Exploring the Role of Persulfate in the Activation Process: Radical Precursor Versus Electron Acceptor

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School of Civil, Environmental, and Architectural Engineering, Korea University, Seoul 136-701, Korea
Department of Civil and Environmental Engineering, Pusan National University, Busan 46241, Korea
§ School of Civil and Environmental Engineering, Yonsei University, Seoul 120-749, Korea
*E-mail: [email protected]. Phone: +82-2-3290-4864. Fax: +82-2-928-7656.
Cite this: Environ. Sci. Technol. 2017, 51, 17, 10090–10099
Publication Date (Web):July 28, 2017
https://doi.org/10.1021/acs.est.7b02519
Copyright © 2017 American Chemical Society
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Abstract

This study elucidates the mechanism behind persulfate activation by exploring the role of various oxyanions (e.g., peroxymonosulfate, periodate, and peracetate) in two activation systems utilizing iron nanoparticle (nFe0) as the reducing agent and single-wall carbon nanotubes (CNTs) as electron transfer mediators. Since the tested oxyanions serve as both electron acceptors and radical precursors in most cases, oxidative degradation of organics was achievable through one-electron reduction of oxyanions on nFe0 (leading to radical-induced oxidation) and electron transfer mediation from organics to oxyanions on CNTs (leading to oxidative decomposition involving no radical formation). A distinction between degradative reaction mechanisms of the nFe0/oxyanion and CNT/oxyanion systems was made in terms of the oxyanion consumption efficacy, radical scavenging effect, and EPR spectral analysis. Statistical study of substrate-specificity and product distribution implied that the reaction route induced on nFe0 varies depending on the oxyanion (i.e., oxyanion-derived radical), whereas the similar reaction pathway initiates organic oxidation in the CNT/oxyanion system irrespective of the oxyanion type. Chronoamperometric measurements further confirmed electron transfer from organics to oxyanions in the presence of CNTs, which was not observed when applying nFe0 instead.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.7b02519.

  • Intermediate and product distributions obtained in the course of 4-CP oxidation by the nFe0/oxyanion and CNT/oxyanion systems, TEM images of iron nanoparticles, metal contents in pristine CNTs, TEM images of fresh and used CNTs, Raman spectra of fresh and used CNTs, Raman spectra of CNTs in the short and long wavenumber ranges, effects of surfactants on CNTs-mediating persulfate activation, DLS size distributions of pristine CNTs and CNTs exposed to ultrasound, effect of sonication on persulfate activating capacity of CNTs, sorption test with CNTs, release of chloride ions during 4-CP degradation by the activated oxyanions, rate of oxyanion consumption by nFe0 and CNTs, XPS spectra of fresh and used CNTs, FT-IR spectra of fresh and used CNTs, formation of formaldehyde during methanol oxidation by the activated oxyanions, initial rates of degradation of various organics by the activated oxyanions, combined two-way clustering analysis of kinetic data and degradation intermediate data, with a heat map, for two oxyanion-activating groups, linear sweep voltammograms of nFe0- and CNT-coated carbon paper electrodes, and rates of 4-CP degradation by CNT/PMS in water and in deuterium oxide (PDF)

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