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电催化产生的羟基自由基对水介质中阿特拉津的降解。动力学和机理研究。

Degradation of atrazine in aqueous medium by electrocatalytically generated hydroxyl radicals. A kinetic and mechanistic study.

作者信息

Balci Beytul, Oturan Nihal, Cherrier Richard, Oturan Mehmet A

机构信息

Université Paris-Est, Laboratoire Géomatériaux et Géologie de l'Ingénieur, 77454 Marne-la-Vallée Cedex 2, France.

出版信息

Water Res. 2009 Apr;43(7):1924-34. doi: 10.1016/j.watres.2009.01.021. Epub 2009 Jan 31.

DOI:10.1016/j.watres.2009.01.021
PMID:19249809
Abstract

Oxidative degradation of atrazine by hydroxyl radicals (()OH) was studied in aqueous medium. ()OH were formed in situ from electrochemically generating Fenton's reagent by an indirect electrochemical advanced oxidation process. Identification and evolution of seven main aromatic metabolites and four short-chain carboxylic acids were performed by using liquid chromatography analyses. Total organic carbon (TOC) and ionic chromatography were used in order to evaluate the mineralization efficiency of treated aqueous solutions. A high mineralization rate of 82% (never reported until now) was obtained. The oxidative degradation of cyanuric acid, the ultimate product of atrazine degradation, was highlighted for the first time. The absolute rate constant of the reaction between atrazine and hydroxyl radicals was evaluated by competition kinetics method as (2.54+/-0.22)x10(9)M(-1)s(-1). Considering all oxidation reaction intermediates and end products a general reaction sequence for atrazine degradation by hydroxyl radicals was proposed.

摘要

在水介质中研究了羟基自由基(·OH)对莠去津的氧化降解。·OH通过间接电化学高级氧化过程由电化学产生的芬顿试剂原位生成。通过液相色谱分析对七种主要芳香族代谢物和四种短链羧酸进行了鉴定和演变分析。使用总有机碳(TOC)和离子色谱法来评估处理后水溶液的矿化效率。获得了高达82%的高矿化率(此前从未报道过)。首次突出了莠去津降解的最终产物氰尿酸的氧化降解。通过竞争动力学方法评估了莠去津与羟基自由基反应的绝对速率常数为(2.54±0.22)×10⁹ M⁻¹ s⁻¹。考虑到所有氧化反应中间体和最终产物,提出了羟基自由基降解莠去津的一般反应序列。

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