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2021 Fiscal Year Annual Research Report

光合成における光収穫アンテナの構造と励起エネルギー伝達・移動機構の解明

Planned Research

Project AreaCreation of novel light energy conversion system through elucidation of the molecular mechanism of photosynthesis and its artificial design in terms of time and space
Project/Area Number 17H06436
Research InstitutionRitsumeikan University

Principal Investigator

民秋 均  立命館大学, 生命科学部, 教授 (00192641)

Project Period (FY) 2017-06-30 – 2022-03-31
Keywords生物物理 / 超分子化学 / ナノ材料 / 光物性 / バイオナノテクノロジー
Outline of Annual Research Achievements

1)緑色細菌由来のクロロゾームの超分子構造・機能解明:光合成細菌である緑色硫黄細菌や糸状酸素非発生型光栄養生物やクロラシドバクテリウムには、膜外ペリフェラルアンテナ部であるクロロゾームを有しているが、その中心部では、構成クロロフィル分子の自己会合によって超分子構造体が形成されている。しかし、その結晶構造解析ができないために、現在でもその超分子構造は未解明なところが多い。そこで、構成クロロフィルの(半)合成モデル分子を利用した人工系を構築し、そこから得られる分光学的や顕微鏡測定情報から超分子構造の解明を行った。特に、20位に電子吸引基を導入した系では、より安定な自己集積体を形成できることが判明し、超分子構造解明にとって有利になることが明らかになった。さらに、31位や132位への置換基の導入にも成功し、サイズや吸収波長を制御しやすいJ型自己会合体の創製にも成功した。
2)光合成細菌の反応中心とアンテナの複合体の調製:光化学系2型の反応中心を有する紅色や緑色非硫黄光合成細菌を培養し、その反応中心を単離・精製した。このような天然反応中心と天然ならびに人工アンテナ系との複合体を巨大リポソームに再構成し、その可視化をおこないつつ、励起エネルギー移動の検出を顕微分光法で行うことに成功した。
3)人工光合成系の創製:自己集積能を有するクロロフィル誘導体を新たに合成し、そのクロロゾーム型自己会合体を調製することで、光吸収・励起エネルギー伝達型巨大集積体を構築した。そのような系にエネルギー受容体を連結することで、励起エネルギーを外部に取り出すことが可能な人工光合成アンテナモデルも創製した。この際に、各コンポーネントの最低励起エネルギー準位を調整することで、可視から近赤外領域の光を効率的に利用できるように検討を行った。特に、固体電極系で光電変換制御を行うことに成功したことは特筆される。

Research Progress Status

令和3年度が最終年度であるため、記入しない。

Strategy for Future Research Activity

令和3年度が最終年度であるため、記入しない。

  • Research Products

    (36 results)

All 2022 2021 Other

All Int'l Joint Research (1 results) Journal Article (25 results) (of which Int'l Joint Research: 11 results,  Peer Reviewed: 25 results,  Open Access: 2 results) Presentation (7 results) (of which Int'l Joint Research: 6 results,  Invited: 7 results) Book (1 results) Remarks (1 results) Funded Workshop (1 results)

  • [Int'l Joint Research] 吉林大学(中国)

    • Country Name
      CHINA
    • Counterpart Institution
      吉林大学
  • [Journal Article] Synthesis of chlorophyll-a derivative inserting an ethynylene group between the carboxylic acid moiety and chlorin π-skeleton and its photosensitizing efficiency in dye-sensitized solar cell2022

    • Author(s)
      Nakano Takeo、Liu Yanxiang、Wang Xiao-Feng、Tamiaki Hitoshi
    • Journal Title

      Journal of Photochemistry and Photobiology A: Chemistry

      Volume: 424 Pages: 113633~113633

    • DOI

      10.1016/j.jphotochem.2021.113633

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Chlorophyll derivatives/MXene hybrids for photocatalytic hydrogen evolution: Dependence of performance on the central coordinating metals2022

    • Author(s)
      Li Yuanlin、Zheng Tianfang、Liu Yanxiang、Dall’Agnese Yohan、Dall’Agnese Chunxiang、Liu Cheng-Liang、Sasaki Shin-ichi、Tamiaki Hitoshi、Wang Xiao-Feng
    • Journal Title

      International Journal of Hydrogen Energy

      Volume: 47 Pages: 3824~3833

    • DOI

      10.1016/j.ijhydene.2021.11.026

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Difluoroboron complexes of peripheral β-diketonates in cyclopheophorbides: Their syntheses and optical properties2022

    • Author(s)
      Ishikawa Haruki、Demise Ayaka、Kitagawa Yuichi、Shinozaki Yoshinao、Kinoshita Yusuke、Tamiaki Hitoshi
    • Journal Title

      Tetrahedron

      Volume: 104 Pages: 132596~132596

    • DOI

      10.1016/j.tet.2021.132596

    • Peer Reviewed
  • [Journal Article] Visible-light-induced hydrogen evolution from water on hybrid photocatalysts consisting of synthetic chlorophyll-a derivatives with a carboxy group in the 20-substituent adsorbed on semiconductors2022

    • Author(s)
      Hashimoto Yuki、Suzuki Hajime、Kondo Tomoki、Abe Ryu、Tamiaki Hitoshi
    • Journal Title

      Journal of Photochemistry and Photobiology A: Chemistry

      Volume: 426 Pages: 113750~113750

    • DOI

      10.1016/j.jphotochem.2021.113750

    • Peer Reviewed
  • [Journal Article] Chlorophyll derivative sensitized monolayer Ti3C2Tx MXene nanosheets for photocatalytic hydrogen evolution2022

    • Author(s)
      Li Yuanlin、Liu Yanxiang、Zheng Tianfang、Sasaki Shin-ichi、Tamiaki Hitoshi、Wang Xiao-Feng
    • Journal Title

      Journal of Photochemistry and Photobiology A: Chemistry

      Volume: 427 Pages: 113792~113792

    • DOI

      10.1016/j.jphotochem.2022.113792

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Incomplete Hydrogenation by Geranylgeranyl Reductase from a Proteobacterial Phototroph Halorhodospira halochloris, Resulting in the Production of Bacteriochlorophyll with a Tetrahydrogeranylgeranyl Tail2022

    • Author(s)
      Tsukatani Yusuke、Harada Jiro、Kurosawa Kanako、Tanaka Keiko、Tamiaki Hitoshi
    • Journal Title

      Journal of Bacteriology

      Volume: 204 Pages: e-00605-21

    • DOI

      10.1128/jb.00605-21

    • Peer Reviewed / Open Access
  • [Journal Article] Quasi-Bilayer All-Small-Molecule Solar Cells Based on a Chlorophyll Derivative and Non-Fullerene Materials with Untraditional Energy Alignments2022

    • Author(s)
      Duan Shengnan、Song Jiaxing、Zhou Erjun、Yang Ke、Lu Shirong、Li Dengfeng、Sasaki Shin-ichi、Tamiaki Hitoshi、Wang Xiao-Feng
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 126 Pages: 4807~4814

    • DOI

      10.1021/acs.jpcc.2c00188

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Improved Li storage capacity of 2D MoS2 upon chlorophyll derivative composition2022

    • Author(s)
      Qi Xin、Xu Wen-Xin、Zhang Chao、Miao Yong-Qiang、Xu Yu-Ting、He Song-Ying、Zhang Dong、Li Liang、Sasaki Shin-ichi、Tamiaki Hitoshi、Wang Xiao-Feng
    • Journal Title

      Materials Today Communications

      Volume: 31 Pages: 103465~103465

    • DOI

      10.1016/j.mtcomm.2022.103465

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Chlorophyll derivative intercalation into Nb2C MXene for lithium-ion energy storage2022

    • Author(s)
      Qi Xin、Xu WenXin、Tang JiaLi、Xu YuTing、Gao Yu、Li Liang、Sasaki Shin-ichi、Tamiaki Hitoshi、Wang XiaoFeng
    • Journal Title

      Journal of Materials Science

      Volume: - Pages: -

    • DOI

      10.1007/s10853-022-06929-y

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Substituted Methylenation at the 132sition of a Chlorophyll‐a Derivative via Mixed Aldol Condensation, Optical Properties of the Synthetic Bacteriochlorophyll‐d Analogs, and Self‐aggregation of Their Zinc Complexes2022

    • Author(s)
      Takeda Toyoho、Kitagawa Yuichi、Tamiaki Hitoshi
    • Journal Title

      Photochemistry and Photobiology

      Volume: - Pages: -

    • DOI

      10.1111/php.13604

    • Peer Reviewed
  • [Journal Article] Synthesis of Chl@Ti3C2 composites as an anode material for lithium storage2021

    • Author(s)
      Xu Wenxin、Zhao Xin、Tang Jiali、Zhang Chao、Gao Yu、Sasaki Shin-ichi、Tamiaki Hitoshi、Li Aijun、Wang Xiao-Feng
    • Journal Title

      Frontiers of Chemical Science and Engineering

      Volume: 15 Pages: 709~716

    • DOI

      10.1007/s11705-020-1984-z

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Synthesis of Highly Fluorescent Cationic Chlorophyll-a Derivatives Possessing a p-Aminopyridinio Group at the 31-Position2021

    • Author(s)
      Ogasawara Shin、Takahashi Tatsuya、Kitagawa Yuichi、Tamiaki Hitoshi
    • Journal Title

      Bulletin of the Chemical Society of Japan

      Volume: 94 Pages: 1201~1203

    • DOI

      10.1246/bcsj.20210009

    • Peer Reviewed
  • [Journal Article] Supramolecular Nanofibers Constructed by Hydrogen Bonding of Chlorophyll Dimer2021

    • Author(s)
      Matsubara Shogo、Tamiaki Hitoshi
    • Journal Title

      Chemistry Letters

      Volume: 50 Pages: 999~1001

    • DOI

      10.1246/cl.210026

    • Peer Reviewed
  • [Journal Article] Physicochemical and biochemical properties of synthetic zinc 131-(un)substituted chlorophyll-a derivatives2021

    • Author(s)
      Hirose Mitsuaki、Harada Jiro、Maeda Hiroaki、Tamiaki Hitoshi
    • Journal Title

      Tetrahedron

      Volume: 88 Pages: 132151~132151

    • DOI

      10.1016/j.tet.2021.132151

    • Peer Reviewed
  • [Journal Article] Self-aggregation of Synthetic 20-O-Substituted Bacteriochlorophyll-d Analogs2021

    • Author(s)
      Sakaguchi Kana、Kishi Masashi、Tamiaki Hitoshi
    • Journal Title

      Chemistry Letters

      Volume: 50 Pages: 1416~1418

    • DOI

      10.1246/cl.210216

    • Peer Reviewed
  • [Journal Article] Synthesis of 20-Deuterated Bacteriochlorophyll-d Homolog and Its 31-Epimerically Controlled Self-Aggregation2021

    • Author(s)
      Shiozaki Mai、Miyanishi Takuya、Tamiaki Hitoshi
    • Journal Title

      Chemistry Letters

      Volume: 50 Pages: 1539~1542

    • DOI

      10.1246/cl.210279

    • Peer Reviewed
  • [Journal Article] 31-Substituent-dependent self-aggregation of bacteriochlorophyll-d analogs in aqueous micelle2021

    • Author(s)
      Tani Shunsuke、Kanehisa Seiji、Tamiaki Hitoshi
    • Journal Title

      Chemistry Letters

      Volume: 50 Pages: 1551~1554

    • DOI

      10.1246/cl.210312

    • Peer Reviewed
  • [Journal Article] Synthesis of 20-substituted chlorophyll derivatives with F-ring and optical properties of their less distorted chlorin π-systems2021

    • Author(s)
      Takarada Yuki、Doi Marie、Ogasawara Shin、Tamiaki Hitoshi
    • Journal Title

      Tetrahedron

      Volume: 93 Pages: 132260~132260

    • DOI

      10.1016/j.tet.2021.132260

    • Peer Reviewed
  • [Journal Article] Aggregate-forming semi-synthetic chlorophyll derivatives / Ti3C2Tx MXene hybrids for photocatalytic hydrogen evolution2021

    • Author(s)
      Li Yuanlin、Liu Yanxiang、Sun Xiaoli、Zheng Tianfang、Dall’Agnese Yohan、Dall’Agnese Chunxiang、Sasaki Shin-ichi、Tamiaki Hitoshi、Wang Xiao-Feng
    • Journal Title

      Dyes and Pigments

      Volume: 194 Pages: 109583~109583

    • DOI

      10.1016/j.dyepig.2021.109583

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Synthesis of deuterated chlorophyll derivatives and their physical properties2021

    • Author(s)
      Shiozaki Mai、Miyanishi Takuya、Tamiaki Hitoshi
    • Journal Title

      Dyes and Pigments

      Volume: 194 Pages: 109618~109618

    • DOI

      10.1016/j.dyepig.2021.109618

    • Peer Reviewed
  • [Journal Article] Hydroquinone redox mediator enhances the photovoltaic performances of chlorophyll-based bio-inspired solar cells2021

    • Author(s)
      Duan Shengnan、Uragami Chiasa、Horiuchi Kota、Hino Kazuki、Wang Xiao-Feng、Sasaki Shin-ichi、Tamiaki Hitoshi、Hashimoto Hideki
    • Journal Title

      Communications Chemistry

      Volume: 4 Pages: 118~118

    • DOI

      10.1038/s42004-021-00556-5

    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Self-aggregation of synthetic zinc 3-hydroxymethyl-chlorophyll-a derivatives possessing electron-withdrawing groups at the 20-position in aqueous micelle solution2021

    • Author(s)
      Sakaguchi Kana、Kishi Masashi、Kinoshita Yusuke、Tamiaki Hitoshi
    • Journal Title

      Journal of Porphyrins and Phthalocyanines

      Volume: 25 Pages: 1104~1110

    • DOI

      10.1142/S1088424621501017

    • Peer Reviewed
  • [Journal Article] Synthesis of 132,173-cyclopheophorbides and their optical properties2021

    • Author(s)
      Kinoshita Yusuke、Demise Ayaka、Ishikawa Haruki、Tamiaki Hitoshi
    • Journal Title

      Journal of Photochemistry and Photobiology A: Chemistry

      Volume: 420 Pages: 113490~113490

    • DOI

      10.1016/j.jphotochem.2021.113490

    • Peer Reviewed
  • [Journal Article] Charge Generation and Transfer Mechanism of Bilayer Organic Photovoltaics with Unconventional Energy Alignment2021

    • Author(s)
      Xiang Tian-Fu、Duan Shengnan、Tamiaki Hitoshi、Sun Yuliang、Liu Ziyan、Sasaki Shin-ichi、Wang Xiao-Feng
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 125 Pages: 25680~25686

    • DOI

      10.1021/acs.jpcc.1c07157

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Effect of the Fabrication Method of Chlorophyll‐Ti3C2Tx‐Based Photocatalysts on Noble Metal‐Free Hydrogen Evolution2021

    • Author(s)
      Zheng Tianfang、Li Yuanlin、Sun Yuliang、Dall’Agnese Yohan、Dall’Agnese Chunxiang、Sasaki Shin-ichi、Tamiaki Hitoshi、Wang Xiao-Feng
    • Journal Title

      Energy Technology

      Volume: 10 Pages: 2100713~2100713

    • DOI

      10.1002/ente.202100713

    • Peer Reviewed / Int'l Joint Research
  • [Presentation] 有機合成法からアプローチする生体外におけるBciC酵素反応の基質特異性の検討2022

    • Author(s)
      廣瀨 光了、原田 二朗、民秋 均
    • Organizer
      原核光合成生物シンポジウム
    • Invited
  • [Presentation] Chlorophyll derivative-based photo-energy conversion systems inspired from Z-scheme process of oxygenic photosynthesis2021

    • Author(s)
      X.-F. Wang, S. Duan, Y. Li, N. Li, S. Sasaki, H. Hashimoto, H. Tamiaki
    • Organizer
      SNCPP21
    • Int'l Joint Research / Invited
  • [Presentation] Intramolecular asymmetric coordination of synthetic zinc chlorophyll-a derivatives possessing a pyridyl group2021

    • Author(s)
      K. Oyagi, S. Ogasawara, H. Tamiaki
    • Organizer
      SNCPP21
    • Int'l Joint Research / Invited
  • [Presentation] BciC enzymatic reactions of synthetic zinc 131-(un)substituted chlorophyll-a derivatives2021

    • Author(s)
      M. Hirose, J. Harada, H. Maeda, H. Tamiaki
    • Organizer
      SNCPP21
    • Int'l Joint Research / Invited
  • [Presentation] Redox mediator to enhance the photovoltaic performance of chlorophyll-based bio-inspired solar cells2021

    • Author(s)
      H. Hashimoto, S. Duan, C. Uragami, K. Horiuchi, K. Hino, X.-F. Wang, S. Sasaki, H. Tamiaki
    • Organizer
      ISPCCS2021
    • Int'l Joint Research / Invited
  • [Presentation] Self-aggregation of bacteriochlorophyll-c/d analogs as models of photosynthetic light-harvesting antennas2021

    • Author(s)
      H. Tamiaki, M. Shiozaki, S. Tani, K. Sakaguchi
    • Organizer
      ISPCCS2021
    • Int'l Joint Research / Invited
  • [Presentation] Synthesis of (bacterio)chlorophylls bearing deuterated substituents and their physical properties2021

    • Author(s)
      H. Tamiaki, S. Matsubara, S. Shoji
    • Organizer
      Pacifichem 2021
    • Int'l Joint Research / Invited
  • [Book] Fundamentals of Porphyrin Chemistry: A 21st Century Approach2022

    • Author(s)
      H. Tamiaki
    • Total Pages
      34
    • Publisher
      John Wiley & Sons
    • ISBN
      978-1-119-12928-8
  • [Remarks] 立命館大学生命科学部応用化学科生物有機化学研究室

    • URL

      http://www.ritsumei.ac.jp/se/rc/staff/tamiaki/lab.html

  • [Funded Workshop] SNCPP212021

URL: 

Published: 2022-12-28  

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