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2014 Fiscal Year Annual Research Report

二次元反応場への金属錯体集積と水を基質とする革新的多電子物質変換

Research Project

Project/Area Number 24655135
Research InstitutionInstitute for Molecular Science

Principal Investigator

正岡 重行  分子科学研究所, 生命・錯体分子科学研究領域, 准教授 (20404048)

Project Period (FY) 2012-04-01 – 2015-03-31
Keywords金属錯体 / 再生可能エネルギー / 超分子
Outline of Annual Research Achievements

現在人類が直面しているエネルギー・環境問題を解決に導くため、太陽光エネルギーを貯蔵可能な化学エネルギーに変換する人工光合成技術が注目されている。中でも、水の完全分解・二酸化炭素還元・窒素還元固定は人工光合成分野における三大ターゲットであり、燃料電池との組み合わせにより、環境調和型物質循環システムの創成が期待されている。本研究では、人工光合成を“光と水の化学”と捉え、太陽光を駆動力とした水が関わる物質変換を自在に操る手法の開拓を目指した。触媒開発の対象として金属錯体、反応場として錯体界面集積体を利用を試みた。具体的には、両親媒性脂質分子を用いて、酸素発生触媒として機能することが知られている金属錯体をリポソーム界面に集積化し、その酸素発生触媒作用を調査した。その結果、錯体触媒に導入した官能基の種類(極性や鎖長など)に応じて、酸素発生触媒挙動が変化することがわかり、リポソーム界面に最適な酸素発生触媒の必要条件を得ることに成功した。また、電極界面への錯体集積も試みた。合理的な集積のため、分子間に有効な非共有結合性相互作用が働く金属錯体モジュールを合成し、その界面集積の可能性を検討した。その結果、非共有結合性相互作用として多点アレーン―パーフルオロアレーン相互作用を用いたところ、金属錯体を目的通りに二次元配列させることに成功した。また、その非共有結合サイトに発光性有機色素を導入した金属錯体の合成も試みた。

  • Research Products

    (13 results)

All 2015 2014

All Journal Article (6 results) (of which Peer Reviewed: 6 results,  Acknowledgement Compliant: 1 results,  Open Access: 1 results) Presentation (7 results) (of which Invited: 7 results)

  • [Journal Article] Design of Mononuclear Ruthenium Catalysts for Low-Overpotential Water Oxidation2015

    • Author(s)
      Masaya Okamura and Shigeyuki Masaoka
    • Journal Title

      Chem. Asian J.

      Volume: 10 Pages: 306-315

    • DOI

      10.1002/asia.201402781

    • Peer Reviewed
  • [Journal Article] Influence of Ligand Flexibility on the Electronic Structure of Oxidized NiIII Phenoxide Complexes2014

    • Author(s)
      Minoru Kawai, Takahide Yamaguchi, Shigeyuki Masaoka, Fumito Tani, Takamitsu Kohzuma, Linus Chiang, Tim Storr, Kaoru Mieda, Takashi Ogura, Robert Szilagyi, and Yuichi Shimazaki
    • Journal Title

      Inorg. Chem.

      Volume: 53 Pages: 10195-10202

    • DOI

      10.1021/ic501181k

    • Peer Reviewed
  • [Journal Article] Three Distinct Redox States of an Oxo-Bridged Dinuclear Ruthenium Complex2014

    • Author(s)
      Masaki Yoshida, Mio Kondo, Toshikazu Nakamura, Ken Sakai, and Shigeyuki Masaoka
    • Journal Title

      Angew. Chem. Int. Ed.

      Volume: 53 Pages: 11519-11523

    • DOI

      10.1002/anie.201406443

    • Peer Reviewed
  • [Journal Article] Electrochemical Behavior of Phosphine-Substituted Ruthenium(II) Polypyridine Complexes with a Single Labile Ligand2014

    • Author(s)
      Go Nakamura, Masaya Okamura, Masaki Yoshida, Takayoshi Suzuki, Hideo D. Takagi, Mio Kondo, and Shigeyuki Masaoka
    • Journal Title

      Inorg. Chem.

      Volume: 53 Pages: 7214-7226

    • DOI

      10.1021/ic5003644

    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Electrochemical response of metal complexes in homogeneous solution under photoirradiation2014

    • Author(s)
      Arisa Fukatsu, Mio Kondo, Masaya Okamura, Masaki Yoshida, and Shigeyuki Masaoka
    • Journal Title

      Sci. Rep.

      Volume: 4 Pages: 5327

    • DOI

      10.1038/srep05327

    • Peer Reviewed / Open Access
  • [Journal Article] Tuning of Metal-Metal Interactions in Mixed-Valence States of Cyclometalated Dinuclear Ruthenium and Osmium Complexes Bearing Tetrapyridylpyrazine or -benzene2014

    • Author(s)
      Takumi Nagashima, Takuya Nakabayashi, Takashi Suzuki, Katsuhiko Kanaizuka, Hiroaki Ozawa, Yu-Wu Zhong, Shigeyuki Masaoka, Ken Sakai, and Masa-aki Haga
    • Journal Title

      Organometallics

      Volume: 33 Pages: 4893-4904

    • DOI

      10.1021/om500142t

    • Peer Reviewed
  • [Presentation] Artificial Molecular Catalysts Designed for Water Oxidation2014

    • Author(s)
      Shigeyuki Masaoka
    • Organizer
      8th International Symposium on Nanomedicine (ISNM2014)
    • Place of Presentation
      Ehime University, Matsuyama, Ehime, Japan
    • Year and Date
      2014-12-04 – 2014-12-04
    • Invited
  • [Presentation] Molecular Catalysts Designed for Water Oxidation2014

    • Author(s)
      Shigeyuki Masaoka
    • Organizer
      2014 International Conference on Artificial Photosynthesis (ICARP2014)
    • Place of Presentation
      Awaji Yumebutai International Conference Center, Awaji, Hyogo, Japan
    • Year and Date
      2014-11-27 – 2014-11-27
    • Invited
  • [Presentation] Electrochemical evaluation of photochemical and catalytic properties of transition metal complexes2014

    • Author(s)
      Shigeyuki Masaoka
    • Organizer
      Annual Meeting on Photochemistry 2014
    • Place of Presentation
      Hokkaido University, Sapporo, Hokkaido, Japan
    • Year and Date
      2014-10-11 – 2014-10-11
    • Invited
  • [Presentation] Molecular Catalysts Designed for Water Oxidation2014

    • Author(s)
      Shigeyuki Masaoka
    • Organizer
      2nd Japan-UK Joint Symposium on Coordination Chemistry
    • Place of Presentation
      Chuo University, Tokyo, Tokyo, Japan
    • Year and Date
      2014-09-17 – 2014-09-17
    • Invited
  • [Presentation] Water Oxidation Catalyzed by Mononuclear and Multinuclear Metal Complexes2014

    • Author(s)
      Shigeyuki Masaoka
    • Organizer
      Symposium on Molecular Catalysis Toward Sustainable Energy
    • Place of Presentation
      Nanyang Technological University, Singapore, Singapore
    • Year and Date
      2014-07-26 – 2014-07-26
    • Invited
  • [Presentation] Water Oxidation Catalyzed by Mononuclear and Multinuclear Metal Complexes2014

    • Author(s)
      Shigeyuki Masaoka
    • Organizer
      41st International Conference on Coordination Chemistry
    • Place of Presentation
      Suntec Singapore Convention & Exhibition Centre, Singapore, Singapore
    • Year and Date
      2014-07-22 – 2014-07-22
    • Invited
  • [Presentation] Water Oxidation Catalyzed by Transition Metal Complexes2014

    • Author(s)
      Shigeyuki Masaoka
    • Organizer
      Supramolecular Coordination Chemistry, Japan-Canada Joint Symposium in CSC2014
    • Place of Presentation
      Vancouver Convention Centre, Vancouver, Canada
    • Year and Date
      2014-06-04 – 2014-06-04
    • Invited

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Published: 2016-06-01  

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