非水溶性铁Schiff碱配合物活化H_(2)O_(2)光催化降解环丙沙星  

Photocatalytic Degradation of Ciprofloxacin by Activation of H_(2)O_(2) with Insoluble Iron Schiff-Base Complexes

作　　者：李张丽 杨健 贾漫珂[1,2] 黄应平 刘铭[1,2] 周后乐[1,2] 田海林 LI Zhangli;YANG Jian;JIA Manke;HUANG Yingping;LIU Ming;ZHOU Houle;TIAN Hailin(College of Biological Pharmaceutical Sciences,China Three Gorges University,Yichang 443002,Hubei,China;Engineering Research Center of Eco-environment in Three Gorges Reservoir Rerion of Ministry of Education,China Three Gorges University,Yichang 443002,Hubei,China;College of Hydraulic and Environmental Engineering,China Three Gorges University,Yichang 443002,Hubei,China)

机构地区：[1]三峡大学生物与制药学院,湖北宜昌443002 [2]三峡大学三峡库区生态环境教育部工程研究中心,湖北宜昌443002 [3]三峡大学水利与环境学院,湖北宜昌443002

出　　处：《武汉大学学报（理学版）》2021年第4期367-374,共8页Journal of Wuhan University:Natural Science Edition

基　　金：国家自然科学基金(21972073);湖北省引进国外人才和智力项目(2019BJH004);高等学校学科创新引智计划(“111”计划,D20015);中国博士后科学基金(2018M640721);三峡大学硕士培优基金(2021SSPY156)。

摘　　要：以3,5-二氯水杨醛和邻苯二胺合成Schiff碱配体,与铁(Ⅲ)配位,得到3,5-二氯水杨醛缩邻苯二胺Schiff碱铁(Fe-3,5ClSPA)光催化剂。以环丙沙星(ciprofloxacin,CIP)为有机污染物,在可见光(λ≥420 nm)照射下通过Fe-3,5ClSPA活化H2O2对CIP进行光催化氧化降解,在光催化反应90 min时对CIP降解率达到98.4%,Fe-3,5ClSPA在偏酸性条件下(pH 3.0~5.0)可有效活化H_(2)O_(2)而降解CIP。通过自由基捕获实验证实,·OH为光催化降解过程中主要的活性氧化物种。通过对CIP降解产物质谱分析,Fe-3,5ClSPA可见光活化H2O2光催化降解CIP经历了脱氟、喹啉羟基化、哌嗪环氧化和脱羧等途径生成5种中间产物。此外,非均相Fe-3,5ClSPA光催化体系在5次重复使用后,对CIP降解率仍达到74.2%,表明Fe-3,5ClSPA光催化剂具有较好的稳定性和重复利用性。In this paper,an iron Schiff-base(Fe-3,5 ClSPA)coordination compound was synthesized with 3,5-dichlorosalicylaldehyde,o-phenylenediamine and iron(Ⅲ).Ciprofloxacin(CIP)was used to the organic pollutant,which was removed by Fe-3,5 ClSPA and activated H2O2 in visible light(λ≥420 nm).The CIP degradation rate of Fe-3,5 ClSPA reached to 98.4% in 90 min,and Fe-3,5 ClSPA could effectively decompose H_(2)O_(2) molecules under acidic conditions(pH 3.0-5.0).Through the radicals capture experiment,it has been demonstrated that·OH was the main active oxidative species in the photocatalytic degradation process.According to the analysis of the mass spectra of CIP degradation,the photocatalytic degradation of CIP by Fe-3,5 ClSPA and H2O2 under visible-light irradiation mainly underwent defluorination,quinolone hydroxylated,piperazine epoxidation and decarboxylation to generate five intermediate products.Additionally,the CIP degradation rate of Fe-3,5 ClSPA was still 74.2% after 5 cycles,indicating that the Fe-3,5 ClSPA photocatalysts have good stability and reusability.

关 键 词：铁Schiff碱配合物 活化H_(2)O_(2) 光催化 环丙沙星 

分 类 号：O643[理学—物理化学]