Development of an iron(II) complex exhibiting thermal- and photoinduced double proton-transfer-coupled spin transition in a short hydrogen bond

Nakanishi, Takumi*; Hori, Yuta*; Shigeta, Yasuteru*; Sato, Hiroyasu*; Kiyanagi, Ryoji; Munakata, Koji*; Ohara, Takashi; Okazawa, Atsushi*; Shimada, Rintaro*; Sakamoto, Akira*; et al.

Journal of the American Chemical Society, 145(35), p.19177 - 19181, 2023/08

https://doi.org/10.1021/jacs.3c06323

Observation of proton-transfer-coupled spin transition by single-crystal neutron-diffraction measurement

Nakanishi, Takumi*; Hori, Yuta*; Shigeta, Yasuteru*; Sato, Hiroyasu*; Wu, S.-Q.*; Kiyanagi, Ryoji; Munakata, Koji*; Ohara, Takashi; Sato, Osamu*

Physical Chemistry Chemical Physics, 25(17), p.12394 - 12400, 2023/05

https://doi.org/10.1039/D3CP00527E

Formation of MPd (M = Gd, Np) by the reaction of MN with Pd and chlorination of MPd using cadmium chloride

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

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

https://doi.org/10.1007/s10967-023-08760-4

The formation of MPd (M = Gd, Np) by the reaction of MN with Pd at 1323 K in Ar gas flow was observed. Cubic AuCu-type GdPd ( = 0.4081 0.0001 nm) and NpPd ( = 0.4081 0.0001 nm) were identified, respectively. The product obtained from the reaction of NpN with Pd contained additional phases including the hexagonal TiNi-type NpPd. Chlorination of the MPd (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 formation.

Stabilization treatment of Pu-bearing organic materials

Morishita, Kazuki; Sato, Takumi; Onishi, Takashi; Seki, Takayuki*; Sekine, Shinichi*; Okitsu, Yuichi*

JAEA-Technology 2021-024, 27 Pages, 2021/10

JAEA-Technology-2021-024.pdf:2.41MB

In the case of Plutonium (Pu)-bearing organic materials, organic materials are decomposed by alpha rays emitted mainly from Pu to generate hydrogen gas and other substances. Therefore, to safely store Pu-bearing organic materials for an extended period of time, organic materials must be eliminated. In addition, carbide and nitride fuels must be converted into oxides for safe storage in order to prevent the exothermal reaction of these fuels with oxygen/moisture in air. A survey of the literature on the stabilization treatment of Pu-bearing organic materials confirmed that organic materials can be decomposed and removed by heating at 950 C (1223.15 K) or greater in air. Furthermore, based on the calculated thermodynamic parameters of oxidation reaction of carbide and nitride fuels in air, it was estimated that these fuels would be oxidized in air at 950 C because the equilibrium oxygen partial pressure in the oxidation reaction at 950 C was lower than 2.110 Pa (oxygen partial pressure in air). Therefore, it was decided to stabilize Pu-bearing organic materials by heating at 950 C in air to remove the organic materials and oxidize the carbide and nitride fuels. As a mock-up test to remove the organic materials, thin sheets of epoxy resin were heated in air. The changes in appearance and weight before and after heating in air showed that organic materials can be removed. After the mock-up test, Pu-bearing organic materials were also stabilized by heating in the similar condition.

Modulation of Dirac electrons in epitaxial BiSe ultrathin films on van der Waals ferromagnet CrSiTe

Kato, Takemi*; Sugawara, Katsuaki*; Ito, Naohiro*; Yamauchi, Kunihiko*; Sato, Takumi*; Oguchi, Tamio*; Takahashi, Takashi*; Shiomi, Yuki*; Saito, Eiji; Sato, Takafumi*

Physical Review Materials (Internet), 4(8), p.084202_1 - 084202_6, 2020/08

https://doi.org/10.1103/PhysRevMaterials.4.084202

Measurement of the angular distribution of -rays after neutron capture by La for a T-violation search

Okudaira, Takuya; Shimizu, Hirohiko*; Kitaguchi, Masaaki*; Hirota, Katsuya*; Haddock, C. C.*; Ito, Ikuya*; Yamamoto, Tomoki*; Endo, Shunsuke*; Ishizaki, Kohei*; Sato, Takumi*; et al.

EPJ Web of Conferences, 219, p.09001_1 - 09001_6, 2019/12

https://doi.org/10.1051/epjconf/201921909001

Parity violating effects enhanced by up to 10 times have been observed in several neutron induced compound nuclei. There is a theoretical prediction that time reversal (T) violating effects can also be enhanced in these nuclei implying that T-violation can be searched for by making very sensitive measurements. However, the enhancement factor has not yet been measured in all nuclei. The angular distribution of the (n,) reaction was measured with La by using a germanium detector assembly at J-PARC, and the enhancement factor was obtained. From the result, the measurement time to achieve the most sensitive T-violation search was estimated as 1.4 days, and a 40% polarized La target and a 70% polarized He spin filter whose thickness is 70 atmcm are needed. Therefore high quality He spin filter is developed in JAEA. The measurement result of the (n,) reaction at J-PARC and the development status of the He spin filter will be presented.

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.

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.

Pyrochemical treatment of spent nitride fuels for MA transmutation

Hayashi, Hirokazu; Sato, Takumi; Shibata, Hiroki; Kurata, Masaki; Iwai, Takashi; Arai, Yasuo

Science China; Chemistry, 57(11), p.1427 - 1431, 2014/11

https://doi.org/10.1007/s11426-014-5205-9

Nitride fuels have several advantages, such as high thermal conductivity and high metal density like metallic fuels, and high melting point and isotropic crystal structure like oxide fuels. Since the late 1990s, the partitioning and transmutation of minor actinides (MA) has been studied to decrease the long term radio-toxicity of high level waste and mitigate the burden on the final disposal. Japan Atomic Energy Agency (JAEA) has been proposing dedicated transmutation cycle using the Accelerator-Driven System (ADS) with the nitride fuels containing MA. We have been developing the nitride fuel cycle including pyrochemical process. Our focus is on electrolysis of nitride fuels and refabrication of nitride fuel from the recovered actinides because other processes are similar to the technology for the metal fuel treatment and have been studied elsewhere. In this paper, we summarized our activity on developments of the pyrochemical treatment of the spent nitride fuels.

Development of the pyrochemical process of spent nitride fuels for ADS; Its elemental technologies and process flow diagram

Hayashi, Hirokazu; Sato, Takumi; Shibata, Hiroki; Iwai, Takashi; Nishihara, Kenji; Arai, Yasuo

Proceedings of International Conference on Toward and Over the Fukushima Daiichi Accident (GLOBAL 2011) (CD-ROM), 6 Pages, 2011/12

R&D on the transmutation of long-lived minor actinides (MA) by the accelerator-driven system (ADS) using nitride fuels is underway at Japan Atomic Energy Agency. In regard to reprocessing technology, pyrochemical process has several advantages in case of treating spent fuel with large decay heat and fast neutron emission, and recovering highly enriched N-15. In the pyrochemical reprocessing, plutonium (Pu) and MA are dissolved in LiCl-KCl eutectic melts and selectively recovered into liquid cadmium (Cd) cathode by molten salt electrorefining. The recovered Pu and MA are converted to nitrides by the nitridation-distillation combined method, in which the Cd alloys containing Pu and MA are heated in nitrogen gas stream. The authors have investigated its elemental technologies such as electrorefining and renitridation. On the other hand, development of the process flow diagram with the material balance sheet of the pyrochemical reprocessing of spent nitride fuel for ADS is in progress. This paper summarized recent progress of the study which aims to prove the technological applicability of pyrochemical process to the nitride fuel cycle for transmutation of MA.