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Development of Molecular Catalysts Promoting Multi-electron Reduction Reactions via Unique Proton-coupled Electron Transfer Pathways

Research Project

Project/Area Number 18K05150
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeMulti-year Fund
Section一般
Review Section Basic Section 34010:Inorganic/coordination chemistry-related
Research InstitutionKyushu University

Principal Investigator

Yamauchi Kosei  九州大学, 理学研究院, 助教 (50631769)

Project Period (FY) 2018-04-01 – 2022-03-31
Project Status Completed (Fiscal Year 2021)
Budget Amount *help
¥4,420,000 (Direct Cost: ¥3,400,000、Indirect Cost: ¥1,020,000)
Fiscal Year 2020: ¥1,430,000 (Direct Cost: ¥1,100,000、Indirect Cost: ¥330,000)
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 / プロトン共役電子移動(PCET) / 錯体触媒 / 水素生成 / プロトン共役電子移動 / 水素発生 / 二酸化炭素還元 / 分子性触媒 / 金属錯体 / 電気化学 / 水素生成反応
Outline of Final Research Achievements

We studied the unique proton-coupled electron transfer (PCET) processes which are promoted at either the metal or ligand center. Specifically, we succeeded in developing the new molecular catalyst which promotes hydrogen evolution from water with the exceptionally overpotential of 173 mV by enhancing PCET at the ligand center. Furthermore, DFT calculations were performed to elucidate the factors controlling the ligand-centered PCET leading to hydrogen evolution from water. In addition, advanced electrochemical reaction analysis was performed to experimentally elucidate the reaction mechanism. On the other hand, we developed the new photochemical system which promotes hydrogen evolution from water via metal-centered PCET.

Academic Significance and Societal Importance of the Research Achievements

プロトンと電子が協奏的に移動するプロトン共役電子移動(PCET)は、生体系の重要反応を担い、これまで多くの研究がなされてきた。一方、PCETを効果的に活用し、高効率な人工光合成系を構築した研究例はほとんどない。本研究では、機能性配位子上で進行する特異なPCETを巧みに制御することにより水素生成錯体触媒の過電圧を劇的に低下させることに成功した。また、機能性錯体上で進行するPCET過程の反応制御因子を実験的並びに計算化学的に解き明かした。このように、特異なPCETを経由し水素生成反応を促進する分子性触媒について多角的な研究を展開し、同分野の発展に貢献する種々の価値ある成果を収めた。

Report

(5 results)
  • 2021 Annual Research Report   Final Research Report ( PDF )
  • 2020 Research-status Report
  • 2019 Research-status Report
  • 2018 Research-status Report
  • Research Products

    (37 results)

All 2021 2020 2019 2018 Other

All Int'l Joint Research (3 results) Journal Article (11 results) (of which Int'l Joint Research: 6 results,  Peer Reviewed: 11 results) Presentation (19 results) (of which Int'l Joint Research: 7 results,  Invited: 5 results) Remarks (4 results)

  • [Int'l Joint Research] ウンム・アル=クラー大学(サウジアラビア)

    • Related Report
      2020 Research-status Report
  • [Int'l Joint Research] Tianjin University of Technology/Sun Yat-Sen University(中国)

    • Related Report
      2019 Research-status Report
  • [Int'l Joint Research] University of Quebec in Trois-Rivieres(カナダ)

    • Related Report
      2019 Research-status Report
  • [Journal Article] Redox tuning in Pt(bpy)-viologen catalyst-acceptor dyads enabling photocatalytic hydrogen evolution from water2021

    • Author(s)
      Yatsuzuka Koichi、Yamauchi Kosei、Sakai Ken
    • Journal Title

      Chemical Communications

      Volume: 57 Issue: 42 Pages: 5183-5186

    • DOI

      10.1039/d1cc00903f

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Improving the overall performance of photochemical H2 evolution catalyzed by the Co-NHC complex via the redox tuning of electron relays2021

    • Author(s)
      Yatsuzuka Koichi、Yamauchi Kosei、Kawano Ken、Ozawa Hironobu、Sakai Ken
    • Journal Title

      Sustainable Energy & Fuels

      Volume: 5 Issue: 3 Pages: 740-749

    • DOI

      10.1039/d0se01597k

    • Related Report
      2020 Research-status Report
    • Peer Reviewed
  • [Journal Article] Unexpected structure of enaminone Pd(II) complex in comparison with Cu(II) complex: Synthesis, characterization, DNA binding and antitumor activity2021

    • Author(s)
      El-Ghamry Hoda A.、Yamauchi Kosei、Sakai Ken、Farghaly Thoraya A.
    • Journal Title

      Inorganica Chimica Acta

      Volume: 516 Pages: 120117-120117

    • DOI

      10.1016/j.ica.2020.120117

    • Related Report
      2020 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] A dinuclear nickel catalyst based on metal-metal cooperation for electrochemical hydrogen production2020

    • Author(s)
      Hamaguchi Tomohiko、Kai Keisuke、Ando Isao、Kawano Ken、Yamauchi Kosei、Sakai Ken
    • Journal Title

      Inorganica Chimica Acta

      Volume: 505 Pages: 119498-119498

    • DOI

      10.1016/j.ica.2020.119498

    • Related Report
      2019 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Highly Efficient and Selective Photocatalytic CO2 Reduction to CO in Water by a Cobalt Porphyrin Molecular Catalyst2019

    • Author(s)
      Call Arnau、Cibian Mihaela、Yamamoto Keiya、Nakazono Takashi、Yamauchi Kosei、Sakai Ken
    • Journal Title

      ACS Catalysis

      Volume: 9 Issue: 6 Pages: 4867-4874

    • DOI

      10.1021/acscatal.8b04975

    • Related Report
      2019 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] A Molecular Cobalt Hydrogen Evolution Catalyst Showing High Activity and Outstanding Tolerance to CO and O22019

    • Author(s)
      Wang Jia‐Wei、Yamauchi Kosei、Huang Hai‐Hua、Sun Jia‐Kai、Luo Zhi‐Mei、Zhong Di‐Chang、Lu Tong‐Bu、Sakai Ken
    • Journal Title

      Angewandte Chemie International Edition

      Volume: 58 Issue: 32 Pages: 10923-10927

    • DOI

      10.1002/anie.201904578

    • Related Report
      2019 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] An earth-abundant system for light-driven CO2 reduction to CO using a pyridinophane iron catalyst2019

    • Author(s)
      Sakaguchi Yuto、Call Arnau、Cibian Mihaela、Yamauchi Kosei、Sakai Ken
    • Journal Title

      Chemical Communications

      Volume: 55 Issue: 59 Pages: 8552-8555

    • DOI

      10.1039/c9cc04191e

    • Related Report
      2019 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Photochemical CO2 Reduction Driven by Water-Soluble Copper(I) Photosensitizer with the Catalysis Accelerated by Multi-Electron Chargeable Cobalt Porphyrin2019

    • Author(s)
      Zhang Xian、Cibian Mihaela、Call Arnau、Yamauchi Kosei、Sakai Ken
    • Journal Title

      ACS Catalysis

      Volume: 9 Issue: 12 Pages: 11263-11273

    • DOI

      10.1021/acscatal.9b04023

    • Related Report
      2019 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Consecutive ligand-based PCET processes affording a doubly reduced nickel pyrazinedithiolate which transforms into a metal hydride required to evolve H22019

    • Author(s)
      Koshiba Keita、Yamauchi Kosei、Sakai Ken
    • Journal Title

      Dalton Transactions

      Volume: 48 Issue: 2 Pages: 635-640

    • DOI

      10.1039/c8dt04497j

    • Related Report
      2018 Research-status Report
    • Peer Reviewed
  • [Journal Article] Ligand‐based PCET Reduction in a Heteroleptic Ni(bpy)(dithiolene) Electrocatalyst Giving Rise to Higher Metal Basicity Required for Hydrogen Evolution2019

    • Author(s)
      Koshiba Keita、Yamauchi Kosei、Sakai Ken
    • Journal Title

      ChemElectroChem

      Volume: - Issue: 8 Pages: 2273-2281

    • DOI

      10.1002/celc.201900400

    • Related Report
      2018 Research-status Report
    • Peer Reviewed
  • [Journal Article] A family of molecular nickel hydrogen evolution catalysts providing tunable overpotentials using ligand-centered proton-coupled electron transfer paths2018

    • Author(s)
      Aimoto Yutaro、Koshiba Keita、Yamauchi Kosei、Sakai Ken
    • Journal Title

      Chemical Communications

      Volume: 54 Issue: 91 Pages: 12820-12823

    • DOI

      10.1039/c8cc07467d

    • Related Report
      2018 Research-status Report
    • Peer Reviewed
  • [Presentation] 錯体化学で理解する人工光合成反応過程2020

    • Author(s)
      山内幸正
    • Organizer
      錯体化学若手の会第1回ウェブ勉強会
    • Related Report
      2020 Research-status Report
    • Invited
  • [Presentation] Electrochemical CO2 Reduction to CO with Low Overpotentials by Co-NHC Complexes2020

    • Author(s)
      Kosei Yamauchi, Toshihiro Koga, Yasunobu Wakafuji, Ken Sakai
    • Organizer
      錯体化学会第70回討論会
    • Related Report
      2020 Research-status Report
  • [Presentation] Electrochemical Hydrogen Evolution from Water Promoted by Metal Complexes2020

    • Author(s)
      Kosei Yamauchi
    • Organizer
      New Trends in Photophysics and Photochemistry and their Applications
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Nickel(II) Dithiolate Molecular Catalysts Promoting Hydrogen Evolution from Water with Low Overpotentials2019

    • Author(s)
      Kosei Yamauchi
    • Organizer
      International Conference on Photocatalysis and Photoenergy 2019 (ICoPP2019)
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] 金属錯体触媒による低過電圧水素生成反応2019

    • Author(s)
      山内幸正
    • Organizer
      九州錯体化学懇談会50周年記念シンポジウム
    • Related Report
      2019 Research-status Report
    • Invited
  • [Presentation] Molecular Catalysts Promoting Hydrogen Production from Water via Unique Proton-coupled Electron Transfer Processes2019

    • Author(s)
      Kosei YAMAUCHI, Keita KOSHIBA, Yutaro AIMOTO, Ken SAKAI
    • Organizer
      錯体化学会第69回討論会
    • Related Report
      2019 Research-status Report
  • [Presentation] コバルトNHC錯体を触媒とした二酸化炭素還元反応2019

    • Author(s)
      古賀俊弘、山内幸正、酒井 健
    • Organizer
      錯体化学会第69回討論会
    • Related Report
      2019 Research-status Report
  • [Presentation] MOLECULAR CATALYSTS PROMOTING HYDROGEN EVOLUTION FROM WATER VIA THE LIGAND-BASED PROTON-COUPLED ELECTRON TRANSFER PROCESSES2019

    • Author(s)
      Kosei Yamauchi, Keita Koshiba, Yutaro Aimoto, Ken Sakai
    • Organizer
      International Conference on Artificial Photosynthesis-2019 (ICARP2019)
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research
  • [Presentation] A Family of Molecular Nickel(II) Dithiolate Catalysts Promoting Hydrogen Evolution from Water with Low Overpotentials via the Ligand-centered PCET Processes2019

    • Author(s)
      K. Yamauchi, Y. Aimoto, K. Koshiba, and K. Sakai
    • Organizer
      日本化学会第99春季年会
    • Related Report
      2018 Research-status Report
  • [Presentation] アントラキノン骨格を有する新規ニッケル錯体の合成と水素生成触媒機能2019

    • Author(s)
      管 昌権、山内幸正、酒井 健
    • Organizer
      日本化学会第99春季年会
    • Related Report
      2018 Research-status Report
  • [Presentation] Molecular Catalyst Promoting Hydrogen Evolution with Low Overpotential2018

    • Author(s)
      K. Yamauchi, K. Koshiba, Y. Aimoto, K. Kawano, and K. Sakai
    • Organizer
      ICCC2018: Post-Conference in Fukuoka “Transition Metal Chemistry towards Sustainable Energy Conversion and Various Advanced Applications
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Nickel Dithiolate Molecular Catalysts Promoting Hydrogen Evolution from Water with Low Overpotentials2018

    • Author(s)
      K. Yamauchi, K. Koshiba, Y. Aimoto, and K. Sakai
    • Organizer
      43rd International Conference on Coordination Chemistry (ICCC2018)
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research
  • [Presentation] 光水素生成反応を促進する白金錯体触媒の速度論的研究2018

    • Author(s)
      山内幸正、脇山史彬、酒井 健
    • Organizer
      第30回配位化合物の光化学討論会
    • Related Report
      2018 Research-status Report
  • [Presentation] Thermodynamic Aspects of Hydrogen Evolution Reactions Catalyzed by Metal-NHC Complexes2018

    • Author(s)
      Kosei Yamauchi, Ken Kawano, Ken Sakai
    • Organizer
      錯体化学会第68回討論会
    • Related Report
      2018 Research-status Report
  • [Presentation] 多座電子供与性配位子を有する金属錯体触媒の合成と水素生成機能2018

    • Author(s)
      古賀俊弘、山内幸正、酒井 健
    • Organizer
      錯体化学会第68回討論会
    • Related Report
      2018 Research-status Report
  • [Presentation] Nickel(II) Dithiolene Complexes Bearing Polyazanaphthalene Units Catalyzing H2 Evolution from Water with Low Overpotentials2018

    • Author(s)
      Yutaro Aimoto, Keita Koshiba, Kosei Yamauchi, Ken Sakai
    • Organizer
      錯体化学会第68回討論会
    • Related Report
      2018 Research-status Report
  • [Presentation] Hydrogen Evolution Catalyzed by New Nickel(II) complexes Having NHC Ligands2018

    • Author(s)
      T. Koga, K. Kawano, K. Yamauchi, K. Sakai
    • Organizer
      43rd International Conference on Coordination Chemistry (ICCC2018)
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research
  • [Presentation] Electrochemical Hydrogen Evolution from Water with Low Overpotentials Catalyzed by Nickel(II) Dithiolene Complexes2018

    • Author(s)
      Y. Aimoto, K. Koshiba, K. Yamauchi, K. Sakai
    • Organizer
      43rd International Conference on Coordination Chemistry (ICCC2018)
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research
  • [Presentation] ピラジンジチオレン錯体触媒による水からの低過電圧水素生成反応2018

    • Author(s)
      相本雄太郎、山内幸正、酒井 健
    • Organizer
      錯体化学若手研究会 錯体化学若手の会夏の学校2018
    • Related Report
      2018 Research-status Report
  • [Remarks] 九州大学大学院理学研究院化学部門 錯体化学研究室

    • URL

      http://www.scc.kyushu-u.ac.jp/Sakutai/jp/index.html

    • Related Report
      2021 Annual Research Report
  • [Remarks] 九州大学 錯体化学研究室

    • URL

      http://www.scc.kyushu-u.ac.jp/Sakutai/jp/index.html

    • Related Report
      2020 Research-status Report
  • [Remarks] 錯体化学研究室

    • URL

      http://www.scc.kyushu-u.ac.jp/Sakutai/jp/index.html

    • Related Report
      2019 Research-status Report
  • [Remarks] 九州大学大学院理学研究院化学部門 錯体化学研究室

    • URL

      http://www.scc.kyushu-u.ac.jp/Sakutai/

    • Related Report
      2018 Research-status Report

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Published: 2018-04-23   Modified: 2023-01-30  

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