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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.
岩瀬 裕希*; 赤松 允顕*; 稲村 泰弘; 坂口 佳史*; 森川 利明*; 笠井 聡*; 大内 啓一*; 小林 一貴*; 酒井 秀樹*
Journal of Applied Crystallography, 56(1), p.110 - 115, 2023/02
被引用回数：2 パーセンタイル：85.44(Chemistry, Multidisciplinary)光応答性材料の重要性が高まる中、光照射によって引き起こされる構造変化とその機能との相関を解析することは極めて重要である。このような構造解析には小角散乱(SAS)が有効であるが、SASによって1nm以下のスケールで局所的な分子構造形成や分子反応を定量的に捉えることは困難である。そこで本研究では、光応答性物質における非平衡現象の構造解析を目的として、紫外可視光照射装置、紫外可視分光光度計から構成される新しい試料環境を開発し、中性子小角・広角散乱装置(TAIKAN)に設置することで中性子小角散乱と紫外可視光吸収の同時測定を実現した。この測定手法を用いることで、光応答性分子であるアゾベンゼンを修飾した陽イオン性界面活性剤が水溶液中で形成するミセルが紫外可視光照射によって構造変化する様子をその場観察することを可能とした。その結果、本測定手法によりミセル構造の変化と分子配置の変化の相互作用に関する直接的な情報を提供することが示された。
藤原 悟*; 松尾 龍人*; 杉本 泰伸*; 柴田 薫
Journal of Physical Chemistry Letters (Internet), 10(23), p.7505 - 7509, 2019/12
被引用回数：4 パーセンタイル：21.85(Chemistry, Physical)無秩序なポリペプチド鎖のダイナミクスの特性評価は、本質的に無秩序状態なタンパク質およびフォールディングプロセスに関連する非ネイティブ状態下のタンパク質の挙動を解明するために必要である。本研究では、小角X線散乱測定データと動的光散乱測定データと組み合わせて準弾性中性子散乱測定データから、タンパク質のセグメント運動と分子全体の拡散および局所側鎖運動を評価する方法を独自に開発した。そしてこの方法を、非フォールディング状態およびメルトグロビュール(MG)状態のタンパク質RNase Aに適用し、セグメント運動から生じる拡散係数を評価し、非フォールディング状態とMG状態で異なる値をとることを明らかにした。またこの方法で得られた値は、蛍光現象を用いた別の測定技術を使用して得られた値と一致していることも確認できた。これらの研究成果は、この方法の、さまざまな無秩序状態でのタンパク質の挙動を特徴付ける実行可能性だけでなく、有用性も示している。
-synuclein related to propensity to amyloid fibril formation藤原 悟*; 河野 史明*; 松尾 龍人*; 杉本 泰伸*; 松本 友治*; 成田 哲博*; 柴田 薫
Journal of Molecular Biology, 431(17), p.3229 - 3245, 2019/08
被引用回数：14 パーセンタイル：49.22(Biochemistry & Molecular Biology)パーキンソン病発症には、脳細胞中の「-シヌクレイン」というタンパク質が線維状に集合した状態(「アミロイド線維」と呼ばれる)となることが関係すると考えられており、どのようなメカニズムでこのアミロイド線維が形成されるのかに強い関心が寄せられている。そこで研究チームは、タンパク質分子の「動き」に着目し、アミロイド線維のできやすさが様々に異なった条件でのタンパク質の動きを、J-PARCの中性子準弾性散乱装置を用いて調べた。その結果、タンパク質分子の動きの違いによりアミロイド線維のできやすさが変わること、特にアミロイド線維ができるためには、タンパク質同士が集合しやすくなるような特定の動きが必要なことを明らかにした。
勅使河原 誠; 土川 雄介*; 市川 豪*; 高田 慎一; 三島 賢二*; 原田 正英; 大井 元貴; 河村 幸彦*; 甲斐 哲也; 河村 聖子; et al.
Nuclear Instruments and Methods in Physics Research A, 929, p.113 - 120, 2019/06
被引用回数：16 パーセンタイル：86.05(Instruments & Instrumentation)ナノダイアモンドは、冷中性子以下のエネルギーにおける反射材として注目されている。ナノダイアモンドを用いた中性子源の高度化には、断面積データの整備が必要である。そのため、この論文では、中性子の透過率の測定から0.2meVから100meVの範囲で全断面積を測定した結果を報告する。測定した全断面積は、エネルギーが低くなるにつれて大きくなり、グラファイトと比較すると0.2meVで約2桁以上高くなることが分かった。その全断面積に占める非弾性散乱の寄与を調べるため、中性子のエネルギー1.2, 1.5, 1.9及び5.9meVで中性子非弾性散乱実験を行った。その結果、測定したエネルギーにおいて、全断面積に占める非弾性散乱の寄与がほぼ無視できることも分かった。さらに、中性子小角散乱実験の結果から、全断面積の高くなる要因として、前方方向、いわゆる小角方向への散乱の寄与が高いことが示された。
大場 洋次郎*; 諸岡 聡; 大石 一城*; 鈴木 淳市*; 高田 慎一; 佐藤 信浩*; 井上 倫太郎*; 土山 聡宏*; Gilbert, E. P.*; 杉山 正明*
Journal of Applied Crystallography, 50(2), p.334 - 339, 2017/04
被引用回数：3 パーセンタイル：29.28(Chemistry, Multidisciplinary)Recent progress of pulsed neutron sources has enabled energy-resolved analysis of neutron attenuation spectra, which include information on neutron scattering. In this study, a new analysis technique for small-angle neutron scattering (SANS) is demonstrated. A clear difference is observed in the neutron attenuation spectra between steels with different nanostructures; this difference can be understood as arising from attenuation due to SANS. The neutron attenuation spectra, calculated from the corresponding SANS profiles, agree well with the experimentally observed attenuation spectra. This result indicates that measurement of neutron attenuation spectra may enable the development of a novel experimental technique, i.e. energy-resolved SANS (ESANS).
岡 弘; 丹野 敬嗣; 大塚 智史; 矢野 康英; 上羽 智之; 皆藤 威二; 大沼 正人*
Nuclear Materials and Energy (Internet), 9, p.346 - 352, 2016/12
被引用回数：21 パーセンタイル：88.83(Nuclear Science & Technology)The effect of thermo-mechanical treatments (TMTs) on the evolution of nano-structure in an oxide dispersion strengthened (ODS) ferritic/martensitic steel (Fe-9Cr-2W-0.22Ti-0.36Y
O
) was investigated. TMTs involve hot extruding and subsequent forging, which are expected to be part of a future industrial-scale manufacturing process of the ODS steel. It was shown that the ODS steel was composed of two phases - a fine-grained residual ferrite phase and a transformable martensite phase. The number density of the nano-sized particles in the residual ferrite phase was significantly higher than that in the martensite phase. The TMTs did not significantly affect the number density, but slightly affected the size distribution of the nano-sized particles in both ferrite phase and martensite phase. Moreover, the volume fraction of the residual ferrite phase decreased after TMTs. In summary, the TMT conditions could be a parameter which affects the nano-structure of the ODS steel.
大場 洋次郎*; 諸岡 聡; 佐藤 博隆*; 佐藤 信浩*; 井上 倫太郎*; 杉山 正明*
波紋, 26(4), p.170 - 173, 2016/11
Based on the time-of-light (TOF) technique, new generation pulsed neutron sources enable novel neutron scattering experiments. Using small-angle neutron scattering (SANS) at the pulsed neutron sources, simultaneous measurements of SANS and Bragg edge transmission can be performed. From the SANS profiles, the precipitates and inclusions in metals and alloys are characterized, while the Bragg edge transmission spectra give crystallographic information about the matrix. This is a powerful tool for quantitative characterization of the microstructures in the metals and alloys. The neutron transmission experiments have potential for further development. Magnetic Bragg edge transmission analysis will be useful for magnetic materials. These new neutron scattering techniques enhance the usability and flexibility of neutron scattering experiments.
大場 洋次郎*; 諸岡 聡; 大石 一城*; 佐藤 信浩*; 井上 倫太郎*; 足立 望*; 鈴木 淳市*; 土山 聡宏*; Gilbert, E. P.*; 杉山 正明*
Journal of Applied Crystallography, 49(5), p.1659 - 1664, 2016/10
被引用回数：13 パーセンタイル：66.73(Chemistry, Multidisciplinary)Pulsed neutron sources enable the simultaneous measurement of small-angle neutron scattering (SANS) and Bragg edge transmission. This simultaneous measurement is useful for microstructural characterization in steel. Since most steels are ferromagnetic, magnetic scattering contributions should be considered in both SANS and Bragg edge transmission analyses. An expression for the magnetic scattering contribution to Bragg edge transmission analysis has been derived. The analysis using this expression was applied to Cu steel. The ferrite crystallite size estimated from this Bragg edge transmission analysis with the magnetic scattering contribution was larger than that estimated using conventional expressions. This result indicates that magnetic scattering has to be taken into account for quantitative Bragg edge transmission analysis. In the SANS analysis, the ratio of magnetic to nuclear scattering contributions revealed that the precipitates consist of body-centered cubic Cu
Fe
and pure Cu, which probably has 9R structure including elastic strain and vacancies. These results show that effective use of the magnetic scattering contribution allows detailed analyses of steel microstructure.
ion conductivity of styrene-ethylene oxide multiblock copolymer electrolytesSarapas, J. M.*; 西条 賢次*; Zhao, Y.; 竹中 幹人*; Tew, G. N.*
Polymers for Advanced Technologies, 27(7), p.946 - 954, 2016/07
被引用回数：10 パーセンタイル：36.08(Polymer Science)A molecular weight series of PS-PEO multiblock copolymers was synthesized by the thiol-norbornene click reaction. These materials were characterized both as neat and lithium 
-trifluorosulfonimide salt loading samples. The neat samples demonstrated the crystallinity increases with PEO contents. The lithium ion-containing samples had broad scattering peaks, half of which displayed disordered scattering. Fitting of disordered scattering peaks by the random phase approximation, yielded the effective Flory-huggins parameter (
) and radius of gyration (
) values that were compared to recent predictive works by Balsara and coworkers. The samples were also analyzed by electrochemical impedance spectroscopy for their potential to conduct lithium ions and those with the volume fraction of PEO larger than 0.5 demonstrated robust conductivity.
Zhao, Y.; 吉田 実留*; 大島 竜也*; 小泉 智*; 陸川 政弘*; Szekely, N.*; Radulescu, A.*; Richter, D.*
Polymer, 86, p.157 - 167, 2016/03
被引用回数：13 パーセンタイル：44.52(Polymer Science)We investigated the structure and the swelling behavior of two synthesized hydrocarbon polymer electrolyte membranes, made of multiblock copolymer poly(sulphonate phenylene)-b-poly(arylene ether ketone) with different block ratios, by using small-angle neutron scattering technique. A scattering maximum (ionomer peak) at high-q range is shown commonly in both dry and wet states, with q being the magnitude of the scattering vector, while it shifts towards low-q region in the wet state due to the swelling of the ionomer domains with water. The swelling effect also results to a second scattering maximum in the middle-q range because of the water-induced microphase separation. The morphology in this q-range was elucidated in terms of Hard-Sphere model with Percus-Yervick interference approximation.
Zhao, Y.; 吉村 公男; 猪谷 秀幸*; 山口 進*; 田中 裕久*; 小泉 智*; Szekely, N.*; Radulescu, A.*; Richter, D.*; 前川 康成
Soft Matter, 12(5), p.1567 - 1578, 2016/02
被引用回数：27 パーセンタイル：79.79(Chemistry, Physical)We investigated the interplay between morphology and properties of a new graft-type of anion exchange membranes (AEMs) containing 2-methylimidazolium groups by using contrast variation small angle neutron scattering (SANS) technique. These AEMs prepared by radiation-induced grafting of 2-methyl-1-vinylimidazole and styrene into poly(ethylene-co-tetrafluoroethylene) (ETFE) films, possessed both high alkaline durability and high conductivity. The SANS measurement reveals that these membranes are consisted of three phases: crystalline lamellar and crystallite domains originating from the pristine ETFE, which offer good mechanical properties, hydrophobic amorphous domains, which offer a matrix to create conducting regions, and interconnected hydrated domains, which are composed of the entire graft chains and water and play a key role to promote the conductivity.
松尾 龍人; 武田 壮一*; 小田 俊郎*; 藤原 悟
Biophysics and Physicobiology (Internet), 12, p.145 - 158, 2015/12
Troponin (Tn), consisting of three subunits, TnC, TnI, and TnT, is a protein that plays a major role in regulation of muscle contraction. Various mutations of Tn cause familial hypertrophic cardiomyopathy. Here we focus on the mutations E244D and K247R of TnT, which induce an increase in the maximum tension of cardiac muscle without changes in Ca
-sensitivity, and carried out small-angle X-ray scattering experiments on the Tn core domain containing the wild type subunits and those containing the mutant TnT in the absence and presence of Ca. Changes in the overall shape induced by the mutations were detected for the first time by the changes in the radius of gyration and the maximum dimension between the wild type and the mutants. Analysis by model calculations shows that TnC adopts a dumbbell structure regardless of the mutations, and that the mutations change the distributions of the conformational ensembles so that the flexible N- and C-terminal regions of TnT become close to the center of the whole molecule.
Zhao, Y.; 小泉 智*; 近藤 哲男*
JPS Conference Proceedings (Internet), 8, p.033002_1 - 033002_6, 2015/09
Incoherent neutron scattering contribution presents a challenge in the structure characterization of many target materials. In this study, we introduce a method of intermediate angle neutron scattering (IANS) to correct the small angle neutron scattering (SANS) data of the water-swollen microbial cellulose (MC) sample, the system of which has significant incoherent contributions from the water solvent, and we describe the effects that the corrections have on the structural analysis. In order to elucidate the structure, the solvent is changed in situ from protonated water to deuterated water to give different scattering contrast, and this water-exchange process has been followed by time-resolved SANS and IANS simultaneously. Our results show that: (1) after incoherent correction, the structure of MC sample is proved to be invariant with solvents; (2) the scattering intensity depends only on the contrast factor, revealing a two-phase system composed of water-resistant crystalline cellulose phase and hydrated phase; (3) The cellulose crystallites have a constant scattering length density of 2.0
10
cm
, determined by the matching point at which the scattering contrast between the two phases is minimum. This value is consistent with that of 1.910cm estimated from its chemical structure.
依田 修
Journal of Applied Crystallography, 17, p.337 - 343, 1984/00
被引用回数：12 パーセンタイル：63.47(Chemistry, Multidisciplinary)全反射ガラスミラーと水晶モノクロメータを組み合わせて、X線を検出器位置に点状に収束させ、散乱強度を一次元位置敏感型検出器(PSPC)によって測定する高分解能小角散乱装置を試作した。この装置の設計、性能を詳述した。
Si土井 健治; 茅野 秀夫*; 増本 健*
Journal of Applied Crystallography, 11(5), P. 605, 1978/00
非晶質合金PdSiをJMTRの速中性子により510
/cmのフルエンスに照射した試料のX線小角散乱を測定した。X線広角散乱には照射による変化は殆ど認められないことはすでに報告した(登録No.A-7199)。CuK線を用い散乱角15'~5°の範囲の測定を行ったところ、照射によりこの範囲の散乱強度が著しく増大していることを見た。未照射試料についてはこの範囲での散乱強度は殆ど0である。この散乱強度分布より、中性子照射により数10
程度の構造のゆらぎが生じたことを結論した。前報の結果と併せて非晶質物質の照射損傷の様子が結晶性物質のそれとどのように異なるかについて一般的な考察を行なう。
Hu, Q.*; Wang, Q.*; Oware, P.*; 舘 幸男; 深津 勇太; Ilavsky, J.*; Almer, J.*
no journal, ,
Pore connectivity is important in controlling fluid flow and mass transport in porous natural rocks. A different extent of pore connectivity can be reflected in the proportion of isolated pore space not connected to the surface of natural rocks. This work presents the multi-approach and multi-scale laboratory studies to investigating the proportion of isolated pore space of, and its resultant anomalous fluid flow and radionuclide movement in, generic geological barrier materials. The samples include mudstone from Wakkanai formation, Opalinus clay from Mt. Terri as well as granodiorite from Grimisel, salt rock from Waste Isolation Pilot Plant in New Mexico, and welded tuff in Yucca Mountain. The independent quantification of both (1) surface-accessible pore space with various probing fluids (e.g., micron-scale tracer mapping using laser ablation-ICP-MS); and (2) total porosity by small angle X-ray scattering. Our complementary approaches provide a rich toolbox for tackling the pore structure characteristics in geological barrier materials, and associated fluid flow and radionuclide transport.
