Advanced Electrochemical Oxidation of 1,4-Dioxane via Dark Catalysis by Novel Titanium Dioxide (TiO2) Pellets

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Department of Chemistry, Department of Soil and Crop Sciences and §Department of Civil and Environmental Engineering, Colorado State University, Fort Collins, Colorado 80523, United States
*Phone: 1-970-491-8880; fax: 1-970-491-8224; e-mail: [email protected]
Cite this: Environ. Sci. Technol. 2016, 50, 16, 8817–8826
Publication Date (Web):July 15, 2016
https://doi.org/10.1021/acs.est.6b02183
Copyright © 2016 American Chemical Society
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Abstract

1,4-dioxane is an emerging groundwater contaminant with significant regulatory implications. Because it is resistant to traditional groundwater treatments, remediation of 1,4-dioxane is often limited to costly ex situ UV-based advanced oxidation. By varying applied voltage, electrical conductivity, seepage velocity, and influent contaminant concentration in flow-through reactors, we show that electrochemical oxidation is a viable technology for in situ and ex situ treatment of 1,4-dioxane under a wide range of environmental conditions. Using novel titanium dioxide (TiO2) pellets, we demonstrate for the first time that this prominent catalyst can be activated in the dark even when electrically insulated from the electrodes. TiO2-catalyzed reactors achieved efficiencies of greater than 97% degradation of 1,4-dioxane, up to 4.6 times higher than noncatalyzed electrolytic reactors. However, the greatest catalytic enhancement (70% degradation versus no degradation without catalysis) was observed in low-ionic-strength water, where conventional electrochemical approaches notoriously fail. The TiO2 pellet’s dark-catalytic oxidation activity was confirmed on the pharmaceutical lamotrigine and the industrial solvent chlorobenzene, signifying that electrocatalytic treatment has tremendous potential as a transformative remediation technology for persistent organic pollutants in groundwater and other aqueous environments.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.6b02183.

  • Details on analytical methods and experimental design, TiO2 pellet fabrication, catalyst characterization, FTER results, and additional mechanistic experiments. Figures showing key steps in the process of making catalytic TiO2 pellets to be used as interelectrode catalysts, photo of a FTER with inter-electrode TiO2 pellets between four working electrodes, experimental set up showing the noncatalyzed control FTER with inter-electrode glass beads and the TiO2-catalyzed FTER, circular Ti–IrO2-Ta2O5 mesh electrode, a top-view of the pulverized TiO2 after shaking pellets in the glass vial, schematic of FTER, chemical structures of persistent organic pollutants, SEM images of TiO2 pellet surface, data characterizing TiO2 pellets sintered for 4 hours, relative distribution of initial TOC, schematic showing the top view of a concentric cylindrical electrode batch reactor with Nafion membrane to separate inner anodic chamber from the outer cathodic chamber, and degradation efficiencies of 1,4-dioxane in 5.0 cm I.D. flow-through electrochemical reactors. Tables showing results and test criteria used to evaluate mechanical stability of finished TiO2 pellets, summary of results from FTER experiments, flow-parameter calculations using hydraulic mass continuity and Darcy equations, triplicate TOC data, and chromatographic retention times and ESI-TOF-MS data for dioxane intermediates. (PDF)

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