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土壤中芘的结合态对其芬顿氧化处理效率的影响。

Influence of pyrene combination state in soils on its treatment efficiency by Fenton oxidation.

作者信息

Sun Hong-wen, Yan Qi-she

机构信息

College of Environmental Science and Engineering, Nankai University, Tianjin 300071, China.

出版信息

J Environ Manage. 2008 Aug;88(3):556-63. doi: 10.1016/j.jenvman.2007.03.031. Epub 2007 May 22.

Abstract

Interactions of hydrophobic organic compounds (HOCs) with soil organic matter (SOM) determine their combination state in soils, and therefore strongly influence their mobility, bioavailability, and chemical reactivity. Contact time (aging) of an HOC in soil also strongly influences its combination state and environmental fate. We studied Fenton oxidation of pyrene in three different soils to reveal the influences of SOM, contact time, and combination state on the efficiency of vigorous chemical reactions. Pyrene degradation efficiency depended strongly on the dose of oxidant (H(2)O(2)) and catalyst (Fe(2+)); the greatest degradation was achieved at an oxidant to catalyst molar ratio of 10:1. Pyrene degradation differed among the three soils, ranging from 65.4% to 88.9%. Pyrene degradation efficiency decreased with increasing SOM content, and the aromatic carbon content in SOM was the key parameter. We hypothesize that pyrene molecules that combine with the compact net structure of aromatic SOM are less accessible to Fenton oxidation. Furthermore, pyrene degradation efficiency decreased considerably after aged for 30 days, but further aging to 60 and 180 days did not significantly change degradation efficiency. The Fenton oxidation efficiency of pyrene in both unaged and aged soils was greater than the corresponding desorption rate during the same period, perhaps because Fenton reaction can make pyrene more accessible to the oxidant through the enhancement of HOCs' desorption by generating reductant species or by destroying SOM through oxidation.

摘要

疏水性有机化合物(HOCs)与土壤有机质(SOM)的相互作用决定了它们在土壤中的结合状态,因此强烈影响它们的迁移性、生物可利用性和化学反应活性。HOCs在土壤中的接触时间(老化)也会强烈影响其结合状态和环境归宿。我们研究了芘在三种不同土壤中的芬顿氧化,以揭示SOM、接触时间和结合状态对剧烈化学反应效率的影响。芘的降解效率强烈依赖于氧化剂(H₂O₂)和催化剂(Fe²⁺)的剂量;在氧化剂与催化剂摩尔比为10:1时实现了最大降解。三种土壤中芘的降解情况不同,范围在65.4%至88.9%之间。芘的降解效率随SOM含量的增加而降低,SOM中的芳香碳含量是关键参数。我们推测,与芳香族SOM紧密网络结构结合的芘分子较难被芬顿氧化。此外,芘老化30天后降解效率大幅下降,但进一步老化至60天和180天并未显著改变降解效率。未老化和老化土壤中芘的芬顿氧化效率均高于同期相应的解吸率,这可能是因为芬顿反应可通过产生还原物种增强HOCs的解吸或通过氧化破坏SOM,使芘更易被氧化剂接触到。

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