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Elucidation of molecular self-assembly processes based on reaction networks

Research Project

Project/Area Number 20K05417
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeMulti-year Fund
Section一般
Review Section Basic Section 32010:Fundamental physical chemistry-related
Research InstitutionThe University of Tokyo

Principal Investigator

Takahashi Satoshi  東京大学, 大学院総合文化研究科, 助教 (20456180)

Project Period (FY) 2020-04-01 – 2023-03-31
Project Status Completed (Fiscal Year 2022)
Budget Amount *help
¥4,290,000 (Direct Cost: ¥3,300,000、Indirect Cost: ¥990,000)
Fiscal Year 2022: ¥780,000 (Direct Cost: ¥600,000、Indirect Cost: ¥180,000)
Fiscal Year 2021: ¥1,820,000 (Direct Cost: ¥1,400,000、Indirect Cost: ¥420,000)
Fiscal Year 2020: ¥1,690,000 (Direct Cost: ¥1,300,000、Indirect Cost: ¥390,000)
Keywords分子自己集合 / 化学反応ネットワーク / 反応速度論 / 化学マスター方程式 / 分子自己集合過程 / 化学反応速度論
Outline of Research at the Start

多数の素反応の複雑な連鎖の末に最終生成物が得られる分子自己集合過程を,化学反応速度と反応ネットワークに着目して解析する.分光学的手法によってモニターされるよりもずっと短い時間スケールを持つ,自己集合反応の詳細を,申請者らが開発した数値手法により明らかにする.分子の自己集合過程において,短寿命の中間体が目まぐるしく生成し,次の反応を導く過程の解明や,実験的に観察することが困難な中間体の同定を行い,反応の予測や制御に関する指針を確立する.さらに,化学反応ネットワークを起点として,個別の反応にとらわれない,自己集合過程の根底にある共通の原則を明らかにする.

Outline of Final Research Achievements

In this research project, based on our developed numerical analysis method, NASAP (numerical analysis of self-assembly process), we performed numerical analyses for some coordination self-assembly systems including M6L3 prism complexes and an M6L4 square-based pyramid complex (M and L stand for the metal ion and the organic multitopic ligand, respectively) and elucidated the detailed reaction processes with main reaction pathways, rate-determining steps, and kinetic traps. It is also revealed from the numerical simulations on the model reaction networks and a more complex self-assembly network that quasi-irreversibility occurs in chemical reaction networks consisting only of reversible elementary reactions as in molecular self-assembly reactions, and that quasi-irreversibility is the key concept for understanding the selection of reaction pathways leading to objective products and kinetic traps.

Academic Significance and Societal Importance of the Research Achievements

構成要素が自発的に特定の構造を構築する分子自己集合の途上で、系がどの経路を優先的に選んで化学反応が進行するのか、実験だけでは明らかにできない詳細を得るために、数値シミュレーションを用いた解析が有用であることを証明した。また、可逆な反応ネットワーク上の自己集合反応ではどのようにして、或いはなぜ目的生成物や速度論トラップに至るのかという、これまで知見や議論が少なく曖昧に捉えられていた問題に対して、可逆性からの準不可逆性の発現の過程を明らかにし、準不可逆性が反応経路選択における重要な概念であることを明らかにしたことは、広く自己集合を支配する根本原理を突き止めるための一歩であると考えられる。

Report

(4 results)
  • 2022 Annual Research Report   Final Research Report ( PDF )
  • 2021 Research-status Report
  • 2020 Research-status Report
  • Research Products

    (12 results)

All 2023 2022 2021 2020

All Journal Article (5 results) (of which Peer Reviewed: 5 results,  Open Access: 5 results) Presentation (7 results)

  • [Journal Article] Theoretical and computational methodologies for understanding coordination self-assembly complexes2023

    • Author(s)
      Takahashi Satoshi、Iuchi Satoru、Hiraoka Shuichi、Sato Hirofumi
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: - Issue: 21 Pages: 14659-14671

    • DOI

      10.1039/d3cp00082f

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Cyclization or bridging: which occurs faster is the key to the self-assembly mechanism of Pd<sub>6</sub>L<sub>3</sub> coordination prisms2022

    • Author(s)
      Zhang Xinman、Takahashi Satoshi、Aratsu Keisuke、Kikuchi Isamu、Sato Hirofumi、Hiraoka Shuichi
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 24 Issue: 5 Pages: 2997-3006

    • DOI

      10.1039/d1cp04448f

    • Related Report
      2021 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Unexpected Self-Assembly Pathway to a Pd(II) Coordination Square-Based Pyramid and Its Preferential Formation beyond the Boltzmann Distribution2021

    • Author(s)
      Tateishi Tomoki、Takahashi Satoshi、Kikuchi Isamu、Aratsu Keisuke、Sato Hirofumi、Hiraoka Shuichi
    • Journal Title

      Inorganic Chemistry

      Volume: 60 Issue: 21 Pages: 16678-16685

    • DOI

      10.1021/acs.inorgchem.1c02570

    • Related Report
      2021 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Towards kinetic control of coordination self-assembly: a case study of a Pd3L6 double-walled triangle to predict the outcomes by a reaction network model2020

    • Author(s)
      Takahashi Satoshi、Tateishi Tomoki、Sasaki Yuya、Sato Hirofumi、Hiraoka Shuichi
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 22 Issue: 45 Pages: 26614-26626

    • DOI

      10.1039/d0cp04623j

    • Related Report
      2020 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Coordination Self‐Assembly Processes Revealed by Collaboration of Experiment and Theory: Toward Kinetic Control of Molecular Self‐Assembly2020

    • Author(s)
      Hiraoka Shuichi、Takahashi Satoshi、Sato Hirofumi
    • Journal Title

      The Chemical Record

      Volume: 21 Issue: 3 Pages: 443-459

    • DOI

      10.1002/tcr.202000124

    • Related Report
      2020 Research-status Report
    • Peer Reviewed / Open Access
  • [Presentation] Switching of self-assembly pathway for Pd6L4 square-based pyramid by NO3-2023

    • Author(s)
      Satoshi Takahashi, Tsukasa Abe, Tomoki Tateishi, Hirofumi Sato, Shuichi Hiraoka
    • Organizer
      日本化学会第103年会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 配位自己集合における反応経路選択の一般原理の理論2022

    • Author(s)
      高橋 聡,佐藤 啓文,平岡 秀一
    • Organizer
      第23回理論化学討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 速度論支配における配位自己集合の反応経路選択の理論2022

    • Author(s)
      高橋 聡,佐藤 啓文,平岡 秀一
    • Organizer
      第16回分子科学討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Numerical study for kinetic control of coordination self-assembly: M4L4 square complex as an example2022

    • Author(s)
      Satoshi Takahashi, Hirofumi Sato, Shuichi Hiraoka
    • Organizer
      日本化学会第102年会
    • Related Report
      2021 Research-status Report
  • [Presentation] Pd6L4正方ピラミッド錯体形成の意外な自己集合経路2021

    • Author(s)
      高橋 聡,立石 友紀,菊池 勇, 新津 敬介,佐藤 啓文,平岡 秀一
    • Organizer
      第23回理論化学討論会
    • Related Report
      2021 Research-status Report
  • [Presentation] 化学反応ネットワークに基づくPd(II)錯体の自己集合経路解析2021

    • Author(s)
      高橋 聡,佐藤 啓文,平岡 秀一
    • Organizer
      第15回分子化学討論会
    • Related Report
      2021 Research-status Report
  • [Presentation] 化学反応ネットワークモデルに基づくPd3L6二重辺三角形錯体の自己集合過程の解明と反応予測2021

    • Author(s)
      Takahashi Satoshi、Tateishi Tomoki、Sasaki Yuya、Sato Hirofumi、Hiraoka Shuichi
    • Organizer
      日本化学会第101春季年会
    • Related Report
      2020 Research-status Report

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Published: 2020-04-28   Modified: 2024-01-30  

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