Co-MIL-101(Fe)活化过硫酸盐降解对乙酰氨基酚

Degradation of acetaminophen using Co-MIL-101(Fe)activated PMS

采用一锅法制备了均质双金属有机骨架材料Co-MIL-101(Fe),并将其用于活化过一硫酸氢钾(PMS)降解溶液中的对乙酰氨基酚(PCT),考察了影响PCT去除率的主要因素,探讨了Co-MIL-101(Fe)活化PMS降解PCT的反应机理,评价了Co-MIL-101(Fe)的活化性能。表征结果显示,掺杂Co后,Co-MIL-101(Fe)由规则的八面体晶体(MIL-101(Fe))变为含有少量纺锤体结构的晶体。实验结果表明:在Co掺杂量3%(原子分数)、初始PCT质量浓度5 mg/L、PMS质量浓度0.10 g/L、Co-MIL-101(Fe)加入量0.10 g/L、初始pH 3~9的最佳工艺条件下,反应30 min后,PCT去除率大于96.5%;Co-MIL-101(Fe)在第5次使用时,反应30 min后,PCT去除率可达91.1%,表现出良好的重复使用性能。浸出金属离子测定结果表明,Co-MIL-101(Fe)具有较好的稳定性。自由基猝灭实验表明,Co-MIL-101(Fe)活化PMS降解PCT的反应体系中,主要活性物种为SO4-·和·OH。Co-MIL-101(Fe)活化PMS降解PCT的动力学过程符合准一级动力学模型。

A homogeneous bimetallic organic framework material Co-MIL-101(Fe)was prepared by one-pot method and used to activate potassium monopersulfate(PMS)for degradation of paracetamol(PCT)in solution.The characterization results show that after doping Co,Co-MIL-101(Fe)changes from a regular octahedral crystal(MIL-101(Fe))to a crystal containing a small amounts spindle structure.The experimental results show that the removal rate of PCT is more than 96.5%under the optimum conditions of Co doping amount 3%,initial PCT mass concentration 5 mg/L,PMS mass concentration 0.10 g/L,Co-MIL-101(Fe)amount 0.10 g/L,initial pH 3-9 and reaction time 30 min,and still reach 91.1%at the 5th use after 30 min of reaction,showing excellent reusability.The results of ICP-MS show that Co-MIL-101(Fe)has good stability.The results of free radical quenching experiments show that the main active species in the reaction system of catalytic degradation of PCT with Co-MIL-101(Fe)activated PMS are SO4-·and·OH.The kinetic process of oxidative degradation of PCT with Co-MIL-101(Fe)activated PMS conforms to the pseudo-first-order kinetic model.