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Development of supramolecular enzymes based on the precise molecular arrangement in crystalline nano-channels

Research Project

Project/Area Number 15H05478
Research Category

Grant-in-Aid for Young Scientists (A)

Allocation TypeSingle-year Grants
Research Field Inorganic chemistry
Research InstitutionThe University of Tokyo

Principal Investigator

Tashiro Shohei  東京大学, 大学院理学系研究科(理学部), 准教授 (80420230)

Project Period (FY) 2015-04-01 – 2019-03-31
Project Status Completed (Fiscal Year 2019)
Budget Amount *help
¥24,050,000 (Direct Cost: ¥18,500,000、Indirect Cost: ¥5,550,000)
Fiscal Year 2018: ¥5,460,000 (Direct Cost: ¥4,200,000、Indirect Cost: ¥1,260,000)
Fiscal Year 2017: ¥5,720,000 (Direct Cost: ¥4,400,000、Indirect Cost: ¥1,320,000)
Fiscal Year 2016: ¥5,590,000 (Direct Cost: ¥4,300,000、Indirect Cost: ¥1,290,000)
Fiscal Year 2015: ¥7,280,000 (Direct Cost: ¥5,600,000、Indirect Cost: ¥1,680,000)
Keywords多孔性結晶 / 分子配列 / ペプチド / 触媒 / 単結晶X線回折 / 触媒反応 / 超分子 / 酵素 / X線回折 / 超分子酵素
Outline of Final Research Achievements

In this research, we aimed at the construction of "supramolecular enzyme" by precise arrangement of multiple functional groups including peptides in a crystalline channel of metal-macrocycle framework (MMF) with shape sorting capability. Specifically, we have achieved (1) development of a size-specific heterogeneous catalyst by arranging acid compounds in the channel, (2) control of photoreaction pathways based on the specific spatial effect of MMF, (3) face-selective adsorption of a prochiral compound on the chiral channel surface, and (4) simultaneous arrangement of two different peptides in the channel with the aid of specific anchor residues.

Academic Significance and Societal Importance of the Research Achievements

金属有機構造体metal-organic framework(MOF)などの既存の多孔性結晶材料では、異種複数の分子を細孔内に位置選択的に精密配列することは極めて困難であるが、本研究ではその課題を実現することにより、超分子酵素構築に向けた大きな一歩を踏み出せたことから、高い学術的意義が見込まれる。また、本研究の実現によって多孔性結晶材料の応用可能性が押し広げられることによる社会的意義も期待できる。

Report

(5 results)
  • 2019 Final Research Report ( PDF )
  • 2018 Annual Research Report
  • 2017 Annual Research Report
  • 2016 Annual Research Report
  • 2015 Annual Research Report
  • Research Products

    (34 results)

All 2020 2019 2018 2017 2016 2015

All Journal Article (7 results) (of which Int'l Joint Research: 1 results,  Peer Reviewed: 7 results,  Acknowledgement Compliant: 1 results) Presentation (25 results) (of which Int'l Joint Research: 5 results,  Invited: 2 results) Book (2 results)

  • [Journal Article] Novel Porous Crystals with Macrocycle-Based Well-Defined Molecular Recognition Sites2020

    • Author(s)
      S. Tashiro, and M. Shionoya
    • Journal Title

      Acc. Chem. Res.

      Volume: 53 Issue: 3 Pages: 632-643

    • DOI

      10.1021/acs.accounts.9b00566

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Face-selective adsorption of a prochiral compound on the chiral pore-surface of metal-macrocycle framework (MMF) directed towards stereoselective reactions2020

    • Author(s)
      S. Tashiro, T. Umeki, R. Kubota, and M. Shionoya
    • Journal Title

      Faraday Discuss.

      Volume: -

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Preferential Photoreaction in a Porous Crystal, Metal-Macrocycle Framework: PdII-Mediated Olefin Migration over [2+2] Cycloaddition2018

    • Author(s)
      H. Yonezawa, S. Tashiro, T. Shiraogawa, M. Ehara, R. Shimada, T. Ozawa, M. Shionoya
    • Journal Title

      Journal of the American Chemical Society

      Volume: 140 Issue: 48 Pages: 16610-16614

    • DOI

      10.1021/jacs.8b08534

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Rational synthesis of benzimidazole[3]arenes by CuII-catalyzed post-macrocyclization transformation2018

    • Author(s)
      Tashiro Shohei、Umeki Tsutomu、Kubota Ryou、Shionoya Mitsuhiko
    • Journal Title

      Chemical Science

      Volume: 9 Issue: 39 Pages: 7614-7619

    • DOI

      10.1039/c8sc03086c

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Arrangement of Proteinogenic α-Amino Acids on a Cyclic Peptide comprising Alternate Biphenyl-Cored ζ-Amino Acids2017

    • Author(s)
      S. Tashiro, M. Chiba, M. Shionoya
    • Journal Title

      Chemistry Asian Journal

      Volume: 12 Issue: 10 Pages: 1087-1094

    • DOI

      10.1002/asia.201700203

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Non-Covalent Immobilisation of p-Toluenesulfonic Acid in a Porous Molecular Crystal for Size-Specific Acid-Catalysed Reactions2016

    • Author(s)
      S. Tashiro, H. Yonezawa, R. Kubota, T. Umeki, M. Shionya
    • Journal Title

      Chem. Commun.

      Volume: 52 Issue: 49 Pages: 7657-7660

    • DOI

      10.1039/c6cc02621d

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Chiral metal-macrocycle frameworks: supramolecular chirality induction and helicity inversion of the helical macrocyclic structures2016

    • Author(s)
      Ryou Kubota, Shohei Tashiro and Mitsuhiko Shionoya
    • Journal Title

      Chemical Science

      Volume: 7 Issue: 3 Pages: 2217-2221

    • DOI

      10.1039/c5sc04570c

    • Related Report
      2015 Annual Research Report
    • Peer Reviewed
  • [Presentation] 多孔性環状錯体結晶MMFのナノチャネルにおける天然テルペノイドの環化反応2019

    • Author(s)
      林 龍之介・林 穎捷・田代 省平・塩谷 光彦
    • Organizer
      日本化学会第99春季年会
    • Related Report
      2018 Annual Research Report
  • [Presentation] Photo-Induced Olefin Migration Reaction at the PdII Sites Arranged on the Channel Surface of a Porous Metal-Macrocycle Framework (MMF)2019

    • Author(s)
      Shohei Tashiro, Hirotaka Yonezawa, Takafumi Shiraogawa, Masahiro Ehara, Mitsuhiko Shionoya
    • Organizer
      The 2nd International Symposium on Soft Crystals
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Construction of discrete and polymeric Ag(I) complexes of benzimidazole[3]arene2018

    • Author(s)
      Shohei Tashiro, Mitsuhiko Shionoya
    • Organizer
      錯体化学会第68回討論会
    • Related Report
      2018 Annual Research Report
  • [Presentation] Metal-Macrocycle Framework (MMF): A Porous Crystal with Multiple Binding Pockets and Active Palladium Sites2018

    • Author(s)
      Shohei Tashiro, Hirotaka Yonezawa, Mitsuhiko Shionoya
    • Organizer
      43rd International Conference on Coordination Chemistry
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 環状Pd(II)錯体集積型多孔性結晶-金ナノ粒子複合体の構築2018

    • Author(s)
      山下 優太郎・田代 省平・塩谷 光彦
    • Organizer
      日本化学会第98春季年会
    • Related Report
      2017 Annual Research Report
  • [Presentation] Development of cycloaddition reactions in chiral porous crystals composed of helical trinuclear Pd(II)-macrocycle complexes2018

    • Author(s)
      Shuhei Nakajima, Shohei Tashiro, Mitsuhiko Shionoya
    • Organizer
      日本化学会第98春季年会
    • Related Report
      2017 Annual Research Report
  • [Presentation] 超分子酵素を志向した環状錯体集積型多孔性結晶の機能化2017

    • Author(s)
      田代 省平
    • Organizer
      第17回リング・チューブ超分子研究会シンポジウム
    • Related Report
      2017 Annual Research Report
    • Invited
  • [Presentation] Metallomacrocycle-assembled Porous Crystal: Dissymmetric Chemical Modification for Designing Precise Nano-reactors2017

    • Author(s)
      Shohei Tashiro
    • Organizer
      Japan-China Joint Interdisciplinary Symposium on Coordination-based Hybrid Materials
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Development and Mechanistic Study of Olefin Migration Reaction with Photo-Activated Pd-Species in Metal-Macrocycle Framework2017

    • Author(s)
      Hirotaka Yonezawa, Takafumi Shiraogawa, Shohei Tashiro, Masahiro Ehara, Mitsuhiko Shionoya
    • Organizer
      第64回有機金属化学討論会
    • Related Report
      2017 Annual Research Report
  • [Presentation] Site-selective recognition of peptides within a metallomacrocycle-assembled porous crystal2017

    • Author(s)
      Shohei Tashiro, Kousuke Nakata, Mitsuhiko Shionoya
    • Organizer
      錯体化学会第67回討論会
    • Related Report
      2017 Annual Research Report
  • [Presentation] 環状多核金属錯体の自己組織化による多孔性機能材料の創製2017

    • Author(s)
      田代 省平
    • Organizer
      錯体化学会第67回討論会
    • Related Report
      2017 Annual Research Report
  • [Presentation] 光還元反応による環状金属錯体集積型多孔性結晶-金ナノ粒子複合体の合成と構造・機能解析2017

    • Author(s)
      山下 優太郎・田代 省平・関根 良輔・原野 幸治・中村 栄一・塩谷 光彦
    • Organizer
      錯体化学会第67回討論会
    • Related Report
      2017 Annual Research Report
  • [Presentation] チャネル型分子結晶内におけるアミノ酸の精密配列に基づく機能性ナノ空間の構築2017

    • Author(s)
      中田 光祐・田代 省平・塩谷 光彦
    • Organizer
      日本化学会第97春季年会
    • Related Report
      2016 Annual Research Report
  • [Presentation] Halogen elimination reaction of an Au(III) complex included in a Pd(II)-macrocycle-assembled porous crystal2016

    • Author(s)
      Shohei Tashiro, Ryoma Ishii, Mitsuhiko Shionoya
    • Organizer
      日本化学会第96春季年会
    • Place of Presentation
      同志社大学・京都府京田辺市
    • Year and Date
      2016-03-24
    • Related Report
      2015 Annual Research Report
  • [Presentation] Construction of size-specific and reaction-selective reaction fields with a porous crystal Metal-Macrocycle Framework (MMF)2016

    • Author(s)
      Hirotaka Yonezawa, Shohei Tashiro, Mitsuhiko Shionoya
    • Organizer
      日本化学会第96春季年会
    • Place of Presentation
      同志社大学・京都府京田辺市
    • Year and Date
      2016-03-24
    • Related Report
      2015 Annual Research Report
  • [Presentation] チャネル型分子結晶の細孔内における異種アミノ酸の位置選択的集積化2016

    • Author(s)
      中田 光祐・田代 省平・塩谷 光彦
    • Organizer
      日本化学会第96春季年会
    • Place of Presentation
      同志社大学・京都府京田辺市
    • Year and Date
      2016-03-24
    • Related Report
      2015 Annual Research Report
  • [Presentation] 多孔性結晶Metal-Macrocycle Framework(MMF)の内部空間における光誘起オレフィン移動反応の反応機構解析2016

    • Author(s)
      米澤 拓孝・田代 省平・塩谷 光彦
    • Organizer
      第27回基礎有機化学討論会
    • Related Report
      2016 Annual Research Report
  • [Presentation] 環状らせん錯体集積型ポーラス結晶による精密反応場の構築2016

    • Author(s)
      田代 省平・米澤 拓孝・中田 光祐・塩谷 光彦
    • Organizer
      第65回高分子討論会
    • Related Report
      2016 Annual Research Report
  • [Presentation] Non-covalent immobilization of acid catalysts in Metal-Macrocycle Framework (MMF) for size-specific reactions2016

    • Author(s)
      Hirotaka Yonezawa, Shohei Tashiro, Ryou Kubota, Tsutomu Umeki, Mitsuhiko Shionoya
    • Organizer
      2nd International Symposium on Center of Excellence for Innovative Material Sciences Based on Supramolecules
    • Related Report
      2016 Annual Research Report
  • [Presentation] Metal-macrocycle frameworks (MMFs): molecular arrangement, transformations, and in situ X-ray observations2016

    • Author(s)
      Shohei Tashiro
    • Organizer
      ETHZ-UTokyo Joint Symposium of Frontier Chemistry
    • Related Report
      2016 Annual Research Report
  • [Presentation] Pd錯体集積型多孔性結晶MMFの内部空間における光反応様式の転換現象とその機構解析2016

    • Author(s)
      米澤 拓孝・田代 省平・塩谷 光彦
    • Organizer
      第6回CSJ化学フェスタ2016
    • Related Report
      2016 Annual Research Report
  • [Presentation] Dynamic aspects of molecular arrangement in a porous crystal with multiple binding pockets2015

    • Author(s)
      Shohei Tashiro, Ryou Kubota, Mitsuhiko Shionoya
    • Organizer
      PACIFICHEM 2015
    • Place of Presentation
      Honolulu
    • Year and Date
      2015-12-15
    • Related Report
      2015 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Size-specific catalytic recognitions based on immobilization of acids in metal-macrocycle framework2015

    • Author(s)
      Hirotaka Yonezawa, Shohei Tashiro, Ryou Kubota, Tsutomu Umeki, Mitsuhiko Shionoya
    • Organizer
      PACIFICHEM 2015
    • Place of Presentation
      Honolulu
    • Year and Date
      2015-12-15
    • Related Report
      2015 Annual Research Report
    • Int'l Joint Research
  • [Presentation] チャネル型分子結晶の細孔内における残基特異的アミノ酸認識2015

    • Author(s)
      中田 光佑・田代 省平・塩谷 光彦
    • Organizer
      錯体化学会第65回討論会
    • Place of Presentation
      奈良女子大学・奈良県奈良市
    • Year and Date
      2015-09-21
    • Related Report
      2015 Annual Research Report
  • [Presentation] 多孔性超分子錯体結晶Metal-Macrocycle Framework (MMF) の内部空間におけるキノリノン誘導体の光反応選択性の制御2015

    • Author(s)
      米澤 拓孝・田代 省平・塩谷 光彦
    • Organizer
      錯体化学会第65回討論会
    • Place of Presentation
      奈良女子大学・奈良県奈良市
    • Year and Date
      2015-09-21
    • Related Report
      2015 Annual Research Report
  • [Book] ナノ空間材料ハンドブック2016

    • Author(s)
      塩谷 光彦・田代 省平
    • Total Pages
      10
    • Publisher
      株式会社エヌ・ティー・エス
    • ISBN
      9784860434335
    • Related Report
      2016 Annual Research Report
  • [Book] 化学2015

    • Author(s)
      窪田 亮・田代 省平・塩谷 光彦
    • Total Pages
      5
    • Publisher
      化学同人
    • Related Report
      2015 Annual Research Report

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Published: 2015-04-16   Modified: 2022-11-04  

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