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Oxidation of 1,1,1-Trichloroethane Stimulated by Thermally Activated Persulfate

化学 过硫酸盐 腐植酸 分解 甲酸 二氯甲烷 无机化学 三羧酸 反应速率常数 二氯乙酸 摩尔浓度 核化学 降级(电信) 动力学 色谱法 有机化学 催化作用 溶剂 物理 肥料 柠檬酸循环 计算机科学 电信 量子力学
作者
Xiaogang Gu,Shuguang Lu,Lin Li,Zhaofu Qiu,Qian Sui,Kuangfei Lin,Qishi Luo
出处
期刊:Industrial & Engineering Chemistry Research [American Chemical Society]
卷期号:50 (19): 11029-11036 被引量:158
标识
DOI:10.1021/ie201059x
摘要

In this study, thermally activated persulfate (PS) to stimulate the oxidation of 1,1,1-trichloroethane (TCA) in groundwater remediation was investigated. The effects of various factors including temperature; initial TCA concentration; PS/TCA molar ratio; solution pH; and common constituents in groundwater such as Cl–, HCO3–, SO42–, and NO3– anions and humic acid (HA) were evaluated. The experimental results showed that TCA can be completely oxidized in 2 h at 50 °C with a PS/TCA molar ratio of 100/1, indicating the effectiveness of thermally activated PS oxidation for TCA removal. TCA oxidation was fitted with a pseudo-first-order kinetic model, and the rate constant was found to increase with increasing temperature and PS/TCA molar ratio, but to decrease with increasing initial TCA concentration. In addition, acidic conditions were favorable to TCA removal and elevating, the initial solution pH value (from pH 3 to 11) decreased the TCA degradation rate. Anions Cl– and HCO3– had negative effects on TCA removal, whereas the effects of both SO42– and NO3– were negligible. With 5–10 mg L–1 concentrations of HA in solution, an inhibitive effect was observed, indicating that dissolved organic matter consumed some of the oxidant. However, the anticipated effective thermally activated PS oxidation of TCA in groundwater from a real contaminated site was not achieved because of the complex solution matrix. On the other hand, the TCA degradation mechanism derived from GC/MS analytical results confirmed formic acid, dichloromethane, and trichloromethane as the primary intermediates, and therefore, two TCA decomposition pathways were proposed. In conclusion, thermally activated PS oxidation is a highly promising technique for TCA-contaminated groundwater remediation, but more complex constituents in in situ groundwater should be carefully considered for its practical application.
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