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氯离子促进基于铁的过乙酸活化体系中萘普生的快速去除:通过形成铁-氯配合物增强反应性氧化物种。

Accelerated removal of naproxen in the iron-based peracetic acid activation system by chloride ions: Enhancement of reactive oxidative species via the formation of iron-chloride complexes.

机构信息

State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China.

State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China.

出版信息

J Hazard Mater. 2024 Jan 15;462:132760. doi: 10.1016/j.jhazmat.2023.132760. Epub 2023 Oct 13.

Abstract

Iron-based PAA activation process is a promising advanced oxidation process for water decontamination which depends on Fe(II) as the main reactive site for PAA activation, resulting in various reactive oxidative species (ROSs) generation. For practical application, the impact of water matrix chloride ion (Cl) on ROSs production and contaminants removal should be carefully considered. In this study, it's found that the introduction of Cl (0.1-10 mM) could significantly enhance the reaction rate of the rapid stage (k) up to 2.15 times at the initial pH of 4.25 in the Fe(II)/PAA system. Further studies demonstrated that the improved removal capacity of NAP resulted from Cl induced R-O generation as indicated by the exposure dose of R-O increasing from 7.74 × 10 M•s to 1.44 × 10 M•s, rather than chlorine-containing radicals' generation. DFT calculation results suggested that the formed Fe(II)-Cl complexes could easily activate PAA to generate more ROSs for NAP removal. Moreover, Fe(II)/PAA treatment can alleviate the biological toxicity of pollutants via both the Escherichia coli test and toxicity assessment. The obtained new knowledge manifested that Cl can boost ROSs generation and conversion in iron-based PAA systems, providing guidance for the efficient decontamination of chlorine-containing sewage with PAA-based AOPs.

摘要

铁基过一硫酸盐(PAA)激活过程是一种有前途的用于水净化的高级氧化工艺,该过程依赖于 Fe(II)作为 PAA 激活的主要反应位点,从而生成各种活性氧化物质(ROSs)。对于实际应用,应仔细考虑水基质氯离子(Cl)对 ROSs 生成和污染物去除的影响。在本研究中,发现 Cl(0.1-10 mM)的引入可在 Fe(II)/PAA 体系的初始 pH 值为 4.25 时将快速阶段(k)的反应速率显著提高至 2.15 倍。进一步的研究表明,Cl 诱导的 R-O 生成导致 NAP 的去除能力得到提高,这表现为 R-O 的暴露剂量从 7.74×10 M•s 增加到 1.44×10 M•s,而不是含氯自由基的生成。DFT 计算结果表明,形成的 Fe(II)-Cl 配合物可容易地激活 PAA 以生成更多的 ROSs 用于 NAP 的去除。此外,Fe(II)/PAA 处理可通过大肠杆菌测试和毒性评估减轻污染物的生物毒性。所获得的新知识表明,Cl 可以促进铁基 PAA 体系中 ROSs 的生成和转化,为基于 PAA 的 AOPs 有效净化含氯污水提供了指导。

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