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碱活化过一硫酸盐降解水中环丙沙星
引用本文:葛勇建,蔡显威,林翰,徐梦苑,沈一挺,周丹,钱梦洁,邓靖.碱活化过一硫酸盐降解水中环丙沙星[J].环境科学,2017,38(12):5116-5123.
作者姓名:葛勇建  蔡显威  林翰  徐梦苑  沈一挺  周丹  钱梦洁  邓靖
作者单位:浙江工业大学建筑工程学院, 杭州 310014,浙江工业大学建筑工程学院, 杭州 310014,浙江工业大学建筑工程学院, 杭州 310014,浙江工业大学建筑工程学院, 杭州 310014,浙江工业大学建筑工程学院, 杭州 310014,浙江工业大学建筑工程学院, 杭州 310014,浙江工业大学建筑工程学院, 杭州 310014,浙江工业大学建筑工程学院, 杭州 310014
基金项目:国家自然科学基金项目(51508509);中国博士后科学基金项目(2015M581936);天津市水质科学与技术重点实验室开放课题项目(TJKLAST-ZD-2017-01);浙江省自然科学基金项目(LY18E080036)
摘    要:采用碱活化过一硫酸盐(peroxymonosulfate,PMS)对环丙沙星(ciprofloxacin,CIP)的去除进行了系统地研究.结果表明,碱活化PMS体系能够高效地去除CIP.通过自由基捕获实验确定了单线态氧(~1O_2)和超氧自由基(O_2~-·)是反应体系中的主要活性物种.NaOH浓度、PMS浓度、反应温度和共存阴离子等对CIP在碱活化PMS体系中的去除均有一定影响.随着NaOH和PMS浓度的增加,CIP的降解均呈现出先增加后降低的趋势.提高反应温度能够加大CIP的反应速率,经过阿伦尼乌斯方程拟合得到的反应活化能为5.09 k J·mol~(-1).不同的阴离子对CIP的去除呈现不同的影响:Cl~-、SO_4~(2-)和NO_3~-对CIP的降解没有呈现明显的作用,H_2PO_4~(2-)能够有效地抑制环丙沙星的去除,而CO_3~(2-)极大地促进了反应进程.通过UPLC-MS/MS可检测到10种降解产物,CIP分子结构中的哌嗪环易于受到活性物种的攻击.

关 键 词:  过一硫酸盐  环丙沙星  降解  氧化产物
收稿时间:2017/4/24 0:00:00
修稿时间:2017/6/29 0:00:00

Base Activation of Peroxymonosulfate for the Degradation of Ciprofloxacin in Water
GE Yong-jian,CAI Xian-wei,LIN Han,XU Meng-yuan,SHEN Yi-ting,ZHOU Dan,QIAN Meng-jie and DENG Jing.Base Activation of Peroxymonosulfate for the Degradation of Ciprofloxacin in Water[J].Chinese Journal of Environmental Science,2017,38(12):5116-5123.
Authors:GE Yong-jian  CAI Xian-wei  LIN Han  XU Meng-yuan  SHEN Yi-ting  ZHOU Dan  QIAN Meng-jie and DENG Jing
Institution:College of Civil Engineering and Architecture, Zhejiang University of Technology, Hangzhou 310014, China,College of Civil Engineering and Architecture, Zhejiang University of Technology, Hangzhou 310014, China,College of Civil Engineering and Architecture, Zhejiang University of Technology, Hangzhou 310014, China,College of Civil Engineering and Architecture, Zhejiang University of Technology, Hangzhou 310014, China,College of Civil Engineering and Architecture, Zhejiang University of Technology, Hangzhou 310014, China,College of Civil Engineering and Architecture, Zhejiang University of Technology, Hangzhou 310014, China,College of Civil Engineering and Architecture, Zhejiang University of Technology, Hangzhou 310014, China and College of Civil Engineering and Architecture, Zhejiang University of Technology, Hangzhou 310014, China
Abstract:The degradation of ciprofloxacin (CIP) in a base activated peroxymonosulfate (PMS) system was investigated. Results showed that a base activated PMS system can efficiently remove CIP. Singlet oxygen (1 O2) and superoxide anion radical (O2-·) were confirmed to be the major reactive oxygen species through radical quenching experiments. The NaOH concentration, PMS concentration, reactive temperature, and coexisting anions also affected CIP removal. Both NaOH and PMS concentration presented a dual effect, which was highly concentration dependent. An improvement in reactive temperature accelerated CIP degradation, and the calculated activation energy (Ea) was determined to be 5.09 kJ·mol-1 through the fitting of the Arrhenius equation. Different anions had different effects on CIP degradation. No obvious change in CIP concentration was observed when Cl-, SO42-, and NO3- were introduced. H2PO42- inhibited the degradation, but CO32- significantly promoted it. Ten oxidation products were identified through UPLC-MS/MS analysis, and the piperazine ring in the molecular structure of CIP was preferentially attacked by reactive oxygen species in the base activated PMS system.
Keywords:base  peroxymonosulfate  ciprofloxacin  degradation  oxidation products
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