宁寻安1,
梁洁莹1,
卢杰1,
陈晓晖1,
宋健1,
陈泓妤1
1.广东工业大学环境科学与工程学院,广州 510006
基金项目: 国家自然科学基金资助项目(21577027)
广州市科技计划项目(201607010330)
广东省科技计划项目(2015A020215032)
Degradation of phenanthrene in aqueous solution by US/Fenton technique
KONG Minyi1,,NING Xunan1,
LIANG Jieying1,
LU Jie1,
CHEN Xiaohui1,
SONG Jian1,
CHEN Hongyu1
1.School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006, China
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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。
关键词: US/Fenton/
菲/
反应动力学/
降解产物/
多环芳烃
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.
Key words:US/Fenton/
phenanthrene/
reaction kinetics/
degradation product/
PAHs.
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[2] | 王靖宇,宁寻安,李锐敬,等.典型印染废水处理过程中芳香烃化合物的污染特征及污泥生态风险评价[J].环境化学,2015,34(6):1201-1208 |
[3] | 王丽.农产品中多环芳烃及卤代多环芳烃残留的检测方法和应用[D].重庆:西南大学,2013 |
[4] | 王艺霏,李亚男,王迪,等.高铁酸钾-Fenton联合氧化法对菲的去除[J].环境工程学报,2016,10(11):6536-6540 10.12030/j.cjee.201603162 |
[5] | 李婷,陈冰,马虹.UV-Fenton催化氧化法对采油废水中多环芳烃的处理效果[J].环境工程学报,2012,6(10):3475-3480 |
[6] | 徐其鹏,罗志龙,李萌,等.超声协同Fenton氧化法降解HMX废水及动力学研究[J].火炸药学报,2016,39(2) :102-106 |
[7] | 戴丽雅,张宏波,王谦,等.超声-芬顿法降解工业染料中间体废水[J].水处理技术,2017,43(4):70-78 10.16796/j.cnki.1000-3770.2017.04.016 |
[8] | 陈昶敏.超声-芬顿联合降解印染污泥中多环芳烃的竞争机理研究[D].广州:广东工业大学,2017 |
[9] | 苟玺莹,张盼月,钱锋,等.UV/H2O2降解水中对乙酰氨基酚的动力学及反应途径[J/OL]. [2017-07-24] 10.13671/j.hjkxxb.2017.0274 |
[10] | 欧晓霞,张凤杰,王崇,等.芬顿氧化法处理水中酸性品红的研究[J].环境工程学报,2010,4(7):1453-1456 |
[11] | BENDOUZ M,TRAN L H,COUDERT L,et al.Degradation of polycyclic aromatic hydrocarbons in different synthetic solutions by Fenton's oxidation[J].Environmental Technology Letters,2017,38(1):116-127 10.1080/09593330.2016.1188161 |
[12] | 陈颖,喻泽斌,孙玲芳,等.准好氧矿化垃圾反应床+超声/芬顿联用技术处理垃圾渗滤液[J].环境工程学报,2013,7(10):3946-3952 |
[13] | HIMANSHU G.Photocatalytic degradation of phenanthrene in the presence of akaganeite nano-rods and the identification of degradation products[J].RSC Advances,2016,6:112721-112727 10.1039/c6ra24602h |
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超声联合芬顿技术对水中菲的降解
孔敏仪1,,宁寻安1,
梁洁莹1,
卢杰1,
陈晓晖1,
宋健1,
陈泓妤1
1.广东工业大学环境科学与工程学院,广州 510006
基金项目: 国家自然科学基金资助项目(21577027) 广州市科技计划项目(201607010330) 广东省科技计划项目(2015A020215032)
关键词: US/Fenton/
菲/
反应动力学/
降解产物/
多环芳烃
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。
English Abstract
Degradation of phenanthrene in aqueous solution by US/Fenton technique
KONG Minyi1,,NING Xunan1,
LIANG Jieying1,
LU Jie1,
CHEN Xiaohui1,
SONG Jian1,
CHEN Hongyu1
1.School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006, China
Keywords: US/Fenton/
phenanthrene/
reaction kinetics/
degradation product/
PAHs
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.