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Devlopment of Molecular Catalysts Promoting Consecutive Reductions of Carbon Dioxide with High Selectivity

Research Project

Project/Area Number 21K05100
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) 2021-04-01 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000)
Fiscal Year 2023: ¥1,430,000 (Direct Cost: ¥1,100,000、Indirect Cost: ¥330,000)
Fiscal Year 2022: ¥1,300,000 (Direct Cost: ¥1,000,000、Indirect Cost: ¥300,000)
Fiscal Year 2021: ¥1,430,000 (Direct Cost: ¥1,100,000、Indirect Cost: ¥330,000)
Keywords二酸化酸素還元 / 人工光合成 / エネルギー変換 / N-ヘテロ環状カルベン(NHC) / 水素発生 / 電気化学 / 光化学 / メタン / 二酸化炭素還元 / コバルト錯体触媒 / NHC配位子 / メタン生成 / 光電子移動 / メタノール / 錯体触媒
Outline of Research at the Start

二酸化炭素(CO2)の逐次多電子還元反応を高選択的に駆動する金属錯体触媒の創出と反応制御を目的として推進する。
光/電気化学的なCO2多電子還元系を構築する上で、CO2の2電子還元により生成するCO(一酸化炭素)の活性化をいかに制御するかが鍵を握る。そのため、COを捕捉する錯体触媒の探索と逐次多電子還元過程への応用に注力する。
また、実験と理論の協奏に基づく多角的な反応機構解析により、逐次多電子還元の制御因子を解明し更なる高活性触媒の創製に挑戦する。

Outline of Final Research Achievements

In this study, photochemical and electrochemical carbon dioxide (CO2) reduction catalyzed by various Co-NHC complexes was investigated in detail. In the photochemical system, the main product is CO, the two-electron reduction product of CO2, and a significant enhancement of catalytic properties in the presence of acid source was observed. In the electrochemical system, methane (CH4) was found to be produced in small amounts during the controlled potential electrolysis of the catalyst solution. This result suggests that the CO captured over the metal center was activated and led to the subsequent consecutive multi-electron reduction process.

Academic Significance and Societal Importance of the Research Achievements

持続可能な社会の実現を目指し、地球温暖化の主要因である二酸化炭素(CO2)の有用化合物への変換反応に関する研究が盛んに行われている。COやギ酸などのCO2の2電子還元生成物を与える分子性触媒反応系の報告は多数あるが、エネルギーキャリアとして真に有用であるメタノール(6電子還元生成物)やメタン(8電子還元生成物)を与える反応系はほとんど無い。本研究では、CO2雰囲気で微量ながらもメタンを生成する分子性触媒系を構築することができ、今後の高選択的なCO2変換系への展開が期待できる。

Report

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

    (33 results)

All 2024 2023 2022 2021 Other

All Int'l Joint Research (2 results) Journal Article (9 results) (of which Int'l Joint Research: 5 results,  Peer Reviewed: 9 results,  Open Access: 2 results) Presentation (19 results) (of which Int'l Joint Research: 2 results,  Invited: 4 results) Remarks (3 results)

  • [Int'l Joint Research] North Dakota State University(米国)

    • Related Report
      2023 Annual Research Report
  • [Int'l Joint Research] University of Gottingen(ドイツ)

    • Related Report
      2022 Research-status Report
  • [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] 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 Research-status 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 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [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 Research-status 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
      2021 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [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 Research-status 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
      2021 Research-status 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 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Presentation] Co-NHC Catalysts Promoting Hydrogen Evolution from Water with High Turnover Number and Frequency2024

    • Author(s)
      Kosei Yamauchi
    • Organizer
      Asian International Symposium - Coordination Chemistry, Organo-metallic Chemistry -, The 104th CSJ Annual Meeting
    • Related Report
      2023 Annual Research Report
    • Invited
  • [Presentation] 塩基性条件下での分子性酸素発生触媒反応に関する研究2024

    • Author(s)
      澁谷篤紀・山内幸正・酒井 健
    • Organizer
      日本化学会第104春季年会
    • Related Report
      2023 Annual Research Report
  • [Presentation] Co-NHC錯体におけるアミン配位部位の構造がアルカリ水素生成触媒特性に与える影響2023

    • Author(s)
      諏訪靖拓・山内幸正・酒井 健
    • Organizer
      錯体化学会第73回討論会
    • Related Report
      2023 Annual Research Report
  • [Presentation] Photocatalytic CO2 Reduction to Formate Promoted by Pentamethylcyclopentadienyl Rhodium Catalysts2023

    • Author(s)
      Dongseb LEE , Yuto SAKAGUCHI, Kosei YAMAUCHI , Ken SAKAI
    • Organizer
      日本化学会第103春季年会
    • Related Report
      2022 Research-status Report
  • [Presentation] 新規Co-NHC錯体の合成と光水素生成触媒機能2023

    • Author(s)
      河村佳央理・山内幸正・酒井 健
    • Organizer
      日本化学会第103春季年会
    • Related Report
      2022 Research-status Report
  • [Presentation] ピリジン誘導体の添加に基づくCo-NHC錯体の水素生成触媒特性制御2023

    • Author(s)
      諏訪靖拓・管 昌権・山内幸正・酒井 健
    • Organizer
      日本化学会第103春季年会
    • Related Report
      2022 Research-status Report
  • [Presentation] N-2-ピリジルイミドイル-2-ピリジルアミジンを有する金属錯体の合成と水素発生触媒機能2023

    • Author(s)
      國久保透真・Jaclyn Brusso・山内幸正・酒井 健
    • Organizer
      日本化学会第103春季年会
    • Related Report
      2022 Research-status Report
  • [Presentation] Photochemical and electrochemical CO2 reduction promoted by cobalt-based molecular catalysts2022

    • Author(s)
      Kosei Yamauchi
    • Organizer
      The 11th Singapore International Chemistry Conference (SICC-11)
    • Related Report
      2022 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Photochemical and Electrochemical Hydrogen Evolution from Water Catalyzed by Co-NHC Complexes2022

    • Author(s)
      Kosei Yamauchi
    • Organizer
      S3: New directions in the use of light and coordination compounds for CO2 reduction, The JSCC 72nd Annual Symposium
    • Related Report
      2022 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Photocatalysis of CO2 reduction by diazapyridinophane complexes of Fe, Co, and Ni2022

    • Author(s)
      Yuto Sakaguchi, Kosei Yamauchi, Ken Sakai
    • Organizer
      The 8th Asian Conference on Coordination Chemistry (ACCC8)
    • Related Report
      2022 Research-status Report
  • [Presentation] Co-NHC錯体を触媒とする光化学的二酸化炭素還元反応2022

    • Author(s)
      前田晃志・山内幸正・酒井 健
    • Organizer
      錯体化学会第72回討論会
    • Related Report
      2022 Research-status Report
  • [Presentation] ピリジン誘導体添加系におけるCo-NHC錯体の水素生成触媒特性2022

    • Author(s)
      諏訪靖拓・管 昌権・山内幸正・酒井 健
    • Organizer
      錯体化学会第72回討論会
    • Related Report
      2022 Research-status Report
  • [Presentation] Photochemical Hydrogen Evolution from Alkaline Water Catalyzed by Co-NHC Complexes2022

    • Author(s)
      Kosei Yamauchi, Yasunobu Wakafuji, Ken Sakai
    • Organizer
      日本化学会第102春季年会
    • Related Report
      2021 Research-status Report
  • [Presentation] 均一系電気化学反応解析で解き明かす金属錯体触媒の化学2021

    • Author(s)
      山内幸正
    • 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 Research-status Report
    • Invited
  • [Presentation] Co-NHC錯体を触媒とする水からの水素生成反応に関する電気化学的研究2021

    • Author(s)
      管 昌権、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 Research-status Report
  • [Presentation] 強アルカリ水からの光化学的な水素生成を駆動する分子性触媒系の開発2021

    • Author(s)
      若藤恭暢、山内幸正、酒井 健
    • Organizer
      第32回配位化合物の光化学討論会
    • Related Report
      2021 Research-status Report
  • [Presentation] Co-NHC錯体を触媒とする水からの水素生成反応に関する電気化学的研究2021

    • Author(s)
      管 昌権、山内幸正、酒井 健
    • Organizer
      錯体化学会第71回討論会
    • Related Report
      2021 Research-status Report
  • [Presentation] 強アルカリ性条件下で高い活性を示すCo-NHCの光水素生成触媒機能2021

    • Author(s)
      若藤恭暢、山内幸正、酒井 健
    • Organizer
      錯体化学会第71回討論会
    • Related Report
      2021 Research-status Report
  • [Presentation] Co-NHCを触媒とする強アルカリ水からの光水素生成反応2021

    • Author(s)
      山内幸正、若藤恭暢、酒井 健
    • Organizer
      第2回複合系の光機能研究会オンラインライジングスター研究会 (ORK2)
    • Related Report
      2021 Research-status Report
  • [Remarks] 山内幸正(九州大学錯体化学研空室)

    • URL

      http://www.scc.kyushu-u.ac.jp/Sakutai/jp/pages/members/yamauchi_kosei.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/pages/members/yamauchi_kosei.html

    • Related Report
      2022 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 Research-status Report

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

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