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首页> 外文期刊>The Science of the Total Environment >Heterogeneous activation of peroxymonosulfate using Mn-Fe layered double hydroxide: Performance and mechanism for organic pollutant degradation
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Heterogeneous activation of peroxymonosulfate using Mn-Fe layered double hydroxide: Performance and mechanism for organic pollutant degradation

机译:Mn-Fe层状双氢氧化物对过氧单硫酸盐的非均相活化:有机污染物降解的性能和机理

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摘要

On account of high oxidation ability of sulfate radical-based advanced oxidation processes (AOPs), the eco-friendly catalysts for peroxymonosulfate (PMS) activation have received considerable attentions. Previous studies mainly focused on Cobalt-based catalyst due to its high activation efficiency, such as Co3O4/MnO2 and FeCo-layered double hydroxide (LDH), whereas Cobalt-based catalyst usually has serious risk to environment. To avoid this risk, MnFe-LDH was primarily synthesized in this research by simple co-precipitation and subsequently utilized as an effective catalyst for peroxymonosulfate (PMS) activation to degrade organic pollutants. The experimental results demonstrated that MnFe-LDH with a lower dosage (0.20 g/L) could efficiently activate PMS to achieve 97.56% removal of target organic pollutants Acid Orange 7 (AO7). The AO7 degradation process followed the pseudo-first-order kinetic well with an activation energy of 21.32 kJ/mol. The intrinsic influencing mechanism was also investigated. The quenching experiment and electron spin resonance (ESR) indicated that sulfate and hydroxyl radicals were produced by the effective activation of PMS by MnFe-LDH, resulting in a high rate of decolorization. The possible AO7 removal pathway in the constructed MnFe-LDH/PMS system was presented on the basis of UV-vis spectrum analysis and GC-MS, which suggested that the AO7 degradation was firstly initiated by breaking azo linkages, then generated phenyl and naphthalene intermediates and finally presented as ring-opening products. This effective MnFe-LDH/PMS system showed great application potential in the purification of wastewater contaminated by refractory organic pollutants. (C) 2019 Elsevier B.V. All rights reserved.
机译:由于基于硫酸根的高级氧化过程(AOP)的高氧化能力,用于过氧一硫酸盐(PMS)活化的生态友好型催化剂已受到广泛关注。以往的研究主要针对钴基催化剂,因为它具有很高的活化效率,例如Co3O4 / MnO2和FeCo层状双氢氧化物(LDH),而钴基催化剂通常会对环境造成严重威胁。为了避免这种风险,在本研究中主要通过简单的共沉淀法合成了MnFe-LDH,随后将其用作过氧化单硫酸盐(PMS)活化以降解有机污染物的有效催化剂。实验结果表明,较低剂量(0.20 g / L)的MnFe-LDH可以有效地激活PMS,以实现97.56%的目标有机污染物酸橙7(AO7)的去除。 AO7降解过程遵循伪一级动力学井,活化能为21.32 kJ / mol。还研究了内在影响机制。淬灭实验和电子自旋共振(ESR)表明,通过MnFe-LDH有效激活PMS会产生硫酸根和羟基自由基,从而导致高脱色率。在紫外可见光谱分析和GC-MS的基础上,提出了构建的MnFe-LDH / PMS系统中可能的AO7去除途径,表明AO7的降解首先是通过破坏偶氮键引发的,然后生成苯基和萘中间体最后作为开环产品展示。这种有效的MnFe-LDH / PMS系统在净化难处理的有机污染物污染的废水中显示出巨大的应用潜力。 (C)2019 Elsevier B.V.保留所有权利。

著录项

  • 来源
    《The Science of the Total Environment》 |2019年第1期|453-464|共12页
  • 作者单位

    Hunan Univ, Coll Environm Sci & Engn, Changsha 410082, Hunan, Peoples R China|Hunan Univ, Minist Educ, Key Lab Environm Biol & Pollut Control, Changsha 410082, Hunan, Peoples R China;

    Hunan Univ, Coll Environm Sci & Engn, Changsha 410082, Hunan, Peoples R China|Hunan Univ, Minist Educ, Key Lab Environm Biol & Pollut Control, Changsha 410082, Hunan, Peoples R China;

    Hunan Univ, Coll Environm Sci & Engn, Changsha 410082, Hunan, Peoples R China|Hunan Univ, Minist Educ, Key Lab Environm Biol & Pollut Control, Changsha 410082, Hunan, Peoples R China;

    Univ Sci & Technol China, Dept Chem, CAS Key Lab Urban Pollutant Convers, Hefei 230026, Anhui, Peoples R China;

    Hunan Univ, Coll Environm Sci & Engn, Changsha 410082, Hunan, Peoples R China|Hunan Univ, Minist Educ, Key Lab Environm Biol & Pollut Control, Changsha 410082, Hunan, Peoples R China;

    Hunan Univ, Coll Environm Sci & Engn, Changsha 410082, Hunan, Peoples R China|Hunan Univ, Minist Educ, Key Lab Environm Biol & Pollut Control, Changsha 410082, Hunan, Peoples R China;

    Hunan Univ, Coll Environm Sci & Engn, Changsha 410082, Hunan, Peoples R China|Hunan Univ, Minist Educ, Key Lab Environm Biol & Pollut Control, Changsha 410082, Hunan, Peoples R China;

    Hunan Univ, Coll Environm Sci & Engn, Changsha 410082, Hunan, Peoples R China|Hunan Univ, Minist Educ, Key Lab Environm Biol & Pollut Control, Changsha 410082, Hunan, Peoples R China;

    Hunan Univ, Coll Environm Sci & Engn, Changsha 410082, Hunan, Peoples R China|Hunan Univ, Minist Educ, Key Lab Environm Biol & Pollut Control, Changsha 410082, Hunan, Peoples R China;

    Hunan Univ, Coll Environm Sci & Engn, Changsha 410082, Hunan, Peoples R China|Hunan Univ, Minist Educ, Key Lab Environm Biol & Pollut Control, Changsha 410082, Hunan, Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    Sulfate radical; Heterogeneous activation; Peroxymonosulfate; Reaction mechanism; Degradation pathway;

    机译:硫酸根;非均相活化;过氧单硫酸盐;反应机理;降解途径;

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