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Development of efficient heterodinuclear water oxidation catalysts based on intramolecular O-O bond formation between different metal ions

Research Project

Project/Area Number 19K21136
Project/Area Number (Other) 18H05990 (2018)
Research Category

Grant-in-Aid for Research Activity Start-up

Allocation TypeMulti-year Fund (2019)
Single-year Grants (2018)
Review Section 0502:Inorganic/coordination chemistry, analytical chemistry, inorganic materials chemistry, energy-related chemistry, and related fields
Research InstitutionNiigata University

Principal Investigator

Tsubonouchi Yuta  新潟大学, 自然科学系, 特任助教 (90823972)

Project Period (FY) 2018-08-24 – 2020-03-31
Project Status Completed (Fiscal Year 2019)
Budget Amount *help
¥2,990,000 (Direct Cost: ¥2,300,000、Indirect Cost: ¥690,000)
Fiscal Year 2019: ¥1,430,000 (Direct Cost: ¥1,100,000、Indirect Cost: ¥330,000)
Fiscal Year 2018: ¥1,560,000 (Direct Cost: ¥1,200,000、Indirect Cost: ¥360,000)
Keywords人工光合成 / 水の酸化反応 / 二核錯体 / 異種金属錯体 / 反応機構解析 / 分子性触媒 / ルテニウム錯体 / 酸素発生反応 / 錯体化学
Outline of Research at the Start

人工光合成の実現には高活性な酸素発生触媒の開発が必要不可欠である。これまで、多く
の酸素発生触媒が報告されているが、分子内O-O カップリング機構により酸素を生成する錯体触媒の報告例は少ない。一方、植物の光合成における酸素発生中心(OEC)は、Mn とCaの二種金属イオンから構成され、それぞれの金属イオンが重要な役割を果たしていると推定されているが、その機構は憶測の域を出ない。本研究では、新奇な異種金属二核錯体を合成し、その酸素発生触媒機能およびO-O 結合形機構に及ぼす異種中心金属イオンの効果を明らかにする。

Outline of Final Research Achievements

This study focuses on the development of efficient water oxidation catalysts based on intramolecular O-O bond formation. We newly synthesized a dinuclear ruthenium complex having an organic bridging ligand and immobilized it on a carbon electrode using hydrophobic interactions. The molecular anode shows a remarkable activity and low overpotential for water oxidation. Furthermore, we successfully prepared and characterized a new series of heterodinuclear complexes inspired by the oxygen-evolving complex of photosystem II.

Academic Significance and Societal Importance of the Research Achievements

本研究では高活性な分子性水の酸化アノードの開発に成功した。これは人工光合成研究の進展に貢献する重要な成果である。また、異種金属二核錯体の合成とその特性評価は、生体の異種金属酵素の反応を解き明かす上で、有用な示唆を与えると期待される。

Report

(3 results)
  • 2019 Annual Research Report   Final Research Report ( PDF )
  • 2018 Annual Research Report
  • Research Products

    (17 results)

All 2020 2019 2018

All Journal Article (7 results) (of which Int'l Joint Research: 7 results,  Peer Reviewed: 7 results,  Open Access: 1 results) Presentation (6 results) (of which Int'l Joint Research: 1 results) Book (4 results)

  • [Journal Article] Molecular aspects, electrochemical properties and water oxidation catalysis on a nanoporous TiO2 electrode anchoring a mononuclear ruthenium(II) aquo complex2020

    • Author(s)
      Tsubonouchi Yuta、Eo Tatsuya、Honta Junichiro、Sato Taisei、Mohamed Eman A.、Zahran Zaki N.、Saito Kenji、Yui Tatsuto、Yagi Masayuki
    • Journal Title

      Journal of Photochemistry and Photobiology A: Chemistry

      Volume: in press Pages: 112696-112696

    • DOI

      10.1016/j.jphotochem.2020.112696

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Multi-potential-step chronocoulospectrometry for electrocatalytic water oxidation by a mononuclear ruthenium aquo complex immobilized on a mesoporous ITO electrode2020

    • Author(s)
      Yuta Tsubonouchi, Junichiro Honta, Taisei Sato, Eman A. Mohamed, Zaki N. Zahran, Kenji Saito, Tatsuto Yui, and Masayuki Yagi
    • Journal Title

      Dalton Trans.

      Volume: 49 Issue: 5 Pages: 1416-1423

    • DOI

      10.1039/c9dt04442f

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Highly Efficient and Selective Electrocatalytic CO2-to-CO Conversion by a Non-heme Iron Complex with an In-Plane N4 Ligand in Heterogeneous Aqueous Media2020

    • Author(s)
      Mohamed Eman A.、Zahran Zaki N.、Tsubonouchi Yuta、Saito Kenji、Yui Tatsuto、Yagi Masayuki
    • Journal Title

      ACS Applied Energy Materials

      Volume: 3 Issue: 5 Pages: 4114-4120

    • DOI

      10.1021/acsaem.9b02548

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Critical Hammett Electron-Donating Ability of Substituent Groups for Efficient Water Oxidation Catalysis by Mononuclear Ruthenium Aquo Complexes2019

    • Author(s)
      Watabe Shunsuke、Tanahashi Yuki、Hirahara Masanari、Yamazaki Hirosato、Takahashi Kosuke、Mohamed Eman A.、Tsubonouchi Yuta、Zahran Zaki N.、Saito Kenji、Yui Tatsuto、Yagi Masayuki
    • Journal Title

      Inorganic Chemistry

      Volume: 58 Issue: 19 Pages: 12716-12723

    • DOI

      10.1021/acs.inorgchem.9b01623

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Characterization and Mechanism of Efficient Visible-Light-Driven Water Oxidation on an in Situ N2-Intercalated WO3 Nanorod Photoanode2019

    • Author(s)
      Chandra Debraj、Li Dong、Sato Tetsuya、Tanahashi Yuki、Togashi Takanari、Ishizaki Manabu、Kurihara Masato、Mohamed Eman A.、Tsubonouchi Yuta、Zahran Zaki N.、Saito Kenji、Yui Tatsuto、Yagi Masayuki
    • Journal Title

      ACS Sustainable Chemistry & Engineering

      Volume: 7 Issue: 21 Pages: 17896-17906

    • DOI

      10.1021/acssuschemeng.9b04467

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Mechanisms of water oxidation using ruthenium, cobalt, copper, and iron molecular catalysts2019

    • Author(s)
      Parent Alexander Rene、Nakazono Takashi、Tsubonouchi Yuta、Taira Natsuki、Sakai Ken
    • Journal Title

      Advances in Inorganic Chemistry

      Volume: 74 Pages: 197-240

    • DOI

      10.1016/bs.adioch.2019.04.001

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Recent Advances in the Development of Molecular Catalyst‐Based Anodes for Water Oxidation toward Artificial Photosynthesis2019

    • Author(s)
      Zaki N. Zahran, Yuta Tsubonouch, Eman A. Mohamed, Masayuki Yagi
    • Journal Title

      ChemSusChem

      Volume: 12 Issue: 9 Pages: 1775-1793

    • DOI

      10.1002/cssc.201802795

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Presentation] Immobilization of a molecular ruthenium catalyst on carbon electrodes for efficient and stable electrochemical water oxidation2019

    • Author(s)
      Y. Tsubonouchi, T. Hayasaka, Y. Wakai, E. A. Mohamed, Z. N. Zahran, K. Saito, Y. Tatsuto, M. Yagi
    • Organizer
      International conference on artificial photosynthesis 2019 (ICARP2019)
    • Related Report
      2019 Annual Research Report
  • [Presentation] Remarkably stable electrocatalysis for water oxidation by a dinuclear ruthenium complex immobilized on carbon electrodes2019

    • Author(s)
      Y. Tsubonouchi, T. Hayasaka, Y. Wakai, E. A. Mohamed, Z. N. Zahran, K. Saito, Y. Tatsuto, M. Yagi
    • Organizer
      錯体化学会第69 回討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Synthesis and Characterization of Multinuclear Complexes as Active Water Oxidation Catalysts2018

    • Author(s)
      Yuta Tsubonouchi, Masayuki Yagi
    • Organizer
      International Conference on Coordination Chemistry, 2018 (ICCC2018)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Physicochemical properties and thermal isomerization reaction of homoleptic mononuclear ruthenium complexes with asymmetric ligands2018

    • Author(s)
      坪ノ内優太、園川大樹、齊藤健二、由井樹人、畑中翼、舩橋靖博、野崎浩一、八木政行
    • Organizer
      日本化学会第99春季年会
    • Related Report
      2018 Annual Research Report
  • [Presentation] Electrochemical water oxidation catalysis by a dinuclear ruthenium complex having a carboxylate-anthyridine ligand2018

    • Author(s)
      園川大樹、坪ノ内優太、齊藤健二、由井樹人、八木政行
    • Organizer
      日本化学会第99春季年会
    • Related Report
      2018 Annual Research Report
  • [Presentation] Synthesis and catalytic water oxidation activities of base metal complexes with conjugated macrocyclic ligands2018

    • Author(s)
      高橋大生、坪ノ内優太、齊藤健二、由井樹人、八木政行
    • Organizer
      日本化学会第99春季年会
    • Related Report
      2018 Annual Research Report
  • [Book] 「酸化イリジウムのナノ構造制御による酸素発生アノード触媒の開発」 エネルギー・資源 5月号2020

    • Author(s)
      坪ノ内優太、江尾達矢、八木政行
    • Total Pages
      7
    • Publisher
      エネルギー・資源学会
    • Related Report
      2019 Annual Research Report
  • [Book] "Catalytic aspects and mechanisms of water oxidation by mononuclear ruthenium(II) aquo complexes", chapter contribution to a book entitled "An introduction to water oxidation"2020

    • Author(s)
      Tsubonouchi Yuta、Tanahashi Yuki、Hirahara Masanari、Mohamed Eman A.、Zahran Zaki N.、Yagi Masayuki
    • Total Pages
      33
    • Publisher
      Nova Science Publishers, Inc.
    • Related Report
      2019 Annual Research Report
  • [Book] “Photoisomerization of polypyridyl ruthenium(II) aquo complexes”, chapter contribution to a book entitled "Photoisomerization: causes, behavior and effects"2019

    • Author(s)
      Tanahashi Yuki、Watabe Shunsuke、Mohamed Eman A.、Tsubonouchi Yuta、Zahran Zaki N.、Yagi Masayuki
    • Total Pages
      30
    • Publisher
      Nova Science Publishers, Inc.
    • Related Report
      2019 Annual Research Report
  • [Book] Photoisomerization: Causes, Behavior and Effects(Photoisomerization of polypyridyl ruthenium(II) aquo complexes)2019

    • Author(s)
      Yuki Tanahashi、Shunsuke Watabe、Eman A. Mohamed、Yuta Tsubonouchi、Zaki N. Zahran、Masanari Hirahara、Masayuki Yagi
    • Total Pages
      30
    • Publisher
      Nova Science Publishers, Inc
    • ISBN
      9781536153132
    • Related Report
      2018 Annual Research Report

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Published: 2018-08-27   Modified: 2024-03-26  

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