Acceleration of levofloxacin degradation by combination of multiple free radicals via MoS2 anchored in manganese ferrite doped perovskite activated PMS under visible light

Acceleration of levofloxacin degradation by combination of multiple free radicals via MoS2 anchored in manganese ferrite doped perovskite activated PMS under visible light
复制标题

可见光下通过锚定在铁酸锰掺杂钙钛矿中的 MoS2 结合多种自由基加速左氧氟沙星降解

DOI:
10.1016/j.cej.2021.133933
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发表时间:
2022-03-01
影响因子:
15.1
通讯作者:
Gao, Pan
Gao, Pan
中科院分区:
工程技术1区
文献类型:
--
作者:
He, Yuxuan;Qian, Jin;Gao, Pan

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以MoS 2为嵌入物,制备了MnFe 2 O 4掺杂的钙钛矿型复合氧化物(SrCoO 3/MnFe 2 O 4/MoS 2,简称SMM),并在可见光下对PMS进行了活化。结果表明,当二硫化钼改性纳米复合材料的质量比为0.3时,SMM-3对PMS具有良好的催化活性,20 min内对左氧氟沙星(LVF)的降解率达到95.1%,且在真实的水体中也能有效降解LVF。猝灭实验和电子顺磁共振(EPR)分析表明,在反应过程中,SO_4 ~(-)和HO ~(-)起主导作用。由于纳米复合材料的光催化性能,可见光可以激发电子与氧气反应生成O-2 &BH;(-),O-2 &BH;(-)进一步与HO &BH;反应生成O-1(2)。在反应过程中,金属离子(包括Co、Mn、Fe和Mo)的快速氧化还原循环促进了PMS的活化,促进了LVF在短时间内的降解。密度泛函理论(DFT)计算和LC-MS/MS分析进一步揭示了哌嗪环氧化、脱羧和脱乙酰基是LVF降解的主要途径。最后,利用毒性评估软件(T.E.S.T)对转化残留物进行了毒性分析,验证了转化残留物的生态风险。
The nanocomposite of MoS2 embedded manganese ferrite doped perovskite (SrCoO3/MnFe2O4/MoS2, abbreviated as SMM) was successfully synthesized for peroxymonosulfate (PMS) activation under visible-light. It was optimized that the SMM-3 (mass ratio of MoS2 modified nanocomposite was 0.3) exhibited excellent catalytic performance to activate PMS for levofloxacin (LVF) degradation, with the degradation efficiency of 95.1% in 20 min. Besides, SMM-3 was able to efficiently degrade LVF under real water matrix. The quenching experiments and electron paramagnetic resonance (EPR) analysis revealed that SO4 & BULL;(-) and HO & BULL; played a dominant role in reaction. Due to the photocatalytic property of nanocomposites, the visible light could excite electrons to react with oxygen and form O-2 & BULL;(-), which further reacted with HO & BULL; to produce O-1(2). In the reaction process, the rapid redox cycle of metal ions (including Co, Mn, Fe and Mo) boosted the activation of PMS and promoted the degradation of LVF in a short time. The Density functional theory (DFT) calculation and LC-MS/MS further revealed that oxidation of piperazine ring, decarboxylation and defluorination processes were the main LVF degradation pathways. Finally, the toxicity analysis based on Toxicity Estimation Software Tool (T.E.S.T) verified the ecological risks of transformation residues.