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过二硫酸盐与亚硫酸氢盐耦合强化水中有机污染物的降解。

Enhanced degradation of organic contaminants in water by peroxydisulfate coupled with bisulfite.

机构信息

State Key Laboratory of Water Environment Simulation, School of Environment, Beijing Normal University, Beijing 100875, PR China; State Key Joint Laboratory of Environment Simulation and Pollution Control (SKLESPC), Beijing Key Laboratory for Emerging Organic Contaminants Control, School of Environment, Tsinghua University, Beijing 100084, PR China.

State Key Laboratory of Water Environment Simulation, School of Environment, Beijing Normal University, Beijing 100875, PR China.

出版信息

J Hazard Mater. 2017 Apr 15;328:98-107. doi: 10.1016/j.jhazmat.2017.01.010. Epub 2017 Jan 10.

Abstract

In this study, the bisulfite-peroxydisulfate system (S(IV)/PDS) widely used in polymerization was innovatively applied for organic contaminants degradation in water. The addition of S(IV) into PDS system remarkably enhanced the degradation efficiency of bisphenol A (BPA, a frequently detected endocrine disrupting chemical in the environments) from 17.0% to 84.7% within 360 min. The degradation efficiency of BPA in the S(IV)/PDS system followed pseudo-first-order kinetics, with rate constant values ranging from 0.00005min to 0.02717min depending on the operating parameters, such as the initial S(IV) and PDS dosage, solution pH, reaction temperature, chloride and water type. Furthermore, nitrogen purging experiment, radical scavenging experiment and electron spin resonance (ESR) analysis were used to elucidate the possible mechanism. The results revealed that sulfate radical was the dominant reactive species in the S(IV)/PDS system. Finally, based on the results of liquid chromatography-mass spectrometry (LC-MS) and gas chromatography-mass spectrometry (GC-MS), the BPA degradation pathway was proposed to involve β-scission (CC), hydroxylation, dehydration, oxidative skeletal rearrangement, and ring opening. This study helps to characterize the combination of PDS and inorganic S(IV), a common industrial contaminant, to generate reactive species to enhance organic contaminants degradation in water.

摘要

在这项研究中,聚合反应中广泛使用的亚硫酸氢盐过二硫酸盐系统(S(IV)/PDS)被创新性地应用于水中有机污染物的降解。在 360 分钟内,向 PDS 系统中添加 S(IV)显著提高了双酚 A(BPA,环境中经常检测到的内分泌干扰化学物质)的降解效率,从 17.0%提高到 84.7%。S(IV)/PDS 体系中 BPA 的降解效率遵循假一级动力学,取决于操作参数(如初始 S(IV)和 PDS 剂量、溶液 pH 值、反应温度、氯离子和水类型),速率常数值范围为 0.00005min 至 0.02717min。此外,还进行了氮气吹扫实验、自由基清除实验和电子自旋共振(ESR)分析,以阐明可能的机制。结果表明,硫酸盐自由基是 S(IV)/PDS 体系中的主要反应性物质。最后,根据液相色谱-质谱(LC-MS)和气相色谱-质谱(GC-MS)的结果,提出了 BPA 的降解途径,涉及β断裂(CC)、羟化、脱水、氧化骨架重排和开环。本研究有助于表征 PDS 与无机 S(IV)的组合,S(IV)是一种常见的工业污染物,可产生反应性物质,以增强水中有机污染物的降解。

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