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Design and systematic synthesis of novel metal-organic polyhedra for controlled integration with enzymes

Research Project

Project/Area Number 24K08447
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

LE・OUAY Benjamin  九州大学, 理学研究院, 助教 (40883179)

Project Period (FY) 2024-04-01 – 2027-03-31
Project Status Granted (Fiscal Year 2024)
Budget Amount *help
¥4,550,000 (Direct Cost: ¥3,500,000、Indirect Cost: ¥1,050,000)
Fiscal Year 2026: ¥1,430,000 (Direct Cost: ¥1,100,000、Indirect Cost: ¥330,000)
Fiscal Year 2025: ¥1,690,000 (Direct Cost: ¥1,300,000、Indirect Cost: ¥390,000)
Fiscal Year 2024: ¥1,430,000 (Direct Cost: ¥1,100,000、Indirect Cost: ¥330,000)
Keywordsmetal-organic polyhedra / coordination cages / protein cross-linking / Enzyme / biocomposite / hybrid materials / 金属-有機多面体 (MOP) / 酵素複合体 / 酵素固定化
Outline of Research at the Start

本課題では、簡便かつ極めて温和な条件で運用可能な「水溶性金属-有機多面体(MOP)を用いた酵素固定化法」を様々な酵素に適用できる技術に成熟させて、酵素固定化法として一般化する。更に、配位子修飾によるMOP表面の設計、MOP-酵素間相互作用の解明およびMOP-酵素複合体の最適化により、異なるスケールの観点から研究を展開し、特定の酵素に対するMOPのカスタムメイド設計指針の確立を目指す。

Outline of Annual Research Achievements

In FY 2024-2025, the research project has been developed along 3 axes:
1) The applications to mixed-protein systems of previously described method. This led to a much higher control of materials composition, and allows co-immobilization of several enzymes to achieve cascades. This results led to one article (ACS Apll. Mater), and one oral presentation at CSJ nenkai.
2) The development of MOP-based salts, to offer more versatility in the immobilization matrices properties, without relying on proteins to form a continuous network. This axes is well advanced, and has been presented at CSJ nenkai.
3) The development of new water-stable and noble-metal-free MOPs based on thiocarboxylate ligands. Significant progress have been done last year.

Current Status of Research Progress
Current Status of Research Progress

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

Reason

For research axis (1), a first article has been published in ACS applied materials Interfaces (IF=8.5). The project is now in a implemenatation stage for technical systems. Good results have also been obtained with the co-immobilization of enzymes (-> cascade reactions), as well as the use of cascade knock-down for sensing, notably of cyanide ions.
- For axis (2), the MOP-salts systems have been established, as-well-as tyhe efficient immobilization of enzymes and performance retention. Now, the project is in the stage of data aquisition for publication.
- For axis (3), new structures have been obtained. Now, systematic modification of the MOP are ongoing, to obtained interesting functional properties and notabvly water-solubility (in addition to stability).

Strategy for Future Research Activity

The three research aspect of the project are going well. With the collaboration of research students, the projects willl be developped further.
- Axis (1) will be driven towards application. In particular, interaction with biocatalysis groups for the implementation of industry relevant cascade reaction are considered. The application of the system to sensing of cyanide is also promising.
- Axis (2) systems demonstrate a high versatility of structure and composition. After a first report (planned this fical year), the system will be developed further to implement additional functional properties.
- Axis (3) systems showed promising properties. Furthermore, the systems showed also very good performance for ammonia capture. The system will be explored systematically before reporting.

Report

(1 results)
  • 2024 Research-status Report
  • Research Products

    (25 results)

All 2025 2024

All Journal Article (7 results) (of which Int'l Joint Research: 7 results,  Peer Reviewed: 7 results,  Open Access: 3 results) Presentation (18 results) (of which Int'l Joint Research: 1 results)

  • [Journal Article] Post‐synthetic Breaking of Inversion Symmetry in Metal Complex‐based Host?guest Systems2025

    • Author(s)
      Shi Yuxin、Iwai Yuudai、Le Ouay Benjamin、Ohba Masaaki、Ohtani Ryo
    • Journal Title

      European Journal of Inorganic Chemistry

      Volume: Early access Issue: 13

    • DOI

      10.1002/ejic.202500059

    • Related Report
      2024 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Metal?organic framework/Nb<sub>4</sub>C<sub>3</sub>T<sub><i>x</i></sub> MXene composites for ultrasensitive detection of dopamine2024

    • Author(s)
      Boruah Purna K.、Sharma Nidhi、Das Manash R.、Ohtani Ryo、Le Ouay Benjamin、Ohba Masaaki
    • Journal Title

      Chemical Communications

      Volume: 60 Issue: 57 Pages: 7307-7310

    • DOI

      10.1039/d4cc00694a

    • Related Report
      2024 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Mechanical Properties of Modulative Undulating Layers in Two-Dimensional Metal-Organic Frameworks2024

    • Author(s)
      Iwai Yuudai、Kusumoto Sotaro、Suzuki Ryo、Tachibana Masaru、Komatsu Kazuki、Kikuchi Takashi、Kawaguchi Saori I.、Kadobayashi Hirokazu、Masubuchi Yuji、Yamamoto Yuzuki、Ozawa Yoshiki、Abe Masaaki、Hirai Kenji、Le Ouay Benjamin、Ohba Masaaki、Ohtani Ryo
    • Journal Title

      Chemistry of Materials

      Volume: 36 Issue: 11 Pages: 5446-5455

    • DOI

      10.1021/acs.chemmater.4c00355

    • Related Report
      2024 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] A novel style of 2D Hofmann-type coordination polymer incorporated trigonal prismatic coordination geometry with bidentate co-ligands2024

    • Author(s)
      Yuki Imamura, Haruka Yoshino, Benjamin Le Ouay, Ryo Ohtani, Masaaki Ohba
    • Journal Title

      Dalton Transaction

      Volume: 9 Issue: 9 Pages: 3970-3974

    • DOI

      10.1039/d3dt03914e

    • Related Report
      2024 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Experimental and Theoretical Investigation of Anisotropic Proton Conduction in Two-Dimensional Metal-Organic Frameworks2024

    • Author(s)
      Shi Yuxin、Kimura Saaya、Iwai Yuudai、Tsuji Yuta、Le Ouay Benjamin、Ohba Masaaki、Ohtani Ryo
    • Journal Title

      Inorganic Chemistry

      Volume: 63 Issue: 46 Pages: 22194-22202

    • DOI

      10.1021/acs.inorgchem.4c03816

    • Related Report
      2024 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Enhancing Performances of Enzyme/Metal?Organic Polyhedra Composites by Mixed-Protein Co-Immobilization2024

    • Author(s)
      Kanzaki Yuri、Minami Ryosuke、Ota Koshiro、Adachi Junya、Hori Yuichiro、Ohtani Ryo、Le Ouay Benjamin、Ohba Masaaki
    • Journal Title

      ACS Applied Materials & Interfaces

      Volume: 16 Issue: 40 Pages: 54423-54434

    • DOI

      10.1021/acsami.4c10146

    • Related Report
      2024 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Giant anisotropic thermal expansion of copper-cyanido flat layers with flexible copper nodes2024

    • Author(s)
      Iwai Yuudai、Nakaya Manabu、Tsuji Yuta、Le Ouay Benjamin、Ohba Masaaki、Ohtani Ryo
    • Journal Title

      Chemical Communications

      Volume: 60 Issue: 51 Pages: 6512-6515

    • DOI

      10.1039/d4cc01232a

    • Related Report
      2024 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Presentation] Enzyme Cascade Immobilization with Porous Coordination Cages: Application to Paper-based Cyanide Detection2025

    • Author(s)
      Benjamin Le Ouay、Yuki Kanzaki、Masaaki Ohba
    • Organizer
      日本化学会第105春季年会
    • Related Report
      2024 Research-status Report
  • [Presentation] 単核クロム(Ⅴ)錯体を用いた分子Qubitのスピン緩和特性2025

    • Author(s)
      岸本悠佑、浅田瑞枝、Benjamin Le Ouay、中村敏和、大場正昭
    • Organizer
      日本化学会第105春季年会
    • Related Report
      2024 Research-status Report
  • [Presentation] 金属有機多面体に基づいての酵素の安定化2025

    • Author(s)
      王 天潤、Benjamin LeOuay、大場正昭
    • Organizer
      日本化学会第105春季年会
    • Related Report
      2024 Research-status Report
  • [Presentation] ビス(ジチオカルボキシレート)リガンドおよび銅イオンを基盤とした導電性配位性フレームワーク2025

    • Author(s)
      古川 廉、Benjamin LeOuay、大場正昭
    • Organizer
      日本化学会第105春季年会
    • Related Report
      2024 Research-status Report
  • [Presentation] Dramatic enhancement of cytochronme c catalytic activity associated with a Rh coordination cage2024

    • Author(s)
      Benjamin Le Ouay、Yuki Kanzaki、Purna Boruah、Ryo Ohtani、Masaaki Ohba
    • Organizer
      錯体化学会第74回討論会
    • Related Report
      2024 Research-status Report
  • [Presentation] Spin Dynamics in Molecular Qubit based on Spin 1/2 Chromium(V) Complexes2024

    • Author(s)
      Naoya Yamamoto、Mizue Asada、Benjamin LeOuay、Ryo Ohtani、Toshikazu Nakamura、Masaaki Ohba
    • Organizer
      錯体化学会第74回討論会
    • Related Report
      2024 Research-status Report
  • [Presentation] ジチオカルボン酸配位子を用いた耐水性MOPの合成2024

    • Author(s)
      下川真依、Benjamin LeOuay、大谷 亮、大場正昭
    • Organizer
      錯体化学会第74回討論会
    • Related Report
      2024 Research-status Report
  • [Presentation] 混合タンパク質の共固定化による酵素/金属-有機多面体複合体の性能向上2024

    • Author(s)
      神﨑友理、Benjamin LeOuay、大谷 亮、大場正昭
    • Organizer
      錯体化学会第74回討論会
    • Related Report
      2024 Research-status Report
  • [Presentation] カチオン性Zr有機金属多面体のポリ酸との集積化と光増感能2024

    • Author(s)
      末田悠太、神﨑友理、Benjamin LeOuay、大谷 亮、大場正昭
    • Organizer
      錯体化学会第74回討論会
    • Related Report
      2024 Research-status Report
  • [Presentation] ZnLn-Re 三元金属MOFの合成と多重発光特性2024

    • Author(s)
      周 堯、Benjamin LeOuay、大谷 亮、大場正昭
    • Organizer
      錯体化学会第74回討論会
    • Related Report
      2024 Research-status Report
  • [Presentation] 無加湿条件下で機能する強誘電イオン伝導体の開発2024

    • Author(s)
      木村紗彩、Benjamin LeOuay、大谷 亮、大場 正昭
    • Organizer
      錯体化学会第74回討論会
    • Related Report
      2024 Research-status Report
  • [Presentation] ニトリドクロム(V)サレン類縁体を用いた分子量子ビットのスピン緩和特性2024

    • Author(s)
      山本直也、浅田瑞枝、Benjamin LeOuay、大谷 亮、中村敏和、大場正昭
    • Organizer
      第61回化学関連支部合同大会
    • Related Report
      2024 Research-status Report
  • [Presentation] 配位子修飾による金属有機多面体の水への安定性の向上2024

    • Author(s)
      下川真依、Benjamin LeOuay、大谷 亮、大場正昭
    • Organizer
      第61回化学関連支部合同大会
    • Related Report
      2024 Research-status Report
  • [Presentation] タンパク質/金属有機多面体ネットワークを用いた高性能酵素固定化法2024

    • Author(s)
      神崎友理、Benjamin LeOuay、大谷 亮、大場 正昭
    • Organizer
      第61回化学関連支部合同大会
    • Related Report
      2024 Research-status Report
  • [Presentation] Ln(III)Zn(II)-Re(V) 三元金属配位高分子の合成と発光特性2024

    • Author(s)
      周 堯、Benjamin LeOuay、大谷 亮、大場正昭
    • Organizer
      第61回化学関連支部合同大会
    • Related Report
      2024 Research-status Report
  • [Presentation] Studies on ferroelectric ion conductors of K2MnN(CN)4.H2O and Na2MnN(CN)4.3H2O2024

    • Author(s)
      時 雨新、Benjamin LeOuay、大谷 亮、大場正昭
    • Organizer
      第61回化学関連支部合同大会
    • Related Report
      2024 Research-status Report
  • [Presentation] 有機カチオンを用いた極性一次元シアノ金属錯体の物性2024

    • Author(s)
      木村紗彩、Benjamin LeOuay、大谷 亮、大場 正昭
    • Organizer
      第61回化学関連支部合同大会
    • Related Report
      2024 Research-status Report
  • [Presentation] Water-soluble ionic metal-organic polyhedra as a versatile platform for enzyme bio-immobilization2024

    • Author(s)
      Benjamin LeOuay
    • Organizer
      MOF 2024 (Singapore)
    • Related Report
      2024 Research-status Report
    • Int'l Joint Research

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Published: 2024-04-05   Modified: 2025-12-26  

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