4.2 Article

Gallic Acid Accelerates the Oxidation Ability of the Peracetic Acid/Fe(III) System for Bisphenol A Removal: Fate of Various Radicals

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ACS ES&T ENGINEERING
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AMER CHEMICAL SOC
DOI: 10.1021/acsestengg.2c00301

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peracetic acid activation; gallic acid; Fe(II); Fe(III) cycle; organic radicals; micropollutant removal

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In this study, it was found that natural polyphenols can assist in the activation of peracetic acid by conveniently obtained Fe(III), leading to efficient removal of bisphenol A. Hydroxyl radicals (center dot OH) are the main contributors to BPA degradation, with superoxide radicals (O2 center dot-) functioning as intermediates. The reaction intermediates between polyphenols and reactive oxygen species play a crucial role in the regeneration of Fe(II) and enhanced activation of peracetic acid.
Conveniently and cost-effectively obtained Fe(III) can be utilized for peracetic acid (PAA) activation in the presence of natural polyphenols. However, the effect of polyphenols on the fate of generated reactive oxygen species (ROS) remains unclear. In this study, it was demonstrated that Fe(III) can efficiently trigger PAA oxidation of pollutants with the assistance of gallic acid (GA), a widely distributed natural polyphenol. The GA/Fe(III)/PAA system efficiently removed bisphenol A (BPA) over a wide initial pH range of 4.0-7.0, with a removal rate of >90% over 20 min. Further, center dot OH played a dominant role in BPA degradation, and O2 center dot- functioned as an intermediate contributing to the partial generation of center dot OH. The generated organic radicals (R-O center dot) did not considerably contribute to BPA removal. Apart from GA itself, both the reaction intermediates (phenoxy radicals) of GA with ROS and BPA degradation intermediates were crucial for the regeneration of Fe(II) from Fe(III) and the subsequent enhanced activation of PAA. Notably, further comprehensive analysis revealed an increase in center dot OH yield, but a decrease in R-O center dot production as the dosage of GA was increased from 10 to 100 mu M. This finding emphasized the importance of properly utilizing GA, considering the reactivity of varied ROS toward different contaminants. R-O center dot (CH3CO2 center dot and CH3CO3 center dot) was quickly consumed by the GA-Fe(II) complex through single-electron transfer (SET) and/or by GA via H-abstraction (HAA). This study proposes a promising strategy for improving the Fe(III)/PAA process and advances the understanding of the trade-off between radical generation and elimination by polyphenols in PAA-based advanced oxidation processes (AOPs).

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