高价铁(Ⅵ)化合物氧化降解磺胺甲噁唑的机理研究
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- 英文论文题名：Oxidative Degradation Mechanism of Sulfamethoxazole Antibiotics by Ferrate(Ⅵ):A DFT Study
- 论文作者：于航 ; 孔庆伟 ; 陈景文 ; 罗一
- 英文论文作者：Hang Yu ; Qingkong Wei ; Jingwen Chen ; Yi Luo ; State Key Laboratory of Fine Chemicals ; School of Pharmaceutical Science and Technology ; Dalian University of Technology ; Key Laboratory of Industrial Ecology and Environmental Engineering (MOE) ; School of Environmental Science and Technology ; Dalian University of Technology
- 年：2016
- 作者机构：大连理工大学精细化工国家重点实验室;大连理工大学环境学院;
- 论文关键词：高价铁[Fe(Ⅵ)]化合物 ; 磺胺甲噁唑 ; 氧化降解 ; 机理研究
- 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;O643.12
- 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：201k
- 原文格式：D
- 会议级别：全国
摘要
高价铁[Fe(Ⅵ)]化合物作为一种环境友好的水处理氧化剂,具有氧化效率高和产物易分离的优点1。该类化合物氧化降解水体中磺胺类药物的研究早已受到广泛关注2。本文选择在水体中具有高检测频率的磺胺甲噁唑(SMX)作为磺胺类药物的模型化合物,采用计算化学的方法探讨了Fe(Ⅵ)化合物氧化降解SMX的反应机理。结果表明,Fe(Ⅵ)化合物氧化SMX的异噁唑环部分时,通过Fe(Ⅵ)化合物中的羰基氧作为氧供体,亲核进攻异噁唑部分,从而发生开环反应。同时,通过计算还发现,Fe(Ⅵ)化合物可以使SMX的异噁唑部分开环的主要原因为Fe(Ⅵ)化合物中存在单电子,更容易离域到异噁唑环上,破坏了异噁唑环的稳定性使其发生开环反应。在探讨反应中水分子的作用时,发现水在反应中以配位络合的形式更有利于反应发生。通过理论研究,揭示了磺胺甲噁唑被Fe(Ⅵ)化合物氧化降解的机理,有利于预测其他磺胺类抗生素在高价铁化合物作用下的氧化降解过程。
Ferrate(Ⅵ) as an environment-friendly oxidant in water treatment.However,the related mechanism of the degradation of micrpollutants such as sulfamethoxazole(SMX) by ferrate(Ⅵ) is ambiguous.This paper indicates an explicit ferrate(Ⅵ)-mediated oxidation mechanism of SMX by density function theory(DFT) calculation.Our results show that the nucleophilic attack of HFe O4-to the isoxazole moiety initiates the ring-opening reaction of the isoxazole moieties,and the O-atom donor is ferrate species Electron delocalization play important roles in the ferrate(Ⅵ)-mediated ring-opening of isoxazole,which sheds light on the difference between ferrate(Ⅵ) and other oxidants such as ozone in sulfonamide pollutants.In addition,the calculations suggest that a water molecule may interact with ferrate species though hydrogen bond interaction during the oxidation process.These results can be extended to predicting the degradation process of other sulfonamides as a kind of pharmaceuticals and personal care products in ferrate(Ⅵ)-mediated treatments.
Ferrate(Ⅵ) as an environment-friendly oxidant in water treatment.However,the related mechanism of the degradation of micrpollutants such as sulfamethoxazole(SMX) by ferrate(Ⅵ) is ambiguous.This paper indicates an explicit ferrate(Ⅵ)-mediated oxidation mechanism of SMX by density function theory(DFT) calculation.Our results show that the nucleophilic attack of HFe O4-to the isoxazole moiety initiates the ring-opening reaction of the isoxazole moieties,and the O-atom donor is ferrate species Electron delocalization play important roles in the ferrate(Ⅵ)-mediated ring-opening of isoxazole,which sheds light on the difference between ferrate(Ⅵ) and other oxidants such as ozone in sulfonamide pollutants.In addition,the calculations suggest that a water molecule may interact with ferrate species though hydrogen bond interaction during the oxidation process.These results can be extended to predicting the degradation process of other sulfonamides as a kind of pharmaceuticals and personal care products in ferrate(Ⅵ)-mediated treatments.
引文
[1]Sharma,V.K.;Zboril,R.;Varma,R.S.Acc.Chem.Res.2015,48,182.
[2]Sharma,V.K.;Mishra,S.K.;Nesnas,N.Environ.Sci.Technol.2006,40,7222.
[2]Sharma,V.K.;Mishra,S.K.;Nesnas,N.Environ.Sci.Technol.2006,40,7222.