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Synthesis of metal complexes containing metal- or organo-hydride moieties directed toward "green" hydrogenation reactions

Research Project

Project/Area Number 25410059
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeMulti-year Fund
Section一般
Research Field Inorganic chemistry
Research InstitutionFukushima University

Principal Investigator

OYAMA DAI  福島大学, 共生システム理工学類, 教授 (20292451)

Co-Investigator(Renkei-kenkyūsha) TAKASE Tsugiko  福島大学, 環境放射能研究所, 特任准教授 (10466641)
Research Collaborator MUN Bisa  
UKAWA Narumi  
NAOI Ryutaro  
ABE Ryosuke  
Project Period (FY) 2013-04-01 – 2016-03-31
Project Status Completed (Fiscal Year 2015)
Budget Amount *help
¥4,810,000 (Direct Cost: ¥3,700,000、Indirect Cost: ¥1,110,000)
Fiscal Year 2015: ¥1,300,000 (Direct Cost: ¥1,000,000、Indirect Cost: ¥300,000)
Fiscal Year 2014: ¥1,560,000 (Direct Cost: ¥1,200,000、Indirect Cost: ¥360,000)
Fiscal Year 2013: ¥1,950,000 (Direct Cost: ¥1,500,000、Indirect Cost: ¥450,000)
Keywords金属錯体化学 / 合成化学 / 再生可能エネルギー / 有機ヒドリド / 金属ヒドリド / ヒドリド移動反応
Outline of Final Research Achievements

The strategy of intramolecular metallacyclization may facilitate the development of organo-hydride chemistry like a coenzyme NADH. In this study, we synthesized novel ruthenium complexes bearing both carbonyls (CO) and naphthyridine derivatives (pynp or paa). We examined redox properties of the complexes using electrochemical and spectroelectrochemical measurements. Chemical reduction of the pynp complex with a reducing agent led to formations of organo-hydride species caused by metallacyclization in addition to conventional metal-hydride one. On the other hand, the corresponding paa complex changed to a “hybrid” compound which involved both metal-hydride and organo-hydride moieties. A hydride transfer reaction between the hybrid hydride-complex and a hydride acceptor was confirmed experimentally.

Report

(4 results)
  • 2015 Annual Research Report   Final Research Report ( PDF )
  • 2014 Research-status Report
  • 2013 Research-status Report
  • Research Products

    (25 results)

All 2016 2015 2014 Other

All Journal Article (7 results) (of which Peer Reviewed: 6 results,  Acknowledgement Compliant: 5 results) Presentation (18 results) (of which Int'l Joint Research: 2 results,  Invited: 1 results)

  • [Journal Article] Ruthenium Complexes Having a Tridentate Polypyridyl Ligand with Non-coordinating Donor Atoms: Construction of a Specific Coordination Environment Involving Noncovalent Interactions2016

    • Author(s)
      Dai Oyama, Takashi Yamanaka, Ryosuke Abe, Tsugiko Takase
    • Journal Title

      ChemistrySelect

      Volume: 1

    • Related Report
      2015 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Reversible Intramolecular Cyclization in Ruthenium Complexes Induced by Ligand-centered One-electron Transfer on Bidentate Naphthyridine: An Important Intermediate for Both Metal- and Organo-Hydride Species2015

    • Author(s)
      Dai Oyama, Narumi Ukawa, Takashi Hamada,Tsugiko Takase
    • Journal Title

      Chemistry Letters

      Volume: 44 Issue: 4 Pages: 533-535

    • DOI

      10.1246/cl.150023

    • NAID

      130005062113

    • Related Report
      2015 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] 高効率色素増感太陽電池開発の鍵となる色素分子:合成化学からの分子設計アプローチ2015

    • Author(s)
      大山 大
    • Journal Title

      ケミカルエンジニヤリング

      Volume: 60 Pages: 847-852

    • NAID

      40020629958

    • Related Report
      2015 Annual Research Report
  • [Journal Article] Isolation and Structural Characterization of a Metallacyclic Compound by Selective Protection of a Single CO Ligand in a Ruthenium Complex2015

    • Author(s)
      Dai Oyama, Takashi Hamada, Narumi Ukawa, Ryuta Mochizuki, Tsugiko Takase
    • Journal Title

      Bulletin of the Chemical Society of Japan

      Volume: 88 Issue: 11 Pages: 1572-1574

    • DOI

      10.1246/bcsj.20150189

    • NAID

      130005108563

    • Related Report
      2015 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Redox-induced reversible intramolecular carbon-nitrogen bond formation of an azopyridylruthenium complex: Control of carbonyl ligand photoreactivity caused by structural change of the complex2015

    • Author(s)
      Dai Oyama, Bisa Mun, Tsugiko Takase
    • Journal Title

      Journal of Organometallic Chemistry

      Volume: 799-800 Pages: 173-178

    • DOI

      10.1016/j.jorganchem.2015.09.017

    • Related Report
      2015 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Synthesis and Crystal Structure of Alkynylplatinum(IV) Complex Containing the Terpyridine Ligand2014

    • Author(s)
      Tsugiko Takase, Dai Oyama
    • Journal Title

      Journal of Crystallography

      Volume: 2014 Pages: 1-5

    • Related Report
      2014 Research-status Report
    • Peer Reviewed
  • [Journal Article] Syntheses of Geometrical Isomers for Comparison of Properties Caused by Steric and Electronic Effects in Carbonylruthenium(II) Complexes2014

    • Author(s)
      Dai Oyama, Kazumi Yuzuriya, Ryutaro Naoi, Takashi Hamada, Tsugiko Takase
    • Journal Title

      Bulletin of the Chemical Society of Japan

      Volume: 87 Issue: 10 Pages: 1107-1115

    • DOI

      10.1246/bcsj.20140125

    • NAID

      130004699183

    • Related Report
      2014 Research-status Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Presentation] 種々のポリピリジル配位子を含むルテニウムカルボニル錯体:酸化還元特性に基づく支持配位子の評価2016

    • Author(s)
      髙橋香澄,高瀬つぎ子,大山 大
    • Organizer
      日本化学会第96春季年会
    • Place of Presentation
      同志社大学(京都府京田辺市)
    • Year and Date
      2016-03-24
    • Related Report
      2015 Annual Research Report
  • [Presentation] 二種のポリピリジル支持配位子を含むルテニウム錯体の選択的な幾何異性体の合成2016

    • Author(s)
      阿部良祐,木村涼太,高瀬つぎ子,大山 大
    • Organizer
      日本化学会第96春季年会
    • Place of Presentation
      同志社大学(京都府京田辺市)
    • Year and Date
      2016-03-24
    • Related Report
      2015 Annual Research Report
  • [Presentation] レドックスが関与する生体反応プロセスに学ぶ:金属錯体で何ができるか2016

    • Author(s)
      大山 大
    • Organizer
      福島化学工学懇話会
    • Place of Presentation
      日本大学工学部(福島県郡山市)
    • Year and Date
      2016-01-19
    • Related Report
      2015 Annual Research Report
    • Invited
  • [Presentation] Ruthenium complexes bearing tridentate polypyridyl with noncoordinating donor atoms: Construction of specific coordination space involving non-covalent interactions2015

    • Author(s)
      Dai Oyama, Takashi Yamanaka, Rie Tokoyoda, Ryosuke Abe, Tsugiko Takase
    • Organizer
      2015 International Chemical Congress of Pacific Basin Societies
    • Place of Presentation
      Honolulu (USA)
    • Year and Date
      2015-12-15
    • Related Report
      2015 Annual Research Report
    • Int'l Joint Research
  • [Presentation] チオシアン酸イオンの配位モード制御に基づく光増感ルテニウム錯体系の構築2015

    • Author(s)
      渡邊勇樹,高瀬つぎ子,大山 大
    • Organizer
      錯体化学会第65回討論会
    • Place of Presentation
      奈良女子大学(奈良県奈良市)
    • Year and Date
      2015-09-21
    • Related Report
      2015 Annual Research Report
  • [Presentation] Redox-induced Reversible Intramolecular C-N Bond Formation Regulates CO-ligand Reactivity in Azopyridylruthenium Complexes2015

    • Author(s)
      Dai Oyama, Bisa Mun, Tsugiko Takase
    • Organizer
      5th Asian Conference on Coordination Chemistry
    • Place of Presentation
      Hong Kong (P. R. China)
    • Year and Date
      2015-07-12
    • Related Report
      2015 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 柔軟な支持配位子を含むルテニウム錯体における反応性と配位様式との関係2015

    • Author(s)
      常世田里恵,阿部良祐,髙橋香澄,高瀬つぎ子,大山 大
    • Organizer
      日本化学会第95春季年会
    • Place of Presentation
      日本大学(千葉県船橋市)
    • Year and Date
      2015-03-26 – 2015-03-29
    • Related Report
      2014 Research-status Report
  • [Presentation] ルテニウム錯体中の酸化還元活性な二座ナフチリジン配位子と反応性との関係2014

    • Author(s)
      鵜川成美,望月龍太,濱田貴志,高瀬つぎ子,大山 大
    • Organizer
      錯体化学会第64回討論会
    • Place of Presentation
      中央大学(東京都文京区)
    • Year and Date
      2014-09-18 – 2014-09-20
    • Related Report
      2014 Research-status Report
  • [Presentation] ポリピリジルルテニウム錯体中のカテコール部位が関与する反応性の検討2014

    • Author(s)
      曽我侑加,木戸正人,高瀬つぎ子,大山 大
    • Organizer
      錯体化学会第64回討論会
    • Place of Presentation
      中央大学(東京都文京区)
    • Year and Date
      2014-09-18 – 2014-09-20
    • Related Report
      2014 Research-status Report
  • [Presentation] Intramolecular Interaction between Coordinated Carbonyl and Polypyridyl Ligands: An Evaluation of Steric and Electronic Effects in New Ruthenium(II) Complexes2014

    • Author(s)
      Dai Oyama, Kazumi Yuzuriya, Ryutaro Naoi, Tsugiko Takase
    • Organizer
      41st International Conference on Coordination Chemistry
    • Place of Presentation
      Singapore (Singapore)
    • Year and Date
      2014-07-21 – 2014-07-25
    • Related Report
      2014 Research-status Report
  • [Presentation] Formation of Organo-Hydride Ruthenium Complexes Caused by Metallacyclization Involving Carbonyl and Polypyridyl Ligands2014

    • Author(s)
      Narumi Ukawa, Ryuta Mochizuki, Takashi Hamada, Tsugiko Takase, Dai Oyama
    • Organizer
      41st International Conference on Coordination Chemistry
    • Place of Presentation
      Singapore (Singapore)
    • Year and Date
      2014-07-21 – 2014-07-25
    • Related Report
      2014 Research-status Report
  • [Presentation] Redox Behavior of Ruthenium Complexes with a Free Catechol Moiety and Conversion Reactions to the Corresponding Quinone Form2014

    • Author(s)
      Yuka Soga, Masato Kido, Tsugiko Takase, Dai Oyama
    • Organizer
      41st International Conference on Coordination Chemistry
    • Place of Presentation
      Singapore (Singapore)
    • Year and Date
      2014-07-21 – 2014-07-25
    • Related Report
      2014 Research-status Report
  • [Presentation] Interconversion between quinone and catecholate caused by photo- or redox reactions on ruthenium polypyridyl complexes

    • Author(s)
      曽我侑加,高瀬つぎ子,大山 大
    • Organizer
      International Symposium for the 70th Anniversary of the Tohoku Branch of the Chemical Society of Japan
    • Place of Presentation
      Sendai (Japan)
    • Related Report
      2013 Research-status Report
  • [Presentation] Design and synthesis of ruthenium complexes for an ideal NADH model compound

    • Author(s)
      鵜川成美,高瀬つぎ子,大山 大
    • Organizer
      International Symposium for the 70th Anniversary of the Tohoku Branch of the Chemical Society of Japan
    • Place of Presentation
      Sendai (Japan)
    • Related Report
      2013 Research-status Report
  • [Presentation] Stereospecific synthesis of carbonyl complexes containing an asymmetrical bidentate ligand

    • Author(s)
      直井龍太郎,譲矢かずみ,高瀬つぎ子,大山 大
    • Organizer
      平成25年度化学系学協会東北大会
    • Place of Presentation
      東北大学(宮城県仙台市)
    • Related Report
      2013 Research-status Report
  • [Presentation] 酸化還元および光に応答した分子内構造変化を利用するRu-CO部位の反応制御

    • Author(s)
      文 比沙,高瀬つぎ子,大山 大
    • Organizer
      錯体化学会第63回討論会
    • Place of Presentation
      琉球大学(沖縄県西原町)
    • Related Report
      2013 Research-status Report
  • [Presentation] ルテニウムカルボニル錯体の配位環境制御による金属-炭素結合の安定化

    • Author(s)
      鵜川成美,小室貴宏,高瀬つぎ子,大山 大
    • Organizer
      日本化学会第94春季年会
    • Place of Presentation
      名古屋大学(愛知県名古屋市)
    • Related Report
      2013 Research-status Report
  • [Presentation] フリーのカテコール部位を有する一連のルテニウム錯体:活性部位の構造に基づく反応性の相違

    • Author(s)
      曽我侑加,木戸正人,高瀬つぎ子,大山 大
    • Organizer
      日本化学会第94春季年会
    • Place of Presentation
      名古屋大学(愛知県名古屋市)
    • Related Report
      2013 Research-status Report

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Published: 2014-07-25   Modified: 2019-07-29  

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