Mechanisms of Sb(III) Oxidation by Pyrite-Induced Hydroxyl Radicals and Hydrogen Peroxide

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State Key Laboratory of Water Environment Simulation, School of Environment, Beijing Normal University, Beijing 100875, P.R. China
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Cite this: Environ. Sci. Technol. 2015, 49, 6, 3499–3505
Publication Date (Web):February 25, 2015
https://doi.org/10.1021/es505584r
Copyright © 2015 American Chemical Society
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Abstract

Antimony (Sb) is an element of growing interest, and its toxicity and mobility are strongly influenced by redox processes. Sb(III) oxidation mechanisms in pyrite suspensions were comprehensively investigated by kinetic measurements in oxic and anoxic conditions and simulated sunlight. Sb(III) was oxidized to Sb(V) in both solution and on pyrite surfaces in oxic conditions; the oxidation efficiency of Sb(III) was gradually enhanced with the increase of pH. The pyrite-induced hydroxyl radical (·OH) and hydrogen peroxide (H2O2) are the oxidants for Sb(III) oxidation. ·OH is the oxidant for Sb(III) oxidation in acidic solutions, and H2O2 becomes the main oxidant in neutral and alkaline solutions. ·OH and H2O2 can be generated by the reaction of previously existing FeIII(pyrite) and H2O on pyrite in anoxic conditions. The oxygen molecule is the crucial factor in continuously producing ·OH and H2O2 for Sb(III) oxidation. The efficiency of Sb(III) oxidation was enhanced in surface-oxidized pyrite (SOP) suspension, more ·OH formed through Fenton reaction in acidic solutions, but Fe(IV) and H2O2 were formed in neutral and alkaline solutions. Under the illumination of simulated sunlight, more ·OH and H2O2 were produced in the pyrite suspension, and the oxidation efficiency of Sb(III) was remarkably enhanced. In conclusion, Sb(III) can be oxidized to Sb(V) in the presence of pyrite, which will greatly influence the fate of Sb(III) in the environment.

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Details of SEM, EDS and XRD analysis of pyrite and SOP, photochemical reactor, Sb(III)/TSb changes in solution in the absence of pyrite, XPS analysis of Sb speciation, ESR spectra in dark and light generated by pyrite, Sb(III) oxidation by H2O2, Fe2+ and Fe3+ and XPS analysis of Fe 2p on the surface of SOP. This material is available free of charge via the Internet at http://pubs.acs.org.

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