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Laser heating induced spatial homogenization of phase separated Na$$_{2}$$O-B$$_{2}$$O$$_{3}$$-SiO$$_{2}$$ glass plate with bearing NiO for heat center and structural probe

富田 夏奈*; 岸 哲生*; 松村 大樹; 矢野 哲司*

Journal of Non-Crystalline Solids, 597, p.121891_1 - 121891_10, 2022/12

 被引用回数:0 パーセンタイル:0.02(Materials Science, Ceramics)

Na$$_{2}$$O-B$$_{2}$$O$$_{3}$$-SiO$$_{2}$$ glass plate phase separated in spinodal was partially remelted and homogenized by laser heating. As heat generation source, 0.8 mol% NiO was added to absorb continuous-wave laser with $$lambda$$=1064 nm. After acid leaching, borate phase with NiO was remaining partially in laser irradiated area. X-ray Absorption Fine Structure (XAFS) spectra revealed that Ni$$^{2+}$$ in laser irradiated area showed coordination change from 6 coordinated octahedral to 5 coordinated in square pyramid along with apparent color change from green to brown. Similar change was observed in water-quenched specimen from 1000$$^{circ}$$C. Ni$$^{2+}$$ transition gave additional structural information in phase separate / homogeneous glass, which was difficult to be distinguished by spectroscopy which focuses on covalent bonding of glass network.


Structural change by phosphorus addition to borosilicate glass containing simulated waste components

岡本 芳浩; 塩飽 秀啓; 嶋村 圭介*; 小林 秀和; 永井 崇之; 猪瀬 毅彦*; 佐藤 誠一*; 畠山 清司*

Journal of Nuclear Materials, 570, p.153962_1 - 153962_13, 2022/11

モリブデンの溶解度を高める効果があるリンを含む模擬核廃棄物ガラス試料を作製し、放射光X線吸収微細構造(XAFS)分析によりいくつかの構成元素を、ラマン分光分析によりその配位構造を分析した。分析では、リンの添加量や廃棄物積載率の違いによる局所構造および化学状態の変化を系統的に調べた。その結果、最大廃棄物量30wt%(MoO$$_3$$ 1.87mol%に相当)においても、モリブデン酸塩化合物による結晶相は観察されなかった。廃棄物充填率を上げると酸化が進行し、リンを添加すると還元が進行した。さらに、それらの酸化と還元の効果が相殺されるケースもみられた。特定元素の周辺局所構造は、主に廃棄物充填率の影響を受けるZn、廃棄物充填率とリン添加の両方の影響を受けるCe、どちらの影響も受けないZr元素に分類された。Moと他の元素の分析結果の比較から、添加したリンは遊離されたPO$$_4$$構造単位として存在し、モリブデン酸イオンに配位するアルカリ金属を奪い取っている可能性があると考えられた。



永井 崇之; 岡本 芳浩; 山岸 弘奈*; 小島 一男*; 猪瀬 毅彦*; 佐藤 誠一*; 畠山 清司*

JAEA-Research 2022-008, 37 Pages, 2022/10




Synergistic hybrid electrocatalysts of platinum alloy and single-atom platinum for an efficient and durable oxygen reduction reaction

Liu, B.*; Feng, R.*; Busch, M.*; Wang, S.*; Wu, H.*; Liu, P.*; Gu, J.*; Bahadoran, A.*; 松村 大樹; 辻 卓也; et al.

ACS Nano, 16(9), p.14121 - 14133, 2022/09

Pt single-atom materials possess an ideal atom economy but suffer from limited intrinsic activity and side reaction of producing H$$_{2}$$O$$_{2}$$ in catalyzing the oxygen reduction reaction (ORR). Here, we demonstrate that anchoring platinum alloys on single-atom Pt-decorated carbon (Pt- SAC) surmounts their inherent deficiencies, thereby enabling a complete four-electron ORR pathway catalysis with high efficiency and durability. Pt$$_{3}$$Co@Pt-SAC demonstrates an exceptional mass and specific activities 1 order of magnitude higher than those of commercial Pt/C. They are durable throughout 50000 cycles, showing only a 10 mV decay in halfwave potential. The superior durability is attributed to the shielding effect of the Pt-SAC coating, which significantly mitigates the dissolution of Pt$$_{3}$$Co cores.


Operando Br K-edge dispersive X-ray absorption fine structure analysis for Br$$^{-}$$/Br$$_{3}$$$$^{-}$$ redox mediator for Li-Air batteries

伊藤 仁彦*; 松村 大樹; Song, C.*; 久保 佳美*

ACS Energy Letters (Internet), 7(6), p.2024 - 2028, 2022/06

 被引用回数:0 パーセンタイル:0.01(Chemistry, Physical)

The behavior of Br$$^{-}$$/Br$$_{3}^{-}$$ redox mediator (RM), which has been shown to suppress charging overpotential in lithium-air batteries, has been detected for the first time using operando Br K-edge dispersive X-ray absorption fine structure. Br$$_{3}^{-}$$ ions in the electrolyte increase monotonically after $$sim$$ 30% charging, which indicates that a part of Br$$_{3}^{-}$$ formed via the oxidation of Br$$^{-}$$ during charging does not oxidize Li$$_{2}$$O$$_{2}$$ as RM but gets accumulated in the cell. Consistent with this result, the O$$_{2}$$ evolution efficiency gradually decreases from the initial 100% as the charging progresses, and CO$$_{2}$$ is emitted at the end of the charging. All these results clearly show that the Br$$^{-}$$/Br$$_{3}^{-}$$ RM functions effectively at the beginning of charging but gradually loses its function as charging proceeds.


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

 被引用回数:1 パーセンタイル:77.26(Chemistry, Analytical)

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.


Influences of hydration-dehydration on local structure in layered perovskite LaSr$$_{3}$$Fe$$_{3}$$O$$_{10}$$

八木 祐太朗*; 脇田 雄大*; 籠宮 功*; 松江 郁弥*; 柿本 健一*; 松村 大樹; 米田 安宏

ChemistrySelect (Internet), 7(21), p.e202104575_1 - e202104575_7, 2022/06

 被引用回数:0 パーセンタイル:0(Chemistry, Multidisciplinary)

The layered perovskite LaSr$$_{3}$$Fe$$_{3}$$O$$_{10}$$ (LSF) easily hydrates under ambient air. The hydrated LSF transports hydroxides in the middle-temperature range of 100 $$^circ$$C - 250 $$^circ$$C. This study used X-ray absorption fine structure analysis on normal and hydrated LSF from room temperature to 350 $$^circ$$C to evaluate the relationship between local structures and ion transport characteristics. The H$$_{2}$$O molecules are mainly intercalated into rock-salt interlayers, which are close to the La1 and O3 sites. The generated OH$$^{-}$$ ions are found at O3 sites, which are closer to Sr ions than La ions. The intercalated H$$_{2}$$O molecules and formed OH$$^{-}$$ ions expand the spaces of the rock-salt interlayers. The temperature dependence of the local crystal structure was also studied in this study. According to the findings, the presence of OH$$^{-}$$ ions on the O3 sites, which are closer to Sr ions, plays a significant role in OH$$^{-}$$ transport in the medium temperature range.


Repeatable photoinduced insulator-to-metal transition in yttrium oxyhydride epitaxial thin films

小松 遊矢*; 清水 亮太*; 佐藤 龍平*; Wilde, M.*; 西尾 和記*; 片瀬 貴義*; 松村 大樹; 齋藤 寛之*; 宮内 雅浩*; Adelman, J. R.*; et al.

Chemistry of Materials, 34(8), p.3616 - 3623, 2022/04

 被引用回数:3 パーセンタイル:66.25(Chemistry, Physical)

Here, we demonstrate such a highly repeatable photoinduced insulator-to-metal transition in yttrium oxyhydride (YO$$_{x}$$H$$_{y}$$) epitaxial thin films. The temperature ($$T$$) dependence of the electrical resistivity ($$rho$$) of the films transforms from insulating to metallic ($$drho/dT > 0$$) under ultraviolet laser illumination. The sample is heated (125 $$^{circ}$$C) under an Ar atmosphere to recover its original insulating state. The films recover their original metallic conductivity when subsequently subjected to ultraviolet laser illumination, showing repeatable photoinduced insulator-to-metal transition. First principles calculations show that the itinerant carriers originate from the variations in the charge states of the hydrogen atoms that occupy octahedral interstitial sites. This study indicates that tuning the site occupancy (octahedral/tetrahedral) of the hydrogen atoms exerts a significant effect on the photoresponse of metal hydrides.


Dispersive XAFS Study on the Laser-Induced Reduction of a Rh$$^{3+}$$ ion complex; Presence of a Rh$$^{+}$$ Intermediate in Direct Photoreduction

佐伯 盛久*; 松村 大樹; 中西 隆造*; 蓬田 匠; 辻 卓也; 齋藤 寛之*; 大場 弘則*

Journal of Physical Chemistry C, 126(12), p.5607 - 5616, 2022/03

 被引用回数:1 パーセンタイル:66.25(Chemistry, Physical)

パルス紫外線レーザー照射によって引き起こされるRh$$^{3+}$$イオン錯体のRh$$^{0}$$種への直接光還元反応機構を、分散型X線吸収微細構造(DXAFS)分光法によって調べた。時間分解X線吸収端近傍構造(XANES)には等吸収点がなく、Rh$$^{3+}$$の直接光還元に2種類以上のRh$$^{n+}$$が寄与することを示した。時間分解XANESデータの特異値解析から、直接光還元には3つのRh$$^{n+}$$種が関与することが示唆された。時間分解XANESデータを、交互最小二乗法による多変量解析(MCR-ALS)により解析したところ、3つのRh$$^{n+}$$種の純粋なスペクトルと濃度プロファイルが得られた。Rh$$^{n+}$$種は、3つのXANESスペクトルの特徴から、Rh$$^{3+}$$, Rh$$^{+}$$, Rh$$^{0}$$種に分類できた。得られた濃度プロファイルから、Rhの直接光還元はRh$$^{3+}$$ $$rightarrow$$ Rh$$^{+}$$ $$rightarrow$$ Rh$$^{0}$$の順で進行することが示唆され、Rh$$^{3+}$$とRh$$^{+}$$の光還元、Rh$$^{3+}$$とRh$$^{+}$$の光による自己触媒的還元、Rh$$^{+}$$の光酸化による反応機構により、3種のRh$$^{n+}$$の濃度プロファイルがよく再現できることが示された。


Mn L$$_{2,3}$$-edge EXAFS and magnetic EXAFS studies on the halfmetallic ferromagnet Co$$_{2}$$MnSi

向後 純也*; 藤原 秀紀*; 関山 明*; 斎藤 祐児; 梅津 理恵*; 二木 かおり*

Journal of the Physical Society of Japan, 91(3), p.034702_1 - 034702_12, 2022/03

 被引用回数:0 パーセンタイル:0(Physics, Multidisciplinary)

We report magnetic circular dichroism in extended X-ray absorption fine structure (EXAFS) in a prototypical halfmetallic ferromagnet, Co$$_{2}$$MnSi. The EXAFS oscillations at the Mn L$$_{2,3}$$ edges are analyzed to obtain parameters used in the analysis of the magnetic EXAFS (MEXAFS). Theoretical calculations of MEXAFS spectra in Co$$_{2}$$MnSi show that the linear-path scatterings have larger contributions than the multiple triangular-path scatterings. Furthermore, the period of the oscillations in the MEXAFS spectra is shorter than that in the EXAFS spectra indicating that the far site contributions from the second to the fourth nearest neighbor Co and the third nearest Si atoms can strongly influence the MEXAFS oscillations, while the Mn atoms, despite the large magnetic moment, can have little contributions due to the interference of the spin components.


Activity enhancement of platinum oxygen-reduction electrocatalysts using ion-beam induced defects

木全 哲也*; 垣谷 健太*; 山本 春也*; 下山 巖; 松村 大樹; 岩瀬 彰宏*; Mao, W.*; 小林 知洋*; 八巻 徹也*; 寺井 隆幸*

Physical Review Materials (Internet), 6(3), p.035801_1 - 035801_7, 2022/03

 被引用回数:2 パーセンタイル:0(Materials Science, Multidisciplinary)

High activity is one of the primary requirements for the catalysts in proton exchange membrane fuel cell applications. Previous computational studies suggested that the catalytic activity of Pt nanoparticles could be enhanced by a Pt-carbon (C) support interaction. We have recently found that an enhanced electronic interaction occurs at the interface between an argon-ion (Ar$$^{+}$$)-irradiated glassy carbon (GC) surface and Pt nanoparticles. Here, we report a more than two-fold increase in specific activity (SA) for the Pt nanoparticles on the Ar$$^{+}$$-irradiated GC substrate compared to that on the non-irradiated GC substrate. The mechanism of this activity enhancement was investigated by local structure analysis of the interface. Ar$$^{+}$$ irradiation of the carbon support led to the formation of the Pt-C bonding, thus protecting the deposited Pt nanoparticles from oxidation.


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。



永井 崇之; 岡本 芳浩; 山岸 弘奈*; 太田 俊明*; 小島 一男*; 猪瀬 毅彦*; 佐藤 誠一*; 畠山 清司*

JAEA-Research 2021-010, 62 Pages, 2022/01




Bayesian sparse modeling of extended X-ray absorption fine structure to determine interstitial oxygen positions in yttrium oxyhydride epitaxial thin film

熊添 博之*; 五十嵐 康彦*; Iesari, F.*; 清水 亮太*; 小松 遊矢*; 一杉 太郎*; 松村 大樹; 齋藤 寛之*; 岩満 一功*; 岡島 敏浩*; et al.

AIP Advances (Internet), 11(12), p.125013_1 - 125013_5, 2021/12

 被引用回数:1 パーセンタイル:22.97(Nanoscience & Nanotechnology)

This letter presents a Bayesian sparse modeling method to analyze extended X-ray absorption fine structure (EXAFS) data with basis functions built on two-body signals. This method allows us to evaluate regression coefficients proportional to the radial distribution functions of the respective elements and their errors and is very effective for analysis of EXAFS with weak absorption intensity and severe signal-to-noise ratio. As an application example, we used it to analyze EXAFS of an yttrium oxyhydride (YO$$_{x}$$H$$_{y}$$) epitaxial thin film. This EXAFS data shows weak absorption intensity due to the small amount of X-ray absorption in the thin film sample. However, this approach revealed that the radial distance ratio of the second neighbor yttrium to the first neighbor oxygen coincides with that of a tetrahedral configuration. This result demonstrates that the interstitial oxygen position is tetrahedral in the YO$$_{x}$$H$$_{y}$$ thin film.


Structural characterization by X-ray analytical techniques of calcium aluminate cement modified with sodium polyphosphate containing cesium chloride

高畠 容子; 渡部 創; 入澤 啓太; 塩飽 秀啓; 渡部 雅之

Journal of Nuclear Materials, 556, p.153170_1 - 153170_7, 2021/12

 被引用回数:0 パーセンタイル:0.01(Materials Science, Multidisciplinary)

The long-time experimental activities on pyroprocessing have generated waste eutectic salts contaminated with nuclear materials. After reprocessing tests, waste salts should be appropriately treated, with a focus on Cl disposal considering its corrosive nature. It is important to construct Cl confinement for the waste salts. Chlorapatite (Ca$$_{10}$$(PO$$_{4}$$)$$_{6}$$Cl$$_{2}$$) has great potential for Cl confinement due to Ca and P. The chemical reactivity of Cl will be drastically reduced if chlorapatite can be synthesized in calcium aluminate cement modified with sodium polyphosphate (CAP) containing CsCl. This study confirms the chemical state of Cl and metal elements in the cement by XRD, XPS, and XANES in the CAP containing CsCl. The analyses results suggest the existence of the Ca-Cl-Cs and Al-Cl-Cs bonds in CAP containing CsCl. The formation of the chemical bonds of Cl with metal elements might be one of important factors for the chlorapatite formation from the CAP containing CsCl.


Distinct variation of electronic states due to annealing in $$T'$$-type La$$_{1.8}$$Eu$$_{0.2}$$CuO$$_{4}$$ and Nd$$_{2}$$CuO$$_{4}$$

浅野 駿*; 石井 賢司*; 松村 大樹; 辻 卓也; 工藤 康太*; 谷口 貴紀*; 齋藤 真*; 春原 稔樹*; 川股 隆行*; 小池 洋二*; et al.

Physical Review B, 104(21), p.214504_1 - 214504_7, 2021/12

 被引用回数:0 パーセンタイル:0(Materials Science, Multidisciplinary)

We performed Cu K-edge X-ray absorption fine-structure measurements on $$T'$$-type La$$_{1.8}$$Eu$$_{0.2}$$CuO$$_{4}$$ (LECO) and Nd$$_{2}$$CuO$$_{4}$$ (NCO) to investigate the variation in the electronic state associated with the emergence of superconductivity due to annealing. The X-ray absorption near-edge structure spectra of as-sintered (AS) LECO are quite similar to those of AS NCO, indicating that the ground state of AS LECO is a Mott insulator. The electron density after annealing $$n_{rm AN}$$ was evaluated for both superconducting LECO and nonsuperconducting NCO and was found to be 0.40 and 0.05 electron per Cu atom, respectively. In LECO but not in NCO, extended X-ray absorption fine-structure analysis revealed a reduction in the strength of the Cu-O bond in the CuO$$_{2}$$ plane due to annealing, which is consistent with the screening effect on phonons in the metallic state. The origin of the difference in doping processes due to annealing is discussed in relation to the size of the charge-transfer gap.


Chromium(VI) adsorption-reduction using a fibrous amidoxime-grafted adsorbent

林 菜月*; 松村 大樹; 保科 宏行*; 植木 悠二*; 辻 卓也; Chen, J.*; 瀬古 典明*

Separation and Purification Technology, 277, p.119536_1 - 119536_8, 2021/12

 被引用回数:5 パーセンタイル:60.29(Engineering, Chemical)

To develop a safe and simple method for the reduction of toxic chromium(VI) to the less harmful chromium(III), we proposed using radiation-induced graft polymerization. This method allows for any functional group to be introduced into conventional polymeric materials. Herein, we synthesized a fibrous adsorbent with amidoxime functional groups that have a high affinity for chromium, and investigated the changes in the chromium valence state over time in the amidoxime-grafted adsorbent. In situ X-ray absorption fine structure analysis revealed that most of the chromium(VI) was reduced to chromium(III) relatively early during the adsorption process, followed by gradual changes in the bonding structure of the amidoxime-chromium complex. It is expected to contribute to the development of practical technologies for wastewater treatment.



永井 崇之; 秋山 大輔*; 桐島 陽*; 佐藤 修彰*; 岡本 芳浩

2020年度「物質・デバイス領域共同研究拠点」および「人・環境と物質をつなぐイノベーション創出ダイナミック・アライアンス」研究成果・活動報告書(CD-ROM), 1 Pages, 2021/11



Mechanistic study on the removal of Cs from contaminated soil by rapid ion exchange in subcritical water

福田 達弥*; 高橋 亮*; 原 卓飛*; 尾原 幸治*; 加藤 和男*; 松村 大樹; 稲葉 優介*; 中瀬 正彦*; 竹下 健二*

Journal of Nuclear Science and Technology, 58(4), p.399 - 404, 2021/04

 被引用回数:3 パーセンタイル:51.02(Nuclear Science & Technology)

As a result of the Fukushima nuclear power plant accident in March 2011, massive amounts of soil were contaminated with radioactive Cs. To remediate the contaminated soil, we are developing a desorption technique for removing Cs from soil using subcritical water. We found that rapid ion exchange of Cs with multivalent cations in subcritical water is an effective desorption technique. To understand the mechanism and structural aspects of this process, in situ observations of the soil layer in subcritical water were carried out by high-energy X-ray diffraction together with pair distribution function analysis, and extended X-ray absorption fine structure analysis. Both the desorption experiments and structural studies indicated that conformational changes of the layer containing Cs$$^{+}$$ under subcritical water conditions promoted intercalation of the hydrated Mg and trapped Cs$$^{+}$$, which facilitated a rapid ion-exchange reaction of Mg$$^{2+}$$ and Cs$$^{+}$$.


Local Ir dedimerization followed by ligand-hole hopping in X-ray irradiated thiospinel

平賀 晴弘*; 松村 大樹; 堀金 和正*; 水木 純一郎*

Journal of Physics and Chemistry of Solids, 150, p.109870_1 - 109870_8, 2021/03

 被引用回数:0 パーセンタイル:0(Chemistry, Multidisciplinary)

The extended X-ray-absorption fine structure of a spinel CuIr$$_{2}$$(S$$_{0.95}$$Se$$_{0.05}$$)$$_{4}$$ powder sample, which has the charge-ordered temperature $$T_{rm{CO}}$$ = 190 K, was determined at the Ir $$L_{3}$$ edge for a wide temperature range. All the local structure parameters on the Ir-Ir bonds signified the second structural change at $$T^{*} sim$$ 70 K. Remarkably, the number of Ir dimers decreased by $$sim$$ 10% below $$T^{*}$$, which indicates partial dedimerization by X-ray irradiation. We also reanalyzed the resistance data of CuIr$$_{2}$$S$$_{4}$$ with the variable-range hopping model by focusing on the density of states. The X-ray-induced decrease in resistance was quantitatively explained as a result of the increase in the density of states, which was attributed to the release of holes from the 10%-dedimerized Ir ions. We suppose that the released holes hop over the ligand chalcogen site.

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