铈酸镧钙钛矿活化亚硫酸盐降解氧氟沙星

Xiangyu Meng, Zhenran Wang, Kerui Li, Yiqing Liu, Dandan Zhao, Yongsheng Fu
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摘要

近年来,氧氟沙星(OFX)的广泛使用导致了水生环境中氧氟沙星化合物浓度的升高。同时,OFX固有的顽固性给OFX的降级带来了巨大的挑战。本研究采用柠檬酸溶胶-凝胶法制备镧铈钙钛矿(LaCeO3),活化亚硫酸氢盐(BS),有效降解OFX。结果表明,LaCeO3/BS体系在180 min内去除了87.5%的OFX,准一级动力学常数为3 × 10−3 min−1。自由基猝灭实验和电子顺磁共振(EPR)谱分析证实,在LaCeO3/BS体系中,硫酸盐自由基(SO4•_)和羟基自由基(HO•)是去除OFX的主要活性物质。反应机理表明,Ce在LaCeO3/BS体系中是BS活化的主要活性位点,并存在一个涉及≡Ce(III)/≡Ce(IV)的再生循环。此外,通过液相色谱-质谱联用(LC-MS)鉴定了可能的中间产物,揭示了OFX的潜在降解途径。循环试验和能谱仪(EDS)数据表明,LaCeO3具有良好的可重复使用性和稳定性。
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Degradation of ofloxacin by lanthanum cerate perovskite activated bisulfite
In recent years, the extensive utilization of ofloxacin (OFX) has led to elevated concentration of OFX compound in the aquatic environment. At the same time, the inherent recalcitrance of OFX has presented a formidable challenge for OFX degradation. In this study, lanthanum cerium perovskite (LaCeO3) was prepared by citric acid sol–gel method to activate bisulfite (BS) for the effective degradation of OFX. The results revealed that the LaCeO3/BS system removed 87.5% of OFX within 180 min with a pseudo-first-order kinetic constant of 3 × 10−3 min −1. Radical quenching experiments and electron paramagnetic resonance (EPR) spectroscopy confirmed that sulfate radicals (SO4•_) and hydroxyl radicals (HO•) were the primary reactive species responsible for OFX removal in LaCeO3/BS system. The reaction mechanism indicated that Ce in LaCeO3/BS system served as the primary active site for BS activation, and a regenerating cycle involving ≡Ce(III)/≡Ce(IV) was present. Additionally, possible intermediate products were identified by a liquid chromatograph-mass spectrometer (LC-MS), revealing potential degradation pathways of OFX. Cycle tests and energy dispersive spectrometer (EDS) data demonstrated the favorable reusability and stability of LaCeO3.
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