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Rational Control for the Reactivity of Low Overpotential Hydrogen-evolving Catalysts and their Application to Water-splitting Molecular Systems

Research Project

Project/Area Number 16K17879
Research Category

Grant-in-Aid for Young Scientists (B)

Allocation TypeMulti-year Fund
Research Field Inorganic chemistry
Research InstitutionKyushu University

Principal Investigator

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

Project Period (FY) 2016-04-01 – 2018-03-31
Project Status Completed (Fiscal Year 2017)
Budget Amount *help
¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000)
Fiscal Year 2017: ¥1,950,000 (Direct Cost: ¥1,500,000、Indirect Cost: ¥450,000)
Fiscal Year 2016: ¥2,210,000 (Direct Cost: ¥1,700,000、Indirect Cost: ¥510,000)
Keywords人工光合成 / 水素発生 / 低過電圧 / ニッケル錯体 / コバルト錯体 / N-ヘテロ環状カルベン / 反応機構解析 / 分子触媒 / 金属錯体 / ヒドリド / プロトン共役電子移動 / 水の可視光分解
Outline of Final Research Achievements

In this study, we focused on the rational control for the activity of molecular catalysts accelerating hydrogen evolution from water via a metal-centered or ligand-centered proton-coupled electron transfer (PCET) process.
As for a Co-NHC complex promoting metal-centered PCET, we realized an efficient photochemical system whose activity is 30 times higher in hydrogen evolution from water by tuning the effect of co-existing anion species and the redox potential of an electron realay employed.
On the other hand, a nickel complex was found to promote hydrogen evolution from water with an overpotential of 330-400 mV via a ligand-centered PCET. Furthermore, the reaction mechanism was successfully clarified in detail.

Report

(3 results)
  • 2017 Annual Research Report   Final Research Report ( PDF )
  • 2016 Research-status Report
  • Research Products

    (31 results)

All 2018 2017 2016 Other

All Journal Article (3 results) (of which Peer Reviewed: 3 results,  Open Access: 1 results,  Acknowledgement Compliant: 1 results) Presentation (26 results) (of which Int'l Joint Research: 4 results,  Invited: 2 results) Remarks (2 results)

  • [Journal Article] Near-Infrared Light-Driven Hydrogen Evolution from Water Using a Polypyridyl Triruthenium Photosensitizer2018

    • Author(s)
      Yutaro Tsuji、Keiya Yamamoto、Kosei Yamauchi、Ken Sakai
    • Journal Title

      Angew. Chem. Int. Ed.

      Volume: 57 Issue: 1 Pages: 208-212

    • DOI

      10.1002/anie.201708996

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Photochemical H2 Evolution Catalyzed by Porphyrin-based Cubic Cages Singly and Doubly Encapsulating PtCl2(4,4′-dimethyl-2,2′-bipyridine)2017

    • Author(s)
      Shota Tanaka、Takashi Nakazono、Kosei Yamauchi、Ken Sakai
    • Journal Title

      Chem. Lett.

      Volume: 46 Issue: 10 Pages: 1573-1575

    • DOI

      10.1246/cl.170692

    • NAID

      130006140028

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] A Nickel Dithiolate Water Reduction Catalyst Providing Ligand-based Proton-coupled Electron Transfer Pathways2017

    • Author(s)
      K. Koshiba, K. Yamauchi, and K. Sakai
    • Journal Title

      Angewandte Chemie International Edition

      Volume: 56 Issue: 15 Pages: 4247-4251

    • DOI

      10.1002/anie.201700927

    • Related Report
      2016 Research-status Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Presentation] Mechanistic Investigation of Hydrogen Evolution Catalysis Promoted by Co-NHC complexes2018

    • Author(s)
      Kosei Yamauchi, Ken Kawano, Ken Sakai
    • Organizer
      日本化学会第98春季年会
    • Related Report
      2017 Annual Research Report
  • [Presentation] ポリピリジルルテニウム(II)三核錯体を光増感剤とした近赤外光水素生成反応2018

    • Author(s)
      辻優太郎、山本啓也、山内幸正、酒井 健
    • Organizer
      日本化学会第98春季年会
    • Related Report
      2017 Annual Research Report
  • [Presentation] ポリアザナフタレン骨格を有するニッケルジチオレン錯体触媒 による水素生成反応とその機構2018

    • Author(s)
      相本雄太郎、小柴慧太、山内幸正、酒井 健
    • Organizer
      日本化学会第98春季年会
    • Related Report
      2017 Annual Research Report
  • [Presentation] NHC配位子を有する金属錯体触媒による多電子還元反応2018

    • Author(s)
      古賀俊弘、河野 健、山内 幸正、酒井 健
    • Organizer
      日本化学会第98春季年会
    • Related Report
      2017 Annual Research Report
  • [Presentation] Mechanistic Studies on Hydrogen Evolution from Water Catalyzed by Ni(II)-based Molecular Catalysts2017

    • Author(s)
      Kosei Yamauchi, Shinataro Nakashima, Keita Koshiba, and Ken Sakai
    • Organizer
      日本化学会第97春季年会
    • Place of Presentation
      慶應義塾大学日吉キャンパス、横浜市
    • Year and Date
      2017-03-16
    • Related Report
      2016 Research-status Report
  • [Presentation] ポリアザナフタレン骨格を有する新規ジチオラトニッケル錯体触媒の電気化学的水素生成反応2017

    • Author(s)
      相本雄太郎、小柴慧太、山内幸正、酒井 健
    • Organizer
      日本化学会第97春季年会
    • Place of Presentation
      慶應義塾大学日吉キャンパス、横浜市
    • Year and Date
      2017-03-16
    • Related Report
      2016 Research-status Report
  • [Presentation] 新規ポリピリジルルテニウム三核錯体を用いた赤色光増感による光水素生成反応2017

    • Author(s)
      辻優太郎、山内幸正、酒井 健
    • Organizer
      日本化学会第97春季年会
    • Place of Presentation
      慶應義塾大学日吉キャンパス、横浜市
    • Year and Date
      2017-03-16
    • Related Report
      2016 Research-status Report
  • [Presentation] A Nickel Dithiolate Molecular Catalyst Promoting Hydrogen Evolution from Water with Low Overpotential2017

    • Author(s)
      Kosei Yamauchi, Keita Koshiba, Ken Sakai
    • Organizer
      NanoMat 2017
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 水からの光水素生成反応を駆動する金属錯体触媒2017

    • Author(s)
      山内幸正、河野 健、八束孝一、酒井 健
    • Organizer
      第38回光化学若手の会
    • Related Report
      2017 Annual Research Report
  • [Presentation] Co-NHC錯体を触媒とする光水素生成反応の活性制御2017

    • Author(s)
      山内幸正、河野 健、八束孝一、酒井 健
    • Organizer
      第29回配位化合物の光化学討論会
    • Related Report
      2017 Annual Research Report
  • [Presentation] Electrocatalytic hydrogen evolution from water with low overpotential even via the formation of low-valent nickel species2017

    • Author(s)
      Kosei YAMAUCHI, Shintaro NAKASHIMA, Keita KOSHIBA, Ken SAKAI
    • Organizer
      錯体化学会第67回討論会
    • Related Report
      2017 Annual Research Report
  • [Presentation] Molecular Catalysts Promoting H2 Evolution from Water with Low Driving Force2017

    • Author(s)
      Kosei Yamauchi, Ken Kawano, Koichi Yatsuduka, Keita Koshiba, Ken Sakai
    • Organizer
      Japan-Italy Joint Symposium on Artificial Photosynthesis
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 高活性水素生成分子触媒の開発と錯体化学2017

    • Author(s)
      山内 幸正
    • Organizer
      第6回錯体化学若手の会九州・沖縄支部勉強会
    • Related Report
      2017 Annual Research Report
    • Invited
  • [Presentation] 単一分子多電子貯蔵デバイスを基盤とした高耐久性光水素発生システムの開発2017

    • Author(s)
      山本啓也、山内幸正、酒井 健
    • Organizer
      第38回光化学若手の会
    • Related Report
      2017 Annual Research Report
  • [Presentation] 新規ポリピリジルルテニウム(II)三核錯体を光増感剤とした近赤外光による光水素生成反応2017

    • Author(s)
      辻優太郎、山本啓也、山内幸正、酒井 健
    • Organizer
      第38回光化学若手の会
    • Related Report
      2017 Annual Research Report
  • [Presentation] オキソ架橋ルテニウム三核錯体による酸素発生触媒反応の機構解析2017

    • Author(s)
      坪ノ内優太、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2017」
    • Related Report
      2017 Annual Research Report
  • [Presentation] 低過電圧で水素生成を行うニッケルジチオレン錯体触媒に関する研究2017

    • Author(s)
      相本雄太郎、小柴慧太、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2017」
    • Related Report
      2017 Annual Research Report
  • [Presentation] ポリアザナフタレン骨格を有するニッケル(II)ジチオレン錯体触媒による低過電圧水素生成反応2017

    • Author(s)
      相本雄太郎、小柴慧太、山内幸正、酒井 健
    • Organizer
      錯体化学会第67回討論会
    • Related Report
      2017 Annual Research Report
  • [Presentation] 近赤外光を増感する新規ポリピリジルルテニウム(II)三核錯体を用いた光水素生成反応2017

    • Author(s)
      辻優太郎、山本啓也、山内幸正、酒井 健
    • Organizer
      錯体化学会第67回討論会
    • Related Report
      2017 Annual Research Report
  • [Presentation] Molecular Catalysis for Hydrogen Evolution Reaction Driven with Low Overpotential2016

    • Author(s)
      Kosei Yamauchi, Keita Koshiba, and Ken Sakai
    • Organizer
      5th International Symposium on Solar Fuels and Solar Cells
    • Place of Presentation
      Dalian International Finance Conference Center, Dalian, China
    • Year and Date
      2016-10-11
    • Related Report
      2016 Research-status Report
    • Int'l Joint Research
  • [Presentation] Mechanistic studies on hydrogen evolution from water catalyzed by metal complexes with low overpotential2016

    • Author(s)
      Kosei Yamauchi, Keita Koshiba, and Ken Sakai
    • Organizer
      錯体化学会第66回討論会
    • Place of Presentation
      福岡大学七隈キャンパス、福岡市
    • Year and Date
      2016-09-10
    • Related Report
      2016 Research-status Report
  • [Presentation] オキソ架橋ルテニウム三核錯体を触媒とする水からの光酸素発生反応2016

    • Author(s)
      坪ノ内優太、林 樹、 Alexander R. Parent、 山内幸正、Gary W. Brudvig、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2016
    • Place of Presentation
      熊本市、火の国ハイツ
    • Year and Date
      2016-08-05
    • Related Report
      2016 Research-status Report
  • [Presentation] 白金錯体触媒による水素生成反応の中間体検出と新規触媒開発2016

    • Author(s)
      脇山史彬、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2016
    • Place of Presentation
      熊本市、火の国ハイツ
    • Year and Date
      2016-08-05
    • Related Report
      2016 Research-status Report
  • [Presentation] 単一分子光電子貯蔵システムにおける光増感部位-電子受容部位間の距離依存性に関する研究2016

    • Author(s)
      山本啓也、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2016
    • Place of Presentation
      熊本市、火の国ハイツ
    • Year and Date
      2016-08-05
    • Related Report
      2016 Research-status Report
  • [Presentation] 可視光水分解系の構築を目指した低過電圧水素生成分子触媒の開発2016

    • Author(s)
      山内幸正、小柴慧太、酒井 健
    • Organizer
      第37回光化学若手の会
    • Place of Presentation
      アイ・アイ・ランド 、大阪府四條畷市
    • Year and Date
      2016-06-17
    • Related Report
      2016 Research-status Report
  • [Presentation] Molecular Systems Driving Hydrogen Evolution from Water with Low Overpotential2016

    • Author(s)
      Kosei Yamauchi, Ken Kawano, Keita Koshiba, and Ken Sakai
    • Organizer
      2nd International Symposium on Chemical Energy Conversion Processes (ISCECP-2)
    • Place of Presentation
      I2CNER Hall, Kyushu University, Fukuoka, Japan
    • Year and Date
      2016-05-22
    • Related Report
      2016 Research-status Report
    • Int'l Joint Research
  • [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
      2017 Annual Research Report
  • [Remarks] 九州大学大学院理学研究院化学部門 酒井グループ

    • URL

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

    • Related Report
      2016 Research-status Report

URL: 

Published: 2016-04-21   Modified: 2019-03-29  

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