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羟胺促进黄铁矿氧化中产生活性羟基自由基和有机污染物降解。

Hydroxylamine promoted hydroxyl radical production and organic contaminants degradation in oxygenation of pyrite.

机构信息

Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing 210008, PR China.

Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing 210008, PR China.

出版信息

J Hazard Mater. 2022 May 5;429:128380. doi: 10.1016/j.jhazmat.2022.128380. Epub 2022 Jan 29.

Abstract

The heterogeneous Fenton-like process using pyrite (FeS) is increasingly recognized as a promising advanced oxidation process for removal of organic contaminants. However, the slow regeneration of Fe(II) limits the generation of reactive oxygen species for environment implication. To overcome this drawback, hydroxylamine was applied to enhance the reactivity of FeS to degrade organic contaminants under oxic conditions. Results showed that hydroxylamine facilitated the regeneration of Fe(II) on FeS surface to promote reactive oxygen species generation, thereby efficiently degrading different organic contaminants. The underlying mechanism was further elucidated that the presence of hydroxylamine enhanced electron transfer from FeS to O to produce superoxide radicals (O), hydrogen peroxide (HO) and hydroxyl radical (HO) via Fenton-like pathways, which induced the rapid degradation of organic contaminants (e.g., sulfamethoxazole (SMX)). The reactivity of FeS for organic contaminant degradation changed negligibly after seven cycles in the presence of hydroxylamine. The effects of pH and inorganic anions on SMX degradation were also clarified in details. The finding of this study would provide a novel strategy to enhance the contaminants degradation by FeS-based advanced oxidation technologies for environmental remediation.

摘要

利用黄铁矿(FeS)的多相类 Fenton 反应过程越来越被认为是一种很有前途的高级氧化工艺,可用于去除有机污染物。然而,Fe(II)的缓慢再生限制了活性氧物质的生成,从而对环境产生影响。为了克服这一缺点,在有氧条件下,使用羟胺来增强 FeS 的反应性,以降解有机污染物。结果表明,羟胺促进了 FeS 表面 Fe(II)的再生,从而促进了活性氧物质的生成,从而有效地降解了不同的有机污染物。进一步阐明了其潜在机制,即在羟胺存在的情况下,增强了从 FeS 到 O 的电子转移,通过类 Fenton 途径产生超氧自由基(O)、过氧化氢(HO)和羟基自由基(HO),从而导致有机污染物(如磺胺甲恶唑(SMX))的快速降解。在羟胺存在的情况下,FeS 对有机污染物降解的反应性在七个循环后几乎没有变化。还详细阐明了 pH 值和无机阴离子对 SMX 降解的影响。本研究的发现将为通过基于 FeS 的高级氧化技术增强污染物降解提供一种新策略,以用于环境修复。

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