uvpms体系中氟甲喹的降解动力学及机理研究(附件)
本文采用紫外（UV）激活过硫酸氢盐（PMS）降解水溶液中的氟甲喹（FLU）方法，研究了氧化剂剂量、溶液初始pH值、典型无机阴阳离子（NH4+、Mg2+、Fe3+、Cl-、NO3-、HCO3-）、腐殖酸及不同水基质对降解效果的影响，并探究了不同的自由基淬灭剂（乙醇和叔丁醇）对反应体系中自由基（硫酸根自由基（SO4·-）和羟基自由基（·OH））的淬灭作用。使用LC-MS/MS分析鉴别得到了17种氧化产物，并推测了可能的反应途径。结果表明，氧化剂PMS的浓度与降解效率呈正相关；FLU的降解速率受到溶液初始pH值的影响，氟甲喹在强酸或强碱体系中的降解效果优于中性环境；体系中Mg2+的存在能显著促进氟甲喹的降解，而腐殖酸、HCO3-及高浓度Fe3+对氟甲喹的降解有抑制作用；氟甲喹在不同水基质中的降解速率排序如下合成废水 > 自来水 > 超纯水 > 九乡河水 > 二沉池出水。乙醇和叔丁醇淬灭实验显示二者的淬灭效果不同，说明本反应体系中可能存在SO4·-和HO·两种活性自由基。
目录
摘要 １
关键词 １
Abstract １
引言
引言
1 材料与方法 ２
1．1 试剂 ２
1．2 实验方法 ３
1．1．1 不同水基质中氟甲喹反应体系的制备 ３
1．1．2 氟甲喹光降解实验 ３
1．3 分析方法 ３
1．3．1 HPLC分析 ３
1．3．2 LC/MSMS分析 ３
2 结果与分析 ４
2．1 氟甲喹在超纯水中降解的动力学分析 ４
2．1．1 PMS浓度的影响 ４
2．1．2 腐殖酸的影响 ４
2．1．3 初始pH值的影响 ５
2．1．4 水体中常见阴、阳离子的影响 ６
2．2 FLU在自然水体和合成水中的降解 ８
2．3 系统自由基的鉴定 ９
2．4 反应机理 １１
3 讨论 １２
3．1 UV/PMS体系对FLU的降解效果 １２
3．2 反应条件对FLU降解效果的影响 １２< *好棒文|www.hbsrm.com +Q: ￥351916072￥
br /> 3．3 FLU在不同水基质中的降解情况 １２
3．4 FLU在UV/PMS体系中降解的反应路径推断 １３
致谢 １３
参考文献 １３
UV/PMS体系中氟甲喹的降解动力学及机理研究
Degradation of flumequine in aqueous by UVactivated peroxymonosulfate:
Kinetics, products and reaction mechanisms
Student majoring in Agricultural Resources and Environment Yumeng Qi
Tutor Yangchun Xu
Abstract: The degradation of flumequine (FLU) in aqueous by ultraviolet (UV)activated peroxymonosulfate (PMS) was investigated in this work. The effects of operating parameters ( the oxidant doses, pH, the presence of typical anions and cations (NH4+、Mg2+、Fe3+、Cl、NO3、HCO3) and humic acid ) were evaluated. The degradation coefficients of FLU in different water matrices (Synthetic wastewater, Tap water, Ultrapure water, Jiuxiang river water, Secondary effluent water) were also explored. It was found that an increase of the PMS and the presence of Mg2+ could accelerate the reaction, while HA, HCO3? and Fe3+ (0.5mM) inhibited the reaction. The degradation constants of FLU were obviously accelerated in strong acid or alkali conditions. The order for FLU removal in various water matrices was as follows: Synthetic wastewater > Tap water > Ultrapure water > Jiuxiang river water > Secondary effluent water. The results of ethanol and tertbutanol effects showed that SO4 and HOall existed in this reaction system.
Key words: flumequine；UV/PMS；degradation kinetics；reaction pathways
引言
氟喹诺酮类抗生素被广泛用于治疗人类和动物的细菌感染，它们进入人或动物体内后40%至90%以母体或代谢物的形式随粪便或尿液进入环境[13]。氟甲喹（FLU）是一种典型的氟喹诺酮类抗生素（图1），该药物已被广泛应用于家禽、家畜和水产养殖行业。传统的废水处理方法不足以完全去除FLU，其在水体环境中的残余浓度可达2.5 50 ng L1[45]。然而，环境中残留的抗生素对人体健康以及整个生态系统存在潜在危害，比如容易引起毒性损伤、过敏反应、三致作用（致癌、致畸、致突变）等，破坏生态平衡，威胁生物多样性[6,38,39]。抗生素的环境污染及其生态毒理效应已成为我国乃至全球所面临的重大环境问题之一[6]。
目录
摘要 １
关键词 １
Abstract １
引言
引言
1 材料与方法 ２
1．1 试剂 ２
1．2 实验方法 ３
1．1．1 不同水基质中氟甲喹反应体系的制备 ３
1．1．2 氟甲喹光降解实验 ３
1．3 分析方法 ３
1．3．1 HPLC分析 ３
1．3．2 LC/MSMS分析 ３
2 结果与分析 ４
2．1 氟甲喹在超纯水中降解的动力学分析 ４
2．1．1 PMS浓度的影响 ４
2．1．2 腐殖酸的影响 ４
2．1．3 初始pH值的影响 ５
2．1．4 水体中常见阴、阳离子的影响 ６
2．2 FLU在自然水体和合成水中的降解 ８
2．3 系统自由基的鉴定 ９
2．4 反应机理 １１
3 讨论 １２
3．1 UV/PMS体系对FLU的降解效果 １２
3．2 反应条件对FLU降解效果的影响 １２< *好棒文|www.hbsrm.com +Q: ￥351916072￥
br /> 3．3 FLU在不同水基质中的降解情况 １２
3．4 FLU在UV/PMS体系中降解的反应路径推断 １３
致谢 １３
参考文献 １３
UV/PMS体系中氟甲喹的降解动力学及机理研究
Degradation of flumequine in aqueous by UVactivated peroxymonosulfate:
Kinetics, products and reaction mechanisms
Student majoring in Agricultural Resources and Environment Yumeng Qi
Tutor Yangchun Xu
Abstract: The degradation of flumequine (FLU) in aqueous by ultraviolet (UV)activated peroxymonosulfate (PMS) was investigated in this work. The effects of operating parameters ( the oxidant doses, pH, the presence of typical anions and cations (NH4+、Mg2+、Fe3+、Cl、NO3、HCO3) and humic acid ) were evaluated. The degradation coefficients of FLU in different water matrices (Synthetic wastewater, Tap water, Ultrapure water, Jiuxiang river water, Secondary effluent water) were also explored. It was found that an increase of the PMS and the presence of Mg2+ could accelerate the reaction, while HA, HCO3? and Fe3+ (0.5mM) inhibited the reaction. The degradation constants of FLU were obviously accelerated in strong acid or alkali conditions. The order for FLU removal in various water matrices was as follows: Synthetic wastewater > Tap water > Ultrapure water > Jiuxiang river water > Secondary effluent water. The results of ethanol and tertbutanol effects showed that SO4 and HOall existed in this reaction system.
Key words: flumequine；UV/PMS；degradation kinetics；reaction pathways
引言
氟喹诺酮类抗生素被广泛用于治疗人类和动物的细菌感染，它们进入人或动物体内后40%至90%以母体或代谢物的形式随粪便或尿液进入环境[13]。氟甲喹（FLU）是一种典型的氟喹诺酮类抗生素（图1），该药物已被广泛应用于家禽、家畜和水产养殖行业。传统的废水处理方法不足以完全去除FLU，其在水体环境中的残余浓度可达2.5 50 ng L1[45]。然而，环境中残留的抗生素对人体健康以及整个生态系统存在潜在危害，比如容易引起毒性损伤、过敏反应、三致作用（致癌、致畸、致突变）等，破坏生态平衡，威胁生物多样性[6,38,39]。抗生素的环境污染及其生态毒理效应已成为我国乃至全球所面临的重大环境问题之一[6]。
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