| 引用本文: | 罗从伟,马军,江进,关朝婷,庞素艳,时玉龙,翟学东,武道吉.UV/H2O2降解三氯生动力学及反应机理[J].哈尔滨工业大学学报,2017,49(2):26.DOI:10.11918/j.issn.0367-6234.2017.02.005 |
| LUO Congwei,MA Jun,JIANG Jin,GUAN Chaoting,PANG Suyan,SHI Yulong,ZHAI Xuedong,WU Daoji.Degradation of triclosan by UV/H2O2：Kinetics and reaction mechanism[J].Journal of Harbin Institute of Technology,2017,49(2):26.DOI:10.11918/j.issn.0367-6234.2017.02.005 |
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| UV/H2O2降解三氯生动力学及反应机理 |
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罗从伟1,2,马军1,2,江进1,2,关朝婷1,2,庞素艳3,时玉龙1,2,翟学东4,武道吉5
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(1. 哈尔滨工业大学 市政环境工程学院,哈尔滨 150090;2.城市水资源与水环境国家重点实验室(哈尔滨工业大学), 哈尔滨 150090;3.绿色化工技术重点实验室(哈尔滨理工大学),哈尔滨 150040;4. 哈尔滨工业大学 科学与工业技术研究院, 哈尔滨 150090;5.山东建筑大学 市政与环境工程学院,济南 250101)
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| 摘要: |
| 为考察紫外催化过氧化氢工艺降解三氯生的降解效能，利用动力学模型对三氯生的表观降解速率进行模拟.考察氧化剂投加量、三氯生浓度、NOM质量浓度和pH对三氯生降解速率的影响.结果表明，H2O2的投加量小于1 mmol/L时，三氯生的降解速率随H2O2浓度的增加而增加，而当H2O2的投加量大于1 mmol/L时，由于H2O2对HO ·的捕获作用增强，三氯生的降解速率随H2O2投加量的增加而降低.当三氯生的初始浓度增加时，体系中HO ·的稳态浓度随之降低，导致三氯生降解的表观速率降低.体系中存在NOM时，三氯生的降解速率显著降低，主要是由于NOM能够与三氯生竞争光子和HO ·.三氯生去质子化后更快地被UV/H2O2降解，其去质子化形态的摩尔吸光系数变大，而且其与HO ·的二级反应速率更快.通过LC/MS-MS检测UV/H2O2氧化TCS得到6种产物，推测TCS的降解途径主要是通过脱氯反应和羟基化反应.
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| 关键词: 三氯生 紫外 过氧化氢 动力学 模拟计算 氧化产物 |
| DOI：10.11918/j.issn.0367-6234.2017.02.005 |
| 分类号:TU991.2 |
| 文献标识码:A |
| 基金项目:国家自然科学基金(3,1)；黑龙江省应用技术研究与开发计划项目(PS13H05)；城市水资源与水环境国家重点实验室开放基金(HIT, 2016DX04)；中国博士后科学基金(2015T80366) |
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| Degradation of triclosan by UV/H2O2：Kinetics and reaction mechanism |
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LUO Congwei1,2, MA Jun1,2, JIANG Jin1,2, GUAN Chaoting1,2, PANG Suyan3, SHI Yulong1,2, ZHAI Xuedong4, WU Daoji5
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(1.School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin 150090, China; 2.State Key Laboratory of Urban Water Resource and Environment (Harbin Institute of Technology), Harbin 150090, China; 3.Key Laboratory of Green Chemical Engineering and Technology of College of Heilongjiang Province (Harbin University of Science and Technology), Harbin 150040, China; 4.School of Science and Industrial Technology, Harbin Institute of Technology, Harbin 150090, China; 5.School of Municipal and Environmental Engineering, Shandong Jianzhu University, Jinan 250101, China)
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| Abstract: |
| The aim of this work is to investigate the transformation efficiency of triclosan (TCS) at the wavelength of 254 nm in the presence of H2O2. The effects of oxidant dosage, TCS concentration, NOM, and pH were evaluated. Most of these kinetic results could be described by a steady-state kinetic model. Increasing dosage of H2O2 increased the observed pseudo-first-order rate constant for TCS degradation (kobs) when H2O2 < 1 mmol/L. However, when H2O2 >1 mmol/L, kobs decreased with H2O2 dosage increased due to the effects of radical scavenging by H2O2. Increasing concentration of TCS decreased the steady-state concentration of HO ·. The presence of NOM significantly decreased kobs due to the effects of UV absorption and radical scavenging. When pH=9, kobs was higher than that when pH=5-7. This could be attributed that the deprotonated TCS was more reactive than protonated TCS. Six products were detected in TCS treated by UV/H2O2. A tentative pathway was proposed, where dechlorination and hydroxylation reaction were involved.
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| Key words: triclosan UV H2O2 kinetics modeling oxidation products |
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