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将环糊精增强的水溶性与间接电化学处理相结合用于五氯苯酚污染土壤的修复。

Coupling enhanced water solubilization with cyclodextrin to indirect electrochemical treatment for pentachlorophenol contaminated soil remediation.

作者信息

Hanna Khalil, Chiron Serge, Oturan Mehmet A

机构信息

Laboratoire des Géomatériaux CNRS-FRE 2455, Université de Marne la Vallée, Cité Descartes, 77454 Marne la Vallée Cedex 2, France.

出版信息

Water Res. 2005 Jul;39(12):2763-73. doi: 10.1016/j.watres.2005.04.057.

Abstract

This study undertakes to examine, at laboratory scale, the technical feasibility, mechanisms and performances provided by coupling the enhanced flushing abilities of cyclodextrin solutions for pentachlorophenol (PCP) removal from contaminated soil with indirect electrochemical treatment for the final disposal of soil extract solutions containing high PCP loads (0.77mmolL(-1)). The hydroxypropyl-beta-cyclodextrin (HPCD) solution increased the aqueous concentration of PCP in soil extract effluents to as much as 3.5 times the concentrations obtained during the water flush of the soil. PCP was treated with electrochemically generated Fenton's reagent in an aqueous medium. The increase in PCP water solubility in the presence of HPCD is balanced by the corresponding decrease in PCP degradation rate under indirect electrochemical treatment. This is due to the high carbon content (HPCD and dissolved natural organic matter) in the soil extract solutions, which compete for the non-selective hydroxyl radical reaction to PCP. However, our results indicate that HPCD has a beneficial effect on the degradation rates of PCP. This relative improvement in PCP degradation could be explained by the formation of the ternary complex (PCP-cyclodextrin-iron) which may direct hydroxyl reaction to PCP and which would, in any case, justify the use of a Fenton -like process for the final treatment of soil extract solutions. Total disappearance of PCP and 90% abatement of the chemical oxygen demand were achieved within an 11h electrolysis treatment time. Elucidation of the PCP degradation pathway indicates that after successive PCP hydroxylations, oxidative opening of the PCP aromatic ring quickly occurred, leading to small unstable non-chlorinated or partially chlorinated short chain carboxylic acids, such as monochloroacetic and dichloromaleic acid. Determination of the concentration of these acids shows that indirect electrochemical treatment leads to oxalic acid accumulation in aqueous solutions treated. A decrease in toxicity was observed at the end of the treatment time.

摘要

本研究旨在通过实验室规模,考察将环糊精溶液增强的冲洗能力与间接电化学处理相结合,从污染土壤中去除五氯苯酚(PCP)的技术可行性、作用机制及性能表现。其中,环糊精溶液用于去除土壤中的PCP,间接电化学处理则用于最终处置含有高浓度PCP(0.77mmolL(-1))的土壤提取液。羟丙基-β-环糊精(HPCD)溶液可使土壤提取液中PCP的水相浓度增加至土壤水洗过程中所得浓度的3.5倍。在水相中,PCP用电化学产生的芬顿试剂进行处理。在间接电化学处理条件下,HPCD存在时PCP水溶性的增加与PCP降解速率的相应降低相平衡。这是由于土壤提取液中高碳含量(HPCD和溶解的天然有机物)与PCP竞争非选择性的羟基自由基反应。然而,我们的结果表明HPCD对PCP的降解速率具有有益影响。PCP降解的这种相对改善可以通过三元络合物(PCP-环糊精-铁)的形成来解释,该络合物可能引导羟基与PCP反应,无论如何,这都证明了采用类芬顿工艺对土壤提取液进行最终处理的合理性。在11小时的电解处理时间内,PCP完全消失,化学需氧量降低了90%。PCP降解途径的阐明表明,在PCP连续羟基化之后,PCP芳香环迅速发生氧化开环,生成不稳定的非氯化或部分氯化的短链羧酸,如一氯乙酸和二氯马来酸。这些酸浓度的测定表明,间接电化学处理导致处理后的水溶液中草酸积累。在处理时间结束时观察到毒性降低。

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