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Development of Highly Robust Catalytic Systems based on Supramolecular Capsules Encapsulating Metal Complexes

Research Project

Project/Area Number 18H01996
Research Category

Grant-in-Aid for Scientific Research (B)

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

Principal Investigator

Sakai Ken  九州大学, 理学研究院, 教授 (30235105)

Project Period (FY) 2018-04-01 – 2021-03-31
Project Status Completed (Fiscal Year 2021)
Budget Amount *help
¥17,290,000 (Direct Cost: ¥13,300,000、Indirect Cost: ¥3,990,000)
Fiscal Year 2020: ¥5,330,000 (Direct Cost: ¥4,100,000、Indirect Cost: ¥1,230,000)
Fiscal Year 2019: ¥5,330,000 (Direct Cost: ¥4,100,000、Indirect Cost: ¥1,230,000)
Fiscal Year 2018: ¥6,630,000 (Direct Cost: ¥5,100,000、Indirect Cost: ¥1,530,000)
Keywords人工光合成 / 分子性触媒 / 超分子 / 二酸化炭素還元 / 酸素発生 / POM / 水素発生 / 白金錯体 / CO2還元 / 水素生成反応 / 金属錯体
Outline of Final Research Achievements

In this study, we aimed to construct durable molecular systems for artificial photosynthetic reactions. As one of the approaches to improve the stability, the encapsulation behaviors of molecular catalysts in supramolecular capsules were evaluated in detail. Furthermore, we succeeded in developing highly active CO2 reduction molecular catalysts which exhibit excellent selectivity even in aqueous media, where hydrogen evolution is favored. The catalyst was found to drive multi-electron reduction processes over the ligand geometry by maintaining the Co(II) oxidation state. Importantly, the Co(II) center promotes the activation of CO2 due to its phase matching character, while the activation of H+ is suppressed because of its phase mismatch. In addition, highly active molecular catalysts for O2 evolution and H2 evolution were also developed.

Academic Significance and Societal Importance of the Research Achievements

生命現象は高度に組織化された生体高分子やタンパク質などが巧みに組み合わさり、様々な化学的現象によって成り立っている。依然人類が太刀打ちできないほど高精度の物質変換過程が高効率に促進されている。植物の行う窒素固定や炭素固定はその代表例と言え、その全てがいわゆる分子性の反応場によって構成されている。本研究では、人工的に開発した金属錯体が人工光合成反応過程を高効率に触媒することを明らかにした。また、その優れた触媒特性の活性制御因子を明らかにした。さらに、より高耐久な反応系の構築に対する設計指針を得ることにも成功した。

Report

(4 results)
  • 2021 Final Research Report ( PDF )
  • 2020 Annual Research Report
  • 2019 Annual Research Report
  • 2018 Annual Research Report
  • Research Products

    (60 results)

All 2021 2020 2019 2018 Other

All Int'l Joint Research (10 results) Journal Article (17 results) (of which Int'l Joint Research: 7 results,  Peer Reviewed: 17 results) Presentation (30 results) (of which Int'l Joint Research: 18 results,  Invited: 15 results) Book (1 results) Remarks (2 results)

  • [Int'l Joint Research] University of Messina(イタリア)

    • Related Report
      2020 Annual Research Report
  • [Int'l Joint Research] College de France(フランス)

    • Related Report
      2020 Annual Research Report
  • [Int'l Joint Research] 天津理工大学/Chinese Academy of Sciences/中山大学(中国)

    • Related Report
      2019 Annual Research Report
  • [Int'l Joint Research] North Dakota State University(米国)

    • Related Report
      2019 Annual Research Report
  • [Int'l Joint Research] University of Messina(イタリア)

    • Related Report
      2019 Annual Research Report
  • [Int'l Joint Research] University of Victoria(カナダ)

    • Related Report
      2018 Annual Research Report
  • [Int'l Joint Research] North Dakota State University(米国)

    • Related Report
      2018 Annual Research Report
  • [Int'l Joint Research] University of Cambridge(英国)

    • Related Report
      2018 Annual Research Report
  • [Int'l Joint Research] University of Messina/University of Bologna(イタリア)

    • Related Report
      2018 Annual Research Report
  • [Int'l Joint Research] 天津工科大学(中国)

    • Related Report
      2018 Annual Research Report
  • [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 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [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 Annual Research Report
    • Peer Reviewed
  • [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
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Earth-Abundant Photocatalytic CO2 Reduction by Multielectron Chargeable Cobalt Porphyrin Catalysts: High CO/H2 Selectivity in Water Based on Phase Mismatch in Frontier MO Association2021

    • Author(s)
      Zhang Xian、Yamauchi Kosei、Sakai Ken
    • Journal Title

      ACS Catalysis

      Volume: 11 Issue: 16 Pages: 10436-10449

    • DOI

      10.1021/acscatal.1c02475

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [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
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] A Molecular-Based Water Electrolyzer Consisting of Two Mesoporous TiO2 Electrodes Modified with Metalloporphyrin Molecular Catalysts Showing a Quantitative Faradaic Efficiency2020

    • Author(s)
      Akamine Katsuhiro、Morita Kohei、Sakai Ken、Ozawa Hironobu
    • Journal Title

      ACS Applied Energy Materials

      Volume: 3 Issue: 5 Pages: 4860-4866

    • DOI

      10.1021/acsaem.0c00443

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [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 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] Room-Temperature Benzylic Alkylation of Benzylic Carbonates: Improvement of Palladium Catalyst and Mechanistic Study2019

    • Author(s)
      Kuwano Ryoichi、Yokogi Masashi、Sakai Ken、Masaoka Shigeyuki、Miura Takashi、Won Sungyong
    • Journal Title

      Organic Process Research & Development

      Volume: 23 Issue: 8 Pages: 1568-1579

    • DOI

      10.1021/acs.oprd.9b00210

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [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 Annual Research 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 Annual Research 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 Annual Research 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 Annual Research Report
    • Peer Reviewed
  • [Journal Article] A New Class of Molecular-Based Photoelectrochemical Cell for Solar Hydrogen Production Consisting of Two Mesoporous TiO2 Electrodes2019

    • Author(s)
      Morita Kohei, Sakai Ken, and Ozawa Hironobu
    • Journal Title

      ACS Applied Energy Materials

      Volume: 2 Issue: 2 Pages: 987-992

    • DOI

      10.1021/acsaem.8b01992

    • Related Report
      2018 Annual Research 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 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Photocatalytic H2 Evolution Using a Ru Chromophore Tethered to Six Viologen Acceptors2018

    • Author(s)
      Yamamoto Keiya, Call Arnau, and Sakai Ken
    • Journal Title

      Chemistry - A European Journal

      Volume: 24 Issue: 62 Pages: 16620-16629

    • DOI

      10.1002/chem.201803662

    • Related Report
      2018 Annual Research 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 Annual Research Report
    • Peer Reviewed
  • [Presentation] Mechanistic Studies on the Photocatalytic CO2 Reduction Promoted by Diazapyridinophane Metal Complexes2020

    • Author(s)
      Yuto Sakaguchi, Arnau Call, Kosei Yamauchi, Ken Sakai
    • Organizer
      錯体化学会第70回討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Molecular Catalysis Relevant to Solar Energy Conversion and Storage2019

    • Author(s)
      Ken Sakai
    • Organizer
      The 23rd International Symposium on the Photochemistry and Photophysics of Coordination Compounds (ISPPCC2019)
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] An Earth-abundant System for the Photocatalytic CO2 Reduction to CO Using an Iron Complex Based on the Pyridinophane Ligand2019

    • Author(s)
      Yuto Sakaguchi, Arnau Call, Mihaela Cibin, Kosei Yamauchi, Ken Sakai
    • Organizer
      The 23rd International Symposium on the Photochemistry and Photophysics of Coordination Compounds (ISPPCC2019)
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 酸化還元活性な配位子Nindigoを配位させた水溶性白金錯体による光水素触媒反応2019

    • Author(s)
      八束孝一, 山内幸正, Robin G. Hicks, 酒井健
    • Organizer
      錯体化学若手の会夏の学校2019
    • Related Report
      2019 Annual Research Report
  • [Presentation] ジアザピリジノファン錯体を触媒とした光化学的CO2還元反応系の開発2019

    • Author(s)
      坂口雄人, Arnau Call, Mihaela Cibian, 山内幸正, 酒井健
    • Organizer
      錯体化学若手の会夏の学校2019
    • Related Report
      2019 Annual Research Report
  • [Presentation] 電子・プロトン受容能を有するNindigo誘導体を配位子として用いた白金錯体触媒による光水素生成反応2019

    • Author(s)
      八束孝一, 山内幸正, Robin G. Hicks, 酒井健
    • Organizer
      第31回配位化合物の光化学討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] ジアザピリジノファン錯体を用いた光化学的CO2還元触媒反応とその機構的研究2019

    • Author(s)
      坂口雄人, Arnau Call, Mihaela Cibian, 山内幸正, 酒井健
    • Organizer
      第31回配位化合物の光化学討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Molecular Catalysis Towards Artificial Solar Generation of Fuels2019

    • Author(s)
      Ken Sakai
    • Organizer
      19th International Conference on Biological Inorganic Chemistry (ICBIC-19)
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Molecular Photocatalysis Towards Solar Water Splitting and CO2 Reduction2019

    • Author(s)
      Ken Sakai
    • Organizer
      2019 ESP-IUPB World Congress
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] ジアザピリジノファン錯体を触媒とした光化学的CO2還元反応の機構的研究2019

    • Author(s)
      坂口雄人, Arnau Call, Mihaela Cibian, 山内幸正, 酒井健
    • Organizer
      錯体化学会第69回討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] 分子内白金間相互作用による触媒活性向上を目指した新規白金二核錯体の合成と水素生成触媒機能2019

    • Author(s)
      山川和馬, 脇山史彬, 山内幸正, 酒井健
    • Organizer
      錯体化学会第69回討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Mechanistic insights into water oxidation catalysis by a mononuclear polypyridyl ruthenium complex2019

    • Author(s)
      Yutaro Aimoto, Alexander Parent, Kosei Yamauchi, Ken Sakai
    • Organizer
      錯体化学会第69回討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Molecular Catalysis for Water Splitting and CO2 Reduction2019

    • Author(s)
      Ken Sakai
    • Organizer
      7th Asian Conference on Coordination Chemistry (ACCC7)
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Molecular Catalysis and Photocatalysis for Water Splitting and CO2 Reduction2019

    • Author(s)
      Ken Sakai
    • Organizer
      12th China-Japan Joint Symposium on metal Cluster Compounds (CJJSMCC2019)
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Molecular Catalysis and Photocatalysis for Water Splitting and CO2 Reduction2019

    • Author(s)
      Ken Sakai
    • Organizer
      International Conference on Artificial Photosynthesis-2019 (ICARP2019)
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Molecular Catalysts and Photocatalysts for Water Splitting Reactions and their Applications in Surface Modified TiO2 Electrodes2018

    • Author(s)
      Ken Sakai
    • Organizer
      I2CNER-UGo, IRTG Proposal Workshop
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Hybrid Molecular Catalysts and Photocatalysts for Solar Water Splitting Reactions2018

    • Author(s)
      Ken Sakai
    • Organizer
      3rd Japan - UK Joint Symposium on Coordination Chemistry
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Catalytic Hydrogen Evolution Reactions Coupled with Proton-Coupled Electron Transfer Processes2018

    • Author(s)
      Ken Sakai
    • Organizer
      3rd International Conference on Proton Coupled Electron Transfer (PCET2018)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Water Oxidation and CO2 Reduction Catalyzed by Co-, Cu- and Ru-Centered Catalysts including Cobalt Porphyrins2018

    • Author(s)
      Ken Sakai
    • Organizer
      Tenth International Conference on Porphyrins and Phthalocyanines(ICPP-10)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Coordination Chemistry focused on Photochemical Water Splitting Molecular Devices2018

    • Author(s)
      Ken Sakai
    • Organizer
      43rd International Conference on Coordination Chemistry(ICCC2018)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Catalysis of metals and metal complexes2018

    • Author(s)
      Ken Sakai
    • Organizer
      Summer Shool 2018 on Young Coordination Chemist's Association Japan
    • Related Report
      2018 Annual Research Report
    • Invited
  • [Presentation] Solar Energy Conversion and Storage using Transition Metal Molecular Systems2018

    • Author(s)
      Ken Sakai
    • Organizer
      CSOM Workshop
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Molecular Catalysts and Photocatalysts towards Artificial Photosynthesis2018

    • Author(s)
      Ken Sakai
    • Organizer
      Department Seminar at School of Science, The University of Tokyo
    • Related Report
      2018 Annual Research Report
    • Invited
  • [Presentation] Molecular Catalysts and Photocatalysts for Solar Energy Conversion and Storage2018

    • Author(s)
      Ken Sakai
    • Organizer
      2nd Kyushu-Mainz Joint Chemistry Symposium
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Syntheses and Catalytic Water Oxidation Activities of Trinuclear Ruthenium Clusters2018

    • Author(s)
      Kosuke Sakota, Yuta Tsubonouchi, Kosei Yamauchi, and Ken Sakai
    • Organizer
      43rd International Conference on Coordination Chemistry(ICCC2018)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Catalytic of Dizapyridinophane First-row Metal Complexes for CO2 Reduction2018

    • Author(s)
      Yuto Sakaguchi, Arnau Call, Mihaela Cibian, and Ken Sakai
    • Organizer
      43rd International Conference on Coordination Chemistry(ICCC2018)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Catalytic Activity of Some Water-soluble Metal Porphyrins for CO2 Reduction in Aqueous Media2018

    • Author(s)
      Xinyi Cheng,Keiya Yamamoto, Mihaela Cibian, Arnau Call, and Ken Sakai
    • Organizer
      43rd International Conference on Coordination Chemistry(ICCC2018)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Toward Metal Complexes with Phosphine Donors as Photosensitizers for Photocatalysis in Aqueous Media2018

    • Author(s)
      Xian Zhang, Mihaela Cibian, Arnau Call, and Ken Sakai
    • Organizer
      43rd International Conference on Coordination Chemistry(ICCC2018)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] ジアザピリジノファン配位子を有する第一遷移金属錯体を用いた光化学的CO2還元触媒反応2018

    • Author(s)
      Yuto Sakaguchi, Arnau Call, Mihaela Cibian, and Ken Sakai
    • Organizer
      錯体化学若手の会夏の学校2018
    • Related Report
      2018 Annual Research Report
  • [Presentation] 近赤外光により水素生成を駆動する新規ルテニウム三核光増感錯体2018

    • Author(s)
      Yutaro Tsuji, Kosei Yamauchi, and Ken Sakai
    • Organizer
      錯体化学若手の会夏の学校2018
    • Related Report
      2018 Annual Research Report
  • [Book] CSJカレントレビュー38 光エネルギー変換における分子触媒の新展開―天然光合成を凌駕する反応系の構築を目指して2020

    • Author(s)
      森田浩平、小澤弘宣、酒井健 日本化学会編
    • Total Pages
      224
    • Publisher
      化学同人
    • ISBN
      9784759813982
    • Related Report
      2020 Annual Research 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 酒井・小澤グループ

    • URL

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

    • Related Report
      2020 Annual Research Report 2019 Annual Research 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/index.html

    • Related Report
      2018 Annual Research Report

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

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