β-内酰胺类抗生素臭氧氧化机理与降解途径  

Ozone oxidation mechanism and degradation pathway ofβ-lactam antibiotics

作　　者：敖蒙蒙 刘利 魏健[2] 宋永会[1,2] 陈婷婷 熊兆锟 赖波[4] 陈忠林[1] AO Mengmeng;LIU Li;WEI Jian;SONG Yonghui;CHEN Tingting;XIONG Zhaokun;LAI Bo;CHEN Zhonglin(College of Environmental Sciences,Liaoning University,Shenyang 110036,P.R.China;Institute of Water Ecology and Environment,Chinese Research Academy of Environmental Sciences,Beijing 100012,P.R.China;Haitian Water Group,Chengdu 610095,P.R.China;College of Architecture&Environment,Sino-German Centre for Water and Health Research,Sichuan University,Chengdu 610065,P.R.China)

机构地区：[1]辽宁大学环境学院,沈阳110036 [2]中国环境科学研究院水生态环境研究所,北京100012 [3]海天水务集团股份公司,成都610041 [4]四川大学建筑与环境学院,中德水环境与健康研究中心,成都610065

出　　处：《土木与环境工程学报（中英文）》2021年第6期187-196,共10页Journal of Civil and Environmental Engineering

基　　金：中央级公益性科研院所基本科研业务专项(2019YSKY-009、2020-JY-003)。

摘　　要：为考察β-内酰胺类抗生素在臭氧氧化过程中的降解规律与特征,采用臭氧直接氧化法处理水中4种典型β-内酰胺类抗生素。研究不同pH值条件下臭氧氧化典型β-内酰胺类抗生素的降解效果,利用淬灭实验探究降解机理,分析中间产物并推测降解路径。研究结果表明:改变pH值对阿莫西林和头孢氨苄降解效果没有显著影响,酸性条件对青霉素钠降解有抑制,碱性条件对头孢曲松钠降解有促进。淬灭实验结果表明:叔丁醇(TBA)对阿莫西林和头孢氨苄的降解有一定的促进作用,说明阿莫西林和头孢氨苄的降解由臭氧分子直接氧化主导;随着TBA浓度的升高,对青霉素钠和头孢曲松钠的抑制效果更加显著,说明青霉素钠和头孢曲松钠以羟基自由基(·OH)间接氧化为主导。阿莫西林、头孢氨苄、青霉素钠和头孢曲松钠臭氧氧化过程中分别生成了4、6、3、3种主要中间产物,降解途径包括β-内酰胺环断裂、去甲基化、水合反应、加成反应等过程。In order to investigate the degradation law and characteristics ofβ-lactam antibiotics during ozone oxidation,four typicalβ-lactam antibiotics in water were treated by direct ozone oxidation.The degradation effect of ozone on typicalβ-lactam antibiotics under different pH values was studied.Quenching experiments were adopted to explore the degradation mechanism,analyze intermediates and speculate the degradation path.Results showed that the degradation of amoxicillin and cephalexin was not significantly affected by changing pH,penicillin sodium was inhibited in acidic condition,and ceftriaxone sodium was promoted in alkaline condition.The results of quenching experiments showed that TBA can promote the degradation of amoxicillin and cephalexin,indicating that the degradation of amoxicillin and cephalexin was dominated by direct oxidation of O 3.With the increase of TBA concentration,the inhibition effect to penicillin and ceftriaxone sodium was more and more significant,which indicated that penicillin and ceftriaxone sodium were indirectly oxidized by·OH.Amoxicillin,cephalexin,penicillin sodium and ceftriaxone sodium produced 4,6,3 and 3 main intermediates during ozonation,respectively.The degradation pathways were composed ofβ-lactam ring breaking,demethylation,hydration and addition etc.

关 键 词：Β-内酰胺类抗生素 臭氧 中间产物 降解途径 

分 类 号：X703.1[环境科学与工程—环境工程]