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亚硫酸氢盐促进了微摩尔级铁对过硫酸盐的活化以降解双酚A。

Hydrogen sulfite promoted the activation of persulfate by μM Fe for bisphenol A degradation.

作者信息

Chen Shiyao, Yan Caixia, Nie Minghua, Wu Leliang, Ding Mingjun, Wang Peng

机构信息

School of Geography and Environment, Key Laboratory of Poyang Lake Wetland and Watershed Research, Ministry of Education, Jiangxi Normal University, Nanchang, 330022, China.

Key Laboratory of Eco-Geochemistry, Ministry of Natural Resource, Beijing, 100037, China.

出版信息

Environ Sci Pollut Res Int. 2022 Dec;29(56):85185-85201. doi: 10.1007/s11356-022-21801-x. Epub 2022 Jul 6.

Abstract

This study evaluated the improvement of bisphenol A (BPA) elimination through hydrogen sulfite (HS) coupling with persulfate (PS) activated by low amounts of Fe. Under the optimum condition (10 μM Fe, 0.6 mM HS, 0.8 mM PS, pH = 4.0), 100% BPA (5 μM) was removed within 15 min. Sulfate radical (SO) and singlet oxygen (O) were confirmed as the primary active species for BPA degradation in the Fe/HS/PS system, and the steady-state concentration of SO and O was 2.43 × 10 M and 1.67 × 10 M, respectively. Besides, FeHSO and FeOHSOH were the main iron species in the Fe/HS/PS system. The removal potency of BPA depended on the operation parameters, such as chemical reagent dosages, reaction temperature, and the solution initial pH. The impact of NO, SO, and humic acid (HA) on BPA removal was negligible, whereas Cl, HCO, and HPO restrained BPA decomposition. Two injections of HS could improve the limitation of BPA degradation efficiency due to the rapid consumption of HS in the reaction process. The lower removal efficiency of BPA was observed in real water matrices than that in ultrapure water. Whatever, up to 58.1%, 66.3%, 68.1%, and 88.1% of BPA were removed from domestic wastewater, lake water, river water, and tap water within 10 min, respectively. In addition, the BPA degradation process was characterized by the 3D fluorescence spectra technique, which indicated the BPA oxidation intermediates also have fluorescence characteristics. Moreover, 6 intermediate products were identified, and the possible degradation pathways of BPA were proposed. Additionally, the Fe/HS/PS system also exerted an excellent performance for the removal of other representative organic contaminants including enrofloxacin, acid orange 7, acetaminophen, and phenol. All results indicated that the Fe/HS/PS system could be a promising method for organic pollutant removal.

摘要

本研究评估了通过低量铁活化的亚硫酸氢盐(HS)与过硫酸盐(PS)耦合来提高双酚A(BPA)的去除效果。在最佳条件(10 μM铁、0.6 mM HS、0.8 mM PS、pH = 4.0)下,15分钟内5 μM的BPA被100%去除。硫酸根自由基(SO)和单线态氧(O)被确认为Fe/HS/PS体系中BPA降解的主要活性物种,且SO和O的稳态浓度分别为2.43×10 M和1.67×10 M。此外,FeHSO和FeOHSOH是Fe/HS/PS体系中的主要铁物种。BPA的去除效能取决于操作参数,如化学试剂用量、反应温度和溶液初始pH。NO、SO和腐殖酸(HA)对BPA去除的影响可忽略不计,而Cl、HCO和HPO则抑制BPA的分解。由于反应过程中HS的快速消耗,分两次注入HS可改善BPA降解效率的限制。在实际水体基质中观察到的BPA去除效率低于超纯水。无论如何,在10分钟内分别从生活污水、湖水、河水和自来水中去除了高达58.1%、66.3%、68.1%和88.1%的BPA。此外,采用三维荧光光谱技术对BPA降解过程进行了表征,结果表明BPA氧化中间体也具有荧光特性。此外,鉴定出6种中间产物,并提出了BPA可能的降解途径。此外,Fe/HS/PS体系对其他代表性有机污染物包括恩诺沙星、酸性橙7、对乙酰氨基酚和苯酚的去除也表现出优异的性能。所有结果表明,Fe/HS/PS体系可能是一种很有前景的有机污染物去除方法。

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