Revisiting the contribution of FeIVO2+ in Fe(II)/peroxydisulfate system

Revisiting the contribution of FeIVO2+ in Fe(II)/peroxydisulfate system
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重新审视 FeIVO2 在 Fe(II)/过二硫酸盐体系中的贡献

DOI:
10.1016/j.cclet.2022.05.069
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发表时间:
2022-05
影响因子:
9.1
通讯作者:
Qi Yang
Qi Yang
中科院分区:
化学1区
文献类型:
--
作者:
Kunjie Hou;Peng Shen;Zhu Wang;Zhoujie Pi;Fei Chen;Xiaoming Li;Haoran Dong;Qi Yang

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近期研究提出,在以甲基苯基亚砜(PMSO)作为Fe⁴⁺O²⁺探针的Fe(II)/过二硫酸盐(PDS)体系中,高价铁物种(如Fe⁴⁺O²⁺)而非硫酸根自由基(SO₄•⁻)和羟基自由基(•OH)是主要的活性氧化物种(ROS)。然而,许多操作因素可能会干扰该方法的准确性,因此通过这种方法计算出的Fe⁴⁺O²⁺的贡献存在争议。在本研究中,详细研究了Fe(II)浓度、污染物类型、还原剂或共存阴离子对Fe⁴⁺O²⁺生成的可能影响以及其对Fe(II)/PDS体系中目标污染物去除的相应贡献,还探讨了所涉及的内在机制。本研究表明,在Fe(II)/PDS体系中,ROS的产生是一个复杂的过程,迫切需要多种组合方法来深入探究ROS对目标污染物去除的贡献。在Fe(II)/PDS体系中,ROS的产生是一个复杂的过程,应用于Fe⁴⁺O²⁺验证的单探针技术可能会导致意想不到的假象。
Recent studies have proposed that the high-valent iron species (such as Fe IV O 2+ ) rather than sulfate radical (SO 4 •− ) and hydroxyl radical ( • OH) are the main reactive oxidant species (ROS) in Fe(II)/peroxydisulfate (PDS) system with the methyl phenyl sulfoxide (PMSO) as the Fe IV O 2+ probe. However, many operational factors may interfere with the accuracy of this method, so the contribution of Fe IV O 2+ calculated by this method is controversial. In this study, the possible effect of Fe(II) concentration, pollutant type, reducing agent, or coexisted anions on Fe IV O 2+ production and its corresponding contribution to the removal of target pollutants in the Fe(II)/PDS system were investigated in detail, and the intrinsic mechanisms involved were also explored. This study shows that ROS generation is a complex process in the Fe(II)/PDS system, and multiple combinatorial approaches are urgently required to deeply explore the contribution of ROS to the elimination of target contaminants. ROS generation is a complex process in the Fe(II)/PDS system, single-probe technique applied to Fe IV O 2+ validation may cause unforeseen artifacts.
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