DNAzyme-Derived Aptamer Reversely Regulates the Two Types of Enzymatic Activities of Covalent-Organic Frameworks for the Colorimetric Analysis of Uranium.

Nanozymes are nanomaterials with enzyme-mimetic activity. It is known that DNA can interact with various nanozymes in different ways, enhancing or inhibiting the activity of nanozymes, which can be used to develop various biosensors. In this work, we synthesized a photosensitive covalent-organic framework (Tph-BT) as a nanozyme, and its oxidase and peroxidase activities could be reversely regulated by surface modification of single-stranded DNA (ssDNA) for the colorimetric detection of UO22+. Tph-BT exhibits excellent oxidase activity and weak peroxidase activity, and it is surprising to find that the UO22+-specific DNA aptamer can significantly inhibit the oxidase activity while greatly enhancing the peroxidase activity. The present UO22+ interacts with the DNA aptamer to form secondary structures and detaches from the surface of Tph-BT, thereby restoring the enzymatic activity of Tph-BT. Based on the reversed regulation effects of the DNA aptamer on the two types of enzymatic activities of Tph-BT, a novel "off-on" and "on-off" sensing platform can be constructed for the colorimetric analysis of UO22+. This research demonstrates that ssDNA can effectively regulate the different types of enzymatic activities of single COFs and achieve the sensitive and selective colorimetric analysis of radionuclides by the naked eye.

[1]  Yongwu Peng,et al.  Ultrathin covalent organic framework nanosheet-based photoregulated metal-free oxidase-like nanozyme , 2022, Nano Research.

[2]  Jianding Qiu,et al.  Construction of D-A-Conjugated Covalent Organic Frameworks with Enhanced Photodynamic, Photothermal, and Nanozymatic Activities for Efficient Bacterial Inhibition. , 2022, ACS applied materials & interfaces.

[3]  Zian Lin,et al.  Construction of Donor-Acceptor Heteroporous Covalent Organic Frameworks as Photoregulated Oxidase-like Nanozymes for Sensing Signal Amplification. , 2022, ACS applied materials & interfaces.

[4]  Yanjun Jiang,et al.  Metal Nanoparticles@Covalent Organic Framework@Enzymes: A Universal Platform for Fabricating a Metal-Enzyme Integrated Nanocatalyst. , 2022, ACS applied materials & interfaces.

[5]  Jianshu Li,et al.  Chemically Grafted Nanozyme Composite Cryogels to Enhance Antibacterial and Biocompatible Performance for Bioliquid Regulation and Adaptive Bacteria Trapping. , 2021, ACS nano.

[6]  Jianding Qiu,et al.  A conveniently synthesized redox-active fluorescent covalent organic framework for selective detection and adsorption of uranium. , 2021, Journal of hazardous materials.

[7]  H. Ju,et al.  Intrareticular charge transfer regulated electrochemiluminescence of donor–acceptor covalent organic frameworks , 2021, Nature Communications.

[8]  Sainan Liu,et al.  Facile Synthesis of a Cubic Porphyrin-Based Covalent Organic Framework for Combined Breast Cancer Therapy. , 2021, ACS applied materials & interfaces.

[9]  Jianding Qiu,et al.  Covalent Organic Frameworks as Advanced Uranyl Electrochemiluminescence Monitoring Platforms. , 2021, Analytical chemistry.

[10]  Zian Lin,et al.  Nanoscale Covalent Organic Frameworks with Donor-Acceptor Structures as Highly Efficient Light-Responsive Oxidase-like Mimics for Colorimetric Detection of Glutathione. , 2021, ACS applied materials & interfaces.

[11]  Huangsheng Yang,et al.  Hydrogen-Bonded Biohybrid Framework-Derived Highly Specific Nanozymes for Biomarker Sensing. , 2021, Analytical chemistry.

[12]  Jianding Qiu,et al.  Facile Construction of Covalent Organic Framework Nanozyme for Colorimetric Detection of Uranium. , 2021, Small.

[13]  Huangsheng Yang,et al.  Biocatalytic Cascade in an Ultrastable Mesoporous Hydrogen-Bonded Organic Framework for Point-of-Care Biosensing. , 2021, Angewandte Chemie.

[14]  Wei Cheng,et al.  Ultrafine Platinum Nanoparticles Supported on Covalent Organic Frameworks As Stable and Reusable Oxidase-Like Catalysts for Cellular Glutathione Detection , 2021 .

[15]  Moon J. Kim,et al.  Nickel-Platinum Nanoparticles as Peroxidase Mimics with a Record High Catalytic Efficiency. , 2021, Journal of the American Chemical Society.

[16]  Jianding Qiu,et al.  Rational design of covalent organic frameworks as a groundbreaking uranium capture platform through three synergistic mechanisms , 2021 .

[17]  Hai‐Long Jiang,et al.  Photocatalytic Molecular Oxygen Activation by Regulating Excitonic Effects in Covalent Organic Frameworks. , 2020, Journal of the American Chemical Society.

[18]  Juanxiu Xiao,et al.  DNA nano-pocket for ultra-selective uranyl extraction from seawater , 2020, Nature Communications.

[19]  P. Mukherjee,et al.  Self-Assembled Pd12 Coordination Cage as Photoregulated Oxidase-Like Nanozyme. , 2020, Journal of the American Chemical Society.

[20]  F. Patolsky,et al.  Direct Detection of Uranyl in Urine by Dissociation from Aptamer-modified Nanosensors Arrays. , 2020, Analytical chemistry.

[21]  S. Dong,et al.  Oxidase-like MOF-818 Nanozyme with High Specificity for Catalysis of Catechol Oxidation. , 2020, Journal of the American Chemical Society.

[22]  Yi He,et al.  Electrostatic-Driven Coordination Interaction Enables High Specificity of UO22+ Peroxidase Mimic for Visual Colorimetric Detection of UO22+ , 2020 .

[23]  Jianding Qiu,et al.  Regenerable Covalent Organic Frameworks for Photo-enhanced Uranium Adsorption from Seawater. , 2020, Angewandte Chemie.

[24]  C. Zhang,et al.  Field-portable ratiometric fluorescence imaging of dual-color label-free carbon dots for uranyl ions detection with cellphone-based optical platform , 2020 .

[25]  Xingguo Chen,et al.  Stable and Reusable Light-responsive Reduced Covalent Organic Framework (COF-300-AR) as Oxidase-mimicking Catalyst for GSH Detection in Cell Lysate. , 2020, ACS applied materials & interfaces.

[26]  Mengxin Zhao,et al.  A highly selective and sensitive colorimetric assay for specific recognition element-free detection of uranyl ion , 2020 .

[27]  Yishan Fang,et al.  Bacterial Detection and Elimination Using a Dual-Functional Porphyrin-Based Porous Organic Polymer with Peroxidase-Like and High Near-Infrared-Light-Enhanced Antibacterial Activity. , 2020, ACS applied materials & interfaces.

[28]  Juewen Liu,et al.  Regenerable and stable sp2 carbon-conjugated covalent organic frameworks for selective detection and extraction of uranium , 2020, Nature Communications.

[29]  Jianding Qiu,et al.  Nanoceria-templated Metal Organic Frameworks with Oxidase-mimicking Activity Boosted by Hexavalent Chromium. , 2019, Analytical chemistry.

[30]  Haijuan Li,et al.  Efficient Electrogenerated Chemiluminescence of Tris(2,2'-bipyridine)ruthenium(II) with N-hydroxysulfosuccinimide as a Coreactant for Selective and Sensitive Detection of L-proline and Mercury (II). , 2019, Analytical chemistry.

[31]  Shaobin He,et al.  Target-triggered inhibiting oxidase-mimicking activity of platinum nanoparticles for ultrasensitive colorimetric detection of silver ion , 2019, Chinese Chemical Letters.

[32]  Christian Ochsenfeld,et al.  Sustained Solar H2 Evolution from a Thiazolo[5,4-d]thiazole-Bridged Covalent Organic Framework and Nickel-Thiolate Cluster in Water , 2019, Journal of the American Chemical Society.

[33]  Min Zhou,et al.  Light-Responsive Metal-Organic Framework as an Oxidase Mimic for Cellular Glutathione Detection. , 2019, Analytical chemistry.

[34]  Xiaogang Qu,et al.  Nanozymes: Classification, Catalytic Mechanisms, Activity Regulation, and Applications. , 2019, Chemical reviews.

[35]  Juewen Liu,et al.  Molecular Imprinting on Inorganic Nanozymes for Hundred-fold Enzyme Specificity. , 2017, Journal of the American Chemical Society.

[36]  N. Khashab,et al.  Colorimetric peroxidase mimetic assay for uranyl detection in sea water. , 2015, ACS applied materials & interfaces.

[37]  H Zhao,et al.  A sensitive resonance light scattering assay for uranyl ion based on the conformational change of a nuclease-resistant aptamer and gold nanoparticles acting as signal reporters , 2014, Microchimica Acta.

[38]  Yi Lu,et al.  A DNAzyme-gold nanoparticle probe for uranyl ion in living cells. , 2013, Journal of the American Chemical Society.

[39]  M. Prodromidis,et al.  An electrochemical sensor for trace uranium determination based on 6-O-palmitoyl-l-ascorbic acid-modified graphite electrodes , 2011 .

[40]  Hoon Sik Kim,et al.  Binding of uranyl ion by a DNA aptamer attached to a solid support. , 2011, Bioorganic & medicinal chemistry letters.

[41]  Yi Lu,et al.  Highly sensitive and selective colorimetric sensors for uranyl (UO2(2+)): development and comparison of labeled and label-free DNAzyme-gold nanoparticle systems. , 2008, Journal of the American Chemical Society.

[42]  R. Shinjo,et al.  Determination of uranium in pore water from coastal sediment by standard addition ICP-MS analysis , 2008 .

[43]  Yi Lu,et al.  A catalytic beacon sensor for uranium with parts-per-trillion sensitivity and millionfold selectivity , 2007, Proceedings of the National Academy of Sciences.