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热活化过硫酸盐对阿替洛尔的氧化降解:动力学、降解途径和转化中间产物的分布。

Oxidative degradation of atenolol by heat-activated persulfate: Kinetics, degradation pathways and distribution of transformation intermediates.

机构信息

State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, People's Republic of China.

State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, People's Republic of China; School of Environment, Henan Normal University, Key Laboratory for Yellow River and Huai River Water Environmental and Pollution Control, Ministry of Education, Henan Key Laboratory for Environmental Pollution Control, Xinxiang, Henan 453007, PR China.

出版信息

Chemosphere. 2018 Sep;207:174-182. doi: 10.1016/j.chemosphere.2018.05.068. Epub 2018 May 17.

Abstract

Atenolol (ATL) has been widely detected in wastewater and aquatic environment. Although satisfactory removal of ATL from wastewater could be achieved, the mineralization ratio is usually low, which may result in the accumulation of its transformation products in the effluent and cause additional ecological risk to the environment. The aim of this study is to explore the effectiveness of heat activated persulfate (PS) in the removal of ATL from wastewater. Influencing factors including temperature, PS dosage, solution pH, existence of NO, Cl, HCO and Suwannee river fulvic acid (SRFA) were examined. Complete removal of ATL was achieved within 40 min at pH 7.0 and 70 °C by using 0.5 mM PS. Inhibitive effects of HCO and FA had been observed on ATL oxidation, which was increased with the increase of their concentration. Sulfate radical (SO) was determined as the main reactive species by quenching experiment. Eight intermediates produced in ATL degradation were identified, and four degradation pathways were proposed based on the analysis of mass spectrum and frontier electron densities. The distribution of major intermediates was influenced by reaction temperature. Hydroxylation intermediates and deamidation intermediate were the most prominent at 50 °C and 60 °C, respectively. All intermediates were completely degraded in 40 min except P134 at 70 °C. Effective removal of TOC (74.12%) was achieved with 0.5 mM PS, pH 7.0 and 70 °C after 240 min. The results proved that heat activation of PS is a promising method to remove organic pollutants in wastewater.

摘要

阿替洛尔(ATL)已广泛存在于废水和水生环境中。尽管从废水中去除 ATL 可以达到令人满意的效果,但矿化率通常较低,这可能导致其转化产物在废水中积累,并对环境造成额外的生态风险。本研究旨在探索热激活过硫酸盐(PS)去除废水中 ATL 的效果。考察了温度、PS 用量、溶液 pH 值、NO、Cl、HCO 和苏万尼河腐殖酸(SRFA)的存在等影响因素。在 pH 值为 7.0 和 70°C 下,只需 0.5mM PS 即可在 40 分钟内完全去除 ATL。HCO 和 FA 的存在对 ATL 氧化有抑制作用,且随着浓度的增加而增加。通过猝灭实验确定硫酸根自由基(SO)是主要的反应性物质。在 ATL 降解过程中生成了 8 种中间体,并根据质谱和前沿电子密度分析提出了 4 种降解途径。主要中间体的分布受反应温度的影响。在 50°C 和 60°C 时,羟基化中间体和脱酰胺化中间体最为突出。除了 70°C 下的 P134,所有中间体在 40 分钟内都完全降解。在 0.5mM PS、pH 值为 7.0 和 70°C 条件下 240 分钟后,TOC(74.12%)的去除效果良好。结果表明,PS 的热激活是去除废水中有机污染物的一种很有前途的方法。

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