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Degradation and mechanism of 2,4-dichlorophenoxyacetic acid (2,4-D) by thermally activated persulfate oxidation

机译:热活化过硫酸盐氧化降解2,4-二氯苯氧基乙酸(2,4-D)的机理

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摘要

The chlorinated phenoxy herbicide of 2,4-dichlorophenoxyacetic acid (2,4-D) was oxidized by thermally activated persulfate (TAP). This herbicide was studied for different persulfate dosages (0.97-7.29 g L-1), for varying initial pH levels (3-12) and temperatures (25-70 degrees C). Compared with Fe2+/PS, TAP could achieve a higher total organic carbon (TOC) removal under wider pH ranges of 3-12. Increasing the mole ratio of PS to 2,4-D favored for the decay of 2,4-D and the best performance was achieved at the ratio of 50. The 2,4-D degradation rate constant highly depended on the initial pH and temperature, in accordance with the Arrhenius model, with an apparent activation energy of 135.24 kJ mol(-1). The study of scavenging radicals and the EPR confirmed the presence of both SO4 center dot- and (OH)-O-center dot. However, SO4 center dot- was the predominant oxidation radical for 2,4-D decay. The presence of both Cl- and CO32- inhibited the degradation of 2,4-D, whereas the effect of NO3- could be negligible. Verified by GC/MS, HPLC and ion chromatography, a possible degradation mechanism was proposed. (C) 2018 Elsevier Ltd. All rights reserved.
机译:2,4-二氯苯氧基乙酸(2,4-D)的氯化苯氧基除草剂被热活化的过硫酸盐(TAP)氧化。研究了该除草剂的不同过硫酸盐剂量(0.97-7.29 g L-1),不同的初始pH值(3-12)和温度(25-70摄氏度)。与Fe2 + / PS相比,TAP在3-12的较宽pH范围内可实现更高的总有机碳(TOC)去除率。将PS与2,4-D的摩尔比增加有利于2,4-D的降解,并在50的比例下获得最佳性能。2,4-D的降解速率常数高度取决于初始pH和温度,根据Arrhenius模型,具有135.24 kJ mol(-1)的表观活化能。对清除自由基和EPR的研究证实了同时存在SO4中心点和(OH)-O中心点。但是,SO4中心点是2,4-D衰变的主要氧化自由基。 Cl-和CO32-的存在均抑制了2,4-D的降解,而NO3-的影响可忽略不计。通过GC / MS,HPLC和离子色谱法的验证,提出了可能的降解机理。 (C)2018 Elsevier Ltd.保留所有权利。

著录项

  • 来源
    《Chemosphere》 |2018年第12期|784-793|共10页
  • 作者单位

    Nankai Univ, Tianjin Key Lab Urban Ecol Environm Remediat & Po, Coll Environm Sci & Engn, Key Lab Pollut Proc & Environm Criteria,Minist Ed, Tianjin 300350, Peoples R China;

    Nankai Univ, Tianjin Key Lab Urban Ecol Environm Remediat & Po, Coll Environm Sci & Engn, Key Lab Pollut Proc & Environm Criteria,Minist Ed, Tianjin 300350, Peoples R China;

    Nankai Univ, Tianjin Key Lab Urban Ecol Environm Remediat & Po, Coll Environm Sci & Engn, Key Lab Pollut Proc & Environm Criteria,Minist Ed, Tianjin 300350, Peoples R China;

    Nankai Univ, Tianjin Key Lab Urban Ecol Environm Remediat & Po, Coll Environm Sci & Engn, Key Lab Pollut Proc & Environm Criteria,Minist Ed, Tianjin 300350, Peoples R China;

    Nankai Univ, Tianjin Key Lab Urban Ecol Environm Remediat & Po, Coll Environm Sci & Engn, Key Lab Pollut Proc & Environm Criteria,Minist Ed, Tianjin 300350, Peoples R China;

    UPS Univ Toulouse, CNRS, Lab Genie Chim, INPT, 118 Route Narbonne, F-31062 Toulouse, France;

  • 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

    2,4-Dichlorophenoxyacetic acid; Thermally activated persulfate; Degradation mechanism; EPR; Fe2+/PS;

    机译:2,4-二氯苯氧基乙酸;热活化过硫酸盐;降解机理;EPR;Fe2 + / PS;

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