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Photochemical activation of seemingly inert SO_4~(2-) in specific water environments

机译:在特定水环境中看似惰性的SO_4〜(2-)的光化学活化

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摘要

Sulfate ions (SO42-) are ubiquitous in aqueous environments and are generally considered to be inert due to their chemical stability. For the first time, we found that SO42- can be activated into SO42--type radicals (e.g., sO(3)(center dot-), SO5 center dot-, SO4 center dot-) in the presence of phenolic compounds under simulated or natural solar irradiation. In turn, the radicals promoted the transformation and mineralization of phenolic compounds compared to that in the absence of SO42- with reaction rate constants ranging from 0.008 h(-1) to 0.021 h(-1). In addition, the activation mechanisms of inert SO42- in the photochemical transformation of phenolic compounds were elucidated. A hydrated electron (e(aq)(-)) is first generated during the photolysis of phenolic compounds and is the most important step in the activation of SO42-. Then, the e(aq)(-) reduces SO42- to SO32-, and SO32- is further photochemical activated to become a reactive species (e.g., erg and SON), which can evolve into strong oxidants (e.g., SO5 center dot- and SO4 center dot-), via a series of radical chain reactions. These oxidants are responsible for the enhanced phenolic compound degradation. The photochemical activation of seemingly inert SO42- sheds new light on studies on the transport, transformation and environmental impact of matter (e.g., phenolic compounds) in specific water environments and provides a novel strategy for the generation of SO4 center dot- and photochemical removal of phenolic pollutants. (C) 2018 Elsevier Ltd. All rights reserved.
机译:硫酸根离子(SO42-)在水性环境中无处不在,由于其化学稳定性,通常被认为是惰性的。首次发现,在模拟下存在酚类化合物的情况下,SO42-可以被激活为SO42-型自由基(例如sO(3)(中心点-),SO5中心点-,SO4中心点-)或自然太阳辐射。反过来,与不存在SO42-的自由基相比,自由基可促进酚类化合物的转化和矿化,其反应速率常数范围为0.008 h(-1)至0.021 h(-1)。此外,阐明了惰性SO42-在酚类化合物光化学转化中的活化机理。在酚类化合物的光解过程中首先生成水合电子(e(aq)(-)),这是SO42-活化中最重要的步骤。然后,e(aq)(-)将SO42-还原为SO32-,并且SO32-被进一步光化学活化以成为反应性物种(例如erg和SON),可以演变成强氧化剂(例如SO5中心点-和SO4中心点-),通过一系列自由基链反应。这些氧化剂负责增加酚类化合物的降解。表面活性呈惰性的SO42的光化学活化为在特定水环境中物质(例如酚类化合物)的运输,转化和环境影响的研究提供了新的思路,并为产生SO4中心点和光化学去除二氧化硫提供了新的策略。酚类污染物。 (C)2018 Elsevier Ltd.保留所有权利。

著录项

  • 来源
    《Chemosphere》 |2019年第1期|399-407|共9页
  • 作者单位

    Nankai Univ, Minist Educ,Key Lab Pollut Proc & Environm Criter, Coll Environm Sci & Engn, Tianjin Key Lab Environm Remediat & Pollut Contro, Tianjin 300071, Peoples R China;

    Nanjing Univ, Sch Environm, State Key Lab Pollut Control & Resource Reuse, Nanjing 210023, Jiangsu, Peoples R China;

    Nanjing Univ, Res Ctr Environm Nandtechnol ReCENT, Nanjing 210023, Jiangsu, Peoples R China;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《化学文摘》(CA);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    Sulfate ions; Phenolic compounds; Photochemical activation; Hydrated electron;

    机译:硫酸根离子;酚类化合物;光化学活化;水合电子;

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