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論文

Local structural changes in V-Ti-Cr alloy hydrides with hydrogen absorption/desorption cycling

池田 一貴*; 佐次田 頌*; 大友 季哉*; 大下 英敏*; 本田 孝志*; 羽合 孝文*; 齋藤 開*; 伊藤 晋一*; 横尾 哲也*; 榊 浩司*; et al.

International Journal of Hydrogen Energy, 51(Part A), p.79 - 87, 2024/01

Low-vanadium-concentration alloys have low durability, and their hydrogen absorption and desorption amounts decrease by 20% after 100 cycles. In this study, we conducted reverse Monte Carlo modeling on X-ray diffraction patterns and neutron pair distribution functions of the hydrogen-absorbed and desorbed samples of a V$$_{0.10}$$Ti$$_{0.36}$$Cr$$_{0.54}$$ alloy to analyze the variations in the local structure. The local structure surrounding the hydrogen atom in the hydrogen-absorbed phase exhibited minimal changes. In contrast, hydrogen occupied both tetrahedral and octahedral sites of the hydrogen-desorbed phase almost equally during the early cycles; however, the amount of hydrogen occupying the tetrahedral sites increased with the number of cycles.

論文

${it In situ}$ Ga K-edge XANES study of Ga-exchanged zeolites at high temperatures under different atmospheres including vacuum, CO, and pressurized H$$_{2}$$

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

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$$_{2}$$, He, CO, vacuum, and C$$_{2}$$H$$_{6}$$). The absorption edge appeared at similarly lower energy values than that of Ga$$_{2}$$O$$_{3}$$ 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$$_{2}$$ and C$$_{2}$$H$$_{6}$$ atmospheres than under CO and vacuum atmospheres.

論文

Weakened oxygen adsorbing the Pt-O bond of the Pt catalyst induced by vacancy introduction into carbon support

岡崎 宏之*; 出崎 亮*; 越川 博*; 松村 大樹; 池田 隆司*; 山本 春也*; 八巻 徹也*

Journal of Physical Chemistry C, 127(49), p.23628 - 23633, 2023/12

The change in the oxygen adsorption states of Pt nanoparticles by ion irradiation of the carbon support is studied by in situ X-ray absorption spectroscopy measurements. The difference spectra around a Pt L$$_{3}$$ edge due to oxygen adsorption are recorded, and a lowering in the Pt-O antibonding level by the ion irradiation is observed, thus resulting in a weakening of the Pt-O bond. This indicates that the introduction of vacancies in the carbon support would result in weak Pt-O bonds assumable through the stronger Pt-C interaction, which is considered to enhance the oxygen reduction reaction activity of the deposited Pt nanoparticles. Theoretical studies have demonstrated that the vacancies affect Pt through the Pt-C interaction and then result in the weakening of the Pt-O bond.

論文

分散型光学系を用いた時間分解X線吸収分光法によるRh金属微粒子触媒のCO酸化反応における自発振動現象の詳細観測

松村 大樹; 木村 優作*; 辻 卓也; 水木 純一郎*

SPring-8/SACLA利用研究成果集(インターネット), 11(5), p.296 - 299, 2023/11

自発振動現象を起こすRh金属微粒子触媒上のCO酸化反応について、分散型光学系による時間分解X線吸収分光法を用いた研究を実施した。定常ガスを一定温度で導入して、触媒反応の振動現象が起こっている最中のRh金属微粒子の構造変化について、1Hz程度のフレームレートで詳細観測した。触媒反応生成物であるCO$$_{2}$$濃度の時間変化とX線吸収分光法によるRh金属微粒子構造の時間変化とを比べると、両者は強く相関していることが見て取れた。振動構造の様式には、Rhの平均価数変化は階段状のものである一方CO$$_{2}$$の生成量はパルス状の変化であるという違いがあり、これは金属Rh表面で短時間のみ吸着COが無い状態が実現されるという考えで解釈できた。

論文

Local atomic displacements and sign of the structural transformation in medium-entropy alloys observed in extended X-ray absorption fine structure spectra

池田 陽一*; 梅本 好日古*; 松村 大樹; 辻 卓也; 橋本 勇輝*; 北澤 崇文*; 藤田 全基*

Materials Transactions, 64(9), p.2254 - 2260, 2023/09

Extended X-ray absorption fine structure (EXAFS) and neutron diffraction experiments were carried out to clarify the typical features of the local structure of a family of medium-entropy alloys (CrCoNi, MnCoNi, and FeCoNi). A simple random cluster model was constructed for analyzing EXAFS spectra, and static and dynamic components of the mean-square relative displacement (MSRD) were separately extracted. In our analysis, the static MSRD of the MnCoNi sample was slightly larger than those of the CrCoNi and FeCoNi samples, whereas the dynamic MSRDs of these samples were almost identical. Based on the complementary neutron diffraction data, we argued that the origin of the large static displacement in the MnCoNi alloy can be associated with a short-range structural transformation through long-term structural relaxation.

論文

Cs ${it L$_{1}$}$吸収端XAFS測定による各種粘土鉱物中におけるセシウムの収着構造

辻 卓也; 松村 大樹; 小林 徹

SPring-8/SACLA利用研究成果集(インターネット), 11(4), p.214 - 217, 2023/08

天然に存在する粘土鉱物は様々な層構造をもち、セシウムイオン等の陽イオン収着サイトは複数存在すると考えられており、層間サイト、表面サイトや端面サイト等が存在すると考えられている。福島第一原子力発電所事故後に放射性セシウムにより汚染された土壌中での詳細な収着構造解明のため、本研究ではセシウムを飽和収着させた粘土鉱物試料に対しCs ${it L$_{1}$}$吸収端X線吸収分光(X-ray absorption fine structure, XAFS)測定を行い、セシウム収着様式の比較を行った。その結果、各種粘土鉱物においてスペクトルの詳細構造に差がみられ、四面体シートや八面体シートへの収着等、収着構造の違いに起因するセシウム収着様式の違いが明らかになった。

論文

Development of hydrogen oxidation reaction catalysts to overcome CO poisoning and elucidation of reaction mechanism

稲川 康平*; 松村 大樹; 谷口 昌司*; 上垣 伸弥*; 中山 智仁*; 浦野 純乃介*; 青谷 拓朗*; 田中 裕久*

Journal of Physical Chemistry C, 127(24), p.11542 - 11549, 2023/06

Passive autocatalytic recombiner (PAR) represents a potential technology for ensuring process safety in the hydrogen society. PARs function through the catalytic oxidation of generated or leaked hydrogen, facilitating its conversion into water and effectively mitigating the risk of hydrogen explosions. CO is recognized as a catalyst poison that hampers surface catalytic reactions. To investigate the negative effects of CO on the local structure of platinum metal nanoparticle catalysts during water formation, in situ and time-resolved X-ray absorption spectroscopy analyses were conducted. The results revealed that the Pt-Fe/CZY catalyst exhibited notable hydrogen oxidation activity even in the presence of CO. The enhanced performance can be attributed to the combined effects of Pt-Fe alloy composition and CZY support materials.

論文

Cu $$K$$-edge X-ray absorption fine structure study of $$T'$$-type $$RE$$$$_{2}$$CuO$$_{4+alpha-delta}$$ ($$RE$$ = Rare Earth); Toward unified understanding of electronic state of $$T'$$-type cuprate

Chen, Y.*; 浅野 駿*; Wang, T.*; Xie, P.*; 北山 慎之介*; 石井 賢司*; 松村 大樹; 辻 卓也; 谷口 貴紀*; 藤田 全基*

JPS Conference Proceedings (Internet), 38, p.011050_1 - 011050_6, 2023/05

To investigate the variation of the electronic state of $$T'$$-type cuprate due to annealing, we performed Cu $$K$$-edge X-ray absorption fine structure measurements on Pr$$_{2}$$CuO$$_{4+alpha-delta}$$ (PCO) and Pr$$_{1.3}$$La$$_{0.7}$$CuO$$_{4+alpha-delta}$$ (PLCO). The induced electrons due to annealing ($$n_{AN}$$) in PCO and PLCO were approximately 2$$delta$$, consistent with a model of electron doping to Mott insulator. Here, $$alpha$$ and $$delta$$ represent the amount of excess oxygen from the stoichiometric composition in the as-sintered compound and that of oxygen loss due to annealing, respectively. Furthermore, the energy of the Einstein oscillator ($$hbaromega_{E}$$) for the Cu-O$$_{p}$$ bond was evaluated by extended X-ray absorption fine structure analysis. (O$$_{p}$$ denotes the in-plane oxygen.) We found a small annealing effect on $$hbaromega_{E}$$ for both PCO and PLCO.

論文

Uranium hydroxide/oxide deposits on uranyl reduction

大内 和希; 松村 大樹; 辻 卓也; 小林 徹; 音部 治幹; 北辻 章浩

RSC Advances (Internet), 13(24), p.16321 - 16326, 2023/05

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

電気化学水晶振動子マイクロバランス、インピーダンススペクトル及びX線吸収微細構造測定の結果から、ウラニルイオン(U$$^{rm VI}$$O$$_{2}$$$$^{2+}$$)の還元に伴う析出物の化学状態変化を明らかにした。U$$^{rm VI}$$O$$_{2}$$$$^{2+}$$の還元に伴い、(1)U$$^{rm V}$$の不均化によりU$$^{rm IV}$$が生成する。(2)U$$^{rm IV}$$はU$$^{rm IV}$$水酸化物として析出物を形成し、(3)最終的に水酸化物より大きな電気抵抗を持つU$$^{rm IV}$$酸化物に変化する析出機構が提案される。

論文

Crystal structure, photomagnetic and dielectric properties of a cyanido-bridged Cu-Mo assembly film

池田 侑典*; 松村 大樹; 辻 卓也; 生井 飛鳥*; 井元 健太*; 所 裕子*; 中林 耕二*; 大越 慎一*

Inorganica Chimica Acta, 550, p.121434_1 - 121434_8, 2023/03

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

A film of a cyanido-bridged Cu-Mo assembly Cu$$_{2}$$[Mo(CN)$$_{8}$$]$$cdot$$8H$$_{2}$$O (CuMo-film) was electrochemically synthesized. Unlike analogs with a formula of M$$_{2}$$[Mo(CN)$$_{8}$$]$$cdot$$zH$$_{2}$$O (M = Mn, Fe, Co), which show tetragonal crystal structures, the CuMo-film shows a monoclinic structure in the C2/m space group with cell parameters of a = 17.2461 $AA, b = 11.1681 AA, c = 11.2618 AA, $beta$$ = 125.1089$$^{circ}$$, and V = 1774.44 $AA$^{3}$$. Extended X-ray absorption fine structure analysis traced the bond distances around the Cu site as 1.93-2.30 $r{A}$ for Cu-N and 2.01-2.40 $r{A}$ for Cu-O. CuMo-film exhibits photo-switchable magnetization with T$$_{C}$$ = 18 K and dielectric relaxation related to the hydrogen bond network. The change of activation energy (E$$_{a}$$) of the dielectric relaxation around 157 K (from E$$_{a}$$ = 49.9 kJ mol$$^{-1}$$ to E$$_{a}$$ = 27.3 kJ mol$$^{-1}$$ on cooling) suggests that the development of the hydrogen bond network occurs below 157 K.

論文

Investigation of hydrogen superoxide adsorption during ORR on Pt/C catalyst in acidic solution for PEFC by ${it in-situ}$ high energy resolution XAFS

山本 直生*; 松村 大樹; 萩原 悠人*; 田中 啓偉*; 長谷川 優太*; 石井 賢司*; 田中 裕久*

Journal of Power Sources, 557, p.232508_1 - 232508_10, 2023/02

 被引用回数:0 パーセンタイル:31.35(Chemistry, Physical)

Oxygen Reduction Reaction (ORR) is one of the key electrochemical reactions, especially in Polymer Electrolyte Fuel Cells (PEFCs). In this work, the reaction pathway and intermediate species such as molecular-type oxygen during ORR were discussed. High energy resolution X-ray absorption fine structure spectra at the Pt L$$_{3}$$-edge were obtained to observe the electronic structure of Pt catalyst. Carbon-supported Pt nanoparticles as powder catalysts were used for measurement as more realistic conditions, and the species adsorbed on the Pt nanoparticles were analyzed while controlling under the potentials in acidic electrolyte solution with N$$_{2}$$ or O$$_{2}$$ gas bubbling. Molecular-type oxygen adsorption species is observed only in the O$$_{2}$$-bubbled electrolyte solution. This intermediate adsorption species is assigned to a hydrogen superoxide.

論文

風化黒雲母およびカオリナイトにおけるセシウム収着構造

辻 卓也; 松村 大樹; 小林 徹; 矢板 毅

SPring-8/SACLA利用研究成果集(インターネット), 11(1), p.15 - 18, 2023/02

風化黒雲母の様な層状粘土鉱物では様々な収着サイトが存在すると考えられており、その中でもCsイオンは層間に取り込まれると考えられている。一方でカオリナイトのような粘土鉱物においては、層間に陽イオンを持たないことから、表面・端面サイトにのみ収着すると考えられている。本研究では福島第一原子力発電所事故後に放射性Csにより汚染された実土壌に近い濃度のCs収着粘土鉱物試料を調製しCs K吸収端におけるX-ray Absorption Fine Structure (XAFS)測定を行い、風化黒雲母とカオリナイトにおけるCs周りの局所構造の違いを観測した。結果、層間サイトに収着していると思われる風化黒雲母と表面・端面サイトに収着していると思われるカオリナイトとでは、特に低濃度領域においてCs周りの局所構造が大きく異なることが判明し、Cs収着様式によってCsイオンの収着安定性が大きく異なることが示唆された。

論文

Electron storage performance of hybrid materials comprising polyoxometalates and carbon nanohorns as cathode-active materials

若松 勝洋*; 関原 輝昇*; 山口 慶彦*; 松島 諒*; 松村 大樹; Kuila, T.*; 吉川 浩史*

Batteries & Supercaps (Internet), 6(1), p.e202200385_1 - e202200385_8, 2023/01

 被引用回数:1 パーセンタイル:31.35(Electrochemistry)

Nanohybrid materials comprising polyoxometalates (POMs) and nanocarbons have attracted considerable attention as electrode-active materials for rechargeable lithium-ion batteries (LIBs). These materials exhibit multi-electron redox reactions, resulting in an improved battery capacity. This study focuses on carbon nanohorns (CNHs) as a nanocarbon material and evaluates the battery performance using POM/CNH hybrids as cathode-active materials. X-ray absorption fine structural analysis was performed to investigate the reaction mechanism of these hybrids. POM/oxidized CNH (CNHox) hybrid materials maintain high capacities at high current densities as the high surface area availability of CNHox leads to high electrical double-layer capacitances. These findings show an improved performance of the as-developed material when compared with those reported in previous papers and can contribute toward an improved design of cathode-active materials for high-performance supercapacitors.

論文

Composite with a glassy nonporous coordination polymer enhances gas adsorption selectivity

Zheng, X.*; 加藤 優*; 上村 洋平*; 松村 大樹; 八木 一三*; 高橋 仁徳*; 野呂 真一郎*; 中村 貴義*

Inorganic Chemistry, 62(3), p.1257 - 1263, 2023/01

 被引用回数:0 パーセンタイル:63.13(Chemistry, Inorganic & Nuclear)

A glass-crystal composite (g-NCP/PCP), comprising a glassy nonporous coordination polymer (g-NCP) and a crystalline porous coordination polymer (PCP)/metal-organic framework, was synthesized by using a melt-quenched method. Compared to that of the PCP itself, g-NCP/PCP has an enhanced gas adsorption selectivity. The results should stimulate further studies of the chemistry of g-NCP/PCP glass-crystal composites.

論文

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:1 パーセンタイル:16.1(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.

論文

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

 被引用回数:23 パーセンタイル:98.03(Chemistry, Multidisciplinary)

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.

論文

Displacement of hydrogen position in di-hydride of V-Ti-Cr solid solution alloys

榊 浩司*; Kim, H.*; Majzoub, E. H.*; 町田 晃彦*; 綿貫 徹*; 池田 一貴*; 大友 季哉*; 水野 正隆*; 松村 大樹; 中村 優美子*

Acta Materialia, 234, p.118055_1 - 118055_10, 2022/08

 被引用回数:6 パーセンタイル:85.3(Materials Science, Multidisciplinary)

Local structure in the di-hydride phases of V-Ti-Cr solid solution alloys were investigated using synchrotron X-ray and neutron total scattering experiments. Both Rietveld refinement and pair distribution function (PDF) refinement of the X-ray scattering data indicated that the crystal structure of the metal lattice was a face centered cubic (FCC) structure and no difference between their local structure and average structure was observed. However, the CaF$$_{2}$$ structure model did not reproduce the first peak corresponding to the metal-hydrogen correlation in neutron PDF patterns. When special quasi-random structure (SQS) models are applied for the refinements, the whole neutron PDF patterns were reproduced. Distribution of interatomic distances between hydrogen and metal atoms in the relaxed SQS models showed that interatomic distance of hydrogen with Cr was shorter than that with V and that with Ti was longer than that with V, independently of the chemical compositions.

論文

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:1 パーセンタイル:31.35(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.

論文

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:2 パーセンタイル:63.02(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.

論文

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.

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