磁性氧化石墨烯活化过一硫酸盐去除水中阿托伐他汀
Efficient removal of atorvastatin in aqueous solution via peroxymonosulfate activated by magnetic graphene oxide
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摘要: 以磁性氧化石墨烯(Fe3O4/GO)为催化剂,研究其活化过一硫酸盐(PMS)对水中阿托伐他汀(ATV)的降解,考察了不同氧化剂、初始pH值、Fe3O4/GO浓度、PMS浓度、反应温度、无机阴离子和溶解有机质(DOM)对Fe3O4/GO+PMS体系催化降解ATV的影响.结果表明,ATV的去除率与溶液初始pH相关,在中性条件时去除率最大;ATV的去除率随着PMS浓度和反应温度的升高而增大,而Fe3O4/GO浓度对ATV去除率的作用不明显;无机阴离子对ATV的去除率起到促进作用,而DOM则表现出不同程度的抑制作用;自由基淬灭实验结果表明,硫酸根自由基(SO4·-)和羟基自由基(·OH)为Fe3O4/GO+PMS体系中主要的氧化活性物质;另外,基于飞行时间液相色谱质谱联用仪(TOF-LC-MS)检测到的9种主要降解中间产物,推测了4种相关反应路径.Abstract: In the present study, the removal of atorvastatin (ATV) in water via peroxymonosulfate (PMS) activated by magnetic graphene oxide (Fe3O4/GO) was systematically investigated. The effects of different oxidant, initial pH, Fe3O4/GO dosage, PMS concentration, reaction temperature, coexisting anions and dissolved organic matters (DOM) on the degradation of ATV in water were examined. Results showed that the ATV degradation efficiency depended on solution initial pH with neutral pH showing the optimum degradation conditions, and the removal of ATV increased with the augment of PMS concentration and temperature, while the effect of Fe3O4/GO dosage was insignificant; inorganic anions promoted the degradation of ATV, while DOM inhibited the removal of ATV. The free radical quenching experiments demonstrated that both sulfate radical (SO4·-) and hydroxyl radical (·OH) were the main reactive oxygen species (ROS) in Fe3O4/GO+PMS system. In addition, nine major intermediates were identified by time of flight liquid chromatography-tandem mass spectrometry (TOF-LC-MS), and four associated reaction pathways were proposed accordingly.
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