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Micheau, C.; 上田 祐生; 元川 竜平; 阿久津 和宏*; 山田 悟史*; 山田 雅子*; Moussaoui, S. A.*; Makombe, E.*; Meyer, D.*; Berthon, L.*; et al.
Journal of Molecular Liquids, 401, p.124372_1 - 124372_12, 2024/05
Supramolecular organization of extractant molecules impacts metal ions separation behavior. Probing bulk and interfacial structures of the relevant systems is expected to provide key insights into the metal ion selectivity and kinetic aspects. The supramolecular features of two solvent extraction systems based on malonamide extractants, N,N,N′,N′-tetrahexylmalonamide (THMA) in toluene and N,N′-dimethyl-N,N′-dibutyl-2-tetradecylmalonamide (DBMA) in n-heptane, were studied using small-angle X-ray scattering for the organic bulk phases, as well as interfacial tension and neutron reflectivity measurements for the interfaces. In the bulk solution, THMA forms dimeric/trimeric associates but no aggregates in toluene, while DBMA forms large aggregates in n-heptane. On the other hand, THMA accumulates in a diffuse layer at the interface at high THMA concentration, whereas DBMA forms a compact but thinner layer. After Pd(II) extraction, the thickness of interfacial layers decreases in the case of THMA, and totally vanishes in the case of DBMA. Based on these new structural information, two mechanisms are proposed for Pd(II) and Nd(III) extraction with malonamides. In toluene, THMA associates slightly accumulate in the vicinity of the interface, then coordinate Pd(II) and diffuse into the organic bulk phase. In n-heptane, DBMA aggregates adsorb at the interface then pick up Nd(III) cations in their polar cores and finally diffuse into the bulk.
水野 るり恵*; 新倉 潤*; 齋藤 岳志*; 松崎 禎市郎*; 櫻井 博儀*; Amato, A.*; 浅利 駿介*; Biswas, S.*; Chiu, I.-H.; Gianluca, J.*; et al.
Nuclear Instruments and Methods in Physics Research A, 1060, p.169029_1 - 169029_14, 2024/03
被引用回数：0 パーセンタイル：0.02(Instruments & Instrumentation)We have developed a photon detection system for muonic X-ray spectroscopy. The detector system consists of high-purity germanium detectors with BGO Compton suppressors. The signals from the detectors are readout with a digital acquisition system. The absolute energy accuracy, energy and timing resolutions, photo-peak efficiency, the performance of the Compton suppressor, and high count rate durability are studied with standard 
-ray sources and in-beam experiment using 
Al(
)
Si resonance reaction. The detection system was demonstrated at Paul Scherrer Institute. A calibration method for a photon detector at a muon facility using muonic X-rays of 
Au and 
Bi is proposed.
Shaimerdenov, A.*; Gizatulin, Sh.*; Sairanbayev, D.*; Bugybay, Zh.*; Silnyagin, P.*; Akhanov, A.*; 冬島 拓実; 広田 憲亮; 土谷 邦彦
Nuclear Instruments and Methods in Physics Research B, 548, p.165235_1 - 165235_6, 2024/03
被引用回数：0原子炉のケーブルの絶縁材は、他の種類の設備における条件と比較して、混合条件(高温、放射線、圧力、湿度、過酷な環境)にさらされ、同時に長期間(約40-50年)の性能特性を維持する必要がある。このような条件下での照射の結果、ケーブル絶縁体の電気的特性は劣化し、電流損失が増大する。これは、放射線によって絶縁体に電荷が誘導されるためである。WWR-K原子炉では、2種類の無機絶縁材(MgOとAl
O
)を使用した信号ケーブルの耐放射線性に関する研究が開始された。これらの研究の一環として、2種類の無機絶縁材を使用した信号ケーブルの混合運転条件(放射線場と高温)における挙動について、新たな実験データを取得する。ケーブルに10
cm
までの高速中性子を照射する予定である。照射温度は(500
50)
Cである。信号ケーブルの絶縁体の電気特性の劣化の研究は、リアルタイムで実施される。このために、実験装置の特別な設計と電気特性の炉内測定技術が開発された。本論文では、キャプセル設計の概略、キャプセル設計開発のための複雑な計算結果、予想される中性子フルエンス、鋼材中のdpa、炉内電気特性測定技術、今後の作業計画を示す。目標中性子フルエンスに到達するまでのケーブル照射時間は、約100日となる。本研究は、国際科学技術センターの助成を受けて実施されている。
坪田 陽一; Porcheron, E.*; Journeau, C.*; Delacroix, J.*; Suteau, C.*; Lallot, Y.*; Bouland, A.*; Roulet, D.*; 三次 岳志
Proceedings of International Conference on Environmental Remediation and Radioactive Waste Management (ICEM2023) (Internet), 6 Pages, 2023/10
福島第一原子力発電所(1F)における燃料デブリ取出しを安全に実施するためには、燃料デブリの切断時に発生する放射性微粒子の定量評価が必要である。我々はウラン含有のIn/Ex-Vessel組成を持つ模擬燃料デブリを作製し、それらを加熱した際に生じるエアロゾルの物理、化学的特性を評価した。それらを基に1F-Unit2の燃料デブリを加熱法の代表例であるレーザー切断した際に生じるエアロゾルの同位体組成と放射能を推定したところ、
Pu、
Am、
Cmを主とするプルトニウムが
核種として、Pu、
Cs-Ba、
Sr-Yが
核種としての着目核種であることが分かった。
Porcheron, E.*; Journeau, C.*; Delacroix, J.*; Berlemont, R.*; Bouland, A.*; Lallot, Y.*; 坪田 陽一; 池田 篤史; 三次 岳志
Proceedings of International Conference on Environmental Remediation and Radioactive Waste Management (ICEM2023) (Internet), 5 Pages, 2023/10
福島第一原子力発電所(1F)の損傷した原子炉の廃止措置における重要な課題である燃料デブリの切断作業における放射性エアロゾルの発生と飛散を評価する目的で行われたURASOLプロジェクトにおいて、模擬燃料デブリの加熱および機械的切断に伴い生成するエアロゾルの質量濃度、リアルタイム数密度、質量基準の粒径分布、形態、および化学的特性の観点からの特性評価について報告する。加熱試験においては温度上昇に伴う粒径増大が観察され、粒子数密度に関しては劣化ウランを用いた模擬燃料デブリを用いた例がHf含有模擬燃料デブリを用いた試験よりも小さい数密度であった。機械的切断においてはエアロゾルの空気動力学的質量中央径は、放射性試料と非放射性試料でほぼ同程度(約3.7
4.4
m)であった。
Micheau, C.; 上田 祐生; 元川 竜平; Bauduin, P.*; Girard, L.*; Diat, O.*
Langmuir, 39(31), p.10965 - 10977, 2023/07
被引用回数：0 パーセンタイル：0(Chemistry, Multidisciplinary)Understanding clay flotation mechanisms has become a major concern because of the increasing level of environmental contamination of soil and ground water by heavy metals and radionuclides. Clays are often used as sorbents for extracting metals in indirect flotation processes but can function simultaneously as defoamers. However, how foam generation and stability depend on the molecular interactions between the clays and surfactant is still controversial. In the present study, an amine polyethoxylated surfactant was used as a bifunctional surfactant that collected clay particles and acted as a foaming agent in the flotation process. The pH conditions strongly affected the surfactant physicochemical properties, allowing the clay extraction efficiency to be tuned. The interfacial recovery factor of the clays almost reached 100 percent under acidic (pH lower than 6) and neutral (pH 6-10) conditions, whereas it was negative under alkaline conditions (pH higher than 10), contrary to expectations. To elucidate the mechanisms involved in the particle flotation process for each of the pH conditions, the bulk and foam phases were analyzed. The effects of electrostatic interactions between the solutes and multiscale structure on the clay extraction behavior were investigated by electrophoretic measurements, dynamic light scattering, small-angle neutron scattering, and image analysis. Based on these results, three flotation processes were found depending on pH range: surfactant foam fractionation at pH higher than 10; clay particle foam flotation at pH 6-10; and particle froth flotation at pH lower than 6.
SnSe
Ren, Q.*; Gupta, M. K.*; Jin, M.*; Ding, J.*; Wu, J.*; Chen, Z.*; Lin, S.*; Fabelo, O.*; Rodriguez-Velamazan, J. A.*; 古府 麻衣子; et al.
Nature Materials, 22, p.999 - 1006, 2023/05
被引用回数：21 パーセンタイル：99.22(Chemistry, Physical)Ultralow thermal conductivity and fast ionic diffusion endow superionic materials with excellent performance both as thermoelectric converters and as solid-state electrolytes. Yet the correlation and interdependence between these two features remain unclear owing to a limited understanding of their complex atomic dynamics. Here we investigate ionic diffusion and lattice dynamics in argyrodite AgSnSe using synchrotron X-ray and neutron scattering techniques along with machine-learned molecular dynamics. We identify a critical interplay of the vibrational dynamics of mobile Ag and a host framework that controls the overdamping of low-energy Ag-dominated phonons into a quasi-elastic response, enabling superionicity. Concomitantly, the persistence of long-wavelength transverse acoustic phonons across the superionic transition challenges a proposed 'liquid-like thermal conduction' picture. Rather, a striking thermal broadening of low-energy phonons, starting even below 50 K, reveals extreme phonon anharmonicity and weak bonding as underlying features of the potential energy surface responsible for the ultralow thermal conductivity (
0.5 Wm
K) and fast diffusion. Our results provide fundamental insights into the complex atomic dynamics in superionic materials for energy conversion and storage.
Lee, S.*; 仲田 光樹; Tchernyshyov, O.*; Kim, S. K.*
Physical Review B, 107(18), p.184432_1 - 184432_12, 2023/05
被引用回数：4 パーセンタイル：90.23(Materials Science, Multidisciplinary)超対称量子力学に基づき、反強磁性スカーミオン構造を有する磁壁中のマグノンのトポロジカル量子輸送物性を明らかにする。スカーミオン型の磁気構造を有する磁壁中を伝搬するマグノンは、一種のゲージ場として作用する有効磁場を獲得する。そこで、この有効磁場中でのマグノンの反射・屈折現象を超対称量子力学に基づいて解析し、その伝搬および束縛マグノン状態を明らかにする。そして、ラウダウアー公式を用いて、磁壁のカイラリティが増加するにつれてマグノンによる熱流が減少することを明らかにする。本研究はスピンホール効果を活用した熱流の制御方法を理論的に提案する。
北垣 徹; Krasnov, V.*; 池田 篤史
Journal of Nuclear Materials, 576, p.154224_1 - 154224_14, 2023/04
被引用回数：1 パーセンタイル：53.89(Materials Science, Multidisciplinary)Nuclear fuel debris is a complex material containing a wide range of elements, compounds, and radiation. This complexity renders all the stages of the treatment of nuclear fuel debris extremely difficult and troublesome in the technical context. The whole treatment of nuclear fuel debris is also an extremely long-term process for tens of thousands of years, during which the aging of nuclear fuel debris is an unavoidable but critical issue. This applies to the decommissioning of the damaged reactors of the Fukushima Daiichi Nuclear Power Station (1F). This review article aims at collecting and summarizing the knowledge and information about the aging of materials containing nuclear fuels (fuel-containing materials) formed as a result of the accident at ChNPP-4 in the light of the decommissioning of 1F and assessing the potential effects of aging on the nuclear fuel debris remaining in the damaged 1F reactors.
間所 寛; 山下 拓哉; Gaus-Liu, X.*; Cron, T.*; Fluhrer, B.*; 佐藤 一憲; 溝上 伸也*
Nuclear Technology, 209(2), p.144 - 168, 2023/02
被引用回数：0 パーセンタイル：0.01(Nuclear Science & Technology)Since the reactor pressure vessel (RPV) lower head failure determines the subsequent ex-vessel accident progression, it is a key issue to understand the accident progression of Fukushima Daiichi Nuclear Power Station (1F). The RPV failure is largely affected by thermal loads on the vessel wall and thus it is inevitable to understand thermal behavior of molten metallic pool with co- existence of solid oxide fuel debris. In the past decades, numerous experiments have been conducted to investigate a homogeneous molten pool behavior. Few experiments, however, addresses the melting and heat transfer process of debris bed consisted of materials with different melting temperatures. LIVE-J2 experiment aimed to provide the experimental data on a solid-liquid mixture pool in a simulated RPV lower head under various conditions. The extensive measurements of the melt temperature indicate the heat transfer regimes in a solid-liquid mixture pool. The test results showed that the conductive heat transfer was dominant during the steady state along the vessel wall boundary and that convective heat transfer takes place inside the mixture pool. Besides the experimental performance, the test case was numerically simulated by using ANSYS Fluent. The simulation results generally agree with the measured experimental data. The flow regime and transient melt evolution were able to be estimated by the calculated velocity field and the crust thickness, respectively.
Micheau, C.; 上田 祐生; 阿久津 和宏*; Bourgeois, D.*; 元川 竜平
Solvent Extraction and Ion Exchange, 41(2), p.221 - 240, 2023/02
被引用回数：1 パーセンタイル：51.1(Chemistry, Multidisciplinary)Malonamide derivatives, which are among the most extensively investigated extractants in solvent extraction of lanthanoids, actinides, and platinum group metal ions, were deuterated by using Pd/C and Rh/C catalysts with a DO/2-propanol mixture. This method enables to replace the hydrogen atoms by deuterium atoms in the malonamide chemical structure with a controllable deuteration rate. The maximum rate reaches 75 percent approximately, determined by nuclear magnetic resonance (NMR) and electrospray ionization mass spectrometry. In addition, it has been demonstrated that extraction behavior of the malonamide molecules remains unchanged after the deuteration procedure. Deuterated malonamides should be a powerful tool for fundamental researches on solvent extraction systems, in particular, for structural analysis of the organic phases. The large difference in the neutron scattering cross-section between hydrogen and deuterium leads to a large difference in neutron scattering length density of the malonamide derivatives before and after the deuteration reaction. Therefore, using deuterated malonamides in small-angle neutron scattering and neutron reflectivity studies could give access to the nanoscopic structure of the specific solute species in the bulk organic phase and at the liquid-liquid interface, respectively. This deuteration method could become a general one and be extended to a wide variety of extractant molecules. In this way this work contributes to the development of the fundamental researches in solvent extraction systems.
Rh
Sn
Opletal, P.; Duverger-N
dellec, E.*; Miliyanchuk, K.*; Malick, S.*; Hossain, Z.*; Custers, J.*
Journal of Alloys and Compounds, 927, p.166941_1 - 166941_7, 2022/12
被引用回数：2 パーセンタイル：32.54(Chemistry, Physical)Single crystals of a new ternary compound CeRhSn were synthesized by flux method and its crystal structure and magnetic properties were studied by single crystal X-ray diffraction and magnetic susceptibility, specific heat and resistivity measurements. CeRhSn crystallizes in a new monoclinic crystal structure, space group 
2
m (No. 11) with Z = 2 and lattice parameters 
= 9.8708(5) 
, 
= 4.5779(3) ; and 
= 14.2381(7) , = 109.535(5), and V = 606.35(6) 
. The structure exhibits three inequivalent Ce-sites. A striking structural motif is the tetragonal pyramid of Rh-ions surrounding the Ce2 yielding an extreme short Ce2-Rh1 spacing of 
= 2.7486(10) . This strong hint to mixed valent cerium behavior is supported by the entropy analysis. We argue that the Ce2-ion is in a nonmagnetic Ce
state while the other 2 Ce-sites are in a trivalent state. At low temperatures these latter become partially Kondo screened (
4 K) and order antiferromagnetic below 
= 2.31 K. The ordering is accompanied by a superzone gap-opening in direction of the magnetic propagation vector Q = (0, 0, l).
BaCo(PO)Sheng, J.*; Wang, L.*; Candini, A.*; Jiang, W.*; Huang, L.*; Xi, B.*; Zhao, J.*; Ge, H.*; Zhao, N.*; Fu, Y.*; et al.
Proceedings of the National Academy of Sciences of the United States of America, 119(51), p.e2211193119_1 - e2211193119_9, 2022/12
被引用回数：3 パーセンタイル：28(Multidisciplinary Sciences)Although considerable progress has been made in the theoretical understanding of the low-dimensional frustrated quantum magnets, experimental realizations of a well-established scaling analysis are still scarce. This is particularly true for the two-dimensional antiferromagnetic triangular lattices. Owing to the small exchange strength, the newly discovered compound NaBaCo(PO) provides a rare opportunity for clarifying the quantum criticality in an ideal triangular lattice with quantum spin S=1/2. In addition to the establishment of the complete phase diagrams, the spin Hamiltonian with a negligible interplane interaction has been determined through the spin wave dispersion in the polarized state, which is consistent with the observation of a two-dimensional quantum critical point with the Bose-Einstein condensation of diluted free bosons.
孫 昊旻; Leblois, Y.*; Gelain, T.*; Porcheron, E.*
Journal of Nuclear Science and Technology, 59(11), p.1356 - 1369, 2022/11
被引用回数：0 パーセンタイル：0.01(Nuclear Science & Technology)PWRのシビアアクシデントシナリオにおいて、格納容器内エアロゾル状放射性物質の除去・保持のために、格納容器スプレイを用いることができる。そのために、高精度な除去効率の予測は安全評価上重要である。PWRの格納容器スプレイでは、84%-95%と高いスプレイカバー率が要求されるのに対して、既往研究では、そのような高いカバー率におけるエアロゾル除去実験はかなり限られている。本論文では、カバー率に着目し、スプレイによるエアロゾル除去現象の理解と除去効率評価モデル高度化のために、大型容器において実機相当のカバー率を有する体系のエアロゾル除去実験を実施し、詳細なエアロゾルと液滴特性の計測結果から除去特性を調査した。また、MELCORの除去モデルと実験結果を比較し、粒子径に対する除去効率の傾向が再現でき、大きい粒子径に対して過小評価となるものの、最小除去効率を有する小さい粒子径(0.52m)において良好な一致が得られることを示した。
Simonnet, M.; Sittel, T.*; We
ling, P.*; Geist, A.*
Energies (Internet), 15(20), p.7724_1 - 7724_10, 2022/10
被引用回数：1 パーセンタイル：10.66(Energy & Fuels)Asse II salt mine, Germany, contains low and intermediate level radioactive waste that must be retrieved in the upcoming years. Potentially contaminated salts and brines will require treatment. Cs would be the main contaminant. Cs
is problematic to selectively recover due to its chemical similarity with Na and K which are present in high quantity in a salt mine. This paper is offering a solution for Cs separation from concentrated chloride salt media by solvent extraction with calixarene-crown-ether extractants in alcoholic diluent.
Porcheron, E.*; Leblois, Y.*; Journeau, C.*; Delacroix, J.*; Molina, D.*; Suteau, C.*; Berlemont, R.*; Bouland, A.*; Lallot, Y.*; Roulet, D.*; et al.
Proceedings of International Topical Workshop on Fukushima Decommissioning Research (FDR2022) (Internet), 5 Pages, 2022/10
福島第一原子力発電所(1F)の事故炉廃止措置における重要な課題の一つが、燃料デブリの取り出しである。ONET Technologies, CEA, IRSNからなるフランスのコンソーシアムがJAEA/CLADSのために実施したURASOLプロジェクトは、燃料デブリ模擬物質の熱的・機械的加工による放射性エアロゾルの生成と特性に関する科学的基礎データの取得に取り組んでいる。VITAE施設で行われる加熱試験はレーザーによる熱的切断の代表的な条件を模擬している。機械的切断では、FUJISAN施設においてコアボーリング試験を実施した。燃料デブリ模擬物質は、非放射性試験と放射性試験のために開発されている。化学的特性評価と粒径情報の取得は、デブリ取り出しで発生する可能性のある放射性粒子の特性推定のために実施された。これらの情報は1Fにおける燃料デブリ取り出し作業において放射線防護上の対策を評価するうえで重要な情報である。
RhGa explored by 
Ga nuclear quadrupole resonance山本 真吾*; 藤井 拓斗*; Luther, S.*; 安岡 弘志*; 酒井 宏典; B
rtl, F.*; Ranjith, K. M.*; Rosner, H.*; Wosnitza, J.*; Strydom, A. M.*; et al.
Physical Review B, 106(11), p.115125_1 - 115125_5, 2022/09
被引用回数：0 パーセンタイル：0(Materials Science, Multidisciplinary)Ga核四重極共鳴法によって、CeRhGaにおける130Kの構造相転移と基底状態について調べた。構造相転移点で、NQR共鳴線の分裂を観測し、構造相転移転移点以下ではGaサイトが結晶学的に2つになることがわかった。NQR周波数は、電子状態計算による予測値を一致した。低温0.3Kまで、磁気秩序が起こらないことを明らかにした。また、構造相転移点以下2Kまでは、NQR緩和率
は一定であるが、2K以下でコリンハ則
の振る舞いにクロスオーバーする。2Kという特徴温度に加えて、は、0.8Kという特徴温度も示しており、2つのCeサイトによる異なる近藤温度の可能性について議論した。
Nguyen, T. H.*; Le Ba, T.*; Tran, C. T.*; Nguyen, T. T.*; Doan, T. T. T.*; Do, V. K.; 渡邉 雅之; Pham, Q. M.*; Hoang, S. T.*; Nguyen, D. V.*; et al.
Hydrometallurgy, 213, p.105933_1 - 105933_11, 2022/08
被引用回数：9 パーセンタイル：83.6(Metallurgy & Metallurgical Engineering)ベトナム・イェンフー希土類精鉱浸出液からトリウム(Th)とウラン(U)を選択的に回収するための連続向流抽出法を系統的に研究した。抽出剤としては、イソパラフィンIP-2028希釈液で調製した一級アミンN1923を用いた。トリウムとウランは、連続ミキサーセトラエクストラクション,スクラビング,逆エクストラクションによって確立された湿式製錬サイクルで選択的に回収され、ラボスケールで実施された。有機相と水相の体積比(O/A比)を管理することにより、ThとUの所望の純度を達成することができる。逆抽出液とラフィネートからそれぞれ高純度のThとUを回収することができ、その後の核物質処理に十分な特性を有している。
Shaimerdenov, A.*; Gizatulin, S.*; Dyussambayev, D.*; Askerbekov, S.*; 植田 祥平; 相原 純; 柴田 大受; 坂場 成昭
Nuclear Engineering and Technology, 54(8), p.2792 - 2800, 2022/08
被引用回数：7 パーセンタイル：88.9(Nuclear Science & Technology)In the core of the WWR-K reactor, a long-term irradiation of tri-structural isotopic (TRISO)-coated fuel particles (CFPs) with a UO kernel was carried out under normal operating conditions of the high-temperature gas-cooled reactor (HTGR). This TRISO fuel was attained at the temperature of 950 to 1,100 C, and the uranium burnup of 9.9% FIMA (fission per initial metal atom) during the irradiation. The release of the gaseous fission product from the fuel was measured in-pile, and its release-to-birth (R/B) ratio was evaluated using the model developed in the High-Temperature Engineering Test Reactor (HTTR) project. After the irradiation test, fuel compacts were subjected to electric dissociation and nondestructive inspections such as X-ray radiography and gamma spectrometry. Finally, it was concluded that integrity of the TRISO fuel irradiated at approximately 9.9% FIMA was demonstrated, and a low fuel failure fraction and a low R/B measured with krypton-88 indicated good performance and reliability of the high burnup TRISO fuel.
仲田 光樹; 大沼 悠一*; Kim, S. K.*
Physical Review B, 105(18), p.184409_1 - 184409_7, 2022/05
被引用回数：2 パーセンタイル：34.67(Materials Science, Multidisciplinary)普遍的熱磁気法則「マグノンWiedemann-Franz則」が非線形応答領域において破れることを理論的に解明することに成功した。
