Visible light and fulvic acid assisted generation of Mn(III) to oxidize bisphenol A: The effect of tetrabromobisphenol A.

Visible light and fulvic acid assisted generation of Mn(III) to oxidize bisphenol A: The effect of tetrabromobisphenol A.
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可见光和黄腐酸辅助生成 Mn(III) 氧化双酚 A:四溴双酚 A 的作用。

DOI:
10.1016/j.watres.2019.115273
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发表时间:
2019-11
期刊:
影响因子:
12.8
通讯作者:
Wang Zunyao
Wang Zunyao
中科院分区:
环境科学与生态学1区
文献类型:
--
作者:
Yao Jiayi;Qu Ruijuan;Wang Xinghao;Sharma Virender K;Shad Asam;Dar Afzal Ahmed;Wang Zunyao

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双酚A (BPA)和四溴双酚A (TBBPA)是内分泌干扰化合物(EDCs),近年来受到越来越多的关注。本文研究了含黄腐酸(FA)和MnSO4(Mn(II))的可见光(VL) (λ ≥ 420 nm)辐照溶液对BPA的去除,并探讨了TBBPA对BPA转化的可能影响。反应72 h后,BPA的去除率为69%。不同的氧化物种鉴定实验结果表明,可溶性锰(Mn(III))在双酚a的转化中起主导作用。VL/FA/Mn(II)体系对BPA的转化是在没有TBBPA共存的情况下通过自齐聚实现的。当BPA与TBBPA共存时,由于与有效态Mn(III)的竞争以及两种EDCs之间可能发生交叉偶联反应,BPA的去除在很大程度上受到抑制。通过产品分析和密度泛函理论(DFT)的计算进一步阐明了这一现象。产生交叉偶联产物的能量差(ΔE)为−23.4 kJ mol−1,远低于BPA或TBBPA自偶联产物ΔEfor的正值,表明BPA和TBBPA之间的交叉偶联反应可能比各自的自偶联反应更容易发生。毒性试验表明,VL/FA/Mn(II)体系显著降低了BPA反应溶液的总雌激素活性。总的来说,我们的研究为共存的EDCs在水溶液中被原位形成的Mn(III)转化提供了新的见解。
Bisphenol A (BPA) and tetrabromobisphenol A (TBBPA), endocrine disrupting compounds (EDCs), are of increasing concerns for many years. This paper presents the elimination of BPA under visible light (VL) (λ ≥ 420 nm) irradiated solutions containing fulvic acid (FA) and MnSO4(Mn(II)), and examines the possible effects of TBBPA on the transformation of BPA. After 72 h of reaction time, the removal efficiency of BPA in the studied system was 69%. Results of different experiments to identify oxidative species suggested the dominate role of soluble manganese (III) (Mn(III)) in the conversion of BPA. The transformation of BPA by the VL/FA/Mn(II) system was through self-oligomerization in absence of co-existence of TBBPA. In the co-existence of BPA with TBBPA, the removal of BPA was largely inhibited due to the competition with available Mn(III) and the possible occurrence of cross-coupling reactions between the two EDCs. This phenomenon was further elucidated by product analyses and density functional theory (DFT) calculations. The energy difference (ΔE) for generating a cross-coupling product was calculated as −23.4 kJ mol−1, much lower than the positive values of ΔEfor self-coupling products of BPA or TBBPA, demonstrating that cross-coupling reactions between BPA and TBBPA likely occurred easier than the respective self-coupling reactions. The toxicity test showed that the overall estrogenic activity of BPA reaction solution was significantly decreased by the VL/FA/Mn(II) system. In general, our study provided new insights into the transformation of co-existing EDCs byin situformed Mn(III) in aqueous solution.
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