Updated on 2024/09/27

Information

 

写真a

 
MATSUMOTO TAKAHIRO
 
Organization
Faculty of Engineering Department of Applied Chemistry Associate Professor
Abolition organization (Concurrent)
School of Engineering (Concurrent)
Graduate School of Engineering (Concurrent)
Title
Associate Professor
Contact information
メールアドレス
Tel
0928022823
Profile
研究は、水中有機金属触媒の新規開発を行っている。 教育では、学部学生を対象とする学生実験やコアセミナーを担当している。
External link

Degree

  • Doctor (Philosophy in Science)

Research Interests・Research Keywords

  • Research theme: Development of a novel catalyst of organometallic complex in water

    Keyword: water・organometal・complex・catalyst

    Research period: 2009.10 - 2014.5

Awards

  • 平成30年度科学技術分野の文部科学大臣表彰若手科学者賞

    2018.4   文部科学省   分子触媒を電極に用いた燃料電池の研究

  • 平成28年度錯体化学会研究奨励賞

    2016.9   錯体化学会   分子燃料電池–ヒドロゲナーゼを範とする水素と酸素の活性化–

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    代表的な研究業績である「基礎研究:錯体化学を基礎とするモデル研究」と「応用研究:錯体化学を基礎とする燃料電池の研究」に基づき、本賞を受賞した。以下に具体的な内容について記述する。
    【基礎研究:錯体化学を基礎とするモデル研究】
    NiFeヒドロゲナーゼモデル錯体の合成:自然界の水素活性化酵素であるNiFeヒドロゲナーゼは、水素を酸化する本来の機能だけでなく、酸素を水に還元する防御機構も有している。本研究では、未解明であったNiFeヒドロゲナーゼの水素と酸素の活性化状態のモデル錯体の合成に初めて成功した。後の酵素研究によって、水素活性化状態モデル錯体の構造が、天然の構造と全く同じであることが報告された。本業績は、酵素研究に先駆けてモデル錯体から未解明構造を予見した意義深い研究である。
    【応用研究:錯体化学を基礎とする燃料電池の研究】
    NiFeヒドロゲナーゼおよびモデル錯体の燃料電池への応用:現行の燃料電池の最重要課題は、白金電極に替わる電極触媒の開発である。本研究では、白金代替電極触媒として、NiFeヒドロゲナーゼS-77(阿蘇山より新規に探索)とそのモデル錯体を用いた燃料電池を新規に開発した。ヒドロゲナーゼS-77の燃料電池では、単位質量あたり白金の637倍の水素酸化電流という酵素燃料電池では最高値を示した。そのモデル錯体を電極触媒に用いた分子燃料電池は、分子触媒を電極に用いた初めての例である。以上の業績は、錯体化学の発展に寄与すると思われる。

Papers

  • Molecular Catalysis in a Fuel Cell Reviewed International journal

    Matsumoto, Takahiro; Kim, Kyoungmok; Ogo, Seiji

    Angew. Chem., Int. Ed.   50 ( 47 )   2011.9

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    Language:English   Publishing type:Research paper (scientific journal)  

    一般的に燃料電池電極触媒には、枯渇資源で高価な白金触媒が使用されているため、その代替触媒の開発が実用化に向けて不可欠である。本論文では、白金の代替となる分子触媒を開発し、世界で初めて分子触媒を用いた燃料電池、分子燃料電池、の開発に成功した。

    DOI: 10.1002/anie.201104498

  • Preparation and Reactivity of a Nickel Dihydride Complex Reviewed International journal

    Takahiro Matsumoto, Takuma Nagahama, Jaeheung Cho, Takuhiro Hizume, Masatatsu Suzuki, and Seiji Ogo

    Angew. Chem. Int. Ed.   50 ( 45 )   2011.9

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    水素酸化酵素であるヒドロゲナーゼは、温和な条件下(水中・常温・常圧)で、水素の酸化を触媒する魅力的な酵素である。その酵素1分子単位での水素酸化の触媒効率は、人工触媒である白金よりも優れているため、ヒドロゲナーゼの反応メカニズムの解明は非常に重要である。しかし、その反応メカニズムの鍵となる活性中間体であるジヒドリド錯体は、これまで観測されていなかった。本研究では世界で初めてその活性中間体のモデル錯体の合成・同定に成功した。

    DOI: 10.1002/anie.201104918

  • Model Study of CO Inhibition of [NiFe]hydrogenase Reviewed International journal

    Matsumoto, Takahiro; Kabe, Ryota; Nonaka, Kyoshiro; Ando, Tatsuya; Yoon, Ki-Seok; Nakai, Hidetaka; Ogo, Seiji

    Inorganic Chemistry   50   2011.8

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    Language:English   Publishing type:Research paper (scientific journal)  

  • Smart Design of Organometallic Catalysts to Induce Innovative Material Transformations

    MATSUMOTO Takahiro

    Journal of the Japan Petroleum Institute   65 ( 4 )   134 - 139   2022.7   ISSN:13468804 eISSN:1349273X

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    Language:Japanese   Publisher:The Japan Petroleum Institute  

    <p>Coordination chemistry has established the principle of “organometallic smart design: metal × ligand” for metal complexes with specific properties and functions based on empirical rules and quantum chemistry considerations. Numerous metal complexes have subsequently been synthesized to catalyze required chemical reactions. This review describes several representative studies, especially concerning the reactions of designed metal complexes with dioxygen, dihydrogen, and methane gases. Copper-mediated dioxygen activation and nickel–iron-mediated dihydrogen activation were inspired by the enzymatic activities of tyrosinase and nickel–iron hydrogenase. Hydroxylation of arene ring, epoxidation of styrene, and oxidation of carbon–hydrogen bonds of hydrocarbons have been achieved using a dinuclear copper peroxide complex derived from dioxygen modelled on tyrosinase. Biomimetic dihydrogen oxidation and dioxygen reduction have been promoted by nickel–iron and nickel–ruthenium complexes in organic solvent and water, based on the oxygen-tolerant nickel–iron hydrogenase. The transformation of methane to methanol and formaldehyde using dioxygen as an oxidant has been achieved by input of light energy into a designed diruthenium dioxide complex.</p>

    DOI: 10.1627/jpi.65.134

    Web of Science

    Scopus

    CiNii Research

  • Light-driven oxidation of CH_4 to C_1 chemicals catalysed by an organometallic Ru complex with O_2

    Nakano Tatsuya, Abe Tsukasa, Matsumoto Takahiro, Kimura Kento, Nakamura Genta, Hayami Shinya, Shiota Yoshihito, Yoshizawa Kazunari, Ogo Seiji

    RSC Advances   12 ( 20 )   12253 - 12257   2022.4   eISSN:20462069

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    Language:English   Publisher:Royal Society of Chemistry  

    CH_4 conversion is one of the most challenging chemical reactions due to its inertness in terms of physical and chemical properties. We have achieved photo-induced C–H bond breaking of CH_4 and successive C–O bond formation to form CH_3OH concomitant with HCHO by an organometallic Ru complex with O_2.

    CiNii Research

  • Light-driven oxidation of CH<sub>4</sub> to C<sub>1</sub> chemicals catalysed by an organometallic Ru complex with O<sub>2</sub>

    Nakano, T; Abe, T; Matsumoto, T; Kimura, K; Nakamura, G; Hayami, S; Shiota, Y; Yoshizawa, K; Ogo, S

    RSC ADVANCES   12 ( 20 )   12253 - 12257   2022.4   eISSN:2046-2069

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    Language:English   Publisher:RSC Advances  

    CH4 conversion is one of the most challenging chemical reactions due to its inertness in terms of physical and chemical properties. We have achieved photo-induced C-H bond breaking of CH4 and successive C-O bond formation to form CH3OH concomitant with HCHO by an organometallic Ru complex with O2

    DOI: 10.1039/d2ra01772e

    Web of Science

    Scopus

    PubMed

  • Light-Driven Oxidation of CH4 to C1 Chemicals Catalysed by an Organometallic Ru Complex with O2. Reviewed International journal

    Nakano, Tatsuya; Abe, Tsukasa; Matsumoto, Takahiro;* Kimura, Kento; Nakamura, Genta; Hayami, Shinya; Shiota, Yoshihito;* Yoshizawa, Kazunari;* Ogo, Seiji.*

    RSC Adv.   12 ( 20 )   12253 - 12257   2022.4

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    Language:English   Publishing type:Research paper (scientific journal)  

    Repository Public URL: https://hdl.handle.net/2324/7160910

  • Smart Design of Organometallic Catalysts to Induce Innovative Material Transformations. Reviewed International journal

    Matsumoto, Takahiro.

    J. Jpn. Petrol. Inst.   65 ( 4 )   134 - 139   2022.3

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  • Hydrogen evolution, electron-transfer, and hydride-transfer reactions in a nickel-iron hydrogenase model complex: a theoretical study of the distinctive reactivities for the conformational isomers of nickel-iron hydride

    Isegawa M., Matsumoto T., Ogo S.

    Dalton Transactions   51 ( 1 )   312 - 323   2022.1   ISSN:14779226

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    Hydrogen fuel is a promising alternative to fossil fuel. Therefore, efficient hydrogen production is crucial to elucidate the distinctive reactivities of metal hydride species, the intermediates formed during hydrogen activation/evolution in the presence of organometallic catalysts. This study uses density functional theory (DFT) to investigate the isomerizations and reactivities of three nickel-iron (NiFe) hydride isomers synthesized by mimicking the active center of NiFe hydrogenase. Hydride transfer within these complexes, rather than a chemical reaction between the complexes, converts the three hydrides internally. Their reactivities, including their electron-transfer, hydride-transfer and proton-transfer reactions, are investigated. The bridging hydride complex exhibits a higher energy level for the highest occupied molecular orbital (HOMO) than the terminal hydride during the electron-transfer reaction. This energy level indicates that the bridging hydride is more easily oxidized and is more susceptible to electron transfer than the terminal hydride. Regarding the hydride-transfer reaction between the NiFe hydride complex and methylene blue, the terminal hydrides exhibit larger hydricity and lower reaction barriers than the bridging hydride complexes. The results of energy decomposition analysis indicate that the structural deformation energy of the terminal hydride in the transition state is smaller than that of the bridging hydride complex, which lowers the reaction barrier of hydride transfer in the terminal hydride. To produce hydrogen, the rate-determining step is represented by the protonation of the hydride, and the terminal hydrides are thermodynamically and kinetically superior to the bridging ones. The differences in the reactivities of the hydride isomers ensure the precise control of hydrogen, and the theoretical calculations can be applied to design catalysts for hydrogen activation/production.

    DOI: 10.1039/d1dt03582g

    Scopus

  • Hydrogen Evolution, Electron-transfer, Hydride-Transfer Reactions in a Nickel-Iron Hydrogenase Model Complex: A Theoretical Study of the Distinctive Reactivities for the Conformational Isomers of Nickel-Iron Hydride. 2021 Reviewed International journal

    Isegawa, Miho;* Matsumoto, Takahiro; Ogo, Seiji.

    Dalton Trans.   51 ( 1 )   312 - 323   2021.12

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  • C–H Arylation of Benzene with Aryl Halides using H2 and a Water-Soluble Rh-Based Electron Storage Catalyst. Reviewed International journal

    Yatabe, Takeshi; Tome, Tamon; Takahashi, Yukina; Matsumoto, Takahiro; Yoon, Ki-Seok; Nakai, Hidetaka; Ogo, Seiji.*

    Chem. Eur. J.   27 ( 69 )   17326 - 17330.   2021.10

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  • H2 Activation by Hydrogenase-Inspired NiFe Catalyst Using Frustrated Lewis Pair: Effect of Buffer and Halide Ion in the Heterolytic H–H Bond Cleavage. Reviewed International journal

    Isegawa, Miho;* Matsumoto, Takahiro; Ogo, Seiji.

    RSC Adv.   11 ( 45 )   28420 - 28432.   2021.8

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  • Synthesis of acetic acid from CO2, CH3I and H2 using a Water-Soluble Electron Storage Catalyst. Reviewed International journal

    Yatabe, Takeshi; Kamitakahara, Kazuki; Higashijima, Kaede; Ando, Tatsuya; Matsumoto, Takahiro; Yoon, Ki-Seok; Enomoto, Takao; Ogo, Seiji.

    Chem. Commun.   57 ( 39 )   4772 - 4774   2021.5

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    DOI: 10.1039/d1cc01611c

  • Direct Synthesis of Hydrogen Peroxide in Water by Means of a Rh-Based Catalyst. Reviewed International journal

    Ogo, Seiji; Thi Minh, Le Tu; Kikunaga, Takahiro; Ando, Tatsuya; Matsumoto, Takahiro; Yatabe, Takeshi; Kato, Kenji.

    Organometallics   39 ( 20 )   3731 - 3741   2020.10

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    DOI: 10.1021/acs.organomet.0c00565

  • A NiRhS Fuel Cell Catalyst – Lessons from Hydrogenase. Reviewed International journal

    Ogo, Seiji; Ando, Tatsuya; Thi Minh, Le Tu; Mori, Yuki; Matsumoto, Takahiro; Yatabe, Takeshi; Yoon, Ki-Seok; Sato, Yukio; Hibino, Takashi; Kaneko, Kenji.

    Chem. Commun.   56 ( 79 )   11787 - 11790   2020.9

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    DOI: 10.1039/d0cc04789a

  • [NiFe], [FeFe], and [Fe] Hydrogenase Models from Isomers. Reviewed

    Ogo, Seiji; Kishima, Takahiro; Yatabe, Takeshi; Miyazawa, Keishi; Yamasaki, Ryunosuke; Matsumoto, Takahiro; Ando, Tatsuya; Kikkawa, Mitsuhiro; Isegawa, Miho; Yoon, Ki-Seok; Hayami, Shinya.

    Sci. Adv.   6 ( 24 )   eaaz8181. - eaaz8181.   2020.3

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    水素の合成や分解を担う3種類の天然ヒドロゲナーゼ酵素の構造をヒントに1つの新しい触媒を開発した。今回開発した触媒は、同じ分子式で構造だけが異なる3種類の異性体によって、3種類のヒドロゲナーゼ酵素のように(i)燃料電池の水素電極の触媒(ii)水素製造の触媒(iii)化学工業の水素化の触媒として働くことを発見した。本研究成果は、これまで不明であったヒドロゲナーゼ酵素の触媒反応と触媒の分子構造との関係を解き明かすことで、次世代のエネルギー源である水素を効率よく利用する道を開いた。

    DOI: 10.1126/sciadv.aaz8181

  • Selective Oxidation of H2 and CO by NiIr Catalyst in Aqueous Solution A DFT Mechanistic Study Reviewed

    Miho Isegawa, Takahiro Matsumoto, Seiji Ogo

    Inorganic chemistry   59 ( 2 )   1014 - 1028   2020.1

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    One of the challenges in utilizing hydrogen gas (H2) as a sustainable fossil fuel alternative is the inhibition of H2 oxidation by carbon monoxide (CO), which is involved in the industrial production of H2 sources. To solve this problem, a catalyst that selectively oxidizes either CO or H2 or one that co-oxidizes H2 and CO is needed. Recently, a NiIr catalyst [NiIICl(X)IrIIICl(Ε5-C5Me5)], (X = N,N′-dimethyl-3,7-diazanonane-1,9-dithiolate), which efficiently and selectively oxidizes either H2 or CO depending on the pH, has been developed (Angew. Chem. Int. Ed. 2017, 56, 9723-9726). In the present work, density functional theory (DFT) calculations are employed to elucidate the pH-dependent reaction mechanisms of H2 and CO oxidation catalyzed by this NiIr catalyst. During H2 oxidation, our calculations suggest that dihydrogen binds to the Ir center and generates an Ir(III)-dihydrogen complex, followed by subsequent isomerization to an Ir(V)-dihydride species. Then, a proton is abstracted by a buffer base, CH3COO-, resulting in the formation of a hydride complex. The catalytic cycle completes with electron transfer from the hydride complex to a protonated 2,6-dichlorobenzeneindophenol (DCIP) and a proton transfer from the oxidized hydride complex to a buffer base. The CO oxidation mechanism involves three distinct steps, i.e., (1) formation of a metal carbonyl complex, (2) formation of a metallocarboxylic acid, and (3) conversion of the metallocarboxylic acid to a hydride complex. The formation of the metallocarboxylic acid involves nucleophilic attack of OH- to the carbonyl-C followed by a large structural change with concomitant cleavage of the Ir-S bond and rotation of the COOH group along the NiIr axis. During the conversion of the metallocarboxylic acid to the hydride complex, intramolecular proton transfer followed by removal of CO2 leads to the formation of the hydride complexes. In addition, the barrier heights for the binding of small molecules (H2, OH-, H2O, and CO) to Ir were calculated, and the results indicated that dissociation from Ir is a faster process than the binding of H2O and H2. These calculations indicate that H2 oxidation is inhibited by CO and OH- and thus prefers acidic conditions. In contrast, the CO oxidation reactions occur more favorably under basic conditions, as the formation of the metallocarboxylic acid involves OH- attack to a carbonyl-C and the binding of OH- to Ni largely stabilizes the triplet spin state of the complex. Taken together, these calculations provide a rationale for the experimentally observed pH-dependent, selective oxidations of H2 and CO.

    DOI: 10.1021/acs.inorgchem.9b02400

  • Computational Study on the Light-Induced Oxidation of Iridium-Aqua Complex to Iridium-Oxo Complex over WO3(001) Surface. Reviewed

    Ikeda, Kei; Mahyuddin, Muhammad Haris; Shiota, Yoshihito; Staykov, Aleksandar; Matsumoto, Takahiro; Ogo, Seiji; Yoshizawa, Kazunari.

    Inorg. Chem.   59 ( 1 )   415 - 422   2019.12

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    DOI: 10.1021/acs.inorgchem.9b02704

  • Dual Catalytic Cycle of H2 and H2O Oxidations by a Half-Sandwich Iridium Complex A Theoretical Study Reviewed

    Kei Ikeda, Yuta Hori, Muhammad Haris Mahyuddin, Yoshihito Shiota, Aleksandar Tsekov Staykov, Takahiro Matsumoto, Kazunari Yoshizawa, Seiji Ogo

    Inorganic Chemistry   58 ( 11 )   7274 - 7284   2019.6

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    While hydrogenase and photosystem II enzymes are known to oxidize H2 and H2O, respectively, a recently reported iridium aqua complex [IrIII5-C5Me5){bpy(COOH)2}(H2O)]2+ is able to oxidize both of the molecules and generate energies as in the fuel and solar cells (Ogo et al. ChemCatChem 2017, 9, 4024-4028). To understand the mechanism behind such an interesting bifunctional catalyst, in the present study, we perform density functional theory (DFT) calculations on the dual catalytic cycle of H2 and H2O oxidations by the iridium aqua complex. In the H2 oxidation, we found that the H-H bond is easily cleaved in a heterolytic fashion, and the resultant iridium hydride complex is significantly stabilized by the presence of H2O molecules, due to dihydrogen bond. The rate-determining step of this reaction is found to be the H2O → H2 ligand substitution with an activation energy of 10.7 kcal/mol. In the H2O oxidation, an iridium oxo complex originating from an oxidation of the iridium aqua complex forms a hydroperoxide complex, where an O-O bond is formed with an activation energy of 21.0 kcal/mol. Such a relatively low activation barrier is possible only when at least two H2O molecules are present in the reaction, allowing the water nucleophilic attack (WNA) mechanism to take place. The present study suggests and discusses in detail six reaction steps required for the dual catalytic cycle to complete.

    DOI: 10.1021/acs.inorgchem.9b00307

  • Dual Catalytic Cycle of H2 and H2O Oxidations by a Half-Sandwich Iridium Complex: A Theoretical Study. Reviewed

    Ikeda, Kei; Hori, Yuta; Mahyuddin, Muhammad Haris; Shiota, Yoshihito; Staykov, Aleksandar; Matsumoto, Takahiro; Yoshizawa, Kazunari; Ogo, Seiji.

    Inorg. Chem. Inorg. Chem.   58 ( 11 )   7274 - 7284   2019.5

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    水素を酸化する酵素「ヒドロゲナーゼ」と水を酸化する酵素「光化学系II」の機能を複合した単一分子触媒を開発し、固体高分子形燃料電池の電極触媒として応用したところ、水素と水を両方燃料にできる電池の作製に成功した。均一系触媒と不均一系触媒の両方の性質を併せ持つ電極触媒の反応メカニズムの解明は極めて困難であるため、密度汎関数理論により、その反応メカニズムの詳細を明らかにした。

    DOI: 10.1021/acs.inorgchem.9b00307

  • Homogeneous catalytic reduction of polyoxometalate by hydrogen gas with a hydrogenase model complex Reviewed

    Takuo Minato, Takahiro Matsumoto, Seiji Ogo

    RSC Advances   9 ( 34 )   19518 - 19522   2019.1

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    The homogeneous catalytic reduction of a polyoxometalate (POM) by hydrogen gas in aqueous media was investigated for the first time by using a [NiRu] hydrogenase model complex (I) under very mild conditions. By bubbling hydrogen gas into the buffer solution containing I and the Dawson-type POM (IIox), the color of the solution turned from pale yellow to dark blue, suggesting the reduction of IIox. The catalytic and kinetic studies revealed that I acted as an efficient catalyst to yield one-electron-reduced Dawson-type POM (IIred) with a low energy barrier for activating dihydrogen and reducing IIoxvia a hydride complex of I. The process for the one-electron reduction of IIox was confirmed by UV-vis spectroscopy, controlled potential electrolysis, and X-ray photoelectron spectroscopy. POM IIred could stably store protons and electrons and release them by addition of oxidants, demonstrating that POMs acted as redox active mediators for transporting protons and electrons from hydrogen gas to acceptors. The recycle study showed that IIox and IIred could be reduced and oxidized by hydrogen and oxygen gases, respectively, at least five times with >99% yield of reduced species, showing a durable system for extracting protons and electrons from hydrogen gas.

    DOI: 10.1039/c9ra04396a

  • Multifunctional Catalysts for H2O2-Resistant Hydrogen Fuel Cells Reviewed

    Yuki Mori, Tatsuya Ando, Takahiro Matsumoto, Takeshi Yatabe, Mitsuhiro Kikkawa, Ki Suk Yoon, Seiji Ogo

    Angewandte Chemie - International Edition   57 ( 48 )   15792 - 15796   2018.11

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    The development of hydrogen fuel cells is greatly hindered by the unwanted generation of H2O2 at the cathode. A non-Pt cathode catalyst is now shown to be capable of simultaneously reducing both O2 and H2O2, thus rendering H2O2 a useful part of the feed stream. The applicability of this unique catalyst is demonstrated by employing it in a fuel cell running on H2/CO and O2/H2O2.

    DOI: 10.1002/anie.201810270

  • Oxidation of Guanosine Monophosphate with O 2 via a Ru-peroxo Complex in Water Reviewed

    Makoto Takenaka, Mitsuhiro Kikkawa, Takahiro Matsumoto, Takeshi Yatabe, Tatsuya Ando, Ki Suk Yoon, Seiji Ogo

    Chemistry - An Asian Journal   13 ( 21 )   3180 - 3184   2018.11

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    Oxidative damage of DNA by reactive oxygen species (ROS) is responsible for aging and cancer. Although many studies of DNA damage by ROS have been conducted, there have been no reports of the oxidation of RNA components, such as guanosine monophosphate, by metal-based species in water. Here, we report the first case of oxidation of guanosine monophosphate to 8-oxoguanosine monophosphate by a metal-based oxygen bound species, derived from O
    2
    and in water.

    DOI: 10.1002/asia.201801267

  • A MnI model for the photoinhibited species of oxygen-evolving complex Reviewed

    Takeshi Yatabe, Taisuke Tokunaga, Takahiro Matsumoto, Mitsuhiro Kikkawa, Ki Suk Yoon, Seiji Ogo

    Chemistry Letters   47 ( 1 )   34 - 36   2018.1

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    We report the reactivity of a new MnI(cyclam) complex (cyclam: 1,4,8,11-tetraazacyclotetradecane) toward O2 and H2O as a model for the photoinhibited species of oxygen-evolving complex (OEC). The reactivity varies according to the number of CO ligands. A MnI dicarbonyl complex, [MnI(cyclam)(CO)2]+ reacts with O2, but not with H2O, to form a bis(μ-oxo)Mn2III,IV complex, though a MnI tricarbonyl complex, [MnI(cyclam)(CO)3]+ does not react with either O2 or H2O. Newly synthesized MnI(cyclam) dicarbonyl complex was characterized by ESI mass spectrometry, UVvis absorption spectroscopy, IR spectroscopy, and X-ray analysis.

    DOI: 10.1246/cl.170869

  • Mechanistic investigation of the formation of H2 from HCOOH with a dinuclear Ru model complex for formate hydrogen lyase Reviewed

    Taisuke Tokunaga, Takeshi Yatabe, Takahiro Matsumoto, Tatsuya Ando, Ki Suk Yoon, Seiji Ogo

    Science and Technology of Advanced Materials   18 ( 1 )   870 - 876   2017.12

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    We report the mechanistic investigation of catalytic H2 evolution from formic acid in water using a formate-bridged dinuclear Ru complex as a formate hydrogen lyase model. The mechanistic study is based on isotope-labeling experiments involving hydrogen isotope exchange reaction.

    DOI: 10.1080/14686996.2017.1379857

  • A Fusion of Biomimetic Fuel and Solar Cells Based on Hydrogenase, Photosystem II, and Cytochrome c Oxidase Reviewed

    Mitsuhiro Kikkawa, Takeshi Yatabe, Takahiro Matsumoto, Ki Suk Yoon, Kazuharu Suzuki, Takao Enomoto, Kenji Kaneko, Seiji Ogo

    ChemCatChem   9 ( 21 )   4024 - 4028   2017.11

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    本論文では、燃料電池と太陽電池を融合する同一触媒の開発について報告した。次世代の電池として、燃料電池と太陽電池はこれまで別々に開発されてきたが、本研究では、「自然界の水素酵素と光合成の機能を融合した新しい触媒」を開発に成功した。この触媒を用いることで、「水素をエネルギー源として燃料電池が、水と光をエネルギー源として太陽電池が駆動する」ことを見出した。本研究成果はエネルギー研究の分野において格段の発展と波及効果をもたらす可能性が十分に期待できる。

    DOI: 10.1002/cctc.201700995

  • Mechanistic Insight into Switching between H2- or O2-Activation by Simple Ligand Effects of [NiFe]hydrogenase Models Reviewed

    Takahiro Matsumoto, Takahiro Kishima, Takeshi Yatabe, Ki Suk Yoon, Seiji Ogo

    Organometallics   36 ( 20 )   3883 - 3890   2017.10

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    We present a mechanistic investigation for the activation of H2 and O2, induced by a simple ligand effect within [NiFe] models for O2-tolerant [NiFe]hydrogenase. Kinetic study reveals Michaelis-Menten type saturation behaviors for both H2 and O2 activation, which is the same behavior as that found in O2-tolerant [NiFe]hydrogenase. Such saturation behavior is caused by H2 complexation followed by heterolytic cleavage of H2 by an outer-sphere base, resulting in the formation of a hydride species showing hydridic character.

    DOI: 10.1021/acs.organomet.7b00471

  • Luminescent Tb(III) and Sm(III) complexes with a 1,4,7-triazacyclononane-based tris-aryloxide ligand for high-performance oxygen sensors Reviewed

    Hidetaka Nakai, Masafumi Kuyama, Juncheol Seo, Takahiro Goto, Takahiro Matsumoto, Seiji Ogo

    Dalton Transactions   46 ( 28 )   9126 - 9130   2017.6

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    Taking advantage of the outstanding oxygen-sensitive luminescence properties of the previously synthesised Tb(iii) complex [{(MeMeArO)3tacn}LnIII(THF)] (1Tb, Ln = Tb), herein, we have prepared an oxygen sensor based on 1Tb embedded in polystyrene film (1Tb/PS) and found that 1Tb/PS shows the highest sensitivity (I0/I100 = 14.9) and the fastest response (response/recovery time = 1.9 s/2.9 s), among the lanthanide(iii)-based oxygen sensors with f-f emission. Moreover, we have prepared the lanthanide(iii)-based colorimetric luminescent oxygen sensor (1TbSm/PS) with green-yellow-red responses, by using 1Tb and a newly synthesised oxygen-insensitive Sm(iii) complex (1Sm, Ln = Sm; Φ = 0.010 and τ = 12.2 μs).

    DOI: 10.1039/c7dt01388d

  • One Model, Two Enzymes Activation of Hydrogen and Carbon Monoxide Reviewed

    Seiji Ogo, Yuki Mori, Tatsuya Ando, Takahiro Matsumoto, Takeshi Yatabe, Ki Suk Yoon, Hideki Hayashi, Masashi Asano

    Angewandte Chemie - International Edition   56 ( 33 )   9723 - 9726   2017.1

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    The ability to catalyze the oxidation of both H2 and CO in one reaction pot would be a major boon to hydrogen technology since CO is a consistent contaminant of H2 supplies. Here, we report just such a catalyst, with the ability to catalyze the oxidation of either or both H2 and CO, based on the pH value. This catalyst is based on a NiIr core that mimics the chemical function of [NiFe]hydrogenase in acidic media (pH 4–7) and carbon monoxide dehydrogenase in basic media (pH 7–10). We have applied this catalyst in a demonstration fuel cell using H2, CO, and H2/CO (1/1) feeds as fuels for oxidation at the anode. The power density of the fuel cell depends on the pH value in the media of the fuel cell and shows a similar pH dependence in a flask. We have isolated and characterized all intermediates in our proposed catalytic cycles.

    DOI: 10.1002/anie.201704864

  • Acetyl-CoA production by encapsulated pyruvate ferredoxin oxidoreductase in alginate hydrogels Reviewed

    Makoto Takenaka, Ki Seok Yoon, Takahiro Matsumoto, Seiji Ogo

    Bioresource Technology   227   279 - 285   2017

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    Pyruvate ferredoxin oxidoreductase from Citrobacter sp. S-77 (PFORS77) was purified in order to develop a method for acetyl-CoA production. Although the purified PFORS77showed high O2-sensitivity, the activity could be remarkably stabilized in anaerobic conditions. PFORS77was effectively immobilized on ceramic hydroxyapatite (PFORS77-HA) with an efficiency of more than 96%, however, after encapsulation of PFORS77-HA in alginate, the rate of catalytic acetyl-CoA production was highly reduced to 36% when compared to that of the free enzyme. However, the operational stability of the PFORS77-HA in alginate hydrogels was remarkable, retaining over 68% initial activity even after ten repeated cycles. The results suggested that the PFORS77-HA hydrogels have a high potential for biotechnological application.

    DOI: 10.1016/j.biortech.2016.12.051

  • Structure and Reactivity of a Ru-based Peroxide Complex as a Reactive Intermediate of O2-Promoted Activation of a C–H Bond in a Cp* Ligand. Reviewed International journal

    Takeshi Yatabe, Takahiro Kishima, Hideaki Nagano, Takahiro Matsumoto, Mikio Yamasaki, YOON KI SUK, Seiji Ogo

    Chem. Lett.   46 ( 1 )   74 - 76   2016.12

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    DOI: 10.1246/cl.160909

  • Acetyl-CoA Production by Encapsulated Pyruvate Ferredoxin Oxidoreductase in Alginate Hydrogels. Reviewed International journal

    Makoto Takenaka, YOON KI SUK, Takahiro Matsumoto, Seiji Ogo

    Bioresour. Technol. 2017, 227, 279–285.   227   279 - 285   2016.12

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    DOI: http://doi.org/10.1016/j.biortech.2016.12.051

  • Control of Lanthanide Coordination Environment: Synthesis, Structure, and Oxygen-Sensitive Luminescence Properties of an Eight-Coordinate Tb(III) Complex. Reviewed International journal

    Nakai Hidetaka, Juncheol Seo, Kazuhiro Kitagawa, Takahiro Goto, Kyoshiro Nonaka, Takahiro Matsumoto, Seiji Ogo

    Inorg. Chem.   55 ( 13 )   6609 - 6615   2016.6

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    DOI: 10.1021/acs.inorgchem.6b00800

  • Inorganic Clusters with a [Fe2MoOS3] Core—A Functional Model for Acetylene Reduction by Nitrogenases. Reviewed International journal

    Koji Yoshimoto, Takeshi Yatabe, Takahiro Matsumoto, TRAN VIET HA, ROBERTSON ANDREW, Nakai Hidetaka, Koichiro Asazawa, Hirohisa Tanaka, Seiji Ogo

    Dalton Trans.   45 ( 37 )   14620 - 14627   2016.6

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    DOI: 10.1039/C6DT01655C

  • An Oxygen-Sensitive Luminescent Dy(III) Complex. Reviewed International journal

    Nakai Hidetaka, Juncheol Seo, Kazuhiro Kitagawa, Takahiro Goto, Takahiro Matsumoto, Seiji Ogo

    Dalton Trans.   45 ( 23 )   9492 - 9496   2016.5

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    DOI: 10.1039/C6DT01057A

  • A Gadolinium(III) Complex That Shows Room-Temperature Phosphorescence in the Crystalline State. Reviewed International journal

    Nakai Hidetaka, Kazuhiro Kitagawa, Juncheol Seo, Takahiro Matsumoto, Seiji Ogo

    Dalton Trans.   45 ( 29 )   11620 - 11623   2016.5

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    DOI: 10.1039/C6DT01303A

  • A Non-precious Metal, Ni Molecular Catalyst for a Fuel Cell Cathode. Reviewed International journal

    Keisuke Takashita, Takahiro Matsumoto, Takeshi Yatabe, Nakai Hidetaka, Seiji Ogo

    Chem. Lett.   45 ( 2 )   137 - 139   2016.2

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    DOI: 10.1246/cl.150988

  • Photoinduced Bending of Rod-like Millimetre-size Crystals of a Rhodium Dithionite Complex with n-Pentyl Moieties. Reviewed International journal

    Nakai Hidetaka, Kengo Matsuba, Masataka Akimoto, Tomonori Nozaki, Takahiro Matsumoto, Kiyoshi Isobe, Masahiro Irie, Seiji Ogo

    Chem. Commun.   52 ( 23 )   4349 - 4352   2016.2

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    DOI: 10.1039/C6CC00059B

  • Synthesis and Reactivity of a Water-soluble NiRu Monohydride Complex with a Tethered Pyridine Moiety. Reviewed International journal

    Takahiro Matsumoto, Koji Yoshimoto, Chunbai Zheng, Yasuhito Shomura, Yoshiki Higuchi, Nakai Hidetaka, Seiji Ogo

    Chem. Lett.   45 ( 2 )   197 - 199   2016.2

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    DOI: 10.1246/cl.151029

  • Synthesis and Structure of a Water-soluble μ-η1:η1-N2 Dinuclear RuII Complex with a Polyamine Ligand. Reviewed International journal

    Koji Yoshimoto, Takeshi Yatabe, Takahiro Matsumoto, ROBERTSON ANDREW, Nakai Hidetaka, Hiromasa Tanaka, Takashi Kamachi, Yoshihito Shiota, Yoshizawa Kazunari, Koichiro Asazawa, Hirohisa Tanaka, Seiji Ogo

    Chem. Lett.   45 ( 2 )   149 - 151   2016.2

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    DOI: 10.1246/cl.150988

  • A Water-soluble Ni Dihydrido Complex That Reduces O2 to H2O in Water. Reviewed International journal

    Keisuke Takashita, Takahiro Matsumoto, Takeshi Yatabe, Nakai Hidetaka, Masatatsu Suzuki, Seiji Ogo

    Chem. Lett.   45 ( 1 )   72 - 74   2016.1

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    DOI: 10.1246/cl.150935

  • Synthesis and structure of a water-soluble μ-η1 η1-N2 dinuclear RuII complex with a polyamine ligand Reviewed

    Koji Yoshimoto, Takeshi Yatabe, Takahiro Matsumoto, Andrew Robertson, Hidetaka Nakai, Hiromasa Tanaka, Takashi Kamachi, Yoshihito Shiota, Kazunari Yoshizawa, Koichiro Asazawa, Hirohisa Tanaka, Seiji Ogo

    Chemistry Letters   45 ( 2 )   149 - 151   2016.1

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    We report the first example of a μ-η11-N2 dinuclear RuII complex with a polyamine ligand and elucidate the structure by means of X-ray analysis. The N=N stretching vibration has been observed at 1994 cm-1 by Raman spectroscopy, which is the lowest value of all the known N2-coordinated RuII complexes. This low value strongly suggests the N=N bond is primed for activation.

    DOI: 10.1246/cl.151004

  • Inorganic clusters with a [Fe2MoOS3] core - A functional model for acetylene reduction by nitrogenases Reviewed

    Koji Yoshimoto, Takeshi Yatabe, Takahiro Matsumoto, Viet Ha Tran, Andrew Robertson, Hidetaka Nakai, Koichiro Asazawa, Hirohisa Tanaka, Seiji Ogo

    Dalton Transactions   45 ( 37 )   14620 - 14627   2016.1

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    We report the first example of a wholly inorganic mimic of a part of the FeMoco active centre of nitrogenases. We detail the synthesis, characterisation and reactivity of two related, transient hydride-containing inorganic clusters, a dihydride complex and a vinyl monohydride complex, which bear the [Fe2MoOS3] portion of FeMoco. The dihydride complex is capable of reducing acetylene to ethylene via the vinyl monohydride complex. In the reaction cycle, a transient low-valent complex was generated by the reductive elimination of H2 or ethylene from dihydride or vinyl monohydride complexes, respectively.

    DOI: 10.1039/c6dt01655c

  • A gadolinium(III) complex that shows room-temperature phosphorescence in the crystalline state Reviewed

    Hidetaka Nakai, Kazuhiro Kitagawa, Juncheol Seo, Takahiro Matsumoto, Seiji Ogo

    Dalton Transactions   45 ( 29 )   11620 - 11623   2016.1

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    This paper presents a gadolinium(iii) complex that shows blue phosphorescence in the crystalline state at room temperature under air atmosphere; color of the crystals can be changed to pale-green from blue by doping of 1-naphthol.

    DOI: 10.1039/c6dt01303a

  • A High-Valent Iron(IV) Peroxo Core Derived from O2 Reviewed

    Takahiro Kishima, Takahiro Matsumoto, Hidetaka Nakai, Shinya Hayami, Takehiro Ohta, Seiji Ogo

    Angewandte Chemie - International Edition   55 ( 2 )   724 - 727   2016.1

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    Dioxygen-tolerant [NiFe] hydrogenases catalyze not only the conversion of H2 into 2 H+ and 2 e- but also the reduction of O2 to H2O. Chemists have sought to mimic such bifunctional catalysts with structurally simpler compounds to facilitate analysis and improvement. Herein, we report a new [NiFe]-based catalyst for O2 reduction via an O2 adduct. Structural investigations reveal the first example of a side-on iron(IV) peroxo complex. Dioxygen-tolerant [NiFe] hydrogenases catalyze not only the conversion of H2 into 2 H+ and 2 e- but also the reduction of O2 to H2O. A new [NiFe]-based complex is a synthetic mimic of such hydrogenases and catalyzes O2 reduction via an O2 adduct, which was shown to be the first example of a side-on iron(IV) peroxo complex.

    DOI: 10.1002/anie.201507022

  • An oxygen-sensitive luminescent Dy(III) complex Reviewed

    Hidetaka Nakai, Juncheol Seo, Kazuhiro Kitagawa, Takahiro Goto, Takahiro Matsumoto, Seiji Ogo

    Dalton Transactions   45 ( 23 )   9492 - 9496   2016

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    This paper presents the first dysprosium(iii) complex, [{(MeMeArO)3tacn}DyIII(THF)] (1Dy), that shows oxygen-sensitive luminescence. The synthesis, structure and oxygen-sensitive luminescence properties of 1Dy are reported (Φ = 0.050 and τ = 17.7 μs under N2, Φ = 0.011 and τ = 4.1 μs under O2 and KSV = 305 M-1 in THF; KSV = 0.0077%-1 in polystyrene film). The oxygen sensitive mechanism of 1Dy is discussed based on the photophysical properties of the corresponding gadolinium(iii) complex, [{(MeMeArO)3tacn}GdIII(THF)].

    DOI: 10.1039/c6dt01057a

  • Photoinduced bending of rod-like millimetre-size crystals of a rhodium dithionite complex with n-pentyl moieties Reviewed

    Hidetaka Nakai, Kengo Matsuba, Masataka Akimoto, Tomonori Nozaki, Takahiro Matsumoto, Kiyoshi Isobe, Masahiro Irie, Seiji Ogo

    Chemical Communications   52 ( 23 )   4349 - 4352   2016

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    Rod-like millimetre-size crystals of a newly prepared rhodium dithionite complex with n-pentyl moieties bend upon photoirradiation and return to the initial shape upon heating; the roles of the flexible n-pentyl moieties as well as the photoreactive dithionite unit (μ-O2SSO2) are disclosed by single crystal X-ray diffraction.

    DOI: 10.1039/c6cc00059b

  • A (Ni-SIr)I model for [NiFe]hydrogenase Reviewed

    Takahiro Matsumoto, Tatsuya Ando, Yuki Mori, Takeshi Yatabe, Hidetaka Nakai, Seiji Ogo

    Journal of Organometallic Chemistry   796   73 - 76   2015.11

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    We report the synthesis and characterization of a μ-hydroxo NiRu complex as a model for the active site of (Ni-SIr)I of [NiFe]hydrogenase. This is the first example of the (Ni-SIr)I model with a bridging hydroxo ligand between dimetal centers and an available coordination site on Ni center cis to the bridging hydroxo ligand. We have determined the structure of the (Ni-SIr)I model complex by X-ray analysis and reported reversible switching between the catalytically inactive (Ni-SIr)I and a catalytically active (Ni-SIr)II models.

    DOI: 10.1016/j.jorganchem.2014.09.025

  • A High-Valent Iron(IV) Peroxo Core Derived from O2. Angew. Chem. Int. Ed. Reviewed International journal

    Takahiro Kishima, Takahiro Matsumoto, Nakai Hidetaka, Shinya Hayami, Takehiro Ohta, Seiji Ogo

    Angew. Chem. Int. Ed.   55 ( 2 )   724 - 727   2015.10

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    DOI: 10.1002/anie.201507022.

  • An IrSi oxide film as a highly active water-oxidation catalyst in acidic media Reviewed

    Viet Ha Tran, Takeshi Yatabe, Takahiro Matsumoto, Hidetaka Nakai, Kazuharu Suzuki, Takao Enomoto, Takashi Hibino, Kenji Kaneko, Seiji Ogo

    Chemical Communications   51 ( 63 )   12589 - 12592   2015.8

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    We report an acid-stable Si oxide-doped Ir oxide film (IrSi oxide film), made by metal organic chemical vapour deposition (MOCVD) of an IrV complex for electrochemical water-oxidation. This is a successful improvement of catalytic ability and stability depending upon the pH of Ir oxide by doping of Si oxide. The turnover frequency (TOF) of the electrochemical water-oxidation by the IrSi oxide film is the highest of any Si oxide-doped Ir oxide materials and higher even than that of Ir oxide in acidic media.

    DOI: 10.1039/c5cc04286k

  • An IrSi Oxide Film as a Highly Active Water-Oxidation Catalyst in Acidic Media. Reviewed International journal

    Viet-Ha Tran, Takeshi Yatabe, Takahiro Matsumoto, Nakai Hidetaka, Kazuharu Suzuki, Takao Enomoto, Takashi Hibino, Kenji Kaneko, Seiji Ogo

    Chem. Commun.   51 ( 63 )   12589 - 12592   2015.7

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    DOI: 10.1039/C5CC04286K

  • An N2-Compatible Ni0 MOCVD precursor. Reviewed International journal

    Viet-Ha Tran, Takeshi Yatabe, Takahiro Matsumoto, Nakai Hidetaka, Kazuharu Suzuki, Takao Enomoto, Seiji Ogo

    Chem. Lett.   44 ( 6 )   794 - 796   2015.6

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    DOI: org/10.1246/cl.150155

  • A macrocyclic tetraamine bearing four phenol groups a new class of heptadentate ligands to provide an oxygen-sensitive luminescent Tb(iii) complex with an extendable phenol pendant arm Reviewed

    Hidetaka Nakai, Kyoshiro Nonaka, Takahiro Goto, Juncheol Seo, Takahiro Matsumoto, Seiji Ogo

    Dalton Transactions   44 ( 24 )   10923 - 10927   2015.6

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    This paper presents a 1,4,7,10-teraazacyclododecane-based tetrakis-phenol as a protonated ligand precursor and its oxygen-sensitive luminescent terbium(iii) complex with an extendable phenol pendant arm (Φ = 0.91 under N2, Φ = 0.031 under air), in which the potentially N4O4-octadentate ligand unprecedentedly coordinates to the Tb3+ ion in a N4O3-heptadentate fashion.

    DOI: 10.1039/c5dt00816f

  • A Macrocyclic Tetraamine bearing Four Phenol Groups: A New Class of Heptadentate Ligands To Provide an Oxygen-Sensitive Luminescent Tb(III) Complex with an Extendable Phenol Pendant Arm. Reviewed International journal

    Nakai Hidetaka, Kyoshiro Nonaka, Juncheol Seo, Takahiro Matsumoto, Seiji Ogo

    Dalton Trans.   44 ( 24 )   10923 - 10927   2015.5

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    DOI: 10.1039/C4CC07717B

  • An Fe-based Model for Metabolism Linking between O2-reduction and H2O-oxidation. Reviewed International journal

    Takeshi Yatabe, Mitsuhiro Kikkawa, Takahiro Matsumoto, Keishi Urabe, ROBERTSON ANDREW, Nakai Hidetaka, Seiji Ogo

    Chem. Lett.   44 ( 9 )   1263 - 1265   2015.5

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    DOI: org/10.1246/cl.150468

  • An N2-compatible Ni0 metal-organic chemical vapor deposition (MOCVD) precursor Reviewed

    Viet Ha Tran, Takeshi Yatabe, Takahiro Matsumoto, Hidetaka Nakai, Kazuharu Suzuki, Takao Enomoto, Seiji Ogo

    Chemistry Letters   44 ( 6 )   794 - 796   2015.1

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    We report the first example of a Ni0 precursor that provides a contamination-free (<1%) nickel film by metal-organic chemical vapor deposition (MOCVD) using N2 as the carrier gas. The structure and physical properties of the Ni0 precursor and subsequent film are described.

    DOI: 10.1246/cl.150155

  • An fe-based model for metabolism linking between O2-reduction and H2O-oxidation Reviewed

    Takeshi Yatabe, Mitsuhiro Kikkawa, Takahiro Matsumoto, Keishi Urabe, Andrew Robertson, Hidetaka Nakai, Seiji Ogo

    Chemistry Letters   44 ( 9 )   1263 - 1265   2015.1

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    Here, we report the first Fe-based model for metabolism linking between the dioxygen reduction of respiration and the water oxidation of photosynthesis. The reaction mechanism was investigated by X-ray analysis, UV-vis spectroscopy, and mass spectrometry.

    DOI: 10.1246/cl.150468

  • A [NiFe]hydrogenase model that catalyses the release of hydrogen from formic acid Reviewed

    Nga T. Nguyen, Yuki Mori, Takahiro Matsumoto, Takeshi Yatabe, Ryota Kabe, Hidetaka Nakai, Ki Seok Yoon, Seiji Ogo

    Chemical Communications   50 ( 87 )   13385 - 13387   2014.11

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    We report the decomposition of formic acid to hydrogen and carbon dioxide, catalysed by a NiRu complex originally developed as a [NiFe]hydrogenase model. This is the first example of H2 evolution, catalysed by a [NiFe]hydrogenase model, which does not require additional energy.

    DOI: 10.1039/c4cc05911e

  • A highly luminescent and highly oxygen-sensitive Tb(III) complex with a tris-aryloxide functionalised 1,4,7-triazacyclononane ligand Reviewed

    Hidetaka Nakai, Takahiro Goto, Kazuhiro Kitagawa, Kyoshiro Nonaka, Takahiro Matsumoto, Seiji Ogo

    Chemical Communications   50 ( 99 )   15737 - 15739   2014.11

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    This communication presents a new terbium(III) complex that shows the highest luminescence quantum yield among the oxygen-sensitive lanthanide complexes (Φ = 0.91 under N2, Φ = 0.054 under air).

    DOI: 10.1039/c4cc07717b

  • A Highly Luminescent and Highly Oxygen-Sensitive Tb(III) Complex with a Tris-Aryloxide Functionalised 1,4,7-Triazacyclononane Ligand. Reviewed International journal

    Nakai Hidetaka, Takahiro Goto, Kazuhiro Kitagawa, Kyoshiro Nonaka, Takahiro Matsumoto, Seiji Ogo

    Chem. Commun.   50 ( 99 )   15737 - 15739   2014.10

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    DOI: 10.1039/C4CC07717B

  • Synthesis and crystal structure of a dinuclear, monomeric MnIIp-semiquinonato complex Reviewed

    Harutaka Nakamori, Takahiro Matsumoto, Takeshi Yatabe, Ki Seok Yoon, Hidetaka Nakai, Seiji Ogo

    Chemical Communications   50 ( 86 )   13059 - 13061   2014.10

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    Herein, we report the first crystal structure of a monomeric p-semiquinonato d-block complex and its reactivity toward dioxygen, closely associated with a biological system of an oxygen evolving centre of photosystem II.

    DOI: 10.1039/c4cc06055e

  • Synthesis and Crystal Structure of a Dinuclear, Monomeric MnII p-Semiquinonato Complex. Reviewed International journal

    Harutaka Nakamori, Takahiro Matsumoto, Takeshi Yatabe, Yoon Ki-Seok, Nakai Hidetaka, Seiji Ogo

    Chem. Commun.   50 ( 86 )   2014.9

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  • Catalytic C-F bond hydrogenolysis of fluoroaromatics by [(η5-C5Me5)RhI(2,2′-bipyridine)] Reviewed

    Hidetaka Nakai, Kihun Jeong, Takahiro Matsumoto, Seiji Ogo

    Organometallics   33 ( 17 )   4349 - 4352   2014.9

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    A new class of efficient catalyst, the Rh(I) complex [(η5-C5Me5)RhI(bpy)] (1; bpy = 2,2′-bipyridine), for the C-F bond hydrogenolysis of fluoroaromatics (C6F5CF3, C6F6, C6F5H, and C6F5CH3) is presented. The best turnover number of 380 for C6F6 is afforded by using 0.1 mol % of 1, 0.8 MPa of H2, and 2 equiv of Et2NH in CH3CN at 25 °C. The successful isolation of the C-F bond cleavage product [(η5-C5Me5)RhIII(bpy)(C6F5)](F) as a plausible intermediate of the catalytic hydrogenolysis of C6F6 by 1 is also described.

    DOI: 10.1021/om500647h

  • A (Ni-SIr)I Model for [NiFe]hydrogenase. Reviewed International journal

    Takahiro Matsumoto, Tatsuya Ando, Yuki Mori, Takeshi Yatabe, Nakai Hidetaka, Seiji Ogo

    J. Organomet. Chem.   2014.9

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  • A [NiFe]hydrogenase Model That Catalyses the Release of Hydrogen from Formic Acid. Reviewed International journal

    Nguyen, Nga T., Yuki Mori, Takahiro Matsumoto, Takeshi Yatabe, Ryota Kabe, Nakai Hidetaka, Yoon Ki-Seok, Seiji Ogo

    Chem. Commun.   50 ( 87 )   2014.9

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  • Synthesis of Aqueous-stable and Water-soluble Mononuclear Nonheme MnV–oxo Complexes Using H2O2 as an Oxidant. Reviewed International journal

    Takeshi Yatabe, Takahiro Kikunaga, Takahiro Matsumoto, Nakai Hidetaka, Yoon Ki-Seok, Seiji Ogo

    Chem. Lett.   43 ( 8 )   2014.8

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  • Hydrogenase from citrobacter sp. S-77 surpasses platinum as an electrode for H2 oxidation reaction Reviewed

    Takahiro Matsumoto, Shigenobu Eguchi, Hidetaka Nakai, Takashi Hibino, Ki Suk Yoon, Seiji Ogo

    Angewandte Chemie - International Edition   53 ( 34 )   8895 - 8898   2014.8

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    Reported herein is an electrode for dihydrogen (H2) oxidation, and it is based on [NiFe]Hydrogenase from Citrobacter sp. S-77 ([NiFe] S77). It has a 637 times higher mass activity than Pt (calculated based on 1 mg of [NiFe]S77 or Pt) at 50 mV in a hydrogen half-cell. The [NiFe]S77 electrode is also stable in air and, unlike Pt, can be recovered 100% after poisoning by carbon monoxide. Following characterization of the [NiFe]S77 electrode, a fuel cell comprising a [NiFe] S77 anode and Pt cathode was constructed and shown to have a a higher power density than that achievable by Pt.

    DOI: 10.1002/anie.201404701

  • Catalytic C−F Bond Hydrogenolysis of Fluoroaromatics by [(η5‑C5Me5)RhI(2,2′-bipyridine)]. Reviewed International journal

    Nakai Hidetaka, Kihun Jeong, Takahiro Matsumoto, Seiji Ogo

    Organometallics   33 ( 17 )   2014.8

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  • [NiFe]Hydrogenase from Citrobacter sp. S-77 Surpasses Platinum as an Electrode for H2 Oxidation Reaction. Reviewed International journal

    Takahiro Matsumoto, Shigenobu Eguchi, Nakai Hidetaka, Takashi Hibino, Yoon Ki-Seok, Seiji Ogo

    Angew. Chem. Int. Ed.   53 ( 34 )   2014.6

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    水素と酸素から電気を作る燃料電池は、排出物として水しか生成しないクリーンな発電装置である。燃料電池はその構造によって数種類に分類され、なかでも低温作動や小型軽量化が可能な固体高分子形燃料電池(polymer electrolyte fuel cell、PEFC)は、家庭用、携帯用、自動車用電源に適している。しかし、PEFCの電極触媒は枯渇資源で高価な白金触媒であり、その代替触媒の開発が行われてきたが、未だに白金に代わる実用触媒の開発には至っていない。本研究では、水素極(水素から電子を取り出す電極)の脱白金触媒として水素酸化酵素であるヒドロゲナーゼを用いたPEFCを初めて作製し、それらの発電実験に成功した。本研究で使用したヒドロゲナーゼS–77(当研究室で新規に探索・精製・単離)は、これまでのヒドロゲナーゼよりも高活性かつ頑丈であり、PEFCの作動条件でも十分にその機能を発揮できる。ヒドロゲナーゼS–77の単位重量あたりの水素酸化活性は、白金触媒に対して637倍であることを明らかにした。

  • A Model for the Water-Oxidation and Recovery Systems of the Oxygen-Evolving Complex. Reviewed International journal

    Takeshi Yatabe, Mitsuhiro Kikkawa, Takahiro Matsumoto, Nakai Hidetaka, Kenji Kaneko, Seiji Ogo

    Dalton Trans.   43 ( 8 )   2014.2

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  • A model for the water-oxidation and recovery systems of the oxygen-evolving complex Reviewed

    Takeshi Yatabe, Mitsuhiro Kikkawa, Takahiro Matsumoto, Hidetaka Nakai, Kenji Kaneko, Seiji Ogo

    Dalton Transactions   43 ( 8 )   3063 - 3071   2014.2

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    We propose a model for the water-oxidation and recovery systems of the oxygen-evolving complex (OEC) of the photosystem II (PSII) enzyme. The whole system is constructed from two catalytic cycles, conducted as a tandem reaction: (i) a water-oxidation loop uses cerium(iv) ammonium nitrate as an oxidant to activate a dimanganese complex for water-oxidation and thereby liberate a molecule of O2 and (ii) a recovery loop begins with photoinhibition of the dimanganese complex but then uses O2 to reactivate the manganese centre. The net result is a catalytic water-oxidation catalyst that can use self-generated O2 for recovery.

    DOI: 10.1039/c3dt52846d

  • Synthesis of aqueous-stable and water-soluble mononuclear nonheme MnV-Oxo complexes using H2O2as an oxidant Reviewed

    Takeshi Yatabe, Takahiro Kikunaga, Takahiro Matsumoto, Hidetaka Nakai, Ki Seok Yoon, Seiji Ogo

    Chemistry Letters   43 ( 8 )   1380 - 1382   2014.1

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    We report the synthesis of mononuclear nonheme manganese(V)oxo complexes in aqueous acetonitrile solution from the reaction of manganese(III) complexes using hydrogen peroxide as an oxidant for the first time. A crystal structure of chloro derivative of manganese(V)oxo complex and its reactivity toward 3,5-di-tert-butyl-catechol are also reported.

    DOI: 10.1246/cl.140376

  • Isolation of a MnIV Acylperoxo Complex and Its Monooxidation Ability. Reviewed International journal

    Takahiro Kikunaga, Takahiro Matsumoto, Takehiro Ohta, Nakai Hidetaka, Yoshinari Naruta, Kwang-Hyun Ahn, Yoshihito Watanabe, Seiji Ogo

    Chem. Commun.   49 ( 75 )   2013.10

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  • Isolation and crystal structure of the proposed low-valent active species in the H2 activation catalytic cycle Reviewed

    Daisuke Inoki, Takahiro Matsumoto, Hidetaka Nakai, Seiji Ogo

    European Journal of Inorganic Chemistry   ( 22-23 )   3978 - 3986   2013.10

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    We provide confirmation of our proposed design principles for a H 2 activation catalytic cycle by constructing a new catalyst. We have been able to obtain a crystal structure to confirm our proposition that a reduced, dinuclear species stores electrons from hydrogen molecules in a metal-metal bond.

    DOI: 10.1002/ejic.201300049

  • Isolation and Crystal Structure of the Proposed Low-Valent Active Species in the H2 Activation Catalytic Cycle. Reviewed International journal

    Daisuke Inoki, Takahiro Matsumoto, Nakai Hidetaka, Seiji Ogo

    Eur. J. Inorg. Chem.   2013(22-23) ( 22-23 )   2013.8

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  • Reversible switching of the luminescence of a photoresponsive gadolinium(III) complex Reviewed

    Hidetaka Nakai, Kazuhiro Kitagawa, Harutaka Nakamori, Taisuke Tokunaga, Takahiro Matsumoto, Koichi Nozaki, Seiji Ogo

    Angewandte Chemie - International Edition   52 ( 33 )   8722 - 8725   2013.8

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    From blue to red: The structure and luminescence properties of the gadolinium(III) complex 1 were investigated. Reversible switching of the luminescence of 1 in THF at room temperature by alternating light irradiation and O2 exposure is presented, during which the emission color changes as shown in the picture. Light-induced phosphorescence of 1 plays a key role in this behavior.

    DOI: 10.1002/anie.201303137

  • Isolation of a MnIV acylperoxo complex and its monooxidation ability Reviewed

    Takahiro Kikunaga, Takahiro Matsumoto, Takehiro Ohta, Hidetaka Nakai, Yoshinori Naruta, Kwang Hyun Ahn, Yoshihito Watanabe, Seiji Ogo

    Chemical Communications   49 ( 75 )   8356 - 8358   2013.8

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    The first example of monooxygenation by a high-valent MnIV complex with a peroxide is described. A key MnIV acylperoxo intermediate, which uses m-chloroperoxybenzoic acid as the oxygen donor, is directly observed by electro-spray ionization mass spectrometry and resonance Raman spectroscopy.

    DOI: 10.1039/c3cc43447h

  • Reversible Switching of the Luminescence of a Photoresponsive Gadolinium(III) Complex. Reviewed International journal

    Nakai Hidetaka, Kazuhiro Kitagawa, Harutaka Nakamori, Taisuke Tokunaga, Takahiro Matsumoto, Koichi Nozaki, Seiji Ogo

    Angew. Chem. Int. Ed.   52 ( 33 )   2013.8

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  • Organometallic Catalysts for Use in a Fuel Cell Reviewed

    Takahiro Matsumoto, Kyoungmok Kim, Hidetaka Nakai, Takashi Hibino, Seiji Ogo

    ChemCatChem   5 ( 6 )   1368 - 1373   2013.6

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    We report the successful increase in performance of a fuel cell based on organometallic catalysis. An organometallic [NiIIRuIV] peroxo complex functions as cathode catalyst and was designed following mechanistic consideration of the cell. It was confirmed that the organometallic [NiIIRuIV] peroxo catalyst could function in the fuel cell with a 240% increase in power output over our previous systems. This organometallic catalyst can act in both solid and solution phases and allows observation of the mechanism, hence providing us further opportunity for future improvement.

    DOI: 10.1002/cctc.201200595

  • Organometallic Catalysts for Use in a Fuel Cell. Reviewed International journal

    Takahiro Matsumoto, Kyoungmok Kim, Nakai Hidetaka, Takashi Hibino, Seiji Ogo

    ChemCatChem   5 ( 6 )   2013.6

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  • A Functional [NiFe]Hydrogenase Mimic That Catalyzes Electron and Hydride Transfer from H2. Reviewed International journal

    Seiji Ogo, Koji Ichikawa, Takahiro Kishima, Takahiro Matsumoto, Nakai Hidetaka, Katsuhiro Kusaka, Takashi Ohhara

    Science   339 ( 6120 )   2013.2

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    ニッケル・鉄ヒドロゲナーゼは、常温・常圧という温和な条件下で触媒的に水素を酸化する酵素である。多くの研究グループが、ニッケル・鉄ヒドロゲナーゼの機能モデル錯体の開発を試みてきたが、これまで達成されることはなかった。本研究では、世界で初めて常温・常圧で水素をヘテロリティックに活性化し、水素を酸化できるニッケル・鉄モデル錯体の開発に成功した。その反応中間体であるヒドリド錯体の構造は、X線構造解析をはじめとする種々の分光学的測定によって決定された。

  • A functional [NiFe]hydrogenase mimic that catalyzes electron and hydride transfer from H2 Reviewed

    Seiji Ogo, Koji Ichikawa, Takahiro Kishima, Takahiro Matsumoto, Hidetaka Nakai, Katsuhiro Kusaka, Takashi Ohhara

    Science   339 ( 6120 )   682 - 684   2013.2

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    Chemists have long sought to mimic enzymatic hydrogen activation with structurally simpler compounds. Here, we report a functional [NiFe]-based model of [NiFe]hydrogenase enzymes. This complex heterolytically activates hydrogen to form a hydride complex that is capable of reducing substrates by either hydride ion or electron transfer. Structural investigations were performed by a range of techniques, including x-ray diffraction and neutron scattering, resulting in crystal structures and the finding that the hydrido ligand is predominantly associated with the Fe center. The ligand's hydridic character is manifested in its reactivity with strong acid to liberate H2.

    DOI: 10.1126/science.1231345

  • Selective redox activation of H2 or O2 in a [NiRu] complex by aromatic ligand effects Reviewed

    Kyoungmok Kim, Takahiro Kishima, Takahiro Matsumoto, Hidetaka Nakai, Seiji Ogo

    Organometallics   32 ( 1 )   79 - 87   2013.1

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    We present two closely related series of a [NiFe] hydrogenase analogue. Based on a [NiRu] core, these complexes demonstrate inactivity, H2 activation, or O2 activation depending only on the nature of the Ru-coordinated aromatic ligand. It is demonstrated that even small changes made to this aromatic ligand can modulate the catalytic activity of the complex. Structural, electrochemical, kinetic, and thermodynamic studies reveal that differences in activation and binding modes of the substrates, combined with differences in σ donation and lability of the aromatic ligands, result in abrupt changes in catalytic activity.

    DOI: 10.1021/om300833m

  • Selective Redox Activation of H2 or O2 in a [NiRu] Complex by Aromatic Ligand Effects. Reviewed International journal

    Kyoungmok Kim, Takahiro Kishima, Takahiro Matsumoto, Nakai Hidetaka, Seiji Ogo

    Organometallics   32 ( 1 )   2012.12

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  • A Neutral Five-coordinated Organoruthenium(0) Complex:X-ray Structure and Unique Solvatochromism. Reviewed International journal

    Jeong, Kihun; Nakamori, Harutaka; Imai, Shunsuke; Matsumoto, Takahiro; Ogo, Seiji;*Nakai, Hidetaka.*

    Chem. Lett.   41 ( 6 )   2012.6

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  • Simple ligand effects switch a hydrogenase mimic between H 2 and O 2 activation Reviewed

    Kyoungmok Kim, Takahiro Matsumoto, Andrew Robertson, Hidetaka Nakai, Seiji Ogo

    Chemistry - An Asian Journal   7 ( 6 )   1394 - 1400   2012.6

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    Herein, we report a [NiRu] biomimetic system for O 2-tolerant [NiFe]hydrogenases and demonstrate that electron donation to the [NiRu] center can switch the system between the activation of H 2 and O 2 through simple ligand effects by using hexamethylbenzene and pentamethylcyclopentadienyl ligands, respectively. Furthermore, we present the synthesis and direct observations of a [NiRu]-peroxo species, which was formed by the oxygenation of a Ni-SIa model [NiRu] complex, that we propose as a biomimetic analogue of O 2-bound species (OBS) of O 2-tolerant [NiFe]hydrogenases. The [NiRu]-peroxo complex was fully characterized by X-ray analysis, X-ray photoelectron spectroscopy (XPS), mass spectrometry, and 1H NMR spectroscopy. The OBS analogue was capable of oxidizing p-hydroquinone and sodium borohydride to turn back into the Ni-SIa model complex.

    DOI: 10.1002/asia.201101020

  • A neutral five-coordinated organoruthenium(0) complex X-ray structure and unique solvatochromism Reviewed

    Kihun Jeong, Harutaka Nakamori, Shunsuke Imai, Takahiro Matsumoto, Seiji Ogo, Hidetaka Nakai

    Chemistry Letters   41 ( 6 )   650 - 651   2012.6

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    The structure of a neutral five-coordinated organoruthenium( 0) complex [(η 6-C 6Me 6)Ru 0(bpy)] (1, bpy: 2,2′-bipyridine) was determined by X-ray diffraction analysis. The solvent-induced reversible color change based on the interconversion between the purple Ru 0 complex 1 and a yellow Ru IIhydride complex [(η 6-C 6Me 6)Ru II(bpy)H] + is presented.

    DOI: 10.1246/cl.2012.650

  • Experimental study of reductive elimination of H 2 from rhodium hydride species Reviewed

    Daisuke Inoki, Takahiro Matsumoto, Hidetaka Nakai, Seiji Ogo

    Organometallics   31 ( 8 )   2996 - 3001   2012.4

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    A Rh III monohydride terpyridine complex undergoes reductive elimination of H 2 in CH 3CN to form a dinuclear Rh II complex with a metal-metal bond. Kinetic studies have revealed that the conversion from the monohydride species to the dinuclear species with evolution of H 2 obeys first-order kinetics and have determined the kinetic deuterium isotope effect value to be 2.0. We discuss the mechanism for the reductive elimination of H 2 from rhodium hydride species.

    DOI: 10.1021/om2009759

  • Establishing the mechanism of Rh-catalysed activation of O 2 by H 2 Reviewed

    Daisuke Inoki, Takahiro Matsumoto, Hideki Hayashi, Keisuke Takashita, Hidetaka Nakai, Seiji Ogo

    Dalton Transactions   41 ( 15 )   4328 - 4334   2012.4

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    Reductive activation of O 2 by H 2 with rhodium terpyridine complexes in H 2O and CH 3CN is described and the mechanism is fully elucidated. The rhodium complex extracts electrons from H 2 and reductively activates O 2 to form a peroxo active intermediate. This intermediate is able to oxidise triphenyl phosphine to triphenyl phosphine oxide. A model system constructed in CH 3CN provides isolable analogues of catalytic intermediates in H 2O, allowing a detailed look at each step in the catalytic cycle.

    DOI: 10.1039/c1dt11599e

  • Experimental Study of Reductive Elimination of H2 from Rhodium Hydride Species Reviewed International journal

    Inoki, Daisuke; Matsumoto, Takahiro; Nakai, Hidetaka; Ogo, Seiji

    Organometallics   31 ( 8 )   2012.3

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  • Simple Ligand Effects Switch a Hydrogenase Mimic between H2 and O2 Activation Invited Reviewed International journal

    Kim, Kyoungmok; Matsumoto, Takahiro; Robertson, Andrew; Nakai, Hidetaka; Ogo, Seiji

    Chem. Asian J.   2012.2

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  • A mer-Triaqua Rh complex with a terpyridine ligand Reviewed

    Daisuke Inoki, Takahiro Matsumoto, Hidetaka Nakai, Seiji Ogo

    Chemistry Letters   41 ( 1 )   116 - 118   2012.1

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    We report the synthesis of a mer-triaqua Rh III complex using terpyridine as a meridional tridentate ligand. This is the first example of a structurally characterized six-coordinated mertriaqua complex for any second- or third-row element from the main transition-metal groups (groups 511). This is also the first example of a structurally characterized mer-triaqua complex with terpyridine for any transition metal. Acid dissociation constants, pK a1 and pK a2, of the triaqua complex are determined to be 3.0 and 6.9, respectively.

    DOI: 10.1246/cl.2012.116

  • A mer-Triaqua Rh Complex with a Terpyridine Ligand Reviewed International journal

    Inoki, Daisuke; Matsumoto, Takahiro; Nakai, Hidetaka; Ogo, Seiji

    Chem. Lett.   41 ( 1 )   2011.12

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  • Establishing the Mechanism of Rh-catalysed Activation of O2 by H2 Reviewed International journal

    Inoki, Daisuke; Matsumoto, Takahiro; Hayashii, Hideki; Takashita, Keisuke; Nakai, Hidetaka; Ogo, Seiji

    Dalton Transactions   2011.11

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    DOI: DOI: 10.1039/c1dt11599e

  • The Development of Aqueous Transfer Hydrogenation Catalysts Reviewed International journal

    Robertson, Andrew; Matsumoto, Takahiro; Ogo, Seiji

    Dalton Transactions   40   2011.10

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  • The development of aqueous transfer hydrogenation catalysts Reviewed

    Andrew Robertson, Takahiro Matsumoto, Seiji Ogo

    Dalton Transactions   40 ( 40 )   10304 - 10310   2011.10

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    This review discusses the development of aqueous phase, homogeneous, transfer hydrogenation catalysis. Transfer hydrogenation catalysts, based on Ru, Ir and Rh, reduce organic substrates in water by assisting the transfer of hydrogen from simple donor species. These catalysts are expected to have significant benefits when compared with organic phase catalysts, including greater activity, greater selectivity and smaller environmental impact. They will therefore be expected to make a significant contribution to homogeneous catalysis and 'green chemistry'. Here, we comprehensively examine these catalysts, paying special attention to structural features.

    DOI: 10.1039/c1dt10544b

  • Ru Ccyclooctatetraene Precursors for MOCVD Reviewed International journal

    Tatsuya Ando, Naoki Nakata, Kazuharu Suzuki, Takahiro Matsumotoa, and Seiji Ogo

    Dalton Trans.   2011.10

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    DOI: 10.1039/c1dt11454a

  • Model study of CO inhibition of [NiFe]hydrogenase Reviewed

    Takahiro Matsumoto, Ryota Kabe, Kyoshiro Nonaka, Tatsuya Ando, Ki Suk Yoon, Hidetaka Nakai, Seiji Ogo

    Inorganic Chemistry   50 ( 18 )   8902 - 8906   2011.9

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    We propose a modified mechanism for the inhibition of [NiFe]hydrogenase ([NiFe]H 2ase) by CO. We present a model study, using a NiRu H 2ase mimic, that demonstrates that (i) CO completely inhibits the catalytic cycle of the model compound, (ii) CO prefers to coordinate to the Ru II center rather than taking an axial position on the Ni II center, and (iii) CO is unable to displace a hydrido ligand from the NiRu center. We combine these studies with a reevaluation of previous studies to propose that, under normal circumstances, CO inhibits [NiFe]H 2ase by complexing to the Fe II center.

    DOI: 10.1021/ic200965t

  • The Useful Properties of H2O as a Ligand of a Hydrogenases Mimic Reviewed International journal

    Zheng, Chunbai; Kim, Kyoungmok; Matsumoto, Takahiro; Ogo, Seiji

    Dalton Transactions   39 ( 9 )   2010.3

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    DOI: 10.1039/b921273f

  • Concerto Catalysis — Harmonising [NiFe]hydrogenase and NiRu Model Catalysts Invited Reviewed International journal

    Ichikawa, Koji; Nonaka, Kyoshiro; Matsumoto, Takahiro; Kure, Bunsho; Yoon, Ki-Seok; Higuchi, Yoshiki; Yagi, Tatsuhiko, Ogo, Seiji

    Dalton Transactions   39 ( 12 )   2010.3

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    DOI: 10.1039/b926061g

  • Dissolved N2 Sensing by pH-dependent Ru Complexes Reviewed International journal

    Kizaki, Tetsuro; Matsumoto, Takahiro; Ogo, Seiji

    Dalton Transactions   39 ( 5 )   2010.2

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    DOI: 10.1039/b918940h

  • A pH-Stable Ruthenium(II)-based Sensing System for Dissolved Dinitrogen Reviewed International journal

    Kizaki, Tetsuro; Abe, Takeru; Matsumoto, Takahiro; Ogo Seiji

    Chemistry Letters   39 ( 2 )   2010.1

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    DOI: 10.1246/cl.2010.128

  • An Acid-Stable Organoruthenium Complex Suitable as a Bidentate Building Block Reviewed International journal

    Zheng, Chunbai; Inoki, Daisuke; Matsumoto, Takahiro; Ogo, Seiji

    Chemistry Letters   39 ( 2 )   2010.1

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    DOI: 10.1246/cl.2010.130

  • Aliphatic C-H bond activation initiated by a (μ-η2 η2-peroxo)dicopper(II) complex in comparison with cumylperoxyl radical Reviewed

    Takahiro Matsumoto, Kei Ohkubo, Kaoru Honda, Akiko Yazawa, Hideki Furutachi, Shuhei Fujinami, Shunichi Fukuzumi, Masatatsu Suzuki

    Journal of the American Chemical Society   131 ( 26 )   9258 - 9267   2009.7

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    A (μ-η22-peroxo)dicopper(II) complex, [Cu2(H-L)(O2)]2+ (1-O2), supported by the dinucleating ligand 1,3-bis[bis(6-methyl-2-pyridylmethyl)aminomethyl] benzene (H-L) is capable of initiating C-H bond activation of a variety of external aliphatic substrates (SHn): 10-methyl-9,10-dihydroacridine (AcrH2), 1,4-cyclohexadiene (1,4-CHD), 9,10-dihydroanthracene (9,10-DHA), fluorene, tetralin, toluene, and tetrahydrofuran (THF), which have C-H bond dissociation energies (BDEs) ranging from ∼75 kcal mol-1 for 1,4-CHD to ∼92 kcal mol-1 for THF. Oxidation of SH n afforded a variety of oxidation products, such as dehydrogenation products (SH(n-2)), hydroxylated and further-oxidized products (SH(n-1)OH and SH(n-2)=O), dimers formed by coupling between substrates (H(n-1)S-SH(n-1)) and between substrate and H-L (H-L-SH(n-1)). Kinetic studies of the oxidation of the substrates initiated by 1-O2 in acetone at -70°C revealed that there is a linear correlation between the logarithms of the rate constants for oxidation of the C-H bonds of the substrates and their BDEs, except for THF. The combination of this correlation and the relatively large deuterium kinetic isotope effects (KIEs), k2H/k2D (13 for 9,10-DHA, ≳29 for toluene, and ∼34 for THF at -70°C and ∼9 for AcrH2 at -94°C) indicates that H-atom transfer (HAT) from SHn (SDn) is the rate-determining step. Kinetic studies of the oxidation of SHn by cumylperoxyl radical showed a correlation similar to that observed for 1-O2, indicating that the reactivity of 1-O2 is similar to that of cumylperoxyl radical. Thus, 1-O 2 is capable of initiating a wide range of oxidation reactions, including oxidation of aliphatic C-H bonds having BDEs from ∼75 to ∼92 kcal mol-1, hydroxylation of the m-xylyl linker of H-L, and epoxidation of styrene (Matsumoto, T.; et al. J. Am. Chem. Soc. 2006, 128, 3874).

    DOI: 10.1021/ja809822c

  • Critical aspects of [NiFe]hydrogenase ligand composition Reviewed

    Koji Ichikawa, Takahiro Matsumoto, Seiji Ogo

    Dalton Transactions   ( 22 )   4304 - 4309   2009.6

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    Structural analysis of the resting state of [NiFe]hydrogenase ([NiFe]H 2ase) shows that the active site has a characteristic bis(μ-thiolato)NiFe unit, where the Ni atom and the Fe atom are bridged by an undetermined oxygen-bearing ligand. This ligand probably derives from the aqueous solvent and is therefore most likely to be H2O, OH - or O2-. Here, we compare the reactivities of a NiFe and a NiRu complex when bearing either acetonitrile or aqueous ligands and demonstrate the critical role of an aqueous ligand in hydrogenase and its mimics. We also make observations on the necessity of organometallic metal-carbon bonds to the supporting frameworks.

    DOI: 10.1039/b819395a

  • Oxidation reactivity of bis(m-oxo) dinickel(iii) complexes Arene hydroxylation of the supporting ligand Reviewed

    Kaoru Honda, Jaeheung Cho, Takahiro Matsumoto, Jungyun Roh, Hideki Furutachi, Takehiko Tosha, Minoru Kubo, Shuhei Fujinami, Takashi Ogura, Teizo Kitagawa, Masatatsu Suzuki

    Angewandte Chemie - International Edition   48 ( 18 )   3304 - 3307   2009.4

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    In the nick(el) of time: Bis(μ-oxo) dinickel(III) complexes 2 (see scheme), generated in the reaction of 1 with H2O2, are capable of hydroxylating the xylyl linker of the supporting ligand to give 3. Kinetic studies reveal that hydroxylation proceeds by electrophilic aromatic substitution. The lower reactivity than the corresponding μ - η2: η2 - peroxo dicopper(II) complexes can be attributed to unfavorable entropy effects.

    DOI: 10.1002/anie.200900222

  • Extraction of electrons from H2 with a NiIRu I catalyst Reviewed

    Takahiro Matsumoto, Bunsho Kure, Seiji Ogo

    Chemistry Letters   37 ( 9 )   970 - 971   2008.9

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    The mechanism of extraction of electrons from H2 catalyzed by hydrogenases has proven challenging to elucidate. Catalytic extraction of electrons from H2 has been achieved by use of a low-valent Ni IRuI complex [NiI(μ-SR)2Ru I6-C6Me6)]{μ-SR) 2 = N,N′-dimethyl-N,N′-bis(2-mercaptoethyl)-1,3- propanediamine) as the active catalyst with evolution of H2 under ambient conditions. The electrons extracted from H2 have been used for a catalytic reduction of Cu2+ to Cu0 with the NiRu complexes.

    DOI: 10.1246/cl.2008.970

  • PH-Dependent isotope exchange and hydrogenation catalysed by water-soluble NiRu complexes as functional models for [NiFe]hydrogenases Reviewed

    Bunsho Kure, Takahiro Matsumoto, Koji Ichikawa, Shunichi Fukuzumi, Yoshiki Higuchi, Tatsuhiko Yagi, Seiji Ogo

    Dalton Transactions   ( 35 )   4747 - 4755   2008.9

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    The pH-dependent hydrogen isotope exchange reaction between gaseous isotopes and medium isotopes and hydrogenation of the carbonyl compounds have been investigated with water-soluble bis(μ-thiolate)(μ-hydride)NiRu complexes, NiII(μ-SR)2(μ-H)RuII {(μ-SR)2 = N,N′-dimethyl-N,N′-bis(2-mercaptoethyl)-1, 3-propanediamine}, as functional models for [NiFe]hydrogenases. In acidic media (at pH 4-6), the μ-H ligand of the NiII(μ-SR) 2(μ-H)RuII complexes has H+ properties, and the complexes catalyse the hydrogen isotope exchange reaction between gaseous isotopes and medium isotopes. A mechanism of the hydrogen isotope exchange reaction between gaseous isotopes and medium isotopes through a low-valent NiI(μ-SR)2RuI complex is proposed. In contrast, in neutral-basic media (at pH 7-10), the μ-H ligand of the Ni II(μ-SR)2(μ-H)RuII complexes acts as H-, and the complexes catalyse the hydrogenation of carbonyl compounds.

    DOI: 10.1039/b807555g

  • Aromatic hydroxylation reactivity of a mononuclear Cu(II)-alkylperoxo complex Reviewed

    Atsushi Kunishita, Junji Teraoka, Joseph D. Scanlon, Takahiro Matsumoto, Masatatsu Suzuki, Christopher J. Cramer, Shinobu Itoh

    Journal of the American Chemical Society   129 ( 23 )   7248 - 7249   2007.6

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    Reaction of copper(II) complex 1X supported by the tridentate bis(pyridylmethyl)amine ligand containing m-substituted phenyl groups at the 6-positions of the pyridine rings (LX) with H2O2 in the presence of triethylamine (NEt3) in acetone generates a copper(II)-alkylperoxo species 2X [2-hydroxy-2-hydroperoxypropane (HHPP) adduct]. The alkylperoxo intermediate 2X undergoes an efficient aromatic ligand hydroxylation reaction, producing a phenolate complex 4X via another intermediate 3X. Kinetic studies on the aromatic hydroxylation process are reported together with spectral characterization of 2X.

    DOI: 10.1021/ja071623g

  • Synthesis and reactivity of (μ-η22-peroxo)dicopper(II) complexes with dinucleating ligands Hydroxylation of xylyl linker with a NIH shift Reviewed

    Takahiro Matsumoto, Hideki Furutachi, Shigenori Nagatomo, Takehiko Tosha, Shuhei Fujinami, Teizo Kitagawa, Masatatsu Suzuki

    Journal of Organometallic Chemistry   692 ( 1-3 )   111 - 121   2007.1

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    New hexadentate dinucleating ligands having a xylyl linker, X-L-R, were synthesized, where X-L-R = 1,3-bis[bis(6-methyl-2-pyridylmethyl)aminomethyl]-2,4,6-trimethybenzene (Me2-L-Me) and 1,3-bis[bis(6-methyl-2-pyridylmethyl)aminomethyl]-2-fluorobenzene (H-L-F). They form dinuclear copper(I) complexes, [Cu2(X-L-R)]2+ (Me2-L-Me (1) and H-L-F (2)). The copper(I) complexes in acetone at -78 °C react with O2 to produce intra- and intermolecular (μ-η22-peroxo)dicopper(II) species depending on the concentrations of the complexes: both complexes generate intramolecular (μ-η22-peroxo)dicopper(II) species [Cu2(O2)(X-L-R)]2+ (1-O2 and 2-O2) at the concentrations below ∼5 mM, whereas at ∼60 mM, both complexes produce intermolecular (μ-η22-peroxo)dicopper(II) species, which were confirmed by the electronic and resonance Raman spectroscopies. The electronic spectrum of 1-O2 in acetone at concentrations below ∼5 mM showed an absorption band at (λmax = 442 nm, ε = 5600 M-1 cm-1) assignable to the πσ*(O-O)-to-Cu(II) ((d x2 - y2 + d x2 - y2) component) LMCT transition in addition to an intense band attributable to the πσ*(O-O)-to-Cu(II) ((d x2 - y2 - d x2 - y2) component) LMCT transition (λmax = 359 nm, ε = 21000 M-1 cm-1), indicating that the (μ-η22-peroxo)Cu(II)2 core of 1-O2 takes a butterfly structure. Decomposition of 1-O2 resulted in hydroxylation of the 2-position of the xylyl linker with 1,2-methyl migration (NIH shift), suggesting that the hydroxylation reaction proceeds via a cationic intermediate as proposed for closely related (μ-η22-peroxo)Cu(II)2 complexes having a xylyl linker. Kinetic study of the decomposition (hydroxylation of the xylyl linker) of 1-O2 suggests that a stereochemical effect of the methyl group in the 2-position of the xylyl linker has a significant influence on a transition state for decomposition (hydroxylation of the xylyl linker).

    DOI: 10.1016/j.jorganchem.2006.05.068

  • A mononuclear alkylperoxocopper(II) complex as a reaction intermediate in the oxidation of the methyl group of the supporting ligand Reviewed

    Masayasu Mizuno, Kaoru Honda, Jaeheung Cho, Hideki Furutachi, Takehiko Tosha, Takahiro Matsumoto, Shuhei Fujinami, Teizo Kitagawa, Masatatsu Suzuki

    Angewandte Chemie - International Edition   45 ( 41 )   6911 - 6914   2006.10

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    Stepwise down : Reaction of[Cu(Me2-tpa)]+ (tpa = bis(6-methyl-2-pyridylmethyl) (2-pyridylmethyl)amine) with H2O 2 results in regioselective oxidation of a methyl group of the Me2-tpa ligand to produce an alkylperoxocopper(II) complex [Cu(Me-tpa-CH2OO)]+ as a reaction intermediate, which undergoes further decomposition to give aldehyde and alcohol copper(I) complexes as well as alkoxo- and carboxylatocopper(II) complexes (see scheme; blue N, green Cu, red O). (Chemical Equation Presented).

    DOI: 10.1002/anie.200602477

  • Intramolecular arene hydroxylation versus intermolecular olefin epoxidation by (μ-η22-peroxo)dicopper(II) complex supported by dinucleating ligand Reviewed

    Takahiro Matsumoto, Hideki Furutachi, Masashi Kobino, Masato Tomii, Shigenori Nagatomo, Takehiko Tosha, Takao Osako, Shuhei Fujinami, Shinobu Itoh, Teizo Kitagawa, Masatatsu Suzuki

    Journal of the American Chemical Society   128 ( 12 )   3874 - 3875   2006.3

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    A discrete (μ-η22-peroxo)Cu(II)2 complex, [Cu2(O2)(H-L)]2+, is capable of performing not only intramolecular hydroxylation of a m-xylyl linker of a dinucleating ligand but also intermolecular epoxidation of styrene via electrophilic reaction to the C=C bond and hydroxylation of THF by H-atom abstraction.

    DOI: 10.1021/ja058117g

  • Poly(N-substituted-acrylamide)-branched schizophyllans are useful for selective recovery of homopolynucleotides through convenient and quick precipitation procedures Reviewed

    Takahiro Matsumoto, Mariko Umeda, Munenori Numata, Teruaki Hasegawa, Kazuo Sakurai, Kazuya Koumoto, Seiji Shinkai

    Polymer Journal   37 ( 3 )   177 - 185   2005.5

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    Schizophyllans carrying poly(N-substituted-acrylamidej-branches were synthesized from native schizophyllan through Ce(IV)-initiated radical homo- or co-polymerization of N-iso-propyl- and N-sec-butyl-acryl-amide. A series of structural analyses including elemental analysis, gel permeation chromatography, 1H NMR, and enzymatic degradation using β-1,3-glucanase revealed that schizophyllans (150 kDa) bearing long poly(N-substituted- acrylamide)-branches (ca. 290 kDa) are obtained. These SPG-conjugates form macromolecular complexes with certain homopolynucleotides such as poly(C), poly(dA), and poly(A) and then efficiently co-precipitate them on heating. For example, schizophyllan carrying poly(N-iso-propylacrylamide)-branches can selectively recover poly(C) from a mixture of poly(C) and poly(U) by simple heating (36°C) followed by centrifugation. HPLC analysis of the recovered polynucleotide revealed the high poly(C)-selectivity (poly(C):poly(U) = 95:5). Similarly, schizophyllan carrying more hydrophobic poly(N-iso-propylacrylamide- co-N-sec-butylacrylamide)-branches precipitates at lower temperature (ca. 20°C) and is applicable to isolation of poly(A) that forms less stable macromolecular complexes with SPG and SPG-derivatives (the dissociation temperatures are around 30°C).

    DOI: 10.1295/polymj.37.177

  • Synthesis and reactivity of a (μ-1,1-hydroperoxo)(μ-hydroxo) dicopper(II) complex Ligand hydroxylation by a bridging hydroperoxo ligand Reviewed

    Kyosuke Itoh, Hideki Hayashi, Hideki Furutachi, Takahiro Matsumoto, Shigenori Nagatomo, Takehiko Tosha, Shoichi Terada, Shuhei Fujinami, Masatatsu Suzuki, Teizo Kitagawa

    Journal of the American Chemical Society   127 ( 14 )   5212 - 5223   2005.4

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    A new tetradentate tripodal ligand (L3) containing sterically bulky imidazolyl groups was synthesized, where L3 is tris(1-methyl-2-phenyl-4- imidazolylmethyl)amine. Reaction of a bis(μ-hydroxo)dicopper(II) complex, [Cu2(L3)2(OH)2]2+ (1), with H 2O2 in acetonitrile at -40 °C generated a (μ-1,1-hydroperoxo)dicopper(II) complex [Cu2(L3) 2(OOH)(OH)]2+ (2), which was characterized by various physicochemical measurements including X-ray crystallography. The crystal structure of 2 revealed that the complex cation has a Cu2(μ-1,1- OOH)(μ-OH) core and each copper has a square pyramidal structure having an N3O2 donor set with a weak ligation of a tertiary amine nitrogen in the apex. Consequently, one pendant arm of L3 in 2 is free from coordination, which produces a hydrophobic cavity around the Cu 2(μ-1,1-OOH)(μ-OH) core. The hydrophobic cavity is preserved by hydrogen bondings between the hydroperoxide and the imidazole nitrogen of an uncoordinated pendant arm in one side and the hydroxide and the imidazole nitrogen of an uncoordinated pendant arm in the other side. The hydrophobic cavity significantly suppresses the H/D and 16O/18O exchange reactions in 2 compared to that in 1 and stabilizes the Cu 2(μ-1,1-OOH)(μ-OH) core against decomposition. Decomposition of 2 in acetonitrile at 0 °C proceeded mainly via disproportionation of the hydroperoxo ligand and reduction of 2 to [Cu(L3)]+ by hydroperoxo ligand. In contrast, decomposition of a solid sample of 2 at 60 °C gave a complex having a hydroxylated ligand [Cu2(L3)(L3-OH)(OH) 2]2+ (2-(L3-OH)) as a main product, where L3-OH is an oxidized ligand in which one of the methylene groups of the pendant arms is hydroxylated. ESI-TOF/MS measurement showed that complex 2-(L3-OH) is stable in acetonitrile at -40 °C, whereas warming 2-(L3-OH) at room temperature resulted in the N-dealkylation from L3-OH to give an N-dealkylated ligand, bis(1-methyl-2-phenyl-4-imidazolylmethyl)amine (L2) in ∼80% yield based on 2, and 1-methyl-2-phenyl-4-formylimidazole (Phim-CHO). Isotope labeling experiments confirmed that the oxygen atom in both L3-OH and Phim-CHO come from OOH. This aliphatic hydroxylation performed by 2 is in marked contrast to the arene hydroxylation reported for some (μ-1,1-hydroperoxo)dicopper(II) complexes with a xylyl linker.

    DOI: 10.1021/ja047437h

  • DNA-photocleaving activities of water-soluble carbohydrate-containing nonionic homooxacalix[3]arene·[60]fullerene complex Reviewed

    Atsushi Ikeda, Akinori Ejima, Koji Nishiguchi, Jun Ichi Kikuchi, Takahiro Matsumoto, Tsukasa Hatano, Seiji Shinkai, Masahiro Goto

    Chemistry Letters   34 ( 3 )   308 - 309   2005.3

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    A new water-soluble carbohydrate-containing "nonionic" homooxacalix[3]arene (2) was synthesized. 2 could solubilize [60]fullerene (C60) into water and the resultant complex acted as an efficient DNA photocleaving reagent.

    DOI: 10.1246/cl.2005.308

  • Schizophyllans carrying oligosaccharide appendages as potential candidates for cell-targeted antisense carrier Reviewed

    Teruaki Hasegawa, Tomohisa Fujisawa, Munenori Numata, Takahiro Matsumoto, Mariko Umeda, Ryouji Karinaga, Masami Mizu, Kazuya Koumoto, Taro Kimura, Shiro Okumura, Kazuo Sakurai, Seiji Shinkai

    Organic and Biomolecular Chemistry   2 ( 21 )   3091 - 3098   2004.11

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    Schizophyllans carrying β-lactoside and α-mannoside appendages were prepared from native schizophyllan through NaIO4 oxidation followed by reductive amination using aminoethyl-β-lactoside and α-mannoside, respectively. The resulting schizophyllans form stable macromolecular complexes with polynucleotides, such as poly(C) and poly(dA). Specific affinity between these macromolecular complexes and saccharide-binding proteins was demonstrated by surface plasmon resonance and agarose gel staining assays. β-Lactoside-appended schizophyllan enhanced an antisense activity in hepatocytes which express lactoside-binding proteins on their cell surfaces.

    DOI: 10.1039/b412124b

  • Single-walled carbon nanotubes acquire a specific lectin-affinity through supramolecular wrapping with lactose-appended schizophyllan Reviewed

    Teruaki Hasegawa, Tomohisa Fujisawa, Munenori Numata, Mariko Umeda, Takahiro Matsumoto, Taro Kimura, Shiro Okumura, Kazuo Sakurai, Seiji Shinkai

    Chemical Communications   ( 19 )   2150 - 2151   2004.11

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    Single-walled carbon nanotubes can be entrapped within a helical superstructure composed of schizophyllan bearing lactoside-appendages to show an excellent water-solubility as well as a specific lectin-affinity.

    DOI: 10.1039/b407409b

  • A polysaccharide carrier for immunostimulatory CpG DNAs to enhance cytokine secretion Reviewed

    Masami Mizu, Kazuya Koumoto, Takahisa Anada, Takahiro Matsumoto, Munenori Numata, Seiji Shinkai, Takeshi Nagasaki, Kazuo Sakurai

    Journal of the American Chemical Society   126 ( 27 )   8372 - 8373   2004.7

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    A β-(1 → 3)-D-glucan schizophyllan (SPG) forms a stoichiometric complex with some polynucleotides. This communication describes our attempt to apply the SPG complex to deliver CpG DNA to endosomes to enhance cytokine secretion. To increase cellular uptake, we introduced spermine, arginine-glycine-aspartic acid tripeptide, octaarginine, or cholesterol to the SPG side chain. The chemically modified SPG showed essentially no cytotoxicity. When CpG DNA complex made therefrom was exposed to macrophages, dramatic enhancement in the cytokine secretion was observed. It increased 5-10 times from the naked dose and 100 times from the background. This performance promises that SPG can be an excellent carrier for CpG DNA.

    DOI: 10.1021/ja031978+

  • Chemically modified polysaccharide schizophyllan for antisense oligonucleotides delivery to enhance the cellular uptake efficiency Reviewed

    Takahiro Matsumoto, Munenori Numata, Takahisa Anada, Masami Mizu, Kazuya Koumoto, Kazuo Sakurai, Takeshi Nagasaki, Seiji Shinkai

    Biochimica et Biophysica Acta - General Subjects   1670 ( 2 )   91 - 104   2004.1

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    Schizophyllan is a natural β-(1→3)-D-glucan existing as a triple helix in water and as a single chain in dimethylsulfoxide (DMSO), respectively. As we already reported, when some homo-phosphodiester polynucleotide (for example, poly(dA) or poly(C)) is added to the schizophyllan/DMSO solution and subsequently DMSO is exchanged for water, the single chain of schizophyllan forms a complex with the polynucleotide. Furthermore, we have already demonstrated that one of the potential applications of this novel complex is an antisense-oligonucleotide (AS ODN) carrier. This work describes a versatile and universal modification technique which enables us to introduce various functional groups only to the side chain of schizophyllan. This technique consists of periodate oxidation of the glucose side chain (it does not react with the main chain because of the absence of the 1,2-diol group in β-(1→3)-glucan) and subsequent introduction of the functional groups into the formyl terminate. In the present work, the introduced functional groups were spermine, octa-arginine (R8), arginine-glycine-aspartic acid tripeptide (RGD) and some amino or α-amino acid compounds. Using these compounds, we made the complexes and carried out an in vitro antisense assay for them, administrating a phosphorothioate AS ODN to the melanoma A375 or leukemia HL-60 cell lines to depress their c-myb mRNA. When we used the R8 or RGD modified schizophyllan as the antisense carrier, the antisense effect was most enhanced among others. Their superiority can be ascribed to enhancement of endocytosis due to these functional peptides. Furthermore, the cytotoxicity for these two modified schizophyllans was negligibly as small as the natural (unmodified) schizophyllan. One of the peculiar features of our system is that the complex (i.e., carrier+AS ODN) is charged negatively in total, which is different from the conventional systems. The present work has thus clarified that schizophyllan can act as a new potential candidate for AS ODN carriers.

    DOI: 10.1016/j.bbagen.2003.10.019

  • Low Mw sulfated curdlan with improved water solubility forms macromolecular complexes with polycytidylic acid Reviewed

    Kazuya Koumoto, Mariko Umeda, Munenori Numata, Takahiro Matsumoto, Kazuo Sakurai, Toyoki Kunitake, Seiji Shinkai

    Carbohydrate Research   339 ( 1 )   161 - 167   2004.1

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    The water solubility of curdlan was enhanced by partial sulfation at O-6. Circular dichroism measurements suggest that the sulfated curdlan with the degree of substitution (DS) from 0 to 8.7mol% forms macromolecular complexes with polycytidylic acid (poly(C)). Although the thermal stability of the complexes decreased with increase in DS, this could be overlapped by addition of NaCl in the concentration above that of serum. The results clearly indicate that the drawback arising from the electrostatic repulsion between the anionic charges can be partially compensated by the presence of salt. Furthermore, the polynucleotide chain complexed with the sulfated curdlan was protected from the enzymatic hydrolysis, corroborating the assumption that the sulfated curdlan has an ability to bind poly(C).

    DOI: 10.1016/j.carres.2003.09.022

  • Lactose-appended schizophyllan is a potential candidate as a hepatocyte-targeted antisense carrier Reviewed

    Teruaki Hasegawa, Mariko Umeda, Takahiro Matsumoto, Munenori Numata, Masami Mizu, Kazuya Koumoto, Kazuo Sakurai, Seiji Shinkai

    Chemical Communications   4 ( 4 )   382 - 383   2004.1

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    A schizophyllan (β-1,3-glucan) derivative carrying lactose-appendages prepared by reductive amination can form stable macromolecular complexes with polynucleotides, shows excellent affinity with a lactose-binding lectin, and effectively mediates gene transfection into hepatocytes.

    DOI: 10.1039/b313426a

  • Polysaccharide-polynucleotide complexes (15) Thermal stability of schizophyllan (SPG)/poly(C) triple strands is controllable by α-amino acid modification Reviewed

    Munenori Numata, Takahiro Matsumoto, Mariko Umeda, Kazuya Koumoto, Kazuo Sakurai, Seiji Shinkai

    Bioorganic Chemistry   31 ( 2 )   163 - 171   2003.4

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    Schizophyllan (SPG), a β-1,3-glucan polysaccharide which is known to form macromolecular complexes with certain polynucleotides, was modified by a reductive amination method with α-amino acids (Arg, Lys, and Ser). The thermal stability of the complexes as estimated by Tm was enhanced in SPG-Arg and SPG-Lys conjugates which have pI values higher than the pH of the medium (8.0). The Tm shift increased with the increase in the percentage of α-amino acid introduced and the highest Tm values attained were 64°C for SPG-Arg conjugate and 62°C for SPG-Lys conjugate, which are higher by 13 and 11°C, respectively, than those of the unmodified SPG+poly(C) complex. In the SPG-Ser conjugate with a pI lower than the medium pH (8.0), the Tm values decreased with an increase in the percentage of Ser. Formation of the macromolecular complex was no longer detected above 13.2% Ser. The findings indicate that the Tm values are easily controllable by the type and percentage of the introduced α-amino acids. We believe, therefore, that the present conjugates, consisting of naturally originated SPG and α-amino acids, provide an important lead for developing nontoxic artificial vectors and to control the affinity with polynucleotides in response to medium pH and temperature.

    DOI: 10.1016/S0045-2068(03)00020-8

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Books

  • メタンと二酸化炭素 ~ その触媒的化学変換技術の現状と展望(「第4節 錯体触媒による液相光酸化(第4章 異種エネルギー負荷型触媒システム、第2部 メタンの触媒的化学変換技術の現状〜新しい化学工業体系を提示できるか)」を担当)

    松本 崇弘(Role:Joint author)

    2023.3 

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    Language:Japanese   Book type:Scholarly book

    本書は、CREST・さきがけ「革新的触媒」の成果をまとめた総説であり(上田渉教授監修)、その中の「第4節 錯体触媒による液相光酸化(第4章 異種エネルギー負荷型触媒システム、第2部 メタンの触媒的化学変換技術の現状〜新しい化学工業体系を提示できるか)」で、均一系触媒によるメタンの酸化についてまとめたものである。自身が開発した光エネルギーと酸素を用いてメタンをメタノールとホルムアルデヒドに酸化した初めての報告例を中心に、これまでの遷移金属錯体による光駆動物質変換反応と酸素を用いたメタンの酸化について系統的に解説している。

  • 錯体化合物事典

    小江 誠司, 松本 崇弘(Role:Joint author)

    2019.9 

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  • フロンティア生物無機化学

    小江 誠司, 松本 崇弘(Role:Joint author)

    2016.12 

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    Language:Japanese   Book type:Scholarly book

Presentations

  • Bioinspired Homogeneous Material Transformations Invited International conference

    Takahiro Matsumoto

    Workshop on Cutting-Edge Research and Future Prospects in Bio- and Bioinspired- Catalysis  2024.3 

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    Event date: 2024.3

    Language:English   Presentation type:Oral presentation (general)  

    Venue:Senri Asahi Hankyu Building   Country:Japan  

  • バイオマス資源からの有用な低分子化合物の製造〜持続可能社会の実現に向けた低コスト・低環境負荷・低エネルギー反応〜 Invited

    Takahiro Matsumoto

    九州大学オープンイノベーションワークショップ  2023.11 

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    Event date: 2023.11

    Language:Japanese   Presentation type:Oral presentation (general)  

    Venue:九州大学伊都キャンパス、椎木講堂   Country:Japan  

  • バイオマス資源からの有用な低分子化合物の製造 Invited

    Takahiro Matsumoto

    JST新技術説明会  2023.10 

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    Event date: 2023.10

    Language:Japanese   Presentation type:Oral presentation (general)  

    Venue:東京、市ケ谷、JST東京本部別館1Fホール   Country:Japan  

  • Sustainable Photosynthesis of NH3 from Environmentally Harmful NO3– Using CH4 with a Homogenous Re Complex Invited International conference

    Takahiro Matsumoto

    International Congress on Pure & Applied Chemistry Bali 2023 (ICPAC Bali 2023)  2023.9 

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    Event date: 2023.9

    Language:English   Presentation type:Oral presentation (general)  

    Venue:Patra Bali Resort & Villas, Bali, Indonesia   Country:Indonesia  

  • Light-Driven Oxidation of CH4 to CH3OH and HCHO using O2 Catalyzed by a Homogenous RuIV2(μ-O)2 Complex International conference

    Takahiro Matsumoto

    20th International Conference on Biological Inorganic Chemistry (ICBIC20)  2023.7 

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    Event date: 2023.7

    Language:English   Presentation type:Oral presentation (general)  

    Venue:Adelaide Convention Centre, South Australia   Country:Australia  

  • Photo-driven Transformations of Methane and Benzene by Organometallic Complexes Invited International conference

    Takahiro Matsumoto

    International Congress on Pure & Applied Chemistry Kota Kinabalu 2022  2022.11 

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    Event date: 2022.11

    Language:English   Presentation type:Oral presentation (general)  

    Venue:The Magellan Sutera Resort, Sabah, Malaysia with online   Country:Malaysia  

  • 有機金属錯体によるメタンとベンゼンの光駆動物質変換 Invited

    Takahiro Matsumoto

    触媒学会 第49回オルガノメタリックセミナー〜有機金属化学のダイバーシティ〜  2022.10 

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    Event date: 2022.10

    Language:Japanese   Presentation type:Oral presentation (general)  

    Venue:福岡、九州大学病院キャンパス   Country:Japan  

  • 有機金属錯体による不活性結合の光活性化 Invited

    Takahiro Matsumoto

    2021年度CREST「革新的触媒」領域・公開シンポジウム「メタン資源利用に向けて」  2022.6 

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    Event date: 2022.6

    Language:Japanese  

    Venue:オンライン   Country:Japan  

  • 錯体化学的スマートデザインでターゲティングする光誘起物質変換反応 – 酸素を用いるメタンとベンゼンの光駆動酸化 Invited

    Takahiro Matsumoto

    日本化学会 第102回春季年会(2022)中長期テーマシンポジウム「革新的触媒:未来へ」  2022.3 

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    Event date: 2022.3

    Language:Japanese   Presentation type:Oral presentation (general)  

    Venue:オンライン   Country:Other  

  • 錯体化学的スマートデザインでターゲティングする分子変換反応 -酸素を用いるメタンとベンゼンの光駆動酸化 Invited

    Takahiro Matsumoto

    九州錯体化学懇談会 第263回例会(2021年度第3回例会)  2022.3 

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    Event date: 2022.3

    Language:Japanese   Presentation type:Oral presentation (general)  

    Venue:オンライン   Country:Other  

  • Photo-Induced Functionalization of Aliphatic and Aromatic C–H Bonds by Transition Metal Complexes Invited International conference

    Takahiro Matsumoto

    Advances in Bioorganometallic Chemistry (#252), Pacifichem 2021  2021.12 

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    Event date: 2021.12

    Language:English   Presentation type:Oral presentation (general)  

    Venue:オンライン   Country:Other  

  • 光で駆動するメタン酸化電池の開発 Invited

    Takahiro Matsumoto

    さきがけ「革新的触媒の科学と創製」領域 3期生勉強会  2021.5 

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    Event date: 2021.5

    Language:Japanese   Presentation type:Oral presentation (general)  

    Venue:オンライン   Country:Japan  

  • 有機金属錯体の光励起状態による脂肪族・芳香族炭化水素の活性化反応 Invited

    Takahiro Matsumoto

    石油学会ジュニアソサイアティ(JPIJS)  2020.11 

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    Event date: 2020.11

    Language:Japanese   Presentation type:Oral presentation (general)  

    Venue:熊本大学(黒髪南地区)+ オンライン   Country:Japan  

  • Photo-Induced Aromatic C-H Functionalization by A Transition Metal Complex Invited International conference

    Takahiro Matsumoto

    Symposium Catalysis Science - Quo Vadis TUM Catalysis Research Center (CRC) and Japan Science and Technology Agency (JST)  2020.7 

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    Event date: 2020.7

    Language:English   Presentation type:Oral presentation (general)  

    Venue:Online Webinar   Country:Other  

  • 有機金属触媒による不活性結合の活性化 Invited

    Takahiro Matsumoto

    JST ・触媒学会共催 オンライン公開シンポジウム-革新的触媒と反応制御の今後-  2020.5 

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    Event date: 2020.5

    Language:Japanese   Presentation type:Oral presentation (general)  

    Venue:オンラインシンポジウム   Country:Japan  

    世界的に脱炭素社会への移行が進む中で、メタンはシェールガス革命以降、ブリッジ・エネルギーとして役割が期待されている。最近では、メタンは再生可能エネルギーであるバイオマスから製造されることから、カーボン・ニュートラル社会の実現に向けたキープレーヤーとしての役割を期待されている。しかし、メタンはその物理化学的性質から、物質変換が最も難しい不活性分子の1つである。本研究では、そのような変換の難しいメタンに対して、光エネルギーを有機化学錯体にインプットしてメタノールに変換する新しい触媒反応を見出した。

  • C–H Bond Activation by Transition Metal Complexes Invited International conference

    Takahiro Matsumoto

    JST–TU Delft Joint Symposium  2019.8 

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    Event date: 2019.8

    Language:English   Presentation type:Oral presentation (general)  

    Venue:オランダ、デルフト、Delft University of Technology (TU Delft)   Country:Netherlands  

  • H2 and O2 Activation by [NiFe]hydrogenase Models Invited International conference

    Takahiro Matsumoto

    The 13th International Symposium on Organic Reactions (ISOR-13)  2018.11 

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    Event date: 2018.11

    Language:English   Presentation type:Oral presentation (general)  

    Venue:台湾、新竹、National Chiao Tung University   Country:Taiwan, Province of China  

  • Mechanistic Investigation of Switching between H2- or O2-Activation by [NiFe]hydrogenase Models Invited International conference

    Takahiro Matsumoto

    43rd International Conference on Coordination Chemistry (ICCC2018)  2018.8 

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    Event date: 2018.7 - 2018.8

    Language:English   Presentation type:Oral presentation (general)  

    Venue:日本、宮城、仙台国際センター   Country:Japan  

  • Mechanistic Insight into Switching between H2- or O2-Activation by Simple Ligand Effects of [NiFe]hydrogenase Models

    Takahiro Matsumoto

    第67回錯体化学会討論会  2017.9 

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    Event date: 2017.9

    Language:English   Presentation type:Oral presentation (general)  

    Venue:札幌、北海道大学   Country:Japan  

  • 自然に学ぶ分子燃料電池の開発 Invited

    Takahiro Matsumoto

    nano tech 2017 〜第16回 国際ナノテクノロジー総合展・技術会議〜  2017.2 

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    Event date: 2017.2

    Language:Japanese   Presentation type:Oral presentation (general)  

    Venue:東京、東京ビッグサイト   Country:Japan  

  • H2 and O2 Activation by a Hydrogenase Model Invited International conference

    Takahiro Matsumoto

    I2CNER International Workshop 2017 Natural and Chemical Catalysts for Technology  2017.2 

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    Event date: 2017.2

    Language:English   Presentation type:Oral presentation (general)  

    Venue:日本、福岡、九州大学 I2CNER   Country:Japan  

  • Hydrogenase and its Mimics for Fuel Cell Electrodes Invited International conference

    Takahiro Matsumoto

    8th Asian Biological Inorganic Chemistry Conference (AsBIC8)  2016.12 

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    Event date: 2016.12

    Language:English   Presentation type:Oral presentation (general)  

    Venue:ニュージーランド、オークランド、The University of Auckland   Country:New Zealand  

  • 分子燃料電池—ヒドロゲナーゼを範とする水素と酸素の活性化— Invited International conference

    Takahiro Matsumoto

    第66回錯体化学会討論会  2016.9 

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    Event date: 2016.9

    Language:Japanese   Presentation type:Oral presentation (general)  

    Venue:福岡、福岡大学   Country:Japan  

  • Hydrogenase and its Mimics for Fuel Cell Electrodes Invited International conference

    Takahiro Matsumoto

    42nd International Conference on Coordination Chemistry (ICCC–42)  2016.7 

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    Event date: 2016.7

    Language:English   Presentation type:Oral presentation (general)  

    Venue:フランス、ブレスト、Le Quartz Convention Center   Country:France  

  • 分子燃料電池 Invited

    Takahiro Matsumoto

    電気化学会第83回大会「シンポジウム:有機電気化学の新しい展開」  2016.3 

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    Event date: 2016.3

    Language:Japanese   Presentation type:Oral presentation (general)  

    Venue:大阪、大阪大学吹田キャンパス   Country:Japan  

  • Molecular Fuel Cell Invited

    Takahiro Matsumoto

    I2CNER International Workshop 2016 Recent Progress in Bio-inspired Catalysisand Utilization of Earth-Abundant Resources  2016.2 

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    Event date: 2016.2

    Language:English   Presentation type:Oral presentation (general)  

    Venue:日本、福岡、九州大学 I2CNER   Country:Japan  

  • 酵素の基礎研究から燃料電池の実用化に向けて Invited

    Takahiro Matsumoto

    第2回物性セミナー(速水研究室)  2015.7 

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    Event date: 2015.7

    Language:Japanese   Presentation type:Oral presentation (general)  

    Venue:熊本、熊本大学   Country:Japan  

  • H2 Activation by Hydrogenase and its Model International conference

    Takahiro Matsumoto

    I2CNER International Workshop 2015 Catalytic Materials Transformations Research Division  2015.2 

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    Event date: 2015.2

    Language:English  

    Venue:日本、福岡、I2CNER Hall   Country:Japan  

  • 酵素の基礎研究から燃料電池の実用化へ

    Takahiro Matsumoto

    第27回生物無機化学夏季セミナー  2014.8 

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    Event date: 2014.8

    Language:Japanese   Presentation type:Oral presentation (general)  

    Venue:兵庫、書写山円教寺会館   Country:Japan  

  • Activation of H2 and O2 by Hydrogenase Mimics in a Fuel Cell International conference

    松本 崇弘

    41st International Conference on Coordination Chemistry (ICCC–41) Activation of Small Molecules by Biomimetic Compounds  2014.7 

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    Event date: 2014.7

    Language:English   Presentation type:Oral presentation (general)  

    Venue:シンガポール、Suntec Shingapore Convention & Exhibition Centre   Country:Singapore  

  • Molecular Fuel Cell International conference

    松本 崇弘

    I2CNER & ACT-C Joint Workshop 2014 CO2 Capture and Utilization, Catalytic Materials Transformation & JST  2014.1 

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    Event date: 2014.1

    Language:English  

    Venue:日本、福岡、I2CNER Hall   Country:Japan  

  • Electron and Hydride Transfer (eHT) from H2 Invited International conference

    松本 崇弘

    I2CNER Symposium: Catalytic Concepts for Energy  2013.9 

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    Event date: 2013.9

    Language:English   Presentation type:Oral presentation (general)  

    Venue:アメリカ、イリノイ、イリノイ大学   Country:Japan  

  • バイオインスパイアード燃料電池触媒の開発

    松本 崇弘

    福岡市産学連携交流センター入居者交流会  2013.5 

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    Event date: 2013.5

    Language:Japanese   Presentation type:Oral presentation (general)  

    Venue:福岡、福岡市産学連携交流センター   Country:Japan  

  • 脱白金分子燃料電池触媒の開発

    松本崇弘・キムギョンモク・中井英隆・日比野高士・小江誠司

    錯体化学会第62回討論会  2012.9 

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    Event date: 2012.9

    Language:Japanese   Presentation type:Oral presentation (general)  

    Venue:富山大学   Country:Japan  

  • Molecular Fuel Cell

    松本崇弘

    Institute Interest Seminar Series(I2CNER)  2012.7 

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    Event date: 2012.7

    Presentation type:Oral presentation (general)  

    Venue:九州大学   Country:Japan  

  • ニッケルジヒドリド錯体からの電子抽出

    松本崇弘・長濵拓磨・趙栽興・樋詰拓洋・鈴木正樹・小江誠司

    錯体化学会第61回討論会  2011.9 

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    Event date: 2011.9 - 2011.10

    Presentation type:Oral presentation (general)  

    Venue:岡山理科大学   Country:Japan  

  • Electron from hydrogen and how to get it International conference

    松本崇弘

    Pacifichem 2010  2010.12 

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    Event date: 2010.12

    Presentation type:Symposium, workshop panel (public)  

    Venue:アメリカ、ハワイ、ホノルル   Country:United States  

    水素社会の到来が迫ってきているが、枯渇資源である白金が未だ最も優れた水素活性化触媒である。水素社会実現のためには、白金の代替触媒の開発が必須である。自然界にはニッケル・鉄ヒドロゲナーゼと呼ばれる水素活性化酵素が存在する。この酵素は水中・常温・常圧で水素を活性化し、水素からの電子抽出を触媒する。しかし、この有用なニッケル・鉄ヒドロゲナーゼの構造・機能を、人工的に再現できたモデル錯体はこれまで報告されていない。本研究では、ニッケル・ルテニウム触媒を用いてその構造・機能を再現することに成功し、これまで知られていなかった水素活性化のメカニズムを解明することに成功した。

  • Extraction of Electrons from H2 International conference

    松本崇弘

    60th Anniversary Conference on Coordination Chemistry in OSAKA, JAPAN  2010.9 

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    Event date: 2010.9

    Presentation type:Oral presentation (general)  

    Venue:日本、大阪、大阪国際交流センター   Country:Japan  

    火力発電と原子力発電に替わる次世代発電システムとして、排出物が水のみであるクリーンな水素燃料電池が期待されている。燃料電池の電極触媒には白金が最適であるが、白金は枯渇資源であるため、白金の代替触媒の開発が求められている。自然界にはニッケル・鉄ヒドロゲナーゼと呼ばれる水素活性化酵素が存在する。この酵素は水中・常温・常圧で水素を活性化し、水素からの電子抽出を触媒する。しかし、この有用なニッケル・鉄ヒドロゲナーゼの構造・機能を、人工的に再現できたモデル錯体はこれまで報告されていない。本研究では、ニッケル・ルテニウム触媒を用いてその構造・機能を再現することに成功した。

  • 水中・常温・常圧での水素からの電子抽出

    松本崇弘

    第3回万有若手交流合宿セミナー  2009.11 

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    Event date: 2009.11

    Presentation type:Symposium, workshop panel (public)  

    Venue:日本、佐賀、唐津ロイヤルホテル   Country:Japan  

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MISC

  • 錯体化学的スマートデザイン「金属×配位子」でターゲティングする物質変換反応

    松本 崇弘

    Bulletin of Japan Society of Coordination Chemistry (BJSCC)   2021.11

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    Language:Japanese  

  • 光エネルギーを利用した有機金属錯体によるメタンの酸化反応

    松本 崇弘

    化学と工業   2021.8

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    Language:Japanese  

  • 分子燃料電池–ヒドロゲナーゼを範とする水素分子と酸素分子の活性化–

    松本 崇弘

    Bulletin of Japan Society of Coordination Chemistry (BJSCC)   2017.11

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    Language:Japanese  

  • 分子および酵素燃料電池

    松本 崇弘, 小江 誠司

    化学と工業   2015.5

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    Language:Japanese  

  • 水素が好き?酸素が好き?̶天然の酵素を模範とする分子燃料電池の開発

    松本 崇弘, 小江 誠司

    現代化学   2013.8

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    Language:Japanese   Publishing type:Article, review, commentary, editorial, etc. (scientific journal)  

    本総説は現代化学(東京化学同人)に掲載されたものである。要旨は下記の通りである。
    水素から電子を取り出す酵素ヒドロゲナーゼの中に、酸素から水をつくる反応を触媒するものがある。この酵素の働きを詳しく解明し、その知見をもとにモデルを構築すれば、燃料電池開発に応用できそうだ。研究者らは、まず貴金属であるルテニウムを使ったモデル構築に成功した。現在は貴金属を使わないモデルの構築に挑んでいる。

  • 新しい水素活性化触媒―[ NiFe]ヒドロゲナーゼに学ぶ水素からの電子抽出

    松本 崇弘, 小江 誠司

    月刊「化学」   2013.8

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    Language:Japanese   Publishing type:Article, review, commentary, editorial, etc. (scientific journal)  

    本総説は化学(化学同人)に掲載されたものである。要旨は下記の通りである。
    水素-水素結合(H-H結合)を切断する触媒が新しく開発された。金属酵素であるヒドロゲナーゼをモデルに五つの水素活性化戦略を打ち立て、ヒドリドイオンから電子を取り出すことに初めて成功した。その戦略とは?

  • 分子燃料電池

    松本 崇弘, 小江 誠司

    化学と工業   2013.2

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    Language:Japanese   Publishing type:Article, review, commentary, editorial, etc. (scientific journal)  

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Industrial property rights

Patent   Number of applications: 4   Number of registrations: 2
Utility model   Number of applications: 0   Number of registrations: 0
Design   Number of applications: 0   Number of registrations: 0
Trademark   Number of applications: 0   Number of registrations: 0

Professional Memberships

  • 錯体化学会

  • 日本化学会

  • 電気化学会

  • 有機合成化学協会

  • 石油学会

  • 日本環境化学会

  • 触媒学会

  • 廃棄物資源循環学会

  • 有機電子移動化学研究会

  • 日本科学振興協会(JAAS)

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Academic Activities

  • 実行委員

    JPIJS討論会 石油産業の役割と若手エンジニアの未来像  ( Japan ) 2023.7

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    Type:Competition, symposium, etc. 

  • 座長

    日本化学会第103春季年会  ( Japan ) 2023.3

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    Type:Competition, symposium, etc. 

  • 世話人

    2022年度 有機化学合成協会 九州山口支部 第2回講演会  ( Japan ) 2022.10

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    Type:Competition, symposium, etc. 

  • 実行委員会委員

    第38回有機合成化学セミナー  ( Japan ) 2022.9

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    Type:Competition, symposium, etc. 

  • 実行委員会委員・プログラム編成委員

    錯体化学会第72回討論会  ( Japan ) 2022.9

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    Type:Competition, symposium, etc. 

  • シンポジウム主催

    錯体化学会第72回討論会  ( Japan ) 2022.9 - 2019.9

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    Type:Competition, symposium, etc. 

  • 座長

    錯体化学会第72回討論会  ( Japan ) 2022.9 - 2019.9

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    Type:Competition, symposium, etc. 

  • 世話人(有機化学)

    第59回化学関連支部合同九州大会  ( Japan ) 2022.7

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    Type:Competition, symposium, etc. 

  • 世話人

    2022年度 有機化学合成協会 九州山口支部 第1回講演会  ( Japan ) 2022.6

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    Type:Competition, symposium, etc. 

  • 世話人

    有機合成化学協会 九州山口支部 第33回若手研究者のためのセミナー  ( Japan ) 2021.8

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    Type:Competition, symposium, etc. 

  • 座長(Chairmanship)

    錯体化学会第69回討論会  ( Japan ) 2019.9

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    Type:Competition, symposium, etc. 

  • セッション編成委員 International contribution

    43rd International Conference on Coordination Chemistry (ICCC2018), S45:Metal Mediated Hydrogen Production and Activation Inspired by Nature  ( Sendai International Center Japan ) 2018.7 - 2018.8

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    Type:Competition, symposium, etc. 

  • 座長(Chairmanship)

    錯体化学会第67回討論会  ( Japan ) 2017.9

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    Type:Competition, symposium, etc. 

  • プログラム編成委員

    錯体化学会第66回討論会  ( Japan ) 2016.9

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    Type:Competition, symposium, etc. 

  • 座長(Chairmanship)

    錯体化学会第66回討論会  ( Japan ) 2016.9

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    Type:Competition, symposium, etc. 

  • 座長(Chairmanship)

    錯体化学会第62回討論会  ( Japan ) 2012.9

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Research Projects

  • 光で駆動するメタン酸化電池の開発

    2017 - 2020

    戦略的創造研究推進事業(JST・さきがけ)

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    Authorship:Principal investigator  Grant type:Contract research

  • 非貴金属分子燃料電池の開発

    Grant number:16K05727  2016 - 2018

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research  Grant-in-Aid for Scientific Research (C)

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    Authorship:Principal investigator  Grant type:Scientific research funding

  • ヒドロゲナーゼと光合成の融合によるエネルギー変換サイクルの創成

    Grant number:26000008  2014 - 2018

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research  Grant-in-Aid for Specially Promoted Research

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    Authorship:Coinvestigator(s)  Grant type:Scientific research funding

  • 酸性耐性能を備えた酵素燃料電池の創製

    Grant number:26810038  2014 - 2015

    Grants-in-Aid for Scientific Research  Grant-in-Aid for Young Scientists (B)

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    Authorship:Principal investigator  Grant type:Scientific research funding

  • ヒドロゲナーゼを範とする脱白金燃料電池酸素極の開発

    Grant number:24750058  2012 - 2013

    Grants-in-Aid for Scientific Research  Grant-in-Aid for Young Scientists (B)

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    Authorship:Principal investigator  Grant type:Scientific research funding

Educational Activities

  • 有機化学

Class subject

  • 有機化学第四

    2023.10 - 2023.12   Fall quarter

  • 有機物質化学Ⅰ

    2023.10 - 2023.12   Fall quarter

  • 有機化学第三

    2023.4 - 2023.6   Spring quarter

  • 有機物質化学Ⅱ

    2022.12 - 2023.2   Winter quarter

  • 有機化学第四および演習

    2022.10 - 2022.12   Fall quarter

  • 有機化学第四および演習

    2022.10 - 2022.12   Fall quarter

  • 有機物質化学Ⅰ

    2022.10 - 2022.12   Fall quarter

  • 有機化学第三

    2022.4 - 2022.6   Spring quarter

  • 有機物質化学Ⅱ

    2021.12 - 2022.2   Winter quarter

  • 有機物質化学Ⅰ

    2021.10 - 2021.12   Fall quarter

  • 有機化学第四および演習

    2021.10 - 2021.12   Fall quarter

  • 有機化学第三

    2021.4 - 2021.6   Spring quarter

  • 小分子の化学

    2020.10 - 2021.3   Second semester

  • 有機化学第四および演習

    2020.10 - 2020.12   Fall quarter

  • 有機化学第三

    2020.4 - 2020.6   Spring quarter

  • 小分子の化学

    2019.10 - 2020.3   Second semester

  • 有機物質化学

    2019.10 - 2020.3   Second semester

  • 有機化学第四および演習

    2019.10 - 2019.12   Fall quarter

  • 有機化学第三

    2019.4 - 2019.6   Spring quarter

  • 自然科学総合実験(発展)

    2018.12 - 2019.2   Winter quarter

  • 小分子の化学

    2018.10 - 2019.3   Second semester

  • 有機化学第四

    2018.10 - 2019.3   Second semester

  • 有機化学第三および演習

    2018.4 - 2018.9   First semester

  • 有機物質化学

    2017.10 - 2018.3   Second semester

  • 安全学

    2017.10 - 2018.3   Second semester

  • 小分子の化学

    2017.10 - 2018.3   Second semester

  • 有機化学第四

    2017.10 - 2018.3   Second semester

  • 有機化学第三および演習

    2017.4 - 2017.9   First semester

  • 課題協学

    2016.10 - 2017.3   Second semester

  • 有機化学第四

    2016.10 - 2017.3   Second semester

  • 小分子の化学

    2016.10 - 2017.3   Second semester

  • 物質科学工学実験第二

    2014.4 - 2014.9   First semester

  • 物質科学工学実験第二

    2013.4 - 2013.9   First semester

  • 物質科学工学実験第二

    2012.4 - 2012.9   First semester

  • 物質科学工学実験第二

    2011.4 - 2011.9   First semester

  • 物質科学工学実験第二

    2010.4 - 2010.9   First semester

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FD Participation

  • 2013.11   Role:Participation   Title:平成25年度 第3回全学FD

    Organizer:University-wide

  • 2013.2   Role:Participation   Title:平成24年度工学部(府)FD

    Organizer:[Undergraduate school/graduate school/graduate faculty]

  • 2011.12   Role:Participation   Title:システム情報科学府・工学府・工学部合同FD

    Organizer:[Undergraduate school/graduate school/graduate faculty]

  • 2011.2   Role:Participation   Title:平成22年度工学部・工学府FD

    Organizer:[Undergraduate school/graduate school/graduate faculty]

  • 2010.3   Role:Participation   Title:平成21年度工学部・工学府FD

    Organizer:[Undergraduate school/graduate school/graduate faculty]

Other educational activity and Special note

  • 2023  Class Teacher  全学

  • 2022  Class Teacher  全学

  • 2021  Class Teacher  全学

  • 2018  Class Teacher  全学

Social Activities

  • オープンキャンパス, 次世代エネルギーをつくろう

    国立大学法人九州大学  2023.8

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    Audience:General, Scientific, Company, Civic organization, Governmental agency

    Type:Other

  • オープンキャンパス, 動画による研究紹介

    国立大学法人九州大学  オンライン  2022.8

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    Audience:General, Scientific, Company, Civic organization, Governmental agency

    Type:Other

  • オープンキャンパス, 動画による研究紹介

    国立大学法人九州大学  オンライン  2021.8

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    Audience:General, Scientific, Company, Civic organization, Governmental agency

    Type:Other

  • オープンキャンパス, 動画による研究紹介

    国立大学法人九州大学  オンライン  2020.8

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    Audience:General, Scientific, Company, Civic organization, Governmental agency

    Type:Other

  • オープンキャンパス, 次世代エネルギーをつくろう

    国立大学法人九州大学  九州大学伊都キャンパス  2019.8

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    Audience:General, Scientific, Company, Civic organization, Governmental agency

    Type:Other

  • オープンキャンパス, 次世代エネルギーをつくろう

    国立大学法人九州大学  九州大学伊都キャンパス  2018.8

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    Audience:General, Scientific, Company, Civic organization, Governmental agency

    Type:Other

  • オープンキャンパス, 次世代エネルギーをつくろう

    国立大学法人九州大学  九州大学伊都キャンパス  2017.8

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    Audience:General, Scientific, Company, Civic organization, Governmental agency

    Type:Other

  • オープンキャンパス, 次世代エネルギーをつくろう

    国立大学法人九州大学  九州大学伊都キャンパス  2016.8

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    Audience:General, Scientific, Company, Civic organization, Governmental agency

    Type:Other

  • 燃料電池をつくってみませんか?

    唐津市  唐津市ふるさと会館アルピノ  2015.12

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    Audience:General, Scientific, Company, Civic organization, Governmental agency

    Type:Other

  • オープンキャンパス, 次世代エネルギーをつくろう

    国立大学法人九州大学  九州大学伊都キャンパス  2015.8

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    Audience:General, Scientific, Company, Civic organization, Governmental agency

    Type:Other

  • オープンキャンパス, 次世代エネルギーをつくろう

    国立大学法人九州大学  九州大学伊都キャンパス  2014.8

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    Audience:General, Scientific, Company, Civic organization, Governmental agency

    Type:Other

  • オープンキャンパス, 次世代エネルギーをつくろう

    国立大学法人九州大学  九州大学伊都キャンパス  2013.8

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    Audience:General, Scientific, Company, Civic organization, Governmental agency

    Type:Other

  • オープンキャンパス, 次世代エネルギーをつくろう

    国立大学法人九州大学  九州大学伊都キャンパス  2012.8

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    Audience:General, Scientific, Company, Civic organization, Governmental agency

    Type:Other

  • オープンキャンパス, 次世代エネルギーをつくろう

    国立大学法人九州大学  九州大学伊都キャンパス  2011.8

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    Audience:General, Scientific, Company, Civic organization, Governmental agency

    Type:Other

  • 水素エネルギー研究最前線についての講演と燃料電池の実験

    西鉄ビルマネージメント株式会社  福岡市産学連携交流センター  2010.11

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    Audience:General, Scientific, Company, Civic organization, Governmental agency

    Type:Other

    福岡市産学連携交流センターにおいて、施設見学会「水素エネルギー研究最前線についての講演と燃料電池の実験」を行った。水素社会の到来が刻々と迫ってきているが、枯渇資源である白金が未だ最も優れた水素活性化触媒である。水素社会実現のためには、白金の代替触媒の開発が必須である。自然界にはニッケル・鉄ヒドロゲナーゼと呼ばれる水素活性化酵素が存在し、この酵素は水中・常温・常圧で水素を活性化し、水素からの電子抽出を触媒する。本施設見学会では、本研究室で水素活性化酵素を範として開発した新規水素活性化分子触媒について解説し、燃料電池を参加者と一緒に実際に組み立て発電実験を行い、燃料電池の仕組みについて説明した。

  • オープンキャンパス, 水素こうそ vs. 燃料電池

    国立大学法人九州大学  九州大学伊都キャンパス  2010.8

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    Audience:General, Scientific, Company, Civic organization, Governmental agency

    Type:Other

  • 水素と燃料電池

    西鉄ビルマネージメント株式会社  福岡市産学連携交流センター  2009.11

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    Audience:General, Scientific, Company, Civic organization, Governmental agency

    Type:Lecture

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