Ga K-edge XANES study of Ga-exchanged zeolites at high temperatures under different atmospheres including vacuum, CO, and pressurized H

Huang, M.*; 金城 哲弥*; 安村 駿作*; 鳥屋尾 隆*; 松村 大樹; 齋藤 寛之*; 清水 研一*; 並木 則和*; 前野 禅*

Catalysis Science & Technology, 13(23), p.6832 - 6838, 2023/12

https://doi.org/10.1039/D3CY01250F

Ga-exchanged zeolites are promising catalysts for dehydrogenative alkane transformations. Reduced Ga species, such as Ga hydrides and Ga cations, are possible active sites for alkane dehydrogenation based on in situ spectroscopic studies. However, most of the reported studies were conducted at lower temperatures compared with those encountered in actual operating conditions. In this study, the in situ Ga K-edge XANES analysis of Ga-exchanged MFI zeolite was performed under actual operating temperatures and different atmospheres (H, He, CO, vacuum, and CH). The absorption edge appeared at similarly lower energy values than that of GaO in all atmospheres, whereas the main absorption peak intensity differed depending on the presence or absence of a hydride source in the gas phase. Higher intensities were observed under H and CH atmospheres than under CO and vacuum atmospheres.

Strain-induced crystallization and phase separation used for fabricating a tough and stiff slide-ring solid polymer electrolyte

橋本 慧*; 塩飽 透*; 青木 裕之; 横山 英明*; 眞弓 皓一*; 伊藤 耕三*

Science Advances (Internet), 9(47), p.eadi8505_1 - eadi8505_8, 2023/11

https://doi.org/10.1126/sciadv.adi8505

The demand for mechanically robust polymer-based electrolytes is increasing for applications to wearable devices. Young's modulus and breaking energy are essential parameters for describing the mechanical reliability of electrolytes. The former plays a vital role in suppressing the short circuit during charge-discharge, while the latter indicates crack propagation resistance. However, polymer electrolytes with high Young's moduli are generally brittle. In this study, a tough slide-ring solid polymer electrolyte (SR-SPE) breaking through this trade-off between stiffness and toughness is designed on the basis of strain-induced crystallization (SIC) and phase separation. SIC makes the material highly tough (breaking energy, 80 to 100 megajoules per cubic meter). Phase separation in the polymer enhanced stiffness (Young's modulus, 10 to 70 megapascals). The combined effect of phase separation and SIC made SR-SPE tough and stiff, while these mechanisms do not impair ionic conductivity. This SIC strategy could be combined with other toughening mechanisms to design tough polymer gel materials.

HTTR1次ヘリウム循環機フィルタの差圧上昇事象,1; 差圧上昇事象の原因調査

根本 隆弘; 荒川 了紀; 川上 悟; 長住 達; 横山 佳祐; 渡部 雅; 大西 貴士; 川本 大樹; 古澤 孝之; 猪井 宏幸; et al.

JAEA-Technology 2023-005, 33 Pages, 2023/05

JAEA-Technology-2023-005.pdf:5.25MB

HTTR (High Temperature engineering Test Reactor) RS-14サイクルの原子炉出力降下において、ヘリウムガス循環機のフィルタ差圧が上昇傾向となった。この原因を調査するため、1次ヘリウム純化設備のガス循環機の分解点検等を実施した結果、ガス循環機内のシリコンオイルミストがチャコールフィルタの性能低下で捕集できなくなり、1次系統に混入したためと推定された。今後は、フィルタ交換を実施するとともに、さらなる調査を進め、再発防止対策を策定する予定である。

Spin and spin current; From fundamentals to recent progress

前川 禎通; 吉川 貴史*; 中堂 博之; 家田 淳一; 齊藤 英治

Journal of Applied Physics, 133(2), p.020902_1 - 020902_24, 2023/01

https://doi.org/10.1063/5.0133335

Along with the progress of spin science and spintronics research, the flow of electron spins, i.e., spin current, has attracted interest. New phenomena and electronic states were explained in succession using the concept of spin current. Moreover, as many of the conventionally known spintronics phenomena became well organized based on spin current, it has rapidly been recognized as an essential concept in a wide range of condensed matter physics. In this article, we focus on recent developments in the physics of spin, spin current, and their related phenomena, where the conversion between spin angular momentum and different forms of angular momentum plays an essential role. Starting with an introduction to spin current, we first discuss the recent progress in spintronic phenomena driven by spin-exchange coupling: spin pumping, topological Hall torque, and emergent inductor. We, then, extend our discussion to the interaction/interconversion of spins with heat, lattice vibrations, and charge current and address recent progress and perspectives on the spin Seebeck and Peltier effects. Next, we review the interaction between mechanical motion and electron/nuclear spins and argue the difference between the Barnett field and rotational Doppler effect. We show that the Barnett effect reveals the angular momentum compensation temperature, at which the net angular momentum is quenched in ferrimagnets.

New isomers in Cf

Orlandi, R.; 牧井 宏之; 西尾 勝久; 廣瀬 健太郎; 浅井 雅人; 塚田 和明; 佐藤 哲也; 伊藤 由太; 洲嵜 ふみ; 永目 諭一郎*; et al.

Physical Review C, 106(6), p.064301_1 - 064301_11, 2022/12

https://doi.org/10.1103/PhysRevC.106.064301

The nuclear structure of Cf produced by the O+Cf multinucleon transfer reaction was investigated using -ray spectroscopy. Analysis of the -ray spectrum of Cf revealed the presence of multiple long-lived (isomeric) excited states at low excitation energies. The energies and half-lives of the isomers contain information on the proton and neutron orbits in the heavy-element region and the deformation of atomic nuclei, and are important data to predict the properties of nuclei in the "island of stability".

Rotation of complex ions with ninefold hydrogen coordination studied by quasielastic neutron scattering and first-principles molecular dynamics calculations

大政 義典*; 高木 茂幸*; 戸嶋 健人*; 横山 凱乙*; 遠藤 亘*; 折茂 慎一*; 齋藤 寛之*; 山田 武*; 川北 至信; 池田 一貴*; et al.

Physical Review Research (Internet), 4(3), p.033215_1 - 033215_9, 2022/09

https://doi.org/10.1103/PhysRevResearch.4.033215

Quasielastic neutron scattering (QENS) and neutron powder diffraction of the complex transition metalhydrides LiMoH and LiNbH were measured in a temperature range of 10-300 K to study their structures and dynamics, especially the dynamics of the hydrogen atoms. These hydrides contain unusual ninefold H coordinated complex ions (MoH or NbH) and hydride ions (H). A QENS signal appeared 150 K due to the relaxation of H atoms. The intermediate scattering functions derived from the QENS spectra are well fitted by a stretched exponential function called the Kohlrausch-Williams-Watts functions with a small stretching exponent 0.3-0.4, suggesting a wide relaxation time distribution. The dependence of the elastic incoherent structure factor is reproduced by the rotational diffusion of MH (M = Mo or Nb) anions. The results are well supported by a van Hove analysis for the motion of H atoms obtained using first-principles molecular dynamics calculations. We conclude that the wide relaxation time distribution of the MH rotation is due to the positional disorder of the surrounding Li ions and a unique rotation with MH anion deformation (pseudorotation).

Uranium chelating ability of decorporation agents in serum evaluated by X-ray absorption spectroscopy

上原 章寛*; 松村 大樹; 辻 卓也; 薬丸 晴子*; 田中 泉*; 城 鮎美*; 齋藤 寛之*; 石原 弘*; 武田(本間) 志乃*

Analytical Methods, 14(24), p.2439 - 2445, 2022/06

https://doi.org/10.1039/D2AY00565D

Internal exposure to actinides such as uranium and plutonium has been reduced using chelating agents for decorporation because of their potential to induce both radiological and chemical toxicities. This study measures uranium chemical forms in serum in the presence and absence of chelating agents based on X-ray absorption spectroscopy (XAS). The chelating agents used were 1-hydroxyethane 1,1-bisphosphonate (EHBP), inositol hexaphosphate (IP6), deferoxamine B (DFO), and diethylenetriaminepentaacetate (DTPA). The main ligands forming complexes with uranium in the serum were estimated as follows: IP6 EHBP bioligands DFO DTPA when the concentration ratio of the chelating agent to uranium was 10. Measurements of uranium chemical forms and their concentrations in the serum would be useful for the appropriate treatment using chelating agents for the decorporation of uranium.

Volatilization of BC control rods in Fukushima Daiichi nuclear reactors during meltdown; B-Li isotopic signatures in cesium-rich microparticles

笛田 和希*; 高見 龍*; 蓑毛 健太*; 諸岡 和也*; 堀江 憲路*; 竹原 真美*; 山崎 信哉*; 斉藤 拓巳*; 塩津 弘之; 大貫 敏彦*; et al.

Journal of Hazardous Materials, 428, p.128214_1 - 128214_10, 2022/04

https://doi.org/10.1016/j.jhazmat.2022.128214

Boron carbide control rods remain in the fuel debris of the damaged reactors in the Fukushima Daiichi Nuclear Power Plant, potentially preventing re-criticality; however, the state and stability of the control rods remain unknown. Sensitive high-resolution ion microprobe analyses have revealed B-Li isotopic signatures in radioactive Cs-rich microparticles (CsMPs) that formed by volatilization and condensation of Si-oxides during the meltdowns. The CsMPs contain 1518-6733 mg kg of B and 11.99-1213 mg kg of Li. The B/B (4.15-4.21) and Li/Li (213-406) isotopic ratios are greater than natural abundances (4.05 and 12.5, respectively), indicating that B(n,)Li reactions occurred in BC prior to the meltdowns. The total amount of B released with CsMPs was estimated to be 0.024-62 g, suggesting that essentially all B remains in reactor Units 2 and/or 3 and is enough to prevent re-criticality; however, the heterogeneous distribution of B needs to be considered during decommissioning.

プルトニウムの体外排出に向けたキレート剤による除染に関する基礎検討; X線吸収分光法によるプルトニウム模擬元素とキレート剤との結合性評価

上原 章寛*; Shuhui, X.*; 佐藤 遼太朗*; 松村 大樹; 辻 卓也; 薬丸 晴子*; 城 鮎美*; 齋藤 寛之*; 田中 泉*; 石原 弘*; et al.

X線分析の進歩,53, p.223 - 229, 2022/03

体内にアクチニドなどの放射性物質が取り込まれると、生体内配位子がアクチニドと化合物を生成し、体内滞留の原因となりうる。本研究では、アクチニドを体外に排出させるためのキレート剤の結合性評価を行うため、キレート剤と結合した元素の局所構造をX線吸収分光法によって解析し結合力を評価した。プルトニウム模擬元素としてジルコニウム(Zr),キレート剤として、EHBP(1-hydroxyethylidene-1,1-diphosphonate)およびDTPA (diethylenetriaminepentaacetate)を用いた。ZrはEHBPと八面体構造の錯体を形成するとともに、Zr-EHBP錯体はZr-DTPA錯体より強い結合を有することが分かった。これらの知見は、放射性元素による内部被ばく線量評価や、放射性元素を体外に取り除くための適切な除染方法の提案につながる。

Improving the safety of the high temperature gas-cooled reactor "HTTR" based on Japan's new regulatory requirements

濱本 真平; 清水 厚志; 猪井 宏幸; 栃尾 大輔; 本間 史隆; 澤畑 洋明; 関田 健司; 渡辺 周二; 古澤 孝之; 飯垣 和彦; et al.

Nuclear Engineering and Design, 388, p.111642_1 - 111642_11, 2022/03

https://doi.org/10.1016/j.nucengdes.2021.111642

日本原子力研究開発機構は、2011年の福島第一原子力発電所事故を契機に作られ2013年12月に施行された新しい規制要件に、高温工学試験研究炉(HTTR)を適合させた。様々な高温ガス炉(HTTR)安全試験を通じて得られたHTGRに関する知見を基に、既存の構造物,系統及び機器の安全性及び耐震分類が議論された。防護の対象となる構築物,系統及び機器が再検討し、安全機能に影響を及ぼす内的・外的脅威への対策が強化された。さらに、設計基準を超える事故として、多量の放射性物質が放出されるおそれのある事故に対する措置を講じた。我々のこの対応が、新しい規制要求に適合していることを、原子力規制委員会は厳格かつ適切に審査した。2014年11月に提出したHTTRの設置許可変更申請書は、9回の修正を経て2020年6月に承認された。この対応は、高温ガス炉の特性を反映すれば、強化された規制要件を満たすためでも合理的に設計できることを示しており、今後の高温ガス炉の開発の参考になると考える。