Mechanism of Base Activation of Persulfate

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Department of Civil & Environmental Engineering, Washington State University, Pullman, Washington 99164-2910
* Corresponding author phone: (509)335-3761; fax: (509)335-7632; e-mail: [email protected]
Cite this: Environ. Sci. Technol. 2010, 44, 16, 6423–6428
Publication Date (Web):July 16, 2010
https://doi.org/10.1021/es1013714
Copyright © 2010 American Chemical Society
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Abstract

Base is the most commonly used activator of persulfate for the treatment of contaminated groundwater by in situ chemical oxidation (ISCO). A mechanism for the base activation of persulfate is proposed involving the base-catalyzed hydrolysis of persulfate to hydroperoxide anion and sulfate followed by the reduction of another persulfate molecule by hydroperoxide. Reduction by hydroperoxide decomposes persulfate into sulfate radical and sulfate anion, and hydroperoxide is oxidized to superoxide. The base-catalyzed hydrolysis of persulfate was supported by kinetic analyses of persulfate decomposition at various base:persulfate molar ratios and an increased rate of persulfate decomposition in D2O vs H2O. Stoichiometric analyses confirmed that hydroperoxide reacts with persulfate in a 1:1 molar ratio. Addition of hydroperoxide to basic persulfate systems resulted in rapid decomposition of the hydroperoxide and persulfate and decomposition of the superoxide probe hexachloroethane. The presence of superoxide was confirmed with scavenging by Cu(II). Electron spin resonance spectroscopy confirmed the generation of sulfate radical, hydroxyl radical, and superoxide. The results of this research are consistent with the widespread reactivity reported for base-activated persulfate when it is used for ISCO.

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Figure S1: effect of ionic strength on persulfate degradation rate (further supports the base-catalyzed hydrolysis of persulfate) and Figure S2: effect of varying base:persulfate ratio on the degradation rate of added H2O2+HO2 (further supports the role of hydroperoxide in persulfate degradation). This material is available free of charge via the Internet at http://pubs.acs.org.

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