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墨田 岳大*; 大澤 崇人; Chiu, I.-H.; 池田 篤史
Analytica Chimica Acta, 1329, p.343256_1 - 343256_10, 2024/11
被引用回数:1 パーセンタイル:40.01(Chemistry, Analytical)The uncertainty including accuracy and precision is the most vital factor that determines the overall quality of quantitative analysis. The objectives of this study are (1) to investigate the analytical uncertainty of a prompt gamma-ray analysis (PGA), a chemical interference-free method in principle, on the quantitative analysis of boron and (2) to evaluate the applicability of inductively coupled plasma optical emission spectrometry (ICP-OES), a common technique for quantitative elemental analysis including boron. PGA provided analytical quantity that is equivalent to the true quantity. The analytical uncertainty in both methods was adequately evaluated by comparing the results from PGA and ICP-OES for a series of boron-containing materials with different physical/chemical properties and the major sources of uncertainty in both methods are specified. The evaluation concept demonstrated in this study could be beneficial to a wide range of analytical chemistry.
小林 大志*; 佐藤 祐太郎*; 頓名 龍太郎*; 松村 大樹; 佐々木 隆之*; 池田 篤史
Dalton Transactions (Internet), 53(46), p.18616 - 18628, 2024/10
被引用回数:0 パーセンタイル:0.00(Chemistry, Inorganic & Nuclear)This study investigates the dissolution behaviour of zirconium-cerium oxide solid solution ((Zr,Ce)O/(Ce,Zr)O
), which contains a redox-active metal of Ce (Ce(III/IV)) and is of particular importance in nuclear industry. The solid phases of the solid-solution were comprehensively characterised by powder X-ray diffraction (PXRD) with the Rietveld analysis and X-ray absorption spectroscopy (XAS) with factor analysis, indicating that the solid-solution is primarily composed of tetragonal-(Zr,Ce)O
and cubic-(Ce,Zr)O
. Water immersion of the solid-solution leads to the dissolution of the solid phase at the solid-liquid interface. The addition of a reductant to the system reduces Ce(IV) in the solid-solution to -(III) at the surface, promoting the dissolution of Ce from the solid-solution phase. The release of Ce from the solid-solution also enriches the Zr content in the remaining solid-solution phase at the surface to be more insoluble.
青柳 登; 元川 竜平; 奥村 雅彦; 上田 祐生; 斉藤 拓巳*; 西辻 祥太郎*; 田口 富嗣*; 蓬田 匠; 佐崎 元*; 池田 篤史
Communications Chemistry (Internet), 7, p.128_1 - 128_13, 2024/06
被引用回数:0 パーセンタイル:0.00(Chemistry, Multidisciplinary)Dissipative structures often appear as an unstable counterpart of ordered structures owing to fluctuations that do not form a homogeneous phase. Even a multiphase mixture may simultaneously undergo one chemical reaction near equilibrium and another one that is far from equilibrium. Here, we observed in real-time crystal seed formation and simultaneous nanocrystal aggregation proceeding from tetravalent cerium complexes to ceria nanoparticles in an acidic aqueous solution and investigated the resultant hierarchical nanoarchitecture. The formed particles exhibited two very different size ranges. The hierarchically assembled structures in solutions were ceria colloids, viz. primary core clusters of crystalline ceria and secondary clusters assembled through surface ions. Such self-assembly is widespread in multi-component complex fluids, paradoxically moderating hierarchical reactions. Stability and instability are not only critical but also complementary for co-optimization around the nearby free energy landscape prior to bifurcation.
池田 篤史
分析化学, 73(4.5), p.147 - 159, 2024/04
多変量解析法の一つである因子分析(Factor analysis: FA)は、複数化学種・化合物が混在している分析データから各化学種・化合物の純成分(主因子)に関する情報を抽出するのに強力な手法である。分析化学の分野では、FAはこれまで主に定量分析で多用されてきたが、定性分析への適用・応用例は少なかった。このような背景を踏まえ、本稿は「FAの定性分析への適用」に焦点を当てる。即ち、定性分析に強力な手法の一つであるX線吸収分光(X-ray absorption spectroscopy: XAS)で得られるスペクトルデータの解析にFAを適用し、測定試料中に含まれる化学種・化合物の純成分定性同定を実施するための基本的な考え方・解析の流れを概説、その適用研究例を紹介する。
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3.74.4
m)であった。
Lau, Y.-C.*; 池田 絢哉*; 藤原 宏平*; 小沢 耀弘*; Zheng, J.*; 関 剛斎*; 野村 健太郎*; Du, L.*; Wu, Q.*; 塚崎 敦*; et al.
Physical Review B, 108(6), p.064429_1 - 064429_11, 2023/08
被引用回数:8 パーセンタイル:74.51(Materials Science, Multidisciplinary)Magnetic Weyl semimetals (mWSMs) are characterized by linearly dispersive bands with chiral Weyl node pairs associated with broken time-reversal symmetry. One of the hallmarks of mWSMs is the emergence of large intrinsic anomalous Hall effect. On heating the mWSM above its Curie temperature, the magnetism vanishes while exchange-split Weyl point pairs collapse into doubly degenerate gapped Dirac states. Here, we reveal the attractive potential of these Dirac nodes in paramagnetic state for efficient spin current generation at room temperature via the spin Hall effect. Ni and In are introduced to separately substitute Co and Sn in a prototypal mWSM CoSn
S
shandite film and tune the Fermi level. Composition dependence of spin Hall conductivity for paramagnetic shandite at room temperature resembles that of anomalous Hall conductivity for ferromagnetic shandite at low temperature; exhibiting peak-like dependence centering around the Ni-substituted Co
Ni
Sn
S
and undoped Co
Sn
S
compositions, respectively. The observed spin Hall and anomalous Hall conductivity maxima at different compositions reflect optimum Fermi-level positioning relative to the paramagnetic Dirac and magnetic Weyl states, suggesting the common origin and intercorrelation between the two Hall effects. Our findings highlight a strategy for the quest of spin Hall materials, guided by the abundant experimental anomalous Hall-effect data of ferromagnets in the literature.
Journeau, C.*; Delacroix, J.*; Guvar, C.*; Testud, V.*; Brackx, E.*; Porcheron, E.*; Bouland, A.*; Berlemont, R.*; 池田 篤史
Science Talks (Internet), 6, p.100215_1 - 100215_9, 2023/05
One of the important challenges for the decommissioning of the damaged reactors of the Fukushima Daiichi Nuclear Power Station (1F) is the fuel debris retrieval. The URASOL (URAnium and aeroSOL) project has been undertaken by the French consortium laboratories consisting of ONET, CEA, and IRSN for JAEA. It aims at acquiring basic data on the generation and characteristics of radioactive aerosols from the thermal or mechanical processing of fuel debris simulant. Prototypic fuel debris samples were fabricated based on the average of the lower head compositions computed in the OECD/BSAF benchmark. Samples were heated in an induction furnace to simulate thermal cutting and released aerosols were collected during three temperature ramps using impactors. The collected aerosols were chemically analyzed by ICP-AES and ICP-MS. Iron and tin are the major elements found in these aerosols, followed by chromium and silicon. Significant releases of tellurium, barium and cerium were observed.
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:6 パーセンタイル:56.80(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.
野中 洋亮*; 若林 勇希*; 芝田 悟朗; 坂本 祥哉*; 池田 啓祐*; Chi, Z.*; Wan, Y.*; 鈴木 雅弘*; 田中 新*; 田中 雅明*; et al.
Physical Review Materials (Internet), 7(4), p.044413_1 - 044413_10, 2023/04
被引用回数:5 パーセンタイル:50.30(Materials Science, Multidisciplinary)We study the electronic and magnetic states of as-grown and annealed Fe
O
(111)/Al
O3(111) (
Co, Ni) thin films with various thicknesses grown on Si(111) substrates with the
-Al
O
(111)buffer layers by using X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD), to investigate magnetically dead layers in these films. Although the magnetically dead layers in the as-grown samples are formed near the interface with the Al
O
buffer layer, we reveal that ferrimagnetic order is partially recovered by postdeposition annealing at 973 K for 48 hours in air. By analyzing the line shapes of the XAS and XMCD spectra, we conclude that, in the dead layers, there are a significant number of vacancies at the
sites of the spinel structure, which may be the microscopic origin of the degraded ferrimagnetic order in the
Fe
O
thin films.
平田 早紀子*; 日下 良二; 明地 省吾*; 為国 誠太*; 奥寺 洸介*; 浜田 昇賢*; 坂本 知優*; 本田 匠*; 松下 高輔*; 村松 悟*; et al.
Inorganic Chemistry, 62(1), p.474 - 486, 2023/01
被引用回数:3 パーセンタイル:28.83(Chemistry, Inorganic & Nuclear)A new technique, surface-enhanced infrared absorption (SEIRA) spectroscopy, was used for the structural investigation of lanthanide (Ln) and actinide (An) complexes containing organic ligands. We synthesized thiol derivatives of organic ligands with coordination sites similar to those of diglycolamide (DGA), Cyanex-272, and -tetrakis(2-pyridinylmethyl)-1,2-ethanediamine (TPEN), which have been used for separating Ln and An through solvent extraction. These ligands were attached on a gold surface deposited on an Si prism through S-Au covalent bonds; the gold surface enhanced the IR absorption intensity of the ligands. Aqueous solutions of Ln (Eu
, Gd
, Tb
) and An (Am
) ions were loaded onto the gold surface to form ion complexes. The IR spectra of the ion complexes were obtained using FT-IR spectroscopy in the attenuated total reflection mode. In this study, we developed a new sample preparation method for SEIRA spectroscopy that enabled us to obtain the IR spectra of the complexes with a small amount of ion solution (5
L). This is a significant advantage for the IR measurement of radiotoxic Am
complexes. In the IR spectra of DGA, the band attributed to C=O stretching vibrations at
1630 cm
shifted to a lower wavenumber by
20 cm
upon complexation with Ln and An ions. Moreover, the amount of the red-shift was inversely proportional to the extraction equilibrium constant reported in previous studies on solvent extraction. The coordination ability of DGA toward Ln and An ions could be assessed using the band position of the C=O band. The Cyanex-272- and TPEN-like ligands synthesized in this report also showed noticeable SEIRA signals for Ln and An complexes. This study indicates that SEIRA spectroscopy can be used for the structural investigation of ion complexes and provides a microscopic understanding of selective extraction of Ln and An.
芝田 悟朗; Won, C.*; Kim, J.*; 野中 洋亮*; 池田 啓祐*; Wan, Y.*; 鈴木 雅弘*; 小出 常晴*; 田中 新*; Cheong, S.-W.*; et al.
Photon Factory Activity Report 2022 (インターネット), 2 Pages, 2023/00
Feをインターカレートした遷移金属ダイカルコゲナイド化合物FeTiS
およびFe
TaS
は、巨大な保磁力および垂直磁気異方性を示す強磁性体になることが知られている。我々は以前、Fe
TiS
についてのX線磁気円二色性(XMCD)実験の結果から、Fe
の凍結していない軌道磁気モーメントが結晶場の1次摂動によって直接磁気異方性エネルギーを生むことを明らかにした。今回、Fe
TiS
よりもさらに強い磁気異方性を示す遷移金属ダイカルコゲナイドFe
TaS
について同様にXMCD実験を行い、磁気異方性の強さが何によって左右されているかを探ることを試みた。
塩貝 淳一*; 池田 絢哉*; 藤原 宏平*; 関 剛斎*; 高梨 弘毅; 塚崎 敦*
Physical Review Materials (Internet), 6(11), p.114203_1 - 114203_9, 2022/11
被引用回数:5 パーセンタイル:34.44(Materials Science, Multidisciplinary)Microscopic understanding of magnetization switching via domain nucleation and/or domain-wall propagation is fundamental knowledge for developing magnetic and spintronic devices. Here, we explore the underlying mechanism of the large coercivity of the magnetic Weyl semimetal CoSn
S
thin films, which is roughly ten times larger than that of Co
Sn
S
bulk single crystal, by measuring Hall resistance in constricted wire devices. The discretized steplike variations appear in the hysteresis loops of the Hall resistance in 0.6 micrometers wide and narrower devices, indicating that the size of the reversed magnetic domain is comparable to the active area of the Hall devices. By counting the number of discrete features, the average diameter of the reversed magnetic domain is estimated to be 80 nm. Individually, the diameter of the reversed domain nucleus is evaluated to be roughly 2 nm. Considering the difference in the diameters of the reversed magnetic domain and the reversed domain nucleus, we ascribed the large coercivity of the Co
Sn
S
thin films to a large nucleation field owing to the uniform crystallinity within grains and strong domain-wall pinning at grain boundaries specific to the thin films. With the large nucleation field in the films, an engineering of the domain-wall pinning sites is a promising approach to control the nucleation, manipulation, and detection of the single domain wall in Co
Sn
S
thin-film devices.
墨田 岳大; 池田 篤史
Isotope News, (783), p.28 - 32, 2022/10
原著論文「High temperature reaction of multiple eutectic-component system; The Case of solid metallic Zr and molten SUS-BC」の解説記事である。
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。
Johansen, M. P.*; Child, D. P.*; Collins, R.*; Cook, M.*; Davis, J.*; Hotchkis, M. A. C.*; Howard, D. L.*; Howell, N.*; 池田 篤史; Young, E.*
Science of the Total Environment, 842, p.156755_1 - 156755_11, 2022/10
被引用回数:6 パーセンタイル:41.40(Environmental Sciences)While they have appeared only recently in earth's history, radioactive particles from anthropogenic sources are widespread in global environments and present radiological harm potentials to living organisms. Here we compare a varied set of particles from past nuclear fission and non-fission sources in Australia of highly diverse magnitudes, release modes, and environments. Numerous radioactive particles persist in soils 60 + years after their release events. Particles can be distinguished by their Ca/Fe and Si/Fe elemental ratios, which in this study range over orders of magnitude and reflect the materials available during their individual formation events. The particles from nuclear testing have dominant Pu activity concentrations, relative to
Sr and
Cs, which increases long-term radiological hazard from alpha emissions if inhaled or ingested, and contrasts with particles from nuclear power accidents (e.g., Fukushima). Internal fracturing is more prevalent than previously reported, and fracturing is greater in Ca-rich vs. Si-dominated matrices.
坪田 陽一; 本田 文弥; 床次 眞司*; 玉熊 佑紀*; 中川 貴博; 池田 篤史
Nuclear Instruments and Methods in Physics Research A, 1030, p.166475_1 - 166475_7, 2022/05
被引用回数:4 パーセンタイル:53.47(Instruments & Instrumentation)福島第一原子力発電所(1F)の長期的な廃止措置において、損傷した原子炉に残存する核燃料デブリの取り出しは、技術的に多くの困難を伴う不可避の重要課題である。デブリ取り出しは機械的な切断を伴い、放射性核種を含む微粒子(
エアロゾル)が高濃度で発生し、吸入時の健康リスクが大きい。1Fの解体・廃止措置における作業員の放射線被ばくを最小化するためには、粒子の発生場所である原子炉格納容器(PCV)内における
エアロゾルの濃度を監視することが重要である。このため、
エアロゾルのin-situモニタリングシステム(in-situ alpha air monitor: IAAM)を開発し、1Fの実環境で想定される条件下でその技術的性能を検証した。IAAMは次の4つの技術的要求を満たすことが確認された。(1)高湿度下での安定動作、(2)フィルターレス動作、(3)高計数率の
線測定能力、(4)高バックグラウンドの
/
線下でも
線が選択的に測定できること。IAAMは、高湿度環境(相対湿度100%)及び
/
線高バックグラウンド(最大100mSv/hの
線)下で、濃度3.3
10
Bq/cm
以上の
エアロゾルを計数の飽和なしに、選択的に測定することが可能であることが確認された。これらの結果は、IAAMが燃料デブリの解体時及び1Fの長期的な廃止措置全体において、信頼性の高い
エアロゾルのモニタリングシステムとして利用できる可能性を示すものである。
上原 章寛*; 秋山 大輔*; 池田 篤史; 沼子 千弥*; 寺田 靖子*; 新田 清文*; 伊奈 稔哲*; 武田 志乃*; 桐島 陽*; 佐藤 修彰*
Journal of Nuclear Materials, 559, p.153422_1 - 153422_11, 2022/02
被引用回数:4 パーセンタイル:53.26(Materials Science, Multidisciplinary)The reaction products were analysed by a combination of powder X-ray diffraction (PXRD) and X-ray absorption spectroscopic measurements of the U L- and Zr K-edges. Under an oxidizing atmosphere, the formation of U
O
and U
Zr
O
was observed in equilibrium with UO
, monoclinic-ZrO
, and tetragonal-ZrO
. However, when O
gas was purged through the reaction tube during the cooling process to room temperature, pentavalent U in ZrU
O
was produced by the oxidation of solid solution UO
formed at
1774 K during the temperature dropped at
1473 K. Under the inert atmosphere, mixed oxides of uranium were found to form at
1673 K due to a low concentration of O
impurity with the Ar gas. This study can pave the way for understanding the interaction between the nuclear fuels and the cladding materials in damaged reactors enabling further simulation of possible decontamination procedures.
墨田 岳大; 須藤 彩子; 高野 公秀; 池田 篤史
Science and Technology of Advanced Materials; Methods (Internet), 2(1), p.50 - 54, 2022/02
Despite a wide variety of its practical applications, handiness, and cost-effectiveness, the advance of lamp-based heating device is obstructed by one technical difficulty in measuring the temperature on a heated material. This difficulty originates in the combination of polychromatic light source and a radiation thermometer that determines temperature from radiation (i.e. light). A new system developed in this study overcomes this intrinsic difficulty by measuring exclusively the radiation from the heated material, allowing us to perform the direct and measurement of temperature in a light-based heating device (an arc image furnace). Test measurements demonstrated the reliability of temperature measurement using the developed system as well as its promising potential for the determination of emissivity at high temperature particularly in the infrared region.
墨田 岳大; 小畠 雅明; 高野 公秀; 池田 篤史
Materialia, 20, p.101197_1 - 101197_11, 2021/12
The eutectic melting, one of the fundamental phenomena in high temperature reactions involving liquid phases, is a primitive but important subject for both scientific and industrial fields associated with metallurgy. The present study aims at revealing the formation and reaction mechanisms of the multiple eutectic-component system consisting of solid metallic Zr and molten stainless steel- boron carbide (SS-BC) by combining multiple analytical methods (i.e. powder X-ray diffraction (PXRD), scanning electron microscopy- energy dispersive X-ray spectroscopy (SEM-EDS), and dynamic secondary ion mass spectrometry (D-SIMS)) with thermodynamical consideration. The results indicate that the solidified Zr-SS-B
C mixture is composed of major phases of (Fe,Cr)
Zr, (Fe,Cr,Ni)
Zr, (Ni,Fe)Zr
, ZrB
, and a minor phase of ZrC. The results also reveal that the eutectic melting between solid metallic Zr and molten SS-B
C can be described as the combination of diffusion kinetics and thermodynamic stability. That is, the initial formation of ZrC and ZrB
layers at the reaction interface significantly retards the diffusion of other SS-B
C components (i.e. Cr, Fe, and Ni) into solid metallic Zr.
Fichter, S.*; Radoske, T.*; 池田 篤史
Acta Crystallographica Section E; Crystallographic Communications (Internet), 77(8), p.847 - 852, 2021/08
A new type of polyoxo cluster complex that contains thirteen uranium atoms, {U}, was synthesised and characterised as [U
(
-O
)
(
-O
)
(
-O
)
Cl
(O
)
] (x = 2.3, MeO = methoxide) (I). The complex crystallises from methanol containing tetravalent uranium (U
) with a basic organic ligand. The characterised {U
} polyoxo cluster complex possesses a single cubic uranium polyhedron at the centre of the cluster core. The observed shortening of U-O bonds, together with BVS calculations and the overall negative charge (2-) of (I), suggests that the central uranium atom in (I), that forms the single cubic polyhedron, is presumably oxidised to the pentavalent state (U
) from the original tetravalent state (U
). Complex I is, hence, the first example of a polyoxo cluster possessing a single cubic coordination polyhedron of U
.