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城市垃圾渗滤液中抗羟基自由基有机物的分子组成

Molecular composition of hydroxyl radical-resistant organics in municipal solid waste leachate.

作者信息

Chen Weiming, Gu Zhepei, He Chen, Li Qibin

机构信息

School of Environmental Science and Engineering, Southwest Jiaotong University, Chengdu, Sichuan 611756, China; Key Laboratory of Treatment for Special Wastewater of Sichuan Province Higher Education System, Chengdu, Sichuan 610066, China.

School of Environmental Science and Engineering, Southwest Jiaotong University, Chengdu, Sichuan 611756, China.

出版信息

J Hazard Mater. 2025 Mar 15;486:137014. doi: 10.1016/j.jhazmat.2024.137014. Epub 2024 Dec 26.

Abstract

Although hydroxyl radicals (OH) degrade organic pollutants nonselectively, their mineralization rate during the treatment of waste leachate biological treatment effluent (BTL) using Fenton or Fenton-like systems is not high, and the reason is unknown. In this study, we investigated three typical Fenton-like systems that act on dissolved organic matter (DOM) in BTL. We analyzed the molecular composition of DOM resistant to OH, using ultrahigh resolution mass spectrometry. We find that DOM resistant to OH is more oxidized, less unsaturated/aromatic, has higher molecular weights, and contains more unsaturated oxygen-containing functional groups than does DOM reactive to OH. Resistant-DOM is further categorized into DOM derived by the action of OH (DOM) and DOM initially present (DOM), whose quantities account for approximately 20 % and 80 %, respectively. The DOM is gradually removed under extended reaction time, while DOM is relatively unreactive with OH and is always present in the treated effluent. Based on the molecular composition of resistant-DOM, we propose a method to increase the mineralization rate (up to 95 % TOC removal with only 5 mM persulfate). This study provides direct evidence for the first time that the presence of resistant-DOM (mainly stemming from DOM) in BTL is an important reason for the unideal mineralization rate in the advanced treatment of Fenton or Fenton-like systems.

摘要

尽管羟基自由基(OH)能非选择性地降解有机污染物,但在使用芬顿或类芬顿系统处理垃圾渗滤液生物处理出水(BTL)时,其矿化率并不高,原因尚不清楚。在本研究中,我们研究了三种作用于BTL中溶解有机物(DOM)的典型类芬顿系统。我们使用超高分辨率质谱分析了抗OH的DOM的分子组成。我们发现,与对OH反应的DOM相比,抗OH的DOM氧化程度更高,不饱和/芳香性更低,分子量更高,且含有更多不饱和含氧官能团。抗DOM进一步分为由OH作用衍生的DOM(DOM)和最初存在的DOM(DOM),其数量分别约占20%和80%。在延长反应时间的情况下,DOM逐渐被去除,而DOM与OH的反应性相对较低,并且始终存在于处理后的出水中。基于抗DOM的分子组成,我们提出了一种提高矿化率的方法(仅用5 mM过硫酸盐即可实现高达95%的总有机碳去除率)。本研究首次提供了直接证据,表明BTL中抗DOM(主要源于DOM)的存在是芬顿或类芬顿系统深度处理中矿化率不理想的重要原因。

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