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作 者:王晨阳 黄文意 连彬惟 周学文 庞义军 田亚洋 WANG Chenyang;HUANG Wenyi;LIAN Binwei;ZHOU Xuewen;PANG Yijun;TIAN Yayang(School of Pharmacy,Hubei University of Science and Techunology,Xianning 437100,Hubei,China)
出 处:《化学研究》2025年第1期32-39,共8页Chemical Research
基 金:湖北省自然科学基金(2022CFB665);湖北省教育厅中青年人才项目(Q20222801);湖北科技学院博士启动项目(BK202305)。
摘 要:为了降解水中抗生素类有机污染物,采用一步水热法制备铜铁矿型催化剂CuMnO_(2),作为过一硫酸盐(PMS)的活化剂,产生活性氧物种降解抗生素。在90 min内实现96%氧氟沙星(OFX)的降解,然而该体系对磺胺甲噁唑(SMX)的降解效率仅为51%。进一步通过淬灭实验、电子自旋共振光谱和材料结构表征,揭示CuMnO_(2)活化PMS降解OFX和SMX两种抗生素的活性氧物种均以单线态氧(^(1)O_(2))为主,发现Cu(Ⅰ)和Mn(Ⅱ)是活化PMS的主要活性位点,并且催化降解体系中^(1)O_(2)的氧化选择性及抗生素的氧化电位差异是两种抗生素降解效率产生差异的主要原因。最后,基于液相色谱质谱联用仪(LC-MS)分析CuMnO_(2)/PMS降解OFX和SMX的可能降解路径。To degrade organic pollutants such as antibiotics in water,CuMnO_(2) catalyst was prepared by one-step hydrothermal method and then used as the activator of peroxymonosulfate(PMS)to produce active oxygen species to degrade antibiotics.The above system achieved 96%degradation efficiency of ofloxacin(OFX)within 90 min,while only 51%removal efficiency was obtained for sulfamethoxazole(SMX).Furthermore,based on quenching experiment,electron spin resonance spectroscopy and material structure characterization,it was found that the active oxygen species of CuMnO_(2) activated PMS to degrade OFX and SMX antibiotics was mainly singlet oxygen(^(1)O_(2)).In addition,Cu(I)and Mn(Ⅱ)were proven to be the main active sites for PMS activation,and selective oxidation of ^(1)O_(2) as well as the difference of oxidation potentials of antibiotics in the catalytic degradation system was involved in activating PMS,which was the main reason for the difference in degradation efficiency between the two antibiotics.Last,the possible degradation pathways of OFX and SMX in CuMnO_(2)/PMS system were analyzed based on liquid chromatography-mass spectrometry(LC-MS).
关 键 词:高级氧化技术 铜铁矿型氧化物 过硫酸盐 氧氟沙星 磺胺甲噁唑
分 类 号:X703.5[环境科学与工程—环境工程]
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