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Fluorescent DNA Probing Nanoscale MnO2: Adsorption, Dissolution by Thiol, and Nanozyme Activity

  • Liu Wang
    Liu Wang
    College of Biosystems Engineering and Food Science, Zhejiang University, Hangzhou 310058, China
    Department of Chemistry, Waterloo Institute for Nanotechnology, University of Waterloo, Waterloo N2L 3G1, Ontario, Canada
    More by Liu Wang
  • , 
  • Zhicheng Huang
    Zhicheng Huang
    Department of Chemistry, Waterloo Institute for Nanotechnology, University of Waterloo, Waterloo N2L 3G1, Ontario, Canada
    More by Zhicheng Huang
  • , 
  • Yibo Liu
    Yibo Liu
    Department of Chemistry, Waterloo Institute for Nanotechnology, University of Waterloo, Waterloo N2L 3G1, Ontario, Canada
    More by Yibo Liu
  • , 
  • Jian Wu*
    Jian Wu
    College of Biosystems Engineering and Food Science, Zhejiang University, Hangzhou 310058, China
    *E-mail: [email protected] (J.W.).
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    Orcidhttp://orcid.org/0000-0003-4518-7027
  • , and 
  • Juewen Liu*
    Juewen Liu
    Department of Chemistry, Waterloo Institute for Nanotechnology, University of Waterloo, Waterloo N2L 3G1, Ontario, Canada
    *E-mail: [email protected] (J.L.).
    More by Juewen Liu
    Orcidhttp://orcid.org/0000-0001-5918-9336
Cite this: Langmuir 2018, 34, 9, 3094–3101
Publication Date (Web):February 19, 2018
https://doi.org/10.1021/acs.langmuir.7b03797
Copyright © 2018 American Chemical Society
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    Abstract

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    Manganese dioxide (MnO2) is an interesting material due to its excellent biocompatibility and magnetic properties. Adsorption of DNA to MnO2 is potentially of interest for drug delivery and sensing applications. However, little fundamental understanding is known about their interactions. In this work, carboxyfluorescein (FAM)-labeled DNA oligonucleotides were used to explore the effect of salt concentration, pH, and DNA sequence and length for adsorption by MnO2, and comparisons were made with graphene oxide (GO). The DNA desorbs from MnO2 by free inorganic phosphate, while it desorbs from GO by adenosine and urea. Therefore, DNA is mainly adsorbed on MnO2 through its phosphate backbone, and DNA has a stronger affinity on MnO2 than on GO based on a salt-shock assay. At the same time, DNA was used to study the effect of thiol containing compounds on the dissolution of MnO2. Adsorbed DNA was released from MnO2 after its dissolution by thiol, but not from other metal oxides with lower solubility such as CeO2, TiO2, and Fe3O4. DNA-functionalized MnO2 was then used for detecting glutathione (GSH) with a detection limit of 383 nM. Finally, DNA was found to inhibit the peroxidase-like activity of MnO2. This study has offered many fundamental insights into the interaction between MnO2 and two important biomolecules: DNA and thiol-containing compounds.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.langmuir.7b03797.

    • DNA sequences employed in this work (Table S1); XRD spectrum of MnO2 (Figure S1); surface area measurement of MnO2 and GO using methylene blue (Figure S2); the effect of MnO2 (Figure S3) and GO (Figure S4) on the fluorescence intensity of free fluorescein and FAM-A15; the fluorescence of FAM-DNA quenched by MnCl2 and MnO2 (Figure S5); and the percentage of DNA adsorbed at pH 5 and pH 7.5 (Figure S6) (PDF)

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