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小澤 沙記*; 塩沢 優大*; 西條 佳孝*; 宮嶋 達也*; 松村 大樹; 辻 卓也; 中瀬 正彦*; 前原 輝敬*
Journal of the American Ceramic Society, 109(3), p.e70621_1 - e70621_10, 2026/03
被引用回数：0 パーセンタイル：0.00(Materials Science, Ceramics)The optical properties of glass are strongly influenced by the redox states of trace multivalent elements. Ce
ions are commonly added to soda-lime glass to remove Fe
-induced coloration via the redox reaction Ce + Fe 
Ce
+ Fe during cooling. Herein, the redox dynamics of cerium ions in soda-lime glass melts during model industrial cooling processes (from 1523 K at 20 K
min
) were investigated using in situ time-resolved Ce K-edge dispersive X-ray absorption fine-structure (DXAFS) spectroscopy. To evaluate the effect of the iron concentration, three soda-lime glass samples containing 2 mass% CeO
were examined: Fe-free, Fe-05 (0.5 mass% FeO
), and Fe-20 (2.0 mass% FeO). Above 1383 K, the Ce/total Ce ratio remained stable for all samples, showing no significant change during cooling. Below 1383 K, the ratio decreased for the Fe-free glass, indicating the oxidation of Ce ions, and increased for the Fe-containing glass owing to the reduction of Ce ions. The temperature dependence of the redox change (
Ce redox) showed Fe-dependent behavior: Fe-20 exhibited more pronounced Ce reduction above 1200 K, while Fe-05 showed accelerated changes mainly below approximately 1100 K. These results indicate that cerium oxidation in Fe-free glass is strongly influenced by oxygen transport limitations, while cerium reduction is closely associated with availability of Fe ions, providing quantitative insights into the control of Ce-based decolorization during industrial cooling.
松村 大樹; 辻 卓也; 瀬古 典明*; 他5名*
Journal of Radioanalytical and Nuclear Chemistry, 335(2), p.1543 - 1552, 2026/02
被引用回数：0 パーセンタイル：0.00(Chemistry, Analytical)The COVID-19 pandemic has underscored the need for protective materials with rapid and durable antiviral properties. We developed silver (Ag)-immobilized fabrics via radiation-induced graft polymerization and tested their activity against SARS-CoV-2. The fabrics reduced 40,000 viral particles to below detection within one hour, showed no Ag leaching after 24 h in water, and retained complete antiviral performance after one year of storage. These findings demonstrate the long-term stability and strong potential of Ag-immobilized fabrics for industrial use in protective equipment.
松村 大樹; 石井 賢司*; 田中 裕久*; 水木 純一郎*
放射光, 39(1), p.28 - 36, 2026/01
燃料電池の開発は二酸化炭素発生抑制のためにも重要な研究課題である。中でも電極反応における酸素還元反応は、電池全体の律速過程であることから、詳しい理解が求められる。高分解能X線吸収分光法を適用し、電極反応の「その場」観察を行うことで、炭素担持白金微粒子(Pt/C)電極触媒に対して表面吸着種の電位依存観測を実施した。その結果、これまで実触媒では同定されていなかった、酸素還元反応の反応中間体としての分子状酸素吸着種の存在を、酸性環境下でもアルカリ性環境下でも見出し、酸素還元反応の理解を一歩進めることができた。
Wang, M.*; 辻 卓也; 松村 大樹; 坂牛 健*; 他9名*
Journal of Physical Chemistry C, 130(2), p.931 - 941, 2026/01
被引用回数：0 パーセンタイル：0.00(Chemistry, Physical)Understanding how compositional complexity influences electrocatalytic kinetics remains a major challenge in the design of multicomponent materials. The multifaceted interactions between constituent elements are able to obscure the factors governing kinetics of electrode processes. Here, we introduce a small compositional change to modulate the rate-determining step of the oxygen evolution reaction (OER) by tuning the binding energies of key intermediates. We combine advanced characterization, including 
electrochemical X-ray absorption spectroscopy, with first-principles calculations to demonstrate that the drastic enhancement in OER activity of MnFeNi-based materials is driven by synergistic interactions among the constituent elements. This enhancement stems from targeted modulation of intrinsic reaction pathways, shifting the rate-determining step via controlled stabilization of key intermediates. Our findings introduce a clear viewpoint for understanding how compositional tuning governs kinetics in complex electrocatalytic systems, offering new design principles for next-generation electrochemical materials.
MnCoNiCu)VO
山本 孟*; 辻 卓也; 松村 大樹; 他16名*
Inorganic Chemistry, 64(34), p.17496 - 17502, 2025/08
被引用回数：0 パーセンタイル：0.00(Chemistry, Inorganic & Nuclear)V-V dimerization in ilmenite-type vanadium oxides is an intriguing phenomenon that induces structural and metal-to-insulator transitions. Herein, we report the high-pressure synthesis, crystal structure, and electronic states of high-entropy ilmenite-type (MgMnCoNiCu)VO. Although all the parent ilmenite-type compounds exhibit triclinic (
) symmetry, this compound crystallizes in a rhombohedral (
) structure, indicating the absence of V-V dimer ordering. The temperature dependence of the resistivity below room temperature follows a variable-range hopping conduction mechanism, suggesting the presence of short-range V-V dimer ordering. Magnetic susceptibility and heat capacity measurements revealed multi-step spin-glass transitions. This study demonstrates that a high-entropy composition hinders electronic and magnetic long-range ordering due to severe lattice distortions and competition between magnetic exchange interactions.
O and/or SiO for methanol synthesis; Deciphering the additive-induced boost in catalytic performance by XAFSIwasaki, Kosei*; Ashida, Yuya*; 松村 大樹; Kawakami, Kotaro*; Shibuya, Kana*; Tazawa, Masaru*; 辻 卓也; Shimizu, Hajime*
Journal of CO Utilization, 97, p.103111_1 - 103111_9, 2025/07
The development of active, long-lived methanol synthesis catalysts can be expedited by thoroughly understanding the operating mechanisms of promoter additives. SiO serves as an effective support and promoter for Cu/ZnO-type methanol synthesis catalysts; however, it has not been studied as extensively as the industrially predominant AlO, despite being similarly potent. Therefore, we conducted X-ray absorption fine structure predominant AlO, despite being similarly potent. Therefore, we conducted X-ray absorption fine structure studies to probe the effects of incorporating AlO and SiO additives into Cu/ZnO-based heterogeneous catalysts. The results revealed that the additive elements primarily affected the ability of the Zn species to generate oxygen vacancies by distorting the local structure around element-doped ZnO and that the number of oxygen vacancies correlated to the catalytic activity. Additionally, the oxygen vacancies in ZnO in the Al/Si-incorporated catalysts diminished under catalytic reaction conditions, thereby providing information on the deactivation of catalytic reactions. Our findings can facilitate the development of highly active industrial-grade methanol synthesis catalysts.
田中 裕久*; 松村 大樹; 他8名*
International Journal of Hydrogen Energy, 141, p.1317 - 1327, 2025/06
被引用回数：1 パーセンタイル：23.08(Chemistry, Physical)The safe removal, transportation, and long-term storage of fuel debris in the decommissioning of Fukushima Daiichi is the biggest challenge facing Japan. In the nuclear power field, passive autocatalytic recombiners (PARs) have become established as a technology to prevent hydrogen explosions inside the containment vessel. To utilize PAR as a measure to reduce the concentration of hydrogen generated in the fuel debris storage canister, which is currently an issue, it is required to perform in a sealed environment with high doses of radiation, low temperature, and high humidity, and there are many challenges different from conventional PAR. A honeycomb-shaped catalyst based on automotive catalyst technology has been newly designed as a PAR, and research has been conducted to solve unique problems such as high dose radiation, low temperature, high humidity, coexistence of hydrogen and low oxygen, and catalyst poisons. This paper summarizes the challenges of hydrogen generation in a sealed container, the results of research, and a guide to how to use the PAR for fuel debris storage canisters.
田中 裕久*; 松村 大樹; 他10名*
International Journal of Hydrogen Energy, 141, p.1088 - 1097, 2025/06
被引用回数：1 パーセンタイル：23.08(Chemistry, Physical)Global efforts are being made to decarbonize the energy sector. Liquefied (cryogenic) hydrogen is suitable for large-scale storage and transportation due to its high storage density, so it is likely to play a fundamental role in the future hydrogen economy. The STACY project, "Towards the Safe Storage and Transport of Cryogenic Hydrogen", is investigating safety aspects of liquid hydrogen in order to overcome potential safety risks. Research is being conducted into passive autocatalytic recombiners using cutting-edge catalyst technology to enable them to be used in conditions where liquid hydrogen escapes, evaporates and forms a cold (
50
C) explosive gas mixture with the ambient air. To this end, the crystal structure of the catalyst was designed at the atomic level, an actual catalyst was prototyped, and repeated tests were carried out on a laboratory scale and in a large reaction vessel. Progress has been made in developing catalysts that can oxidize hydrogen even at very low temperatures, high expansion, and low-oxygen environments, are resistant to catalyst poisons, and can prevent spontaneous unintended ignition. The tested catalyst technologies use different carrier materials (alumina and ceria) to control the surface state of precious metals and suppress hydrogen ignition through a multilevel configuration.
田中 裕久*; 松村 大樹; 他9名*
SAE Technical Paper 2025-01-8474 (Internet), 8 Pages, 2025/04
On-board diagnosis (OBD) of gasoline vehicle emissions is detected by measuring the fluctuations of the rear oxygen sensor due to the time-dependent deterioration of the oxygen storage capacity (OSC) contained in the automotive catalyst materials. To detect OBD in various driving modes of automobiles with an order of magnitude higher accuracy than before, it is essential to understand the OSC mechanism based on fundamental science. In this study, time-resolved dispersive X-ray absorption fine structure (DXAFS) using synchrotron radiation was used to carry out a detailed analysis not only of the OSC of ceria-based complex oxides, which had previously been roughly understood, but also of how differences in design parameters such as the type of precious metals, reducing gases (CO and H), detection temperatures, and mileages (degree of deteriorations) affect the OSC rate in a fluctuating redox atmosphere. A fundamental characteristic was clearly demonstrated in ceria-based complex oxides: the oxygen release rate accompanying the generation of oxygen vacancies is overwhelmingly slower than the oxygen storage rate that restores the crystal structure. Another interesting result was revealed: when precious metals are supported, a competitive reaction occurs between the precious metal and the ceria-based complex oxide in the release/storage of oxygen, and the change in cerium valence from tetravalent to trivalent actually slows down. Furthermore, it was proven that CZY is more durable than CZ in terms of both OSC rate and amount. In this way, the basic scientific properties of ceria-based complex oxides, which are necessary for designing OBD logic, have been clarified.
濱田 翔太*; 松村 大樹; 他10名*
SAE Technical Paper 2025-01-8476 (Internet), 6 Pages, 2025/04
In order to comply with the tightening of global regulations on automobile exhaust gas, further improvements to exhaust gas control catalysts and upgrades to on-board diagnostics (OBD) systems must be made. Currently, oxygen storage capacity (OSC) is monitored by front and rear sensors before and after the catalyst, and deterioration is judged by a decrease in OSC, but it is possible that catalyst deterioration may cause the rear sensor to detect gas that has not been sufficiently purified. It is important to observe the activity changes when the catalyst deteriorates in more detail and to gain a deeper understanding of the catalyst mechanism in order to create guidelines for future catalyst development. In this study, we used a 
-TG (micro thermogravimetric balance) to analyze in detail how differences in design parameters such as the type of precious metal, detection temperature, and mileage (degree of deterioration) affect the OSC rate in addition to the OSC of the ceria-based composite oxide of the entire catalyst. It was found that CZY has better durability in terms of both OSC rate and amount than CZ. Furthermore, by comparing the results of experiments using time-resolved dispersive X-ray absorption fine structure (DXAFS) using synchrotron radiation, the reduction behavior of ceria was analyzed in more detail.
by solvent extraction as a potential method to determine Fe in glass containing Sn菅野 直樹*; 中瀬 正彦*; 西條 佳孝*; 松村 大樹; 辻 卓也; 竹下 健二*; 塚原 剛彦*
Progress in Nuclear Science and Technology (Internet), 7, p.154 - 160, 2025/03
The amounts of Fe and Fe present in glass are important indicators of its optical properties because even small amounts have significant effects. However, it is challenging to use wet chemical analysis to determine the concentration and the ratio of Fe and Fe in glass when it contains Sn because of the redox reaction between Sn and Fe in the glass decomposition solution. A two-step approach was tested to determine the concentrations of Fe and Fe in a glass decomposition solution in the presence of Sn. In the first step, the redox reaction between Sn and Fe was suppressed by increased pH. In the second step, Sn was removed from the glass decomposition solution by solvent extraction. To understand the kinetics of the redox reaction between Sn and Fe, time-resolved dispersive X-ray absorption fine structure and ultraviolet-visible absorption spectroscopy (UV-vis) were used with standard chloride solutions of Sn and Fe in respective valences. We found that lowering the acid concentration suppressed redox reactions. The partitioning behaviors of Sn, Sn, Fe, and Fe by bis(2-ethylhexyl) hydrogen phosphate (D2EHPA) as an extractant in 
-dodecane were investigated to see the removal ability of Sn from the glass decomposition solution. As a result, D2EHPA in -dodecane could extract Sn, Sn, and Fe into the organic phase, and Fe remained in the aqueous phase. The simultaneous removal of Sn and Sn and the separation of Fe and Fe became possible. This method can potentially apply to the rapid analysis of the concentration of Fe and Fe in a glass containing tin oxide.
-orbital transition metal multielemental alloy nanoparticles by atomically dispersed 4-orbital Pd for a 100-fold extended lifetimeZhu, B.*; Huang, S.*; Seo, O.*; Cao, M.*; 松村 大樹; Gu, H.*; Wu, D.*
Journal of the American Chemical Society, 147(13), p.11250 - 11256, 2025/02
被引用回数：68 パーセンタイル：99.72(Chemistry, Multidisciplinary)Earth-abundant 3-orbital late transition metals are the most used and highly desired catalysts for the oxygen evolution reaction (OER) but are prone to quick oxidative dissolution, leading to poor durability. We first report that FeCoNiCu multielemental alloy nanoparticles (MEANPs) can be stabilized with only 0.3 at.%Pd, a 4-orbital element. Although pure Pd is known for extremely poor OER activity and durability, Pd-FeCoNiCu sustains 1000 h at 10 mA cm
. In an accelerating durability test (ADT) at 100 mA cm, it exhibits a mere 8.9 mV increase over 25 h with a degradation rate of 0.356 mVh, which is 1/350th that of FeCoNiCu (125 mVh) and among the most stable OER catalysts reported so far. Aberration-corrected HAADF-STEM and X-ray absorption fine structure (XAFS) reveal that atomically dispersed Pd atoms, surrounded by Fe, Co, Ni, and Cu atoms, contributed to a more delocalized electronic structure and stronger bonding via strong -/
hybridization and the vibronic coupling induced by atomic displacement. The altered local density of states (LDOS) of Fe, Co, Ni, and Cu mitigates the oxidation of FeCoNiCu in OER by over 50%, quantified by hard X-ray photoelectron spectroscopy (HAXPES), making the combination of these five dissoluble elements a durable catalyst.
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：2 パーセンタイル：26.40(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.
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), 12(5), p.259 - 262, 2024/10
2:1型層状粘土鉱物には層を構成する陽イオンが同形置換することで層電荷を持ち、層間に陽イオンを取り込むことで電荷を補償する。また、層電荷の大小により異なる膨潤性を示す。風化黒雲母は比較的大きい層電荷をもつため膨潤性が低く、モンモリロナイトは層電荷が小さいため膨潤性が高い。アルミノケイ酸塩であるゼオライトは様々な細孔を持ち、その内部に水分子を持つ。これらの粘土鉱物中では、降雨等の環境の変化により異なるセシウム収着構造をとることが考えられるため、本研究では湿潤・乾燥・再湿潤状態の粘土鉱物試料に対し、Cs K吸収端X線吸収分光(X-ray Absorption Fine Structure, XAFS)測定によりセシウム近傍の局所構造解析を行った。その結果、湿潤・乾燥試料においては水分子の存在により、一部の収着サイトではセシウムを収着しにくくなり、乾燥・再湿潤試料においては収着構造に差はなく、不可逆的にセシウムが収着していることが示唆された。
Krajewska, A.*; 辻 卓也; 松村 大樹; 他15名*
Science Advances (Internet), 10(41), p.eadn3880_1 - eadn3880_10, 2024/10
被引用回数：5 パーセンタイル：56.92(Multidisciplinary Sciences)The interplay of spin-orbit coupling with other relevant parameters gives rise to the rich phase competition in complex ruthenates featuring octahedrally coordinated Ru. While locally, spin-orbit coupling stabilizes a non-magnetic 
= 0 state, intersite interactions resolve one of two distinct phases at low temperatures: an excitonicmagnet stabilized by the magnetic exchange of upper-lying = 1 states or Ru molecular orbital dimers driven by direct orbital overlap. Pyrochlore ruthenates ARuO
(A = rare earth, Y) are candidate excitonic magnets with geometrical frustration. We synthesized InRuO with covalent In-O bonds. This pyrochlore ruthenate hosts alocal = 0 state at high temperatures; however, at low temperatures, it forms a unique nonmagnetic ground state with nearly linear Ru-O-Ru molecules, in stark contrast to other ARuO compounds. The disproportionation of covalent In-O bonds drives RuO molecule formation, quenching not only the local spin-orbit singlet but also geometrical frustration.
, AgNbO, and KNbO米田 安宏; 小林 徹; 辻 卓也; 松村 大樹; 斎藤 祐児; 野口 祐二*
Japanese Journal of Applied Physics, 63(9), p.09SP12_1 - 09SP12_10, 2024/09
被引用回数：3 パーセンタイル：33.64(Physics, Applied)NaNbO、AgNbO、KNbOのABO型ペロブスカイト系は良好な強誘電特性を持つことが知られている。我々は局所構造解析により各原子のラットリング空間を直接決定した。この解析により、大きな揺らぎを持つ結合サイトがイオンサイズの変化によって変化することを明らかにした。軟X線吸収分光法を含む実験から、Aサイトイオンは酸素と混成していることがわかった。
山本 孟*; 池田 理*; 本田 孝志*; 木村 健太*; 青山 拓也*; 大串 研也*; 鈴木 昭夫*; 石井 賢司*; 松村 大樹; 辻 卓也; et al.
Physical Review Materials (Internet), 8(9), p.094402_1 - 094402_6, 2024/09
被引用回数：5 パーセンタイル：34.77(Materials Science, Multidisciplinary)We investigate the crystal and electronic structures as well as magnetic properties of ilmenite-type NiVO, which has attracted research interest as an 
= 1 honeycomb lattice magnet. Ilmenite-type NiVO samples were synthesized under high-pressure and high-temperature conditions. Synchrotron X-ray diffraction and Rietveld refinement results demonstrated that NiVO underwent a continuous structural phase transition from the triclinic (
) phase to the rhombohedral (
) phase at 450 K. This transition is concomitant with the decomposition of the V-V dimers formed by the tetravalent V ions. X-ray absorption spectroscopy measurements confirmed that the Ni and V ions were divalent and tetravalent, respectively. Magnetic and specific heat measurements revealed that NiVO underwent an antiferromagnetic transition at 140 K, and a zigzag-type magnetic order with magnetic propagation vector 
=(0,1/2,0) was observed by neutron diffraction measurements.
O-BO-SiO glass and melt through high-temperature Ni K-edge XAFS and time-resolved SAXS measurements富田 夏奈*; 岸 哲生*; 大坂 恵一*; 松村 大樹; 矢野 哲司*
Journal of Non-Crystalline Solids, 634, p.122975_1 - 122975_19, 2024/06
被引用回数：4 パーセンタイル：34.97(Materials Science, Ceramics)High-temperature in-situ Ni-K edge XAFS and SAXS measurements were conducted on borosilicate glasses with low alkali content with/without phase separation tendency, which have been investigated to understand immiscibility into silica-rich phase and borate-rich one on the samples heat-treated at certain temperature followed by fast quenching. In this work, using in-situ analyzing techniques, in-situ time-domain evolution of phases along temperature and time was obtained to understand high-temperature behavior. Ni ion probes phase separation behavior using its high selectivity favoring borate-rich phase and sensitivity to electron donating ability of surrounding oxygens. Taking advantage of these characters, local compositional change was tracked during phase separation under heat treatment. Time-resolved SAXS profiles revealed the speed of phase transformation in addition to changes of morphology at respective temperature. The phase-separation transformation mechanism via different phase separation scheme (homogeneous spinodal binodal homogeneous) was clearly described, revealing effect of NiO clustering at higher temperature.
Jung, H.*; 松村 大樹; 他12名*
ACS Energy Letters (Internet), 9(5), p.2162 - 2172, 2024/04
被引用回数：23 パーセンタイル：89.54(Chemistry, Physical)A strategic approach has been proposed for designing robust, high-performing oxygen evolution reaction (OER) catalysts tailored for saline water splitting. By employing a density functional theory (DFT)-based computational screening process, a set of promising dopants were identified from a range of 26 3d to 5d transition metals, with the aim of enhancing the activity and saline water resilience of the catalysts. The screening methodology was 3-fold, encompassing evaluations of OER energetics, chlorine evolution reaction (ClER) energetics, and chloride-corrosion energetics. The screening led to the selection of Sc as a promising dopant, which substantially elevated the performance of the NiFeOOH catalysts. This improvement was validated by an 87 mV decrease in OER overpotential at 100 mA/cm
and a 100 h stability test under 1 M KOH + 0.5 M NaCl conditions. This study contributes to the understanding of the alkaline ClER and chloride-corrosion mechanisms, providing insights into catalyst behavior under saline conditions.
Lei, Y.-J.*; 松村 大樹; 他15名*
Nature Communications (Internet), 15, p.3325_1 - 3325_12, 2024/04
被引用回数：93 パーセンタイル：99.01(Multidisciplinary Sciences)The effective flow of electrons through bulk electrodes is crucial for achieving high-performance batteries, although the poor conductivity of homocyclic sulfur molecules results in high barriers against the passage of electrons through electrode structures. This phenomenon causes incomplete reactions and the formation of metastable products. To enhance the performance of the electrode, it is important to place substitutable electrification units to accelerate the cleavage of sulfur molecules and increase the selectivity of stable products during charging and discharging. Herein, we develop a single-atom-charging strategy to address the electron transport issues in bulk sulfur electrodes. The establishment of the synergistic interaction between the adsorption model and electronic transfer helps us achieve a high level of selectivity towards the desirable short-chain sodium polysulfides during the practical battery test. These finding indicates that the atomic manganese sites have an enhanced ability to capture and donate electrons. Additionally, the charge transfer process facilitates the rearrangement of sodium ions, thereby accelerating the kinetics of the sodium ions through the electrostatic force. These combined effects improve pathway selectivity and conversion to stable products during the redox process, leading to superior electrochemical performance for room temperature sodium-sulfur batteries.
