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Development of G4DNA-based switchable metalloenzymes

Research Project

Project/Area Number 18K05315
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeMulti-year Fund
Section一般
Review Section Basic Section 37010:Bio-related chemistry
Research InstitutionKyoto University

Principal Investigator

Park Soyoung  京都大学, 理学研究科, 助教 (10628556)

Project Period (FY) 2018-04-01 – 2021-03-31
Project Status Completed (Fiscal Year 2020)
Budget Amount *help
¥4,420,000 (Direct Cost: ¥3,400,000、Indirect Cost: ¥1,020,000)
Fiscal Year 2020: ¥1,300,000 (Direct Cost: ¥1,000,000、Indirect Cost: ¥300,000)
Fiscal Year 2019: ¥1,300,000 (Direct Cost: ¥1,000,000、Indirect Cost: ¥300,000)
Fiscal Year 2018: ¥1,820,000 (Direct Cost: ¥1,400,000、Indirect Cost: ¥420,000)
KeywordsDNA / Amino acid / Hybrid catalyst / quadruplex / Asymmetric catalysis / peroxidase / ハイブリッド触媒 / 四重鎖ー二本鎖ハイブリッド / アミノ酸ー核酸ハイブリッド / 金属酵素 / 不斉合成 / グアニン四重鎖構造 / 核酸 / DNA金属酵素
Outline of Final Research Achievements

Asymmetric catalysis based on DNA/RNA scaffolds has been actively studied and the field has consistently expanded. Our group has site-specifically introduced a metal-binding bipyridine ligand and steric moieties into double-stranded DNA. In this study, we focused on the potential of quadruplex-duplex (QD) hybrids to facilitate the structural engineering of DNA-based hybrid catalysts. We devised modular DNA QD hybrids with a bipyridine ligand (X) and a hydrogen (H)-bond donor moiety (Y) on the G-quadruplex core and investigated their conformation and thermal stability. The QD hybrid-based DNA catalysts have been successfully applied to the asymmetric Michael addition reactions. We also demonstrated that enantioselectivity could be controlled by a spatial arrangement of a metal-binding ligand and a functional group in the active site, without the inversion of overall DNA structure.

Academic Significance and Societal Importance of the Research Achievements

地球の資源を有効に活用することや環境に負荷をかけない不斉触媒の開発は持続可能な社会の実現のため重要な課題になっている. 本研究は, 生体高分子であるDNAを用いてハイブリッド触媒を開発し, 環境調和型合成プロセスを確立するという学術的重要性と社会的な貢献を満たすプロジェクトである. また, 申請者の研究はDNAナノテクノロジーと融合することにより, 疾患に関連する特定の配列を切断するDNAナノ酵素を開発することが期待できる. さらに, アミノ酸-DNAコンジュゲートは生理活性を持つペプチドをミミックした機能性分子としてバイオメディカル領域への貢献が期待できる.

Report

(4 results)
  • 2020 Annual Research Report   Final Research Report ( PDF )
  • 2019 Research-status Report
  • 2018 Research-status Report
  • Research Products

    (18 results)

All 2021 2020 2019 2018

All Journal Article (12 results) (of which Int'l Joint Research: 5 results,  Peer Reviewed: 12 results,  Open Access: 1 results) Presentation (6 results) (of which Int'l Joint Research: 5 results,  Invited: 6 results)

  • [Journal Article] Systematic Approach to DNA Aptamer Design Using Amino Acid?Nucleic Acid Hybrids (ANHs) Targeting Thrombin2021

    • Author(s)
      Yum Ji Hye、Ishizuka Takumi、Fukumoto Koyuki、Hori Daisuke、Bao Hong-Liang、Xu Yan、Sugiyama Hiroshi、Park Soyoung
    • Journal Title

      ACS Biomaterials Science & Engineering

      Volume: 7 Issue: 4 Pages: 1338-1343

    • DOI

      10.1021/acsbiomaterials.1c00060

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Synthesis and application of a 19F-labeled fluorescent nucleoside as a dual-mode probe for i-motif DNAs2021

    • Author(s)
      Wee Wen Ann、Yum Ji Hye、Hirashima Shingo、Sugiyama Hiroshi、Park Soyoung
    • Journal Title

      RSC Chemical Biology

      Volume: 1 Issue: 3 Pages: 1-1

    • DOI

      10.1039/d1cb00020a

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Modular quadruplex-duplex hybrids as biomolecular scaffolds for asymmetric Michael addition reactions2020

    • Author(s)
      Yum Ji Hye、Sugiyama Hiroshi、Park Soyoung
    • Journal Title

      Organic & Biomolecular Chemistry

      Volume: 18 Issue: 35 Pages: 6812-6817

    • DOI

      10.1039/d0ob01362e

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Histidine-conjugated DNA as a biomolecular depot for metal ions2020

    • Author(s)
      Park Soyoung、Matsui Haruka、Fukumoto Koyuki、Yum Ji Hye、Sugiyama Hiroshi
    • Journal Title

      RSC Advances

      Volume: 10 Issue: 16 Pages: 9717-9722

    • DOI

      10.1039/d0ra01267j

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] G-quadruplexes as versatile scaffolds for catalysis2019

    • Author(s)
      Yum Ji Hye、Park Soyoung、Sugiyama Hiroshi
    • Journal Title

      Organic & Biomolecular Chemistry

      Volume: 17 Issue: 44 Pages: 9547-9561

    • DOI

      10.1039/c9ob01876j

    • Related Report
      2019 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Highly sensitive and selective mercury sensor based on mismatched base pairing with dioxT2019

    • Author(s)
      Han Ji Hoon、Hirashima Shingo、Park Soyoung、Sugiyama Hiroshi
    • Journal Title

      Chemical Communications

      Volume: 55 Issue: 69 Pages: 10245-10248

    • DOI

      10.1039/c9cc05123f

    • Related Report
      2019 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] New Size‐Expanded Fluorescent Thymine Analogue: Synthesis, Characterization, and Application2019

    • Author(s)
      Hirashima Shingo、Han Ji Hoon、Tsuno Hitomi、Tanigaki Yusuke、Park Soyoung、Sugiyama Hiroshi
    • Journal Title

      Chemistry ? A European Journal

      Volume: 25 Issue: 42 Pages: 9913-9919

    • DOI

      10.1002/chem.201900843

    • Related Report
      2019 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Binding of a Telomestatin Derivative Changes Mechanical Anisotropy of Human Telomeric G-quadruplex2019

    • Author(s)
      Jonchhe, S.; Chimire, C.; Cui, Y.; Park, S.; Iida, K.; Nagasawa, K.; Sugiyama, H.; Mao, H.
    • Journal Title

      Angewandte Chemie international edition

      Volume: 58 Issue: 3 Pages: 877-877

    • DOI

      10.1002/anie.201811046

    • Related Report
      2019 Research-status Report 2018 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Modular DNA-based hybrid catalysts as a toolbox for enantioselective hydration of α,β-unsaturated ketones2019

    • Author(s)
      Yum, J. H.; Park, S.; Hiraga, R.; Okamura, I.; Notsu, S.; Sugiyama, H.
    • Journal Title

      Organic & biomolecular chemistry

      Volume: 17 Issue: 9 Pages: 2548-2548

    • DOI

      10.1039/c9ob00196d

    • Related Report
      2018 Research-status Report
    • Peer Reviewed
  • [Journal Article] Approach to the Investigation of Nucleosome Structure by Using the Highly Emissive Nucleobase thdG-tC FRET Pair2018

    • Author(s)
      Han, J. H.; Park, S.; Hashiya, F.; Sugiyama, H.
    • Journal Title

      Chemistry a European journal

      Volume: 24 Issue: 64 Pages: 1709-1709

    • DOI

      10.1002/chem.201803382

    • Related Report
      2018 Research-status Report
    • Peer Reviewed
  • [Journal Article] Sequence Preference and Structural Heterogeneity of BZ junctions2018

    • Author(s)
      Kim, D.; Hur, J.; Han, J. H.; Ha, S. C.; Shin, D.; Lee, S.; Park, S.; Sugiyama, H.; Kim, K. K.
    • Journal Title

      Nucleic acids research

      Volume: 46 Issue: 19 Pages: 10504-10504

    • DOI

      10.1093/nar/gky784

    • Related Report
      2018 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Biomimetic Artificial Epigenetic Code for Targeted Acetylation of Histones2018

    • Author(s)
      Taniguchi, J.; Feng, Y.; Pandian, G.; Hashiya, F.; Hidaka, T.; Hashiya, K.; Park, S.; Bando, T.; Ito, S.; Sugiyama, H.
    • Journal Title

      Journal of American chemical society

      Volume: 140 Issue: 23 Pages: 7108-7108

    • DOI

      10.1021/jacs.8b01518

    • NAID

      120006715542

    • Related Report
      2018 Research-status Report
    • Peer Reviewed
  • [Presentation] Synthesis and Application of Highly Emissive Nucleic Acid Analogues2020

    • Author(s)
      Soyoung Park
    • Organizer
      Sino-Japan Medical Textiles Forum
    • Related Report
      2020 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] DNA as a Versatile Biomolecular Scaffold for Asymmetric Catalysis2020

    • Author(s)
      Soyoung Park
    • Organizer
      KIChE Fall Meeting and International Symposium
    • Related Report
      2020 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] DNA as a Versatile Biomolecular Scaffold for Asymmetric Catalysis2020

    • Author(s)
      Soyoung Park
    • Organizer
      2020 International Symposium on Blue Carbon
    • Related Report
      2020 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Modular DNA-based Hybrid Catalyst as a Toolbox for Asymmetric Catalysis2019

    • Author(s)
      Soyoung Park
    • Organizer
      ACC2019 (The 18th Asian Chemical Congress and The 20th General Assembly of the Federation of Asian Chemical Societies)
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] DNA as a Versatile Biomolecular Scaffold for Asymmetric Catalysis2019

    • Author(s)
      Soyoung Park
    • Organizer
      Sogang University
    • Related Report
      2019 Research-status Report
    • Invited
  • [Presentation] Development of New Biohybrid Materials by Merging of DNA and Amino Acids2019

    • Author(s)
      Soyoung Park
    • Organizer
      ISNAC2019 (The 46th International Symposium on Nucleic Acids Chemistry)
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research / Invited

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Published: 2018-04-23   Modified: 2022-01-27  

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