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高等学校化学研究 ›› 2020, Vol. 36 ›› Issue (2): 301-306.doi: 10.1007/s40242-020-0110-6

• Articles • 上一篇    下一篇

Programmable and Reversible Regulation of Catalytic Hemin@MOFs Activities with DNA Structures

LIU Shuo, YANG Mingjie, GUO Weiwei   

  1. College of Chemistry, Research Centre for Analytical Sciences, Tianjin Key Laboratory of Biosensing and Molecular Recognition, Nankai University, Tianjin 300071, P. R. China
  • 收稿日期:2019-12-25 修回日期:2020-03-02 出版日期:2020-04-01 发布日期:2020-03-02
  • 通讯作者: GUO Weiwei E-mail:weiweiguo@nankai.edu.cn
  • 基金资助:
    Supported by the National Natural Science Foundation of China(Nos.21505078, 21874076), the Natural Science Foundation of Tianjin City, China(No.18JCZDJC37800), the Fundamental Research Funds for Central Universities(China) and the National Program for Support of Top-notch Young Professionals, China.

Programmable and Reversible Regulation of Catalytic Hemin@MOFs Activities with DNA Structures

LIU Shuo, YANG Mingjie, GUO Weiwei   

  1. College of Chemistry, Research Centre for Analytical Sciences, Tianjin Key Laboratory of Biosensing and Molecular Recognition, Nankai University, Tianjin 300071, P. R. China
  • Received:2019-12-25 Revised:2020-03-02 Online:2020-04-01 Published:2020-03-02
  • Contact: GUO Weiwei E-mail:weiweiguo@nankai.edu.cn
  • Supported by:
    Supported by the National Natural Science Foundation of China(Nos.21505078, 21874076), the Natural Science Foundation of Tianjin City, China(No.18JCZDJC37800), the Fundamental Research Funds for Central Universities(China) and the National Program for Support of Top-notch Young Professionals, China.

摘要: Metal-organic frameworks(MOFs)-based nanozyme plays an important role in biosensing, therapy and catalysis. In this study, the effects of single-stranded DNA(ssDNA) with programmable sequences and its complementary DNA(TDNA) on the intrinsic peroxidase-like activity of hemin loaded MOFs(UiO-66-NH2), denoted as hemin@UiO-66-NH2, were investigated. The hemin@UiO-66-NH2 exhibited improved catalytic activity compared with free hemin. However, the catalytic activity is inhibited in the presence of ssDNA, as ssDNA can be adsorbed by MOFs and therefore protected the active sites from contact with substrates. Upon the addition of the TDNA, double-stranded DNA(dsDNA) was formed and detached from the MOFs, resulting in the recovery of catalytic activity. Sequentially adding ssDNA or its complementary DNA strands can achieve the reversible regulation of the catalytic activity of MOFs nanozymes. Moreover, the DNA hybridization-based regulation was further applied to a cascaded catalytic system composed of the nanozyme, hemin@UiO-66-NH2, and glucose oxidase. These nanozyme based programmable and reversibly regulated catalytic systems may have potential applications in future smart biosensing and catalysis systems.

关键词: Nanozyme, Catalytic metal-organic framework, Hemin, DNA hybridization, Dynamic modification

Abstract: Metal-organic frameworks(MOFs)-based nanozyme plays an important role in biosensing, therapy and catalysis. In this study, the effects of single-stranded DNA(ssDNA) with programmable sequences and its complementary DNA(TDNA) on the intrinsic peroxidase-like activity of hemin loaded MOFs(UiO-66-NH2), denoted as hemin@UiO-66-NH2, were investigated. The hemin@UiO-66-NH2 exhibited improved catalytic activity compared with free hemin. However, the catalytic activity is inhibited in the presence of ssDNA, as ssDNA can be adsorbed by MOFs and therefore protected the active sites from contact with substrates. Upon the addition of the TDNA, double-stranded DNA(dsDNA) was formed and detached from the MOFs, resulting in the recovery of catalytic activity. Sequentially adding ssDNA or its complementary DNA strands can achieve the reversible regulation of the catalytic activity of MOFs nanozymes. Moreover, the DNA hybridization-based regulation was further applied to a cascaded catalytic system composed of the nanozyme, hemin@UiO-66-NH2, and glucose oxidase. These nanozyme based programmable and reversibly regulated catalytic systems may have potential applications in future smart biosensing and catalysis systems.

Key words: Nanozyme, Catalytic metal-organic framework, Hemin, DNA hybridization, Dynamic modification