超声联合芬顿技术对水中菲的降解
Degradation of phenanthrene in aqueous solution by US/Fenton technique
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摘要: 利用超声联合芬顿（US/Fenton）降解模拟水中的菲，考察降解过程中菲的反应动力学影响因素，如初始pH、H2O2投量、反应温度、H2O2:Fe2+比值、超声功率。进一步通过气相色谱/质谱（GC/MS）检测其中间产物，并推测降解途径。结果表明：US/Fenton可有效降解水中的菲，符合伪一级反应动力学模型，菲的降解速率随H2O2投量和温度的升高而增大；随H2O2:Fe2+比值和超声功率的增大而降低；酸性条件（pH=3.0）是降解体系的最适宜环境，此时反应速率常数达到最大值0.035 min-1。通过分析可知，菲降解的中间产物有9,10菲醌、2-羟基-9-芴、(1,1′)-二苯基-2,2′-二甲醛、9-芴酮，菲结构中的9,10位首先受到攻击，进而断链，再被氧化生成醛、羧酸、酚类物质，最后矿化成CO2和H2O。Abstract: The degradation kinetics and pathway of phenanthrene (Phe) in aqueous solution by US/Fenton were investigated. The effects of the important factors on phenanthrene degradation including the initial pH, the dosage of H2O2, the temperature, H2O2: Fe2+ moral rations as well as the ultrasonic power were evaluated. The results indicated that the Phe was removed effectively using US/Fenton, and the degradation of Phe could be well fitted with the pseudo-first-order kinetics model. The Phe degradation rate constant increased with increasing both of the dosage of H2O2 and temperature. However, the degradation rate constant decreased by the increasing of H2O2: Fe2+ moral rations and ultrasonic power. The optimum pH for the degradation of phenanthrene was pH 4.0, and 0.022 min-1 of the maximum degradation rate constant was achieved. The intermediate products by gas chromatography-mass spectrometry (GC/MS) were 9,10-phenanthrenedione, 2-hydroxy-9H-fluoren-9-one, (1,1′-Biphenyl)-2,2′-dicarboxaldehyde, 9H-fluoren-9-one.It indicated that the 9,10 bits in the structure of phenanthrene was attacked first through breaking, which broke the chain and were oxidized to aldehydes, carboxylic acids, phenols and mineralized into CO2 and H2O.
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Key words:
- US/Fenton /
- phenanthrene /
- reaction kinetics /
- degradation product /
- PAHs
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