双氯芬酸在高铁酸钾氧化过程的反应动力学和降解效能研究
详细信息 查看官网全文
- 英文论文题名：Reaction Kinetics and Degradation Efficiency of Ferrate(Ⅵ) Oxidation of Diclofenac in Water
- 论文作者：袁建梅 ; 汪应灵 ; 谢友海 ; 刘国光
- 英文论文作者：Jianmei Yuan ; Yingling Wang ; Youhai Xie ; Guoguang Liu ; Key Laboratory of Medical Molecular Probes ; School of Basic Medical Sciences ; Xinxiang Medical University ; School of Environment ; Henan Normal University
- 年：2016
- 作者机构：新乡医学院基础医学院医用分子探针重点实验室;河南师范大学环境学院;
- 论文关键词：双氯芬酸 ; 高铁酸钾 ; 反应动力学 ; 影响因素
- 会议召开时间：2016-07-01
- 会议录名称：中国化学会第30届学术年会摘要集-第二十六分会：环境化学
- 语种：中文
- 分类号：X52;O643.1
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第二十六分会 ; 环境化学
- 会议地点：中国辽宁大连
- 主办单位：中国化学会
- 学会名称：中国化学会
- 页数：1
- 文件大小：119k
- 原文格式：D
- 会议级别：全国
摘要
双氯芬酸药物是一种难以生物降解的环境污染物,传统的絮凝、沉淀和砂滤过程对其去除率并不高,导致部分污染物进入到自来水消毒阶段[1-2]。本文研究了Fe(Ⅵ)氧化双氯芬酸的反应动力学、去除效果及影响因素。结果表明,Fe(Ⅵ)能够有效氧化降解水体中的双氯芬酸,反应遵循二级反应动力学模式。当pH 9.0,反应温度为25℃时,反应速率常数为5.04 M~(-1)·s~(-1)。pH值、反应温度和Fe(Ⅵ)投加量对Fe(Ⅵ)氧化双氯芬酸反应影响显著,在pH 7.0~11.0范围内,反应速率常数和降解率随pH值升高而逐渐降低,其中HFe O4-和Fe O42-与双氯芬酸之间的比反应速率常数分别为16.8 M~(-1)·s~(-1)和3.61 M~(-1)·s~(-1)。Fe(Ⅵ)氧化双氯芬酸的活化能、焓变和熵变分别为23.3 k J·mol~(-1)、20.9 k J·mol~(-1)、~(-1)61.0 J·mol~(-1)·K~(-1)。水体共存无机离子和天然有机物的影响实验结果表明:不同程度促进效应的共存因子有NO3-、HCO3-、NH4+、Ca~(2+)、Fe3+、CTAB和腐殖酸,起抑制作用的有Cl-、SDBS和Tween-80,SO42-、Mg~(2+)对反应影响甚微,同时提出了各个环境因子发挥效应的作用机制。
The reaction kinetics,removal efficiency and influence factors on the oxidation of DCF by ferrate were investigated.The study demonstrated that Fe(Ⅵ) could be applied to effectively remove DCF in the disinfection of potable water.The reaction between DCF and Fe(Ⅵ) followed second-order kinetics.The value of rate constant was measured to be 5.04 M~(-1)·s~(-1),at pH 9.0 and 298 K.The concentration of Fe(Ⅵ),pH and temperature exhibited significant influences on the DCF-Fe(Ⅵ) reactivity.The rate constants and degradation rates gradually decreased as pH was increased from 7.0 to 11.0,and the species-specific rate constants were 16.8 M~(-1)·s~(-1) for HFe O4-and 3.61 M~(-1)·s~(-1) for Fe O42-respectively.Ea,△H and △S were determined to be 23.3 k J·mol~(-1),20.9 k J·mol~(-1),~(-1)61.0 J·mol~(-1)·K~(-1),respectively.The experiments of coexisting substances in nature water showed that the presence of NO3-,HCO3-,NH4+,Ca~(2+),Fe3+,CTAB and humic acid clearly initiated its promotion,whereas the presence of Cl-,SDBS and Tween-80 had some inhibition effect on the removal of DCF,the addition of SO42-and Mg~(2+) conveyed little influences on the reaction.Furthermore,the causal effects of the relevant factors were interpreted.
The reaction kinetics,removal efficiency and influence factors on the oxidation of DCF by ferrate were investigated.The study demonstrated that Fe(Ⅵ) could be applied to effectively remove DCF in the disinfection of potable water.The reaction between DCF and Fe(Ⅵ) followed second-order kinetics.The value of rate constant was measured to be 5.04 M~(-1)·s~(-1),at pH 9.0 and 298 K.The concentration of Fe(Ⅵ),pH and temperature exhibited significant influences on the DCF-Fe(Ⅵ) reactivity.The rate constants and degradation rates gradually decreased as pH was increased from 7.0 to 11.0,and the species-specific rate constants were 16.8 M~(-1)·s~(-1) for HFe O4-and 3.61 M~(-1)·s~(-1) for Fe O42-respectively.Ea,△H and △S were determined to be 23.3 k J·mol~(-1),20.9 k J·mol~(-1),~(-1)61.0 J·mol~(-1)·K~(-1),respectively.The experiments of coexisting substances in nature water showed that the presence of NO3-,HCO3-,NH4+,Ca~(2+),Fe3+,CTAB and humic acid clearly initiated its promotion,whereas the presence of Cl-,SDBS and Tween-80 had some inhibition effect on the removal of DCF,the addition of SO42-and Mg~(2+) conveyed little influences on the reaction.Furthermore,the causal effects of the relevant factors were interpreted.
引文
[1]Evgenidou E N,Konstantinou I K,Lambropoulou D A.Science of the Total Environment,2015,505:905-926
[2]Michael I,Achilleos A,Lambropoulou D,et al.Applied Catalysis B:Environmental,2014,147:1015-1027
[2]Michael I,Achilleos A,Lambropoulou D,et al.Applied Catalysis B:Environmental,2014,147:1015-1027