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Ground State Reactions of nC60 with Free Chlorine in Water

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    Ground State Reactions of nC60 with Free Chlorine in Water
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    † Department of Energy, Environmental and Chemical Engineering, Washington University in St. Louis, St. Louis, Missouri 63130, United States
    ‡ Department of Chemistry, Rice University, Houston, Texas 77005, United States
    *Phone: +1-314-935-9293; fax: +1-314-935-5464; e-mail: [email protected]
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    Environmental Science & Technology

    Cite this: Environ. Sci. Technol. 2016, 50, 2, 721–731
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    https://doi.org/10.1021/acs.est.5b04368
    Published December 14, 2015
    Copyright © 2015 American Chemical Society
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    Abstract

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    Facile, photoenhanced transformations of water-stable C60 aggregates (nC60) to oxidized, soluble fullerene derivatives, have been described as key processes in understanding the ultimate environmental fate of fullerene based materials. In contrast, fewer studies have evaluated the aqueous reactivity of nC60 during ground-state conditions (i.e., dark conditions). Herein, this study identifies and characterizes the physicochemical transformations of C60 (as nC60 suspensions) in the presence of free chlorine, a globally used chemical oxidant, in the absence of light under environmentally relevant conditions. Results show that nC60 undergoes significant oxidation in the presence of free chlorine and the oxidation reaction rates increase with free chlorine concentration while being inversely related to solution pH. Product characterization by FTIR, XPS, Raman Spectroscopy, TEM, XRD, TOC, collectively demonstrates that oxidized C60 derivatives are readily formed in the presence of free chlorine with extensive covalent oxygen and even chlorine additions, and behave as soft (or loose) clusters in solution. Aggregation kinetics, as a function of pH and ionic strength/type, show a significant increase in product stabilities for all cases evaluated, even at pH values approaching 1. As expected with increased (surface) oxidation, classic Kow partitioning studies indicate that product clusters are relatively more hydrophilic than parent (reactant) nC60. Taken together, this work highlights the importance of understanding nanomaterial reactivity and the identification of corresponding stable daughter products, which are likely to differ significantly from parent material properties and behaviors.

    Copyright © 2015 American Chemical Society

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.5b04368.

    • Seven supporting figures and one supporting table. This material is available free of charge via the Internet at http://pubs.acs.org/ (PDF)

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    This article is cited by 21 publications.

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    Environmental Science & Technology

    Cite this: Environ. Sci. Technol. 2016, 50, 2, 721–731
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.est.5b04368
    Published December 14, 2015
    Copyright © 2015 American Chemical Society
    Request reuse permissions

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