Gallic Acid Accelerates the Oxidation Ability of the Peracetic Acid/Fe(III) System for Bisphenol A Removal: Fate of Various Radicals
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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DOI：
10.1021/acsestengg.2c00301
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发表时间：
2023-01
期刊：
影响因子：
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通讯作者：
Shurun Yang;Zi-Han Liang;Yaning Wen;Chuanshu He;Z. Xiong;Yelei Du;Yang Liu;Heng Zhang
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文献类型：
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作者：
Shurun Yang;Zi-Han Liang;Yaning Wen;Chuanshu He;Z. Xiong;Yelei Du;Yang Liu;Heng Zhang
在天然多酚的存在下，方便且成本有效地获得的Fe（III）可用于过乙酸（PAA）活化。然而，多酚对产生的活性氧（ROS）的命运的影响仍然不清楚。在这项研究中，它被证明，铁（III）可以有效地触发PAA氧化污染物的援助，没食子酸（GA），一种广泛分布的天然多酚。GA/Fe（III）/PAA体系在较宽的初始pH范围内（4.0-7.0）对双酚A（BPA）的去除率均大于90%。此外，·OH在BPA的降解过程中起主导作用，O2·-作为中间体参与了·OH的部分生成。生成的有机自由基（R-O·）对BPA的去除没有显著贡献。除了GA本身之外，GA与ROS和BPA降解中间体的反应中间体（苯氧基自由基）对于从Fe（III）再生Fe（II）和随后增强PAA的活化都是至关重要的。进一步的综合分析表明，随着GA用量从10 μ M增加到100 μM，·OH产量增加，但R-O·产量下降。这一发现强调了适当利用GA的重要性，考虑到不同的ROS对不同污染物的反应性。R-O·（CH_3CO_2·和CH_3CO_3·）通过单电子转移（SET）和（或）通过抽氢（HAA）被GA-Fe（II）络合物迅速消耗。这项研究提出了一个很有前途的策略，为改善Fe（III）/PAA过程和进步的自由基生成和消除之间的权衡PAA为基础的高级氧化过程（AOPs）的多酚的理解。
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, •OH played a dominant role in BPA degradation, and O2•–functioned as an intermediate contributing to the partial generation of •OH. The generated organic radicals (R-O•) 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 •OH yield, but a decrease in R-O• production as the dosage of GA was increased from 10 to 100 μM. This finding emphasized the importance of properly utilizing GA, considering the reactivity of varied ROS toward different contaminants. R-O• (CH3CO2• and CH3CO3•) 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).