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Development of Molecular Devices for Solar Fuels Generation based on Carbon Nitride Composites

Research Project

Project/Area Number 21H01952
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)

Co-Investigator(Kenkyū-buntansha) 山内 幸正  九州大学, 理学研究院, 助教 (50631769)
Project Period (FY) 2021-04-01 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥17,420,000 (Direct Cost: ¥13,400,000、Indirect Cost: ¥4,020,000)
Fiscal Year 2023: ¥5,590,000 (Direct Cost: ¥4,300,000、Indirect Cost: ¥1,290,000)
Fiscal Year 2022: ¥5,590,000 (Direct Cost: ¥4,300,000、Indirect Cost: ¥1,290,000)
Fiscal Year 2021: ¥6,240,000 (Direct Cost: ¥4,800,000、Indirect Cost: ¥1,440,000)
Keywords人工光合成 / カーボンナイトライド / ポリオキソメタレート / 酸素発生反応 / 二酸化炭素還元反応 / 光触媒 / 反応機構解析 / DFT計算 / 水素発生 / 二酸化炭素還元 / 酸素発生 / 錯体触媒 / 水素生成 / 酸素生成 / 反応機構 / 光エネルギー変換 / 分子デバイス
Outline of Research at the Start

本課題では、カーボンナイトライド(C3N4)を光増感触媒とする人工光合成デバイスの開発を推進する。申請者は、最近の研究により優れた触媒特性を示す酸素発生触媒、並びにCO2還元触媒を見出し、それら触媒反応の詳細な機構的研究を展開してきた。そこで本研究では、これら分子性触媒を酸化側と還元側の両触媒に適用したカーボンナイトライド基盤の光酸素発生デバイスおよびCO2光還元デバイスをそれぞれ構築し、最終的にはそれらを融合させた光炭酸ガス還元デバイスの開発、機能評価、並びに優れたデバイス設計指針の探求と確立を試みる。

Outline of Final Research Achievements

We have developed molecular catalysts of oxygen evolution and CO2 reduction reactions under low overpotential conditions. In addition, we elucidated the reaction mechanisms in detail with the aim of realizing artificial photosynthetic systems. Next, these molecular catalysts were physisorbed over carbon nitride (C3N4), a metal-free semiconductor photocatalyst responsive to visible light. It was succeeded to construct and demonstrate hybrid photocatalysts which can drive these reactions with high efficiency in the presence of sacrificial reagents.

Academic Significance and Societal Importance of the Research Achievements

炭素と窒素から構成される有機半導体カーボンナイトライド(C3N4)は、可視光を吸収し水の酸化および二酸化炭素(CO2)還元の両反応を駆動可能なバンド構造を有する。本研究では、高活性な分子性酸素発生触媒(WOC)を開発し、C3N4光触媒への修飾を行った。光触媒性能試験の結果、犠牲試薬存在下で、分子性WOC修飾C3N4光触媒の中で最も高い触媒回転数/頻度が示された。CO2還元触媒修飾C3N4光触媒の構築にも成功し、水を電子源とする人工光合成系実現への道筋をつけた。

Report

(4 results)
  • 2023 Annual Research Report   Final Research Report ( PDF )
  • 2022 Annual Research Report
  • 2021 Annual Research Report
  • Research Products

    (57 results)

All 2024 2023 2022 2021 Other

All Int'l Joint Research (8 results) Journal Article (12 results) (of which Int'l Joint Research: 5 results,  Peer Reviewed: 11 results,  Open Access: 3 results) Presentation (34 results) (of which Int'l Joint Research: 9 results,  Invited: 7 results) Remarks (3 results)

  • [Int'l Joint Research] Sun Yat-sen University(中国)

    • Related Report
      2023 Annual Research Report
  • [Int'l Joint Research] ICMM-CSIC(スペイン)

    • Related Report
      2023 Annual Research Report
  • [Int'l Joint Research] University of Ottawa(カナダ)

    • Related Report
      2023 Annual Research Report
  • [Int'l Joint Research] Tianjin University of Technology(中国)

    • Related Report
      2022 Annual Research Report
  • [Int'l Joint Research] Georg-August-Universitat Gottingen(ドイツ)

    • Related Report
      2022 Annual Research Report
  • [Int'l Joint Research] ICIQ(スペイン)

    • Related Report
      2022 Annual Research Report
  • [Int'l Joint Research] Tianjin University of Technology(中国)

    • Related Report
      2021 Annual Research Report
  • [Int'l Joint Research] Georg-August-Universitat Gottingen(ドイツ)

    • Related Report
      2021 Annual Research Report
  • [Journal Article] Efficient Visible-Light-Driven Water Oxidation by a Carbon Nitride Modified with Cobalt Polyoxometalate Molecular Catalyst2024

    • Author(s)
      Tomita Yuki、Taira Natsuki、Sakai Ken、Ozawa Hironobu
    • Journal Title

      ACS Catalysis

      Volume: 14 Issue: 8 Pages: 5788-5794

    • DOI

      10.1021/acscatal.4c00627

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Synthesis of the MN Ring of Caribbean Ciguatoxin C-CTX-1 via Desymmetrization by Acetal Formation2024

    • Author(s)
      Kaneko Masahiro、Yamashita Atsuhiro、Yasuno Yoko、Yamauchi Kosei、Sakai Ken、Oishi Tohru
    • Journal Title

      Organic Letters

      Volume: 26 Issue: 4 Pages: 855-859

    • DOI

      10.1021/acs.orglett.3c04013

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Precious-Metal-Free CO2 Photoreduction Boosted by Dynamic Coordinative Interaction between Pyridine-Tethered Cu(I) Sensitizers and a Co(II) Catalyst2023

    • Author(s)
      Wang Jia-Wei、Zhang Xian、Velasco Lucia、Karnahl Michael、Li Zizi、Luo Zhi-Mei、Huang Yanjun、Yu Jin、Hu Wenhui、Zhang Xiaoyi、Yamauchi Kosei、Sakai Ken、Moonshiram Dooshaye、Ouyang Gangfeng
    • Journal Title

      JACS Au

      Volume: 3 Issue: 7 Pages: 1984-1997

    • DOI

      10.1021/jacsau.3c00218

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Highly Efficient and Stable Molecular-Based TiO2 Photoanodes for Photoelectrochemical Water Splitting Achieved by Pyridyl Anchoring Technique2023

    • Author(s)
      Yan Xin、Sakai Ken、Ozawa Hironobu
    • Journal Title

      ACS Catalysis

      Volume: 13 Issue: 20 Pages: 13456-13465

    • DOI

      10.1021/acscatal.3c03136

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Theoretical study on the mechanism of the hydrogen evolution reaction catalyzed by platinum subnanoclusters2023

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

      Dalton Transactions

      Volume: 52 Issue: 3 Pages: 583-597

    • DOI

      10.1039/d2dt02645g

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Controlling the Photofunctionality of a Polyanionic Heteroleptic Copper(I) Photosensitizer for CO2 Reduction Using Its Ion‐pair Formation with Polycationic Ammonium in Aqueous Media2023

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

      Angewandte Chemie International Edition

      Volume: 62 Issue: 9

    • DOI

      10.1002/anie.202217807

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Efficient syngas production with controllable CO:H2 ratios based on aqueous electrocatalytic CO2 reduction over mesoporous TiO2 films modified with a cobalt porphyrin molecular catalyst2023

    • Author(s)
      Ozawa Hironobu、Kikunaga Ryoma、Suzuki Hajime、Abe Ryu、Sakai Ken
    • Journal Title

      Sustainable Energy & Fuels

      Volume: 7 Issue: 7 Pages: 1627-1632

    • DOI

      10.1039/d2se01595a

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Intracluster O-O Coupling Pathway Evidenced for an Anderson-Type Single-Cobalt Polymolybdate Water Oxidation Catalyst2023

    • Author(s)
      Taira Natsuki、Yamauchi Kosei、Sakai Ken
    • Journal Title

      ACS Catalysis

      Volume: 13 Issue: 5 Pages: 3211-3223

    • DOI

      10.1021/acscatal.2c05925

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Visible-light-driven reduction of CO<sub>2</sub> to CO in fully aqueous media using a water-soluble cobalt porphyrin2022

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

      Sustainable Energy & Fuels

      Volume: - Issue: 9 Pages: 2160-2164

    • DOI

      10.1039/d2se00291d

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [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
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Catalysis of CO<sub>2</sub> reduction by diazapyridinophane complexes of Fe, Co, and Ni: CO<sub>2</sub> binding triggered by combined frontier MO associations involving a SOMO2021

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

      Dalton Transactions

      Volume: 50 Issue: 44 Pages: 15983-15995

    • DOI

      10.1039/d1dt01877a

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Two-Electrode Solar Water Splitting Permitting H2 Separation at a Dark Cathode2021

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

      AsiaChem

      Volume: 2 Issue: 1 Pages: 80-87

    • DOI

      10.51167/acm00027

    • Related Report
      2021 Annual Research Report
    • Open Access
  • [Presentation] 水溶性ロジウム錯体の光化学的CO2還元触媒反応2023

    • Author(s)
      Dongseb LEE, Kosei YAMAUCHI1, Ken SAKAI
    • Organizer
      錯体化学若手研究会「錯体化学若手の会夏の学校2023」
    • Related Report
      2023 Annual Research Report
  • [Presentation] 水素生成触媒反応の観察を志向した白金ナノクラスター修飾電極の作製2023

    • Author(s)
      池田達紀, 山内幸正, 小澤弘宜, 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2023」
    • Related Report
      2023 Annual Research Report
  • [Presentation] 高耐久性を示す白金二核錯体型光水素発生分子デバイスの開発2023

    • Author(s)
      國久保 透真・Jaclyn Brusso・Muralee Murugesu・山内幸正・小澤弘宜・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2023」
    • Related Report
      2023 Annual Research Report
  • [Presentation] 水溶性ロジウム錯体の光化学的CO2還元反応2023

    • Author(s)
      Dongseb LEE, Kosei YAMAUCHI, Ken SAKAI
    • Organizer
      第34回配位化合物の光化学討論会
    • Related Report
      2023 Annual Research Report
  • [Presentation] 高い耐久力を備えた白金二核錯体型光水素発生分子デバイスの開発2023

    • Author(s)
      國久保透真・Jaclyn Brusso・Muralee Murugesu・山内幸正・小澤弘宜・酒井 健
    • Organizer
      第34回配位化合物の光化学討論会
    • Related Report
      2023 Annual Research Report
  • [Presentation] 白金ナノクラスター修飾電極の作製及び水素生成触媒反応の観察2023

    • Author(s)
      池田達紀, 山内幸正, 小澤弘宜, 酒井 健
    • Organizer
      錯体化学会第73回討論会
    • Related Report
      2023 Annual Research Report
  • [Presentation] A Novel Platinum-Dimer-Based Photo-Hydrogen Evolving Molecular Device Showing Outstanding Long-Term Stability2023

    • Author(s)
      Toma KUNIKUBO, Jaclyn BRUSSO, Muralee MURUGESU, Kosei YAMAUCHI, Hironobu OZAWA, Ken SAKAI
    • Organizer
      錯体化学会第73回討論会
    • Related Report
      2023 Annual Research Report
  • [Presentation] Highly Efficient Photocatalytic Water Oxidation by Carbon Nitride Photocatalyst Modified with a Cobalt Polymolybdate Molecular Catalyst2023

    • Author(s)
      Yuki TOMITA, Natsuki TAIRA, Ken SAKAI, Hironobu OZAWA
    • Organizer
      錯体化学会第73回討論会
    • Related Report
      2023 Annual Research Report
  • [Presentation] 白金ナノクラスター修飾電極の作製と水素生成触媒特性2023

    • Author(s)
      池田達紀・山内幸正・小澤弘宣・酒井健
    • Organizer
      日本化学会第103春季年会
    • Related Report
      2022 Annual Research Report
  • [Presentation] ポリモリブデン酸コバルト触媒を修飾したカーボンナイトライドの光化学的酸素生成触媒2023

    • Author(s)
      冨田侑樹・多伊良夏樹・小澤弘宜・酒井健
    • Organizer
      日本化学会第103春季年会
    • Related Report
      2022 Annual Research Report
  • [Presentation] イオン会合体形成に基づく水溶性銅錯体の光機能制御2023

    • Author(s)
      末吉史佳・Xian Zhang・山内幸正・酒井健
    • Organizer
      日本化学会第103春季年会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Mechanistic Studies on Water Splitting and CO2 Reduction Towards Solar Fuels Production2022

    • Author(s)
      Ken Sakai
    • Organizer
      The 24th International Symposium on the Photochemistry and Photophysics of Coordination Compounds(ISPPCC)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Photocatalytic Water Splitting and CO2 Reduction2022

    • Author(s)
      Ken Sakai
    • Organizer
      The 8th Asian Conference on Coordination Chemistry (ACCC8)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Controlling the photofunctionality of polyanionic heteroleptic copper(I) photosensitizer using the ionic interactions with polycationic alkylammonium ions in aqueous media2022

    • Author(s)
      Fumika Sueyoshi, Xian Zhang, Kosei Yamauchi, Ken Sakai
    • Organizer
      The 8th Asian Conference on Coordination Chemistry (ACCC8)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Photocatalytic Water Oxidation by Carbon Nitride Modified with Rubda-type Water Oxidation Catalyst2022

    • Author(s)
      Yuki Tomita, Hironobu Ozawa, Ken Sakai
    • Organizer
      The 8th Asian Conference on Coordination Chemistry (ACCC8)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Photoelectrochemical water oxidation by TiO2 photoanode modified with molecular ruthenium photosensitizer and catalyst2022

    • Author(s)
      Xin Yan, Ken Sakai, Hironobu Ozawa
    • Organizer
      The 8th Asian Conference on Coordination Chemistry (ACCC8)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Cobalt Porphyrin Catalysts for Water Oxidation and Fuel Generation2022

    • Author(s)
      Ken Sakai
    • Organizer
      The 44th International Conference on Coordination Chemistry(ICCC2022)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 溶液内イオン会合体形成による燐光発光性銅錯体の光機能制御2022

    • Author(s)
      末吉史佳・ Xian Zhang・山内幸正・酒井健
    • Organizer
      第33回配位化合物の光化学討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Photoelectrochemical Water Oxidation by TiO2 Photoanode Modified with Molecular Ruthenium Photosensitizer and Catalyst2022

    • Author(s)
      ケン キン ・ 酒井 健・小澤 弘宜
    • Organizer
      第33回配位化合物の光化学討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Sustainable Energy Cycles based on Water Splitting and CO2 Reduction2022

    • Author(s)
      Ken Sakai
    • Organizer
      錯体化学会第72回討論会
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] Development of the Naphthyridine-bridged Dinuclear Co Complex for Highly Selective CO2 Reduction Catalysis in the Presence of Proton Source2022

    • Author(s)
      Yuto Sakaguchi, Kosei Yamauchi, Ken Saka
    • Organizer
      錯体化学会第72回討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Luminescence Enhancement of a Copper(I) Diimine-Diphosphine Complex in Water by Hydrophobic Encapsulation2022

    • Author(s)
      Fumika Sueyoshi, Xian Zhang, Kosei Yamauchi, Ken Sakai
    • Organizer
      錯体化学会第72回討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Rubda型分子性酸素生成触媒を修飾したカーボンナイトライド光触媒の機能評価2022

    • Author(s)
      Yuki Tomita, Hironobu Ozawa, Ken Sakai
    • Organizer
      錯体化学会第72回討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Coポルフィリン修飾TiO2電極を用いたCO2還元反応による合成ガス生成2022

    • Author(s)
      合屋 祐輝・菊永 竜馬・酒井 健・小澤弘宜
    • Organizer
      錯体化学会第72回討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Photoelectrochemical Water Oxidation by a Molecular-based TiO2 Photoanode Modified with Ruthenium Photosensitizer and Catalys2022

    • Author(s)
      Xin Yan, Ken Sakai, Hironobu Ozawa
    • Organizer
      錯体化学会第72回討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Photocatalytic CO2 Reduction to Formate Promoted by the Pentamethylcyclopentadienyl Rhodium Catalyst2022

    • Author(s)
      Dongseb LEE , Kosei YAMAUCHI , Ken SAKAI
    • Organizer
      錯体化学会第72回討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Znポルフィリン修飾TiO2電極をフォトアノードとして用いた太陽光水素生成2022

    • Author(s)
      中島直人・酒井健・小澤弘宜
    • Organizer
      錯体化学会第72回討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Advanced Aspects on the Mechanisms of Catalytic Water Splitting and CO2 Reduction2022

    • Author(s)
      Ken Sakai
    • Organizer
      The 11th Singapore International Chemistry Conference (SICC-11
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Advanced Aspects on the Mechanisms of Catalytic Water Splitting and CO2 Reduction2022

    • Author(s)
      Ken Sakai
    • Organizer
      Workshop on Catalytic Approaches for Carbon Capture, Utilization, and Renewable Energy
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] ジアザピリジノファン錯体を用いたCO2還元反応におけるDFT法およびフロンティア軌道論を用いた触媒反応機構解析2021

    • Author(s)
      坂口雄人・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2021」
    • Related Report
      2021 Annual Research Report
  • [Presentation] DFT Study on Hydrogen Evolution Reaction Catalyzed by Platinum Clusters2021

    • Author(s)
      Keita Kuge, Kosei Yamauchi, Ken Sakai
    • Organizer
      錯体化学会第71回討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] CO2 Reduction Catalysis of Naphthyridine-bridged Dinuclear Metal Complexes2021

    • Author(s)
      Yuto Sakaguchi, Kosei Yamauchi, Ken Sakai
    • Organizer
      錯体化学会第71回討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] Co-NHC錯体触媒を用いた光CO2還元反応系における生成物評価 Evaluation of products in photocatalytic CO2 reduction system with Co-NHC complex.2021

    • Author(s)
      前田晃志・山内幸正・酒井健
    • Organizer
      錯体化学会第71回討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] Earth-abundant and environmentally friendly molecular photocatalysts for CO2 reduction in aqueous media2021

    • Author(s)
      Ken Sakai
    • Organizer
      Virtual Global Renewable Energy Researchers Meet
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research / Invited
  • [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
      2023 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/jp/index.html

    • Related Report
      2022 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
      2021 Annual Research Report

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Published: 2021-04-28   Modified: 2025-01-30  

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