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LABORATORY COMPARISON OF nZVI / S-nZVI EFFICIENCY IN SYSTEMS WITH AND WITHOUT POWER
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Iron-based materials used in water treatment and groundwater remediation—especially micro- and nano-sized zerovalent iron (nZVI)—can be more effective when modified with lower-valent forms of sulfur (i.e., “sulfidated”). Controlled sulfidation for this purpose (using sulfide, dithionite, etc.) is the main topic of this review, but insights are derived by comparison with related and comparatively well-characterized processes such as corrosion of iron in sulfidic waters and abiotic natural attenuation by iron sulfide minerals. Material characterization shows that varying sulfidation protocols (e.g., concerted or sequential) and key operational variables (e.g., S/Fe ratio and sulfidation duration) result in materials with structures and morphologies ranging from core-shell to multiphase. A meta-analysis of available kinetic data for dechlorination under anoxic conditions, shows that sulfidation usually increases dechlorination rates, and simultaneously hydrogen production is suppressed. Therefore, sulfidation can greatly improve the efficiency of utilization of reducing equivalents for contaminant removal. This benefit is most likely due to inhibited corrosion as a result of sulfidation. Sulfidation may also favor desirable pathways of contaminant removal, such as (i) dechlorination by reductive elimination rather than hydrogenolysis and (ii) sequestration of metals as sulfides that could be resistant to reoxidation. Under oxic conditions, sulfidation is shown to enhance heterogeneous catalytic oxidation of contaminants. These net effects of sulfidation on contaminant removal by iron-based materials may substantially improve its practical utility for water treatment and remediation of contaminated groundwater.
Direct injection of reactive nanoscale zerovalent iron particles (NZVI) is considered to be a promising approach for remediation of aquifers contaminated by chlorinated organic pollutants. In this study we show that the extent of sulfidation of NZVI enhances the rate of dechlorination of trichloroethylene (TCE) compared to that by unamended NZVI, and the enhancement depends on the Fe/S molar ratio. Experiments where TCE was reacted with NZVI sulfidated to different extents (Fe/S molar ratios 0.62-66) showed that the surface-area normalized first-order TCE degradation rate constant increased up to 40 folds compared to non-sulfidated NZVI. Fe/S ratios in the range of 12-25 provided the highest TCE dechlorination rates, and rates decreased at both higher and lower Fe/S. In contrast, sulfidated NZVI exposed to water in the absence of TCE showed significantly lower hydrogen evolution rate (2.75 μmol L(-1) h(-1)) compared to that by an unamended NZVI (6.92 μmol L(-1) h(-1)), indicating that sulfidation of NZVI suppressed corrosion reactions with water. Sulfide (HS(-)) ions reacted rapidly with NZVI and X-ray photoelectron spectroscopy analyses showed formation of a surface layer of FeS and FeS2. We propose that more electrons are preferentially conducted from sulfidated NZVI than from unamended NZVI to TCE, likely because of greater binding of TCE on the reactive sites of the iron sulfide outer layer. Resuspending sulfidated NZVI in sulfide-free or sulfide containing solutions altered the TCE degradation rate constants because of changes in the FeS layer thickness. Sulfidated NZVI maintained its high reactivity in the presence of multiple mono and divalent ions and with polyelectrolyte coatings. Thus, sulfide ions in groundwater can significantly alter NZVI reactivity.
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Recent industrial and urban activities have led to elevated concentrations of a wide range of contaminants in groundwater and wastewater, which affect the health of millions of people worldwide. In recent years, the use of zero-valent iron (ZVI) for the treatment of toxic contaminants in groundwater and wastewater has received wide attention and encouraging treatment efficiencies have been documented. This paper gives an overview of the recent advances of ZVI and progress obtained during the groundwater remediation and wastewater treatment utilizing ZVI (including nanoscale zero-valent iron (nZVI)) for the removal of: (a) chlorinated organic compounds, (b) nitroaromatic compounds, (c) arsenic, (d) heavy metals, (e) nitrate, (f) dyes, and (g) phenol. Reaction mechanisms and removal efficiencies were studied and evaluated. It was found that ZVI materials with wide availability have appreciable removal efficiency for several types of contaminants. Concerning ZVI for future research, some suggestions are proposed and conclusions have been drawn.
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