4.8 Article

Effect of Metal Ions on Oxidation of Micropollutants by Ferrate(VI): Enhancing Role of FeIV Species

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ENVIRONMENTAL SCIENCE & TECHNOLOGY
卷 55, 期 1, 页码 623-633

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AMER CHEMICAL SOC
DOI: 10.1021/acs.est.0c04674

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  1. National Science Foundation [CBET 1802944, CBET 1802800]

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This study investigated the oxidation of recalcitrant micropollutants by combining Fe-VI and Fe(III), finding that the addition of Fe(III) enhances the oxidation process. Fe-IV was identified as the main species contributing to the increase in ATL removal, with natural organic matter inhibiting the removal of pollutants.
This paper investigated the oxidation of recalcitrant micropollutants [i.e., atenolol (ATL), flumequine, aspartame, and diatrizoic acid] by combining ferrate(VI) ((FeO42-)-O-VI, Fe-VI) with a series of metal ions [i.e., Fe(III), Ca(II), Al(III), Sc(III), Co(II), and Ni(II)]. An addition of Fe(III) to Fe-VI enhanced the oxidation of micropollutants compared solely to Fe-VI. The enhanced oxidation of studied micropollutants increased with increasing [Fe(III)]/[Fe-VI] to 2.0. The complete conversion of phenyl methyl sulfoxide (PMSO), as a probe agent, to phenyl methyl sulfone (PMSO2) by the Fe-VI-Fe(III) system suggested that the highly reactive intermediate Fe-IV/Fe-V species causes the increased oxidation of all four micropollutants. A kinetic modeling of the oxidation of ATL demonstrated that the major species causing the increase in ATL removal was Fe-IV, which had an estimated rate constant as (6.3 +/- 0.2) x 10(4) M-1 s(-1), much higher than that of Fe-VI [(5.0 +/- 0.4) x 10(-1) M-1 s(-1)]. Mechanisms of the formed oxidation products of ATL by Fe-IV, which included aromatic and/or benzylic oxidation, are delineated. The presence of natural organic matter significantly inhibited the removal of four pollutants by the Fe-VI-Fe(III) system. The enhanced effect of the Fe-VI-Fe(III) system was also seen in the oxidation of the micropollutants in river water and lake water.

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