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Compartmentalization of catalysts into metal-organic polyhedra gel for cascade reactions

Research Project

Project/Area Number 20K15366
Research Category

Grant-in-Aid for Early-Career Scientists

Allocation TypeMulti-year Fund
Review Section Basic Section 36010:Inorganic compounds and inorganic materials chemistry-related
Research InstitutionKyoto University

Principal Investigator

Legrand Alex  京都大学, 高等研究院, 特定研究員 (00836372)

Project Period (FY) 2020-04-01 – 2023-03-31
Project Status Completed (Fiscal Year 2022)
Budget Amount *help
¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000)
Fiscal Year 2021: ¥1,950,000 (Direct Cost: ¥1,500,000、Indirect Cost: ¥450,000)
Fiscal Year 2020: ¥2,210,000 (Direct Cost: ¥1,700,000、Indirect Cost: ¥510,000)
KeywordsPorous material / supramolecular system / metal organic cages / host-guest system / metal nanoparticles / Metal-organic cages / Metal nanoparticles / Host-guest system / metal-organic polyhedra / self-assembly / soft matter / catalysis / metal nanoparticle
Outline of Research at the Start

I will use porous molecular cages (MOPs) to immobilize catalyticaly active metal nanoparticles (MNPs) within host cage. In addition, metal-organic cages offer the advantages such as flexibility and processability, which will be use to control the assembly of the hybrid system MNPs(guest)/MOPs(host) into porous gels. The system will be used as bifunctional membrane offering extra free hierarchical porosity for optimal reaction-diffusion and perform one-pot multi-steps catalysis.
This work could lead to high impact journals publication and presentation in international conferences.

Outline of Final Research Achievements

As porous molecular solids, MOPs present improved prospects for materials processing. They have been used as templates to accommodate and control properties of various guests. However, the joint use of (i) the intrinsic cage porosity with the extrinsic porosity of MOP-assembled structure and (ii) the compartmentalized catalytic sites into a MOP-based gel for tandem catalytic applications has never been described. The originality of the project lies in the use of MOPs to (i) isolate multiple catalytic species; (ii) control their spatial organization during gel formation and (iii) use the mesoporosity created by the gel networks as diffusion channels for reactants to create a bifunctional catalytic porous membrane for continuous reactions. The work will demonstrate new applications for porous molecules not only in the field of catalysis but also for selective sensing and chiral separation.

Academic Significance and Societal Importance of the Research Achievements

The developed system will be used as bifunctional membrane offering extra free hierarchical porosity for optimal reaction-diffusion and perform one-pot multi-steps catalysis. This work could lead to high impact journals publication and presentation in international conferences.

Report

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

    (11 results)

All 2023 2022 2021 2020

All Journal Article (5 results) (of which Int'l Joint Research: 4 results,  Peer Reviewed: 4 results,  Open Access: 2 results) Presentation (6 results) (of which Int'l Joint Research: 5 results,  Invited: 4 results)

  • [Journal Article] Controlled sequential assembly of metal-organic polyhedra into colloidal gels with high chemical complexity2022

    • Author(s)
      Tsang Min Ying、Tokuda Shun、Han Po-Chun、Wang Zaoming、Legrand Alexandre、Kawano Marina、Tsujimoto Masahiko、Ikeno Yuki、Urayama Kenji、Wu Kevin C.-W.、Furukawa Shuhei
    • Journal Title

      Small Structures

      Volume: 3 Pages: 2100197-2100197

    • DOI

      10.26434/chemrxiv-2021-6dhhs

    • Related Report
      2022 Annual Research Report
  • [Journal Article] Directional asymmetry over multiple length scales in reticular porous materials2021

    • Author(s)
      Legrand Alexandre、Wang Zaoming、Troyano Javier、Furukawa Shuhei
    • Journal Title

      Chemical Science

      Volume: 12 Issue: 1 Pages: 18-33

    • DOI

      10.1039/d0sc05008c

    • Related Report
      2020 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Spatiotemporal Control of Supramolecular Polymerization and Gelation of Metal?Organic Polyhedra2021

    • Author(s)
      Legrand Alexandre、Liu Li-Hao、Royla Philipp、Aoyama Takuma、Craig Gavin A.、Carn?-S?nchez Arnau、Urayama Kenji、Weigand Jan J.、Lin Chia-Her、Furukawa Shuhei
    • Journal Title

      Journal of the American Chemical Society

      Volume: 143 Issue: 9 Pages: 3562-3570

    • DOI

      10.1021/jacs.1c00108

    • Related Report
      2020 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Synthetic and computational assessment of a chiral metal?organic framework catalyst for predictive asymmetric transformation2020

    • Author(s)
      Canivet Jerome、Bernoud Elise、Bonnefoy Jonathan、Legrand Alexandre、Todorova Tanya K.、Quadrelli Elsje Alessandra、Mellot-Draznieks Caroline
    • Journal Title

      Chemical Science

      Volume: 11 Issue: 33 Pages: 8800-8808

    • DOI

      10.1039/d0sc03364b

    • Related Report
      2020 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] A selective ionic rectifier2020

    • Author(s)
      Legrand Alexandre、Furukawa Shuhei
    • Journal Title

      Nature Materials

      Volume: 19 Issue: 7 Pages: 701-702

    • DOI

      10.1038/s41563-020-0686-8

    • Related Report
      2020 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Presentation] Controlled assembly of Metal Organic Cages into hierarchical structures and their applications2023

    • Author(s)
      A. Legrand
    • Organizer
      RSC Porous Material Interest Group
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Controlled assembly of Metal Organic Cages into hierarchical structures and their applications2023

    • Author(s)
      A. Legrand
    • Organizer
      MOF thematic day of the Catalysis and Solid State Chemistry Unit
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Stimuli-responsive gelation of linked metal-organic cages using pH and light2023

    • Author(s)
      A. Legrand
    • Organizer
      the 38th meeting of the Zeolite French Group
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Stimuli-responsive gelation of linked metal-organic cages using pH and light2022

    • Author(s)
      A. Legrand, S. Furukawa
    • Organizer
      the international conference on Metal-Organic Frameworks
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Effect of linker structures on materials properties of linked metal-organic polyhedra gels2022

    • Author(s)
      A. Legrand, S. Furukawa
    • Organizer
      SPIRITS/LIMNI joint workshop
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Towards the creation of complex hierarchical structures starting from MOFs or MOPs as initial building blocks2020

    • Author(s)
      Alexandre Legrand
    • Organizer
      Laboratory of Infrared and Raman Spectroscopy Seminar
    • Related Report
      2020 Research-status Report
    • Invited

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

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