation of minor actinides

Hayashi, Hirokazu; Nishi, Tsuyoshi*; Sato, Takumi; Kurata, Masaki

Proceedings of 21st International Conference & Exhibition; Nuclear Fuel Cycle for a Low-Carbon Future (GLOBAL 2015) (USB Flash Drive), p.1811 - 1817, 2015/09

Transmutation of long-lived radioactive nuclides including minor actinides (MA: Np, Am, Cm) has been studied in Japan Atomic Energy Agency (JAEA). Accelerator-driven system (ADS) is regarded as one of the powerful tools for transmutation of MA under the double strata fuel cycle concept. Uranium-free nitride fuel was chosen as the first candidate fuel for MA transmutation using ADS. To improve the transmutation ratio of MA, reprocessing of spent fuel and reusing MA recovered from the spent fuels is necessary. Our target is to transmute 99% of MA arisen from commercial power reactor fuel cycle, with which the period until the radiotoxicity drops below that of natural uranium can be shorten from about 5000 years to about 300 years. A pyrochemical process has been proposed as the first candidate for reprocessing of the spent nitride fuel. This paper overviews the current status of the nitride fuel cycle technology. Our recent study on fuel fabrication, fuel property measurements, reprocessing of spent fuel, development of the property database of MA nitride fuel, and fuel behavior simulation code are introduced. Our research and development (R&D) plan based on the roadmap of the development is also introduced.

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