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2017 Fiscal Year Annual Research Report

Fine controlf of Multi-Electron Transfer of Ground and Excited States of Metal-Oxygen Complexes

Research Project

Project/Area Number 16H02268
Research InstitutionMeijo University

Principal Investigator

福住 俊一  名城大学, 理工学研究科, 特任教授 (40144430)

Co-Investigator(Kenkyū-buntansha) 山田 裕介  大阪市立大学, 大学院工学研究科, 教授 (30358270)
大久保 敬  大阪大学, 工学(系)研究科(研究院), その他 (00379140)
Project Period (FY) 2016-04-01 – 2021-03-31
Keywords電子移動 / 光合成 / 水の酸化 / 金属酸素錯体 / 光励起状態
Outline of Annual Research Achievements

電子移動過程は光合成、呼吸プロセスなどのエネルギー変換において非常に重要な役割を果たしている。光合成は水を4電子酸化することで酸素を生成して4電子と4プロトンを得る過程であり、呼吸は逆に酸素を4電子還元して水に戻すことによりエネルギーを獲得する過程である。水と酸素との間の4電子・4プロトンの相互変換の間には、様々な金属酸素錯体が活性種として関与している。しかし、金属酸素錯体の電子移動特性、特に多電子移動過程については、エネルギー変換において最も基本的かつ重要なものであるにもかかわらず、まだ不明な点が多い。本基盤研究では、申請者が行って来た金属イオン共役電子移動研究の成果を基に「基底状態及び励起状態の金属酸素錯体の多電子移動精密制御」を行うことを目的としている。平成29年度では、マンガン(IV)-オキソ錯体によるアントラセンの6電子酸化反応機構を明らかにした。また、酸素の分子の活性化による鉄(IV)-オキソ錯体及びマンガン(V)-オキソコロール錯体の生成機構を解明した。さらにスカンジウムイオンが結合したマンガン(IV)-オキソ錯体を光励起すると長寿命の励起状態が得られることを見出し、その電子移動特性を明らかにした。

Current Status of Research Progress
Current Status of Research Progress

1: Research has progressed more than it was originally planned.

Reason

本研究課題では「基底状態及び励起状態の金属酸素錯体の多電子移動精密制御」を行うことを目的としている。基底状態の金属酸素錯体の多電子移動精密制御については多くの研究成果を得た。しかし、これまで金属酸素錯体の励起状態の電子移動過程については全くと言って良いほど未開拓の分野であった。しかし、上述のように平成29年度にはスカンジウムイオンが結合したマンガン(IV)-オキソ錯体を光励起すると長寿命の励起状態が得られることを見出し、その電子移動特性を明らかにすることができた。これを契機として金属オキソ錯体の励起状態について研究が飛躍的に進展することが期待される。平成29年度の査読付き論文の発表数は、J. Am. Chem. Soc., Angew. Chem. Int. Ed., Nature Chemistry などの国際誌に30報となり、論文の引用数も42000回を越している。平成29年度はアメリカ電気化学会のSmalley賞を受賞し、受賞講演を行った。このように本研究成果は国際的に高く評価された。

Strategy for Future Research Activity

本基盤研究では、申請者が行って来た金属イオン共役電子移動研究の成果を基に「基底状態及び励起状態の金属酸素錯体の多電子移動精密制御」を行うことを目的としている。基底状態の金属酸素錯体の多電子移動精密制御についてはこれまで数多くの研究成果をあげてきた。金属酸素錯体の励起状態の電子移動過程についてもブレークスルーとなる研究成果を得たので、今後は励起状態の金属酸素錯体の多電子移動精密制御についても研究をさらに発展させていきたいと考えている。一般に金属酸素錯体は不安定であるので、低温での測定が必要となるが、低温で秒レーザー時間分解分光を測定する装置をフルに活用して金属酸素錯体の励起状態の新しい化学を開拓していく予定である。

  • Research Products

    (35 results)

All 2018 2017 Other

All Int'l Joint Research (1 results) Journal Article (28 results) (of which Int'l Joint Research: 25 results,  Peer Reviewed: 26 results) Presentation (6 results) (of which Int'l Joint Research: 5 results,  Invited: 6 results)

  • [Int'l Joint Research] Wha Womans University(韓国)

    • Country Name
      KOREA (REP. OF KOREA)
    • Counterpart Institution
      Wha Womans University
  • [Journal Article] A supramolecular photocatalyst composed of a polyoxometalate and a photosensitizing water-soluble porphyrin diacid for the oxidation of organic substrates in water2018

    • Author(s)
      Ishizuka, Tomoya; Ohkawa, Shumpei; Ochiai, Hidemi; Hashimoto, Muneaki; Ohkubo, Kei; Kotani, Hiroaki; Sadakane, Masahiro; Fukuzumi, Shunichi; Kojima, Takahiko
    • Journal Title

      Green Chemistry

      Volume: 20 Pages: in press

    • DOI

      10.1039/c8gc00295a

    • Peer Reviewed
  • [Journal Article] Amphoteric reactivity of metal-oxygen complexes in oxidation reactions2018

    • Author(s)
      Sankaralingam, Muniyandi; Lee, Yong-Min; Nam, Wonwoo; Fukuzumi, Shunichi
    • Journal Title

      Coordination Chemistry Reviews

      Volume: 365 Pages: 41-59

    • DOI

      10.1016/j.ccr.2018.03.003

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Assemblies of Boron Dipyrromethene/Porphyrin, Phthalocyanine, and C60 Moieties as Artificial Models of Photosynthesis: Synthesis, Supramolecular Interactions, and Photophysical Studies2018

    • Author(s)
      Chen, Xiao-Fei; El-Khouly, Mohamed E.; Ohkubo, Kei; Fukuzumi, Shunichi; Ng, Dennis K. P.
    • Journal Title

      Chemistry - A European Journal

      Volume: 24 Pages: 3862-3872

    • DOI

      10.1002/chem.201705843

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Immobilization of Molecular Catalysts for Enhanced Redox Catalysis2018

    • Author(s)
      Fukuzumi, Shunichi; Lee, Yong-Min; Nam, Wonwoo
    • Journal Title

      ChemCatChem

      Volume: 10 Pages: 1687-1702

    • DOI

      10.1002/cctc.201701786

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Solar-Driven Production of Hydrogen Peroxide from Water and Dioxygen2018

    • Author(s)
      Fukuzumi, Shunichi; Lee, Yong-Min; Nam, Wonwoo
    • Journal Title

      Chemistry - A European Journal

      Volume: 24 Pages: 5016-5031

    • DOI

      10.1002/chem.201704512

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] A Triphenylamine-Naphthalenediimide-Fullerene Triad: Synthesis, Photoinduced Charge Separation and Solution-Processable Bulk Heterojunction Solar Cells2018

    • Author(s)
      Srivani, Doli; Gupta, Akhil; Bhosale, Sidhanath V.; Ohkubo, Kei; Bhosale, Rajesh S.; Fukuzumi, Shunichi; Bilic, Ante; Jones, Lathe A.; Bhosale, Sheshanath V.
    • Journal Title

      Asian Journal of Organic Chemistry

      Volume: 7 Pages: in press

    • DOI

      10.1002/ajoc.201700689

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Artificial Photosynthesis for Production of ATP, NAD(P)H, and Hydrogen Peroxide2018

    • Author(s)
      Fukuzumi, Shunichi; Lee, Yong-Min; Nam, Wonwoo
    • Journal Title

      ChemPhotoChem

      Volume: 2 Pages: 121-135

    • DOI

      10.1002/cptc.201700146

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Mechanisms of Two-Electron versus Four-Electron Reduction of Dioxygen Catalyzed by Earth-Abundant Metal Complexes2018

    • Author(s)
      Fukuzumi, Shunichi; Lee, Yong-Min; Nam, Wonwoo
    • Journal Title

      ChemCatChem

      Volume: 10 Pages: 9-28

    • DOI

      10.1002/cctc.201701064

  • [Journal Article] Inter- and Intramolecular Electron-Transfer Reduction Properties of Coronenediimide Derivatives via Photoinduced Processes2018

    • Author(s)
      Yoshida, Motoki; Sakai, Hayato; Ohkubo, Kei; Fukuzumi, Shunichi; Hasobe, Taku
    • Journal Title

      Journal of Physical Chemistry C

      Volume: 122 Pages: in press

    • DOI

      10.1021/acs.jpcc.7b09817

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Thermal and photocatalytic production of hydrogen with earth-abundant metal complexes2018

    • Author(s)
      Fukuzumi, Shunichi; Lee, Yong-Min; Nam, Wonwoo
    • Journal Title

      Coordination Chemistry Reviews

      Volume: 355 Pages: 54-73

    • DOI

      10.1016/j.ccr.2017.07.014

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Fuel Production from Seawater and Fuel Cells Using Seawater2017

    • Author(s)
      Fukuzumi, Shunichi; Lee, Yong-Min; Nam, Wonwoo
    • Journal Title

      ChemSusChem

      Volume: 10 Pages: 4264-4276

    • DOI

      10.1002/cssc.201701381

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Dioxygen Activation and O-O Bond Formation Reactions by Manganese Corroles2017

    • Author(s)
      Guo, Mian; Lee, Yong-Min; Gupta, Ranjana; Seo, Mi Sook; Ohta, Takehiro; Wang, Hua-Hua; Liu, Hai-Yang; Dhuri, Sunder N.; Sarangi, Ritimukta; Fukuzumi, Shunichi; Nam, Wonwoo
    • Journal Title

      Journal of the American Chemical Society

      Volume: 139 Pages: 15858-15867

    • DOI

      10.1021/jacs.7b08678

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Photocatalytic oxidation of benzene to phenol using dioxygen as an oxygen source and water as an electron source in the presence of a cobalt catalyst2017

    • Author(s)
      Han, Ji Won; Jung, Jieun; Lee, Yong-Min; Nam, Wonwoo; Fukuzumi, Shunich
    • Journal Title

      Chemical Science

      Volume: 8 Pages: 7119-7125

    • DOI

      10.1039/C7SC02495A

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Ionic manipulation of charge-transfer and photodynamics of [60]fullerene confined in pyrrolo-tetrathiafulvalene cage2017

    • Author(s)
      Bahring, Steffen; Larsen, Karina R.; Supur, Mustafa; Nielsen, Kent A.; Poulsen, Thomas; Ohkubo, Kei; Marlatt, Craig W.; Miyazaki, Eigo; Takimiya, Kazuo; Flood, Amar H.; Fukuzumi, Shunichi; Jeppesen, Jan O.
    • Journal Title

      Chemical Communications

      Volume: 53 Pages: 9898-9901

    • DOI

      10.1039/C7CC03775A

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Bicyclic Baird-type aromaticity2017

    • Author(s)
      Cha, Won-Young; Kim, Taeyeon; Ghosh, Arindam; Zhang, Zhan; Ke, Xian-Sheng; Ali, Rashid; Lynch, Vincent M.; Jung, Jieun; Kim, Woojae; Lee, Sangsu; Fukuzumi, Shunichi; Park, Jung Su; Sessler, Jonathan L.; Chandrashekar, Tavarekere K.; Kim, Dongho
    • Journal Title

      Nature Chemistry

      Volume: 9 Pages: 1243-1248

    • DOI

      10.1038/nchem.2834

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Direct oxygen atom transfer versus electron transfer mechanisms in the phosphine oxidation by nonheme Mn(IV)-oxo complexes2017

    • Author(s)
      Lee, Yong-Min; Yoo, Mi; Yoon, Heejung; Nam, Wonwoo; Fukuzumi, Shunichi
    • Journal Title

      Chemical Communications

      Volume: 53 Pages: 9352-9355

    • DOI

      10.1039/C7CC04035K

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] A subphthalocyanine-pyrene dyad: electron transfer and singlet oxygen generation2017

    • Author(s)
      El-Khouly, Mohamed E.; El-Refaey, Ahmed; Nam, Wonwoo; Fukuzumi, Shunichi; Goktug, Ozge; Durmus, Mahmut
    • Journal Title

      Photochemical & Photobiological Sciences

      Volume: 16 Pages: 1512-1518

    • DOI

      10.1039/C7PP00166E

  • [Journal Article] Autocatalytic dioxygen activation to produce an iron(V)-oxo complex without any reductants2017

    • Author(s)
      Sankaralingam, Muniyandi; Lee, Yong-Min; Lu, Xiaoyan; Vardhaman, Anil Kumar; Nam, Wonwoo; Fukuzumi, Shunichi
    • Journal Title

      Chemical Communications

      Volume: 53 Pages: 8348-8351

    • DOI

      10.1039/C7CC03742B

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Preface-JSS Focus Issue on Nanocarbons - In Memory of Sir Harry Kroto2017

    • Author(s)
      Weisman, R. Bruce; Fukuzumi, Shunichi; D'Souza, Francis
    • Journal Title

      ECS Journal of Solid State Science and Technology

      Volume: 6 Pages: Y5

    • DOI

      10.1149/2.0341706jss

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Nanocarbons as Electron Donors and Acceptors in Photoinduced Electron-Transfer Reactions2017

    • Author(s)
      Fukuzumi, Shunichi
    • Journal Title

      ECS Journal of Solid State Science and Technology

      Volume: 6 Pages: M3055-M3061

    • DOI

      10.1149/2.0061706jss

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Multi-Electron Oxidation of Anthracene Derivatives by Nonheme Manganese(IV)-Oxo Complexes2017

    • Author(s)
      Sharma, Namita; Jung, Jieun; Lee, Yong-Min; Seo, Mi Sook; Nam, Wonwoo; Fukuzumi, Shunichi
    • Journal Title

      Chemistry - A European Journal

      Volume: 23 Pages: 7125-7131

    • DOI

      10.1002/chem.201700666

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Selective Oxygenation of Cyclohexene by Dioxygen via an Iron(V)-Oxo Complex-Autocatalyzed Reaction2017

    • Author(s)
      Sankaralingam, Muniyandi; Lee, Yong-Min; Nam, Wonwoo; Fukuzumi, Shunichi
    • Journal Title

      Inorganic Chemistry

      Volume: 56 Pages: 5096-5104

    • DOI

      10.1021/acs.inorgchem.7b00220

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Multi-level non-volatile organic transistor-based memory using lithium-ion-encapsulated fullerene as a charge trapping layer2017

    • Author(s)
      Tran, Cuong Manh; Sakai, Heisuke; Kawashima, Yuki; Ohkubo, Kei; Fukuzumi, Shunichi; Murata, Hideyuki
    • Journal Title

      Organic Electronics

      Volume: 45 Pages: 234-239

    • DOI

      10.1016/j.orgel.2017.03.018

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Synthesis of methylated quercetin analogues for enhancement of radical-scavenging activity2017

    • Author(s)
      Imai, Kohei; Nakanishi, Ikuo; Ohkubo, Kei; Ohba, Yusuke; Arai, Takuya; Mizuno, Mirei; Fukuzumi, Shunichi; Matsumoto, Ken-ichiro; Fukuhara, Kiyoshi
    • Journal Title

      RSC Advances

      Volume: 7 Pages: 17968-17979

    • DOI

      10.1039/C7RA02329D

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Tunneling Effect That Changes the Reaction Pathway from Epoxidation to Hydroxylation in the Oxidation of Cyclohexene by a Compound I Model of Cytochrome P4502017

    • Author(s)
      Gupta, Ranjana; Li, Xiao-Xi; Cho, Kyung-Bin; Guo, Mian; Lee, Yong-Min; Wang, Yong; Fukuzumi, Shunichi; Nam, Wonwoo
    • Journal Title

      Journal of Physical Chemistry Letters

      Volume: 8 Pages: 1557-1561

    • DOI

      10.1021/acs.jpclett.7b00461

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Thermodynamics and Photodynamics of a Monoprotonated Porphyrin Directly Stabilized by Hydrogen Bonding with Polar Protic Solvents2017

    • Author(s)
      Suzuki, Wataru; Kotani, Hiroaki; Ishizuka, Tomoya; Ohkubo, Kei; Shiota, Yoshihito; Yoshizawa, Kazunari; Fukuzumi, Shunichi; Kojima, Takahiko
    • Journal Title

      Chemistry - A European Journal

      Volume: 23 Pages: 4669-4679

    • DOI

      10.1002/chem.201606012

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] A Chromium(III)-Superoxo Complex as a Three-Electron Oxidant with a Large Tunneling Effect in Multi-Electron Oxidation of NADH Analogues2017

    • Author(s)
      Devi, Tarali; Lee, Yong-Min; Jung, Jieun; Sankaralingam, Muniyandi; Nam, Wonwoo; Fukuzumi, Shunichi
    • Journal Title

      Angewandte Chemie, International Edition

      Volume: 56 Pages: 3510-3515

    • DOI

      10.1002/anie.201611709

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Production of Liquid Solar Fuels and Their Use in Fuel Cells2017

    • Author(s)
      Fukuzumi, Shunichi
    • Journal Title

      Joule

      Volume: 1 Pages: 689-738

    • DOI

      10.1016/j.joule.2017.07.007

    • Peer Reviewed / Int'l Joint Research
  • [Presentation] Solar-Driven Production of Hydrogen Peroxide from Water and Dioxygen and Its Usage in Fuel Cells and Green Oxidation2018

    • Author(s)
      Shunichi Fukuzumi
    • Organizer
      121st General Meeting of KCS
    • Int'l Joint Research / Invited
  • [Presentation] Liquid Solar Fuels and Fuel Cells2018

    • Author(s)
      Shunichi Fukuzumi
    • Organizer
      E-COST BIO
    • Int'l Joint Research / Invited
  • [Presentation] Production and Usage of Liquid Solar Fuels2018

    • Author(s)
      Shunichi Fukuzumi
    • Organizer
      Girona Seminar 2018
    • Int'l Joint Research / Invited
  • [Presentation] Production and Utilization of Liquid Solar Fuels2018

    • Author(s)
      Shunichi Fukuzumi
    • Organizer
      Egypt-Japan University of Science and Technology
    • Int'l Joint Research / Invited
  • [Presentation] 液体太陽燃料の製造と利用2017

    • Author(s)
      福住俊一
    • Organizer
      第50回酸化反応討論会
    • Invited
  • [Presentation] Artificial Photosynthesis Utilizing Nanocarbons2017

    • Author(s)
      Shunichi Fukuzumi
    • Organizer
      Nanocarbons, 231st ECS Meeting, Nanocarbons Division Richard E. Smalley Award Address
    • Int'l Joint Research / Invited

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Published: 2018-12-17  

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