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沉积物氧化过程中•OH对污染物的降解作用:含水层中丰富固体基质的影响

Contaminant degradation by •OH during sediment oxygenation: Effect of abundant solid matrix in aquifer.

作者信息

Zheng Yunsong, Lu Yuxi, Yuan Songhu

机构信息

State Key Laboratory of Biogeology and Environmental Geology, China University of Geosciences, 68 Jincheng Street, Wuhan 430078, PR China.

State Key Laboratory of Biogeology and Environmental Geology, China University of Geosciences, 68 Jincheng Street, Wuhan 430078, PR China; Hubei Key Laboratory of Yangtze Catchment Environmental Aquatic Science, School of Environmental Studies, China University of Geosciences, 68 Jincheng Street, Wuhan 430078, PR China.

出版信息

J Hazard Mater. 2024 Mar 5;465:133322. doi: 10.1016/j.jhazmat.2023.133322. Epub 2023 Dec 20.

Abstract

Aquifer oxygenation for hydroxyl radical (•OH) production has been recently proposed as a promising strategy for in-situ remediation. However, the high performance of this process was justified at low solid-to-liquid ratios (SLRs) of suspension systems. It remains unclear whether and how the performance is affected by abundant solid matrixes. Here we assessed the influence of SLR on •OH production and contaminant degradation during sediment oxygenation. Cumulative •OH increased from 21.8 to 165.2 μM when the SLR increased from 200 to 1600 g/L, while phenol degradation increased with the increase in SRL at the values lower than 1200 g/L and decreased at higher SLRs. As the main sediment component, silica exhibited a negligible effect on •OH production and phenol degradation because of the weak adsorption towards aqueous Fe(II). Whereas, the other component, alumina, significantly inhibited •OH production and phenol degradation because it strongly adsorbed Fe(II). •OH scavenging by solid reactive matrixes was mainly responsible for the inhibition at high SLRs. The scavenging effect could be mitigated by mediating the main reactive Fe(II) species from solid-adsorbed to dissolved phase with ligand addition. Our findings are important for understanding the side reactions and optimizing the remediation performance during aquifer oxygenation.

摘要

最近,有人提出通过含水层充氧来产生羟基自由基(•OH),这是一种很有前景的原位修复策略。然而,该过程在悬浮体系的低固液比(SLR)条件下具有高性能。目前尚不清楚丰富的固体基质是否以及如何影响其性能。在此,我们评估了固液比对沉积物充氧过程中•OH产生和污染物降解的影响。当固液比从200增加到1600 g/L时,累积•OH从21.8 μM增加到165.2 μM,而苯酚降解在固液比低于1200 g/L时随其增加而增加,在较高固液比时则下降。作为沉积物的主要成分,二氧化硅对•OH产生和苯酚降解的影响可忽略不计,因为其对水相Fe(II)的吸附较弱。而另一种成分氧化铝则显著抑制•OH产生和苯酚降解,因为它强烈吸附Fe(II)。固体反应性基质对•OH的清除是高固液比下抑制作用的主要原因。通过添加配体将主要反应性Fe(II)物种从固体吸附相介导到溶解相,可以减轻清除效应。我们的研究结果对于理解含水层充氧过程中的副反应和优化修复性能具有重要意义。

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