改性有序介孔碳活化过硫酸盐非自由基降解扑热息痛

Non-radical degradation of paracetamol by persulfate activation with modified ordered mesoporous carbon

通过热处理对有序介孔碳(CMK-3)材料进行改性,并将改性后的材料用于活化过二硫酸盐(PDS)降解药物扑热息痛(ACT).结果表明600℃热处理的CMK-3(CMK-3-600)具有最优的催化性能.该CMK-3-600/PDS氧化体系30 min内可去除100%ACT,其反应速率常数(k)远高于CMK-3/PDS,这可能是由于改性后的CMK-3-600比表面积显著增大,表面缺陷、C-OH官能团以及芳香环中的π-π*shake up增多.CMK-3-600不仅显示出良好的稳定性,其催化氧化过程还不受水中的无机阴离子(Cl^(-)、NO_(3)^(-)、HCO_(3)^(-))及腐殖酸(HA)等影响.此外,自由基淬灭实验和电子顺磁共振(EPR)测试结果表明,该氧化体系降解ACT的主要活性氧物种(ROS)是单线态氧(^(1)O_(2)).

In this study,ordered mesoporous carbon(CMK-3)was modified by heat treatment,and the obtained material was used for activating peroxydisulfate(PDS)to degrade pharmaceutical acetaminophen(ACT).The results showed that the CMK-3 treated at 600 ℃(CMK-3-600)had the best catalytic performance.The CMK-3-600/PDS oxidation system can remove 100% of ACT within 30 min,and the reaction rate constant(k)was much higher than that of CMK-3/PDS.The probable contributing factors are with the features of the modified material,such as the significantly increases in the specific surface area,the growth of the quantity of surface defects and C-OH functional groups,and the raises of the number of π-π*shake up in the aromatic ring,etc.CMK-3-600 showed not only good stability,but also excellent degradation performance.Its oxidation system was not affected by inorganic anions(Cl^(-)、NO_(3)^(-)、HCO_(3)^(-))and humic acid(HA)in water.In addition,radical quenching experiment and electron paramagnetic resonance(EPR)measurement both showed that singlet oxygen(^(1)O_(2))was the main reactive oxygen species(ROS)in the oxidation system.