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氯离子对模拟太阳光活化过一硫酸氢钾氧化卡马西平的影响规律
引用本文:竺哲欣,马晓吉,尚志国,吕汪洋,陈文兴.氯离子对模拟太阳光活化过一硫酸氢钾氧化卡马西平的影响规律[J].环境科学学报,2021,41(6):2131-2137.
作者姓名:竺哲欣  马晓吉  尚志国  吕汪洋  陈文兴
作者单位:浙江理工大学材料科学与工程学院,杭州 310018
基金项目:国家自然科学基金(No.22006136);浙江省自然科学基金(No.LQ19E090023)
摘    要:研究了氯离子存在条件下模拟太阳光活化过一硫酸盐(PMS)催化氧化模型污染物卡马西平(CBZ)的效果及机理.结果表明,无氯离子存在时,光活化PMS在30 min内只能转化25%左右的CBZ;随着氯离子浓度的增加,PMS/氯离子光催化体系对CBZ的氧化速率也迅速增加.通过电子顺磁共振(EPR)测试、活性种捕获实验等方式确定了氯离子/PMS光催化体系是以HClO为主要的氧化活性种.在无氯离子存在时,光活化PMS以1O2活性种为主.随着氯离子浓度的增加,1O2的EPR信号强度逐渐减弱,表明PMS在光照下生成的1O2易与氯离子反应生成HClO.结合超高效液相色谱-质谱法对不同反应时间的中间产物进行分析,发现CBZ转化为氯代有机副产物.

关 键 词:氯离子  过一硫酸盐  光催化反应  中间产物  催化机理
收稿时间:2021/1/22 0:00:00
修稿时间:2021/3/8 0:00:00

Effect of chloride ion on oxidation of carbamazepine by simulated sunlight activation of peroxymonosulfate
Institution:School of Materials Science & Engineering, Zhejiang Sci-Tech University, Hangzhou 310018
Abstract:The activation of peroxomonosulfate (PMS) by simulated sunlight to oxidize model pollutant carbamazepine (CBZ) in the presence of chloride ions was studied. The results showed that the photoactivated PMS could only oxidize about 25% of CBZ in 30 minutes. With increase of chloride ion concentration, the oxidation rate of CBZ enhanced obviously. It was determined that the main reaction species in chloride ion/PMS photocatalytic system was HClO by electron paramagnetic resonance (EPR) test and active species capture experiment. 1O2 played the primary role in the system without chloride ion. When the chloride ion concentration increased, the EPR intensity of 1O2 gradually weakened, indicating that PMS easily reacted with chloride ions to generate HClO. Combined with ultra-high performance liquid chromatography-mass spectrometry analysis in different reaction time, the intermediates, chlorinated organic by-products were detected.
Keywords:chloride ion  peroxomonosulfate  photocatalytic reaction  intermediates  catalytic mechanism
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