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Structure–Property–Toxicity Relationships of Graphene Oxide: Role of Surface Chemistry on the Mechanisms of Interaction with Bacteria

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Download Hi-Res ImageDownload to MS-PowerPointCite This:Environ. Sci. Technol. 2019, 53, 24, 14679-14687
    Article

    Structure–Property–Toxicity Relationships of Graphene Oxide: Role of Surface Chemistry on the Mechanisms of Interaction with Bacteria
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    • Ana C. Barrios
      Ana C. Barrios
      School of Sustainable Engineering and the Built Environment  and  Nanosystems Engineering Research Center for Nanotechnology-Enabled Water Treatment, Arizona State University, Tempe 85287-3005, Arizona, United States
      More by Ana C. Barrios
    • Yan Wang
      Yan Wang
      Department of Civil and Environmental Engineering, University of Pittsburgh, Pittsburgh 15260, Pennsylvania, United States
      More by Yan Wang
      Orcidhttp://orcid.org/0000-0002-9147-1136
    • Leanne M. Gilbertson
      Leanne M. Gilbertson
      Department of Civil and Environmental Engineering  and  Department of Chemical and Petroleum Engineering, University of Pittsburgh, Pittsburgh 15260, Pennsylvania, United States
      More by Leanne M. Gilbertson
    • François Perreault*
      François Perreault
      School of Sustainable Engineering and the Built Environment  and  Nanosystems Engineering Research Center for Nanotechnology-Enabled Water Treatment, Arizona State University, Tempe 85287-3005, Arizona, United States
      *E-mail: [email protected]
      More by François Perreault
      Orcidhttp://orcid.org/0000-0002-4756-8205
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    Environmental Science & Technology

    Cite this: Environ. Sci. Technol. 2019, 53, 24, 14679–14687
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    https://doi.org/10.1021/acs.est.9b05057
    Published November 7, 2019
    Copyright © 2019 American Chemical Society
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    Abstract

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    Graphene oxide (GO) is an antimicrobial agent with tunable surface chemistry. To identify the physicochemical determinants of GO’s antimicrobial activity, we generated different modified Hummer’s GO materials thermally annealed at 200, 500, or 800 °C (TGO200, TGO500, and TGO800, respectively) to modify the surface oxygen groups on the material. Plating assays show that as-received GO (ARGO) and TGO200, TGO500, and TGO800 reduce Escherichia coli viability by 50% (EC50) at 183, 143, 127, and 86 μg/mL, respectively, indicating higher bacterial toxicity as ARGO is reduced. To uncover the toxicity mechanism of GO, fluorescent dye-based assays were used to measure oxidative stress at the EC50. ARGO showed an increase in intracellular reactive oxygen species, measured as an increase in 2′,7′-dichlorodihydrofluorescein diacetate fluorescence, whereas TGO500 and TGO800 induced an increase in the fluorescence of fluorescein diacetate (FDA) by 30 and 42%, suggesting a decrease in cell permeability. Because of a possible wrapping mechanism, plating assays after post-exposure sonication were performed to explain TGO’s low oxidative response and high FDA levels. Results show no difference in colony-forming units, indicating that inhibition of cell growth is a result of the adsorption of bacterial cells on the GO material. By comparing different GO samples at their EC50, this study reveals that reduction of GO alters both the mechanisms of cellular interaction and the degree of toxicity to bacteria.

    Copyright © 2019 American Chemical Society

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    • Impurities in ARGO and TGOs; XPS peak deconvolution of ARGO and TGOs; EC50 values of ARGO and TGOs; statistical data and parameters of ARGO and TGOs after sigmoidal dose–response fit; dye fluorescence of FDA, BODIPY, and ROS with statistical data; SEM micrographs and size distribution histograms of ARGO and TGO800; sigmoidal fit of dose–response curves for ARGO and TGOs; linear fit of EC50 values for ARGO and TGOs with respect to oxygen functional groups; and SEM micrographs of E. coli cells exposed to ARGO and TGO800 (PDF)

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    Cite this: Environ. Sci. Technol. 2019, 53, 24, 14679–14687
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.est.9b05057
    Published November 7, 2019
    Copyright © 2019 American Chemical Society
    Request reuse permissions

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