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水相中的乙撑硫脲的臭氧化和过氧单磺酸盐氧化:操作参数优化和副产物鉴定。

Ozonation and peroxone oxidation of ethylenethiourea in water: operational parameter optimization and by-product identification.

机构信息

Department of Sanitary and Environmental Engineering, Universidade Federal de Minas Gerais, Belo Horizonte, 31270-901, Brazil.

出版信息

Environ Sci Pollut Res Int. 2015 Jan;22(2):903-8. doi: 10.1007/s11356-014-3616-y. Epub 2014 Sep 27.

Abstract

The objective of this work was to study the degradation and mineralization of ethylenethiourea (ETU) in water by ozonation at different pH values and in the presence of hydrogen peroxide. Degradation experiments were performed using an initial ETU concentration of 50 ppm for 180 min with a gas flux of 0.25 dm(3) min(-1) and an O3 production rate of 12.1 mg min(-1). Degradation of by-products was monitored by direct injection electrospray ionization mass spectrometry (ESI-MS), ETU concentration was determined by HPLC-UV, and its mineralization was detected by total organic carbon (TOC) analysis. Optimum degradation of ETU in water was observed at pH = 11, whereas at pH = 3, the degradation of ETU was slowest, indicating that the reaction occurred through different mechanisms. The additional effects of hydroxyl radicals formed at the highest pH can be used to explain the results obtained in this study. Peroxone experiments were carried out in the presence of 400 and 800 mg L(-1) H2O2; the degradation of ETU was faster at 400 mg L(-1) H2O2. This was attributed to the scavenging effect of the excess H2O2. ETU treatment by ozonation produced several by-products of degradation such as ethylene urea and 2-imidazoline.

摘要

本工作旨在研究乙硫脲(ETU)在不同 pH 值和过氧化氢存在下通过臭氧化的降解和矿化。降解实验在初始 ETU 浓度为 50ppm 下进行 180min,气体流速为 0.25dm³min⁻¹,臭氧生成速率为 12.1mgmin⁻¹。通过直接注入电喷雾电离质谱(ESI-MS)监测副产物的降解,通过 HPLC-UV 测定 ETU 浓度,并通过总有机碳(TOC)分析检测其矿化。在 pH=11 时观察到 ETU 在水中的最佳降解,而在 pH=3 时,ETU 的降解最慢,表明反应通过不同的机制发生。在最高 pH 值下形成的羟基自由基的附加作用可以用来解释本研究中得到的结果。在存在 400 和 800mgL⁻¹H2O2 的过氧单磺酸盐实验中,在 400mgL⁻¹H2O2 时,ETU 的降解更快。这归因于过量 H2O2 的清除作用。臭氧化处理 ETU 产生了几种降解副产物,如乙烯脲和 2-咪唑啉。

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