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Iron and Sulfur Precursors Affect Crystalline Structure, Speciation, and Reactivity of Sulfidized Nanoscale Zerovalent Iron

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    Treatment and Resource Recovery

    Iron and Sulfur Precursors Affect Crystalline Structure, Speciation, and Reactivity of Sulfidized Nanoscale Zerovalent Iron
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    • Jiang Xu
      Jiang Xu
      Department of Civil and Environmental Engineering, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States
      Center for Environmental Implications of NanoTechnology, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States
      More by Jiang Xu
      Orcidhttp://orcid.org/0000-0003-0369-4848
    • Astrid Avellan
      Astrid Avellan
      Department of Civil and Environmental Engineering, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States
      Center for Environmental Implications of NanoTechnology, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States
      More by Astrid Avellan
      Orcidhttp://orcid.org/0000-0001-6081-4389
    • Hao Li
      Hao Li
      Department of Chemistry and the Oden Institute for Computational Engineering and Sciences, The University of Texas at Austin, Austin, Texas 78712, United States
      More by Hao Li
    • Elizabeth A. Clark
      Elizabeth A. Clark
      Department of Materials Science and Engineering, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States
      More by Elizabeth A. Clark
    • Graeme Henkelman
      Graeme Henkelman
      Department of Chemistry and the Oden Institute for Computational Engineering and Sciences, The University of Texas at Austin, Austin, Texas 78712, United States
      More by Graeme Henkelman
      Orcidhttp://orcid.org/0000-0002-0336-7153
    • Rälf Kaegi
      Rälf Kaegi
      Eawag, Swiss Federal Institute of Aquatic Science and Technology, Überlandstrasse 133, 8600 Dübendorf, Switzerland
      More by Rälf Kaegi
      Orcidhttp://orcid.org/0000-0002-2430-4733
    • Gregory V. Lowry*
      Gregory V. Lowry
      Department of Civil and Environmental Engineering, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States
      Center for Environmental Implications of NanoTechnology, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, United States
      *Email: [email protected]. Phone: (412) 268-2948. Fax: (412) 268-7813.
      More by Gregory V. Lowry
      Orcidhttp://orcid.org/0000-0001-8599-008X
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    Cite this: Environ. Sci. Technol. 2020, 54, 20, 13294–13303
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    https://doi.org/10.1021/acs.est.0c03879
    Published September 23, 2020
    Copyright © 2020 American Chemical Society
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    Abstract

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    The reactivity of sulfidized nanoscale zerovalent iron (SNZVI) is affected by the amount and species of sulfur in the materials. Here, we assess the impact of the Fe (Fe2+ and Fe3+) and S (S2O42–, S2–, and S62–) precursors used to synthesize both NZVI and SNZVI on the resulting physicochemical properties and reactivity and selectivity with water and trichloroethene (TCE). X-ray diffraction indicated that the Fe precursors altered the crystalline structure of both NZVI and SNZVI. The materials made from the Fe3+ precursor had an expanded lattice in the Fe0 body-centered-cubic (BCC) structure and lower electron-transfer resistance, providing higher reactivity with water (∼2–3 fold) and TCE (∼5–13 fold) than those made from an Fe2+ precursor. The choice of the S precursor controlled the S speciation in the SNZVI particles, as indicated by X-ray absorption spectroscopy. Iron disulfide (FeS2) was the main S species of SNZVI made from S2O42–, whereas iron sulfide (FeS) was the main S species of SNZVI made from S2–/S62–. The former SNZVI was more hydrophobic, reactive with, and selective for TCE compared to the latter SNZVI. These results suggest that the Fe and S precursors can be used to select the conditions of the synthesis process and provide selected physicochemical properties (e.g., S speciation, hydrophobicity, and crystalline structure), reactivity, and selectivity of the SNZVI materials.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.0c03879.

    • Dechlorination rate of antibiotic florfenicol by NZVI and SNZVI with Fe2+ or Fe3+ precursors, properties and reactivity of NZVI and SNZVI made from FeCl2, TEM images and elemental distribution of NZVI and SNZVI; surface area, XRD patterns and Rietveld refinement, XPS analysis, EIS analysis, accumulated H2 with or without TCE, TCE and its main degradation products of NZVI and SNZVI with different precursors (PDF)

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    Cite this: Environ. Sci. Technol. 2020, 54, 20, 13294–13303
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