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研究报告

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

基金项目：国家自然科学基金项目（No.21607058）；浙江省自然科学基金项目（No.LY21B070007，LY21B070008）；浙江省教育厅科技计划项目（No.Y201840526）；嘉兴市科技计划项目（No.2021AY10069，2021AD10008，2020AY10005）

摘要：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^-、NO₃^-、HCO₃^-）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（¹O₂）.

Abstract：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^-、NO₃^-、HCO₃^-） and humic acid （HA） in water. In addition， radical quenching experiment and electron paramagnetic resonance （EPR） measurement both showed that singlet oxygen （¹O₂） was the main reactive oxygen species （ROS） in the oxidation system.

Key words：ordered mesoporous carbon peroxydisulfate （PDS） acetaminophen （ACT） non-radical oxidation singlet oxygen