| 纳米核壳Co@NC催化剂活化过氧乙酸降解磺胺甲（口恶）唑 |
| 摘要点击 2389 全文点击 2207 投稿时间：2022-05-18 修订日期：2022-07-26 |
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| 中文关键词 纳米核壳Co@NC催化剂 过氧乙酸 磺胺甲（口恶）唑(SMX) 高级氧化技术 有机自由基 |
| 英文关键词 nanocore-shell Co@NC catalyzer peracetic acid sulfamethoxazole(SMX) advanced oxidation process organic radical |
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| 中文摘要 |
| 过氧乙酸［PAA，CH3 C （O） OOH］作为一种新兴的氧化剂，在处理污水中难降解有机污染物中受到了越来越多的关注.通过蚀刻方法制备出纳米核壳Co@NC催化剂，并将其用于活化PAA降解污水中磺胺甲（口恶）唑（SMX）.结果表明，当控制催化剂投加量为0.02 g ·L-1、PAA浓度为0.12 mmol ·L-1和SMX浓度为10 μmol ·L-1时，反应5 min时SMX的去除率即可达到98%，且降解SMX的速率常数为0.80 min-1.SMX降解效率随催化剂添加量和PAA浓度提高而显著增加.结果发现核壳Co@NC/PAA体系在近中性条件下（pH为6.0~8.0）可获得最佳的SMX降解效果，酸性或碱性条件均不利于SMX去除.HCO3-和腐殖酸对该催化体系存在显著抑制，而Cl-抑制作用较弱.此外，通过自由基淬灭实验和电子顺磁共振（EPR）研究发现，乙酰氧自由基（CH3 CO2 ·）和乙酰过氧自由基（CH3 CO3 ·）为该体系中降解SMX的主要活性氧物种.进一步采用U-HPLC-Q-Exactive Orbitrap HRMS测定了该体系中SMX的降解产物，并提出了SMX可能的降解路径.同时，催化剂循环利用实验表明，纳米核壳Co@NC催化剂具有较好的催化稳定性和重复利用性. |
| 英文摘要 |
| Peracetic acid (PAA), as a new oxidant, has attracted increasing attention in the treatment of refractory organic pollution in sewage. In this study, the nano core-shell Co@NC catalyst was prepared via etching and used to activate PAA to degrade sulfamethoxazole (SMX) in sewage. The results indicated that the degradation rate of SMX reached 98%, and its reaction rate constant was 0.80 min-1 under optimal conditions (catalyst dosage=0.02 g·L-1, PAA concentration=0.12 mmol·L-1, pH=7, SMX concentration=10 μmol·L-1). With the increase in PAA concentration and core-shell Co@NC dosage, the degradation efficiency of SMX increased. The study found that the core-shell Co@NC/PAA system had the best degradation effect on SMX under near-neutral conditions (pH 6.0-8.0), and both acidic and alkaline environments were not conducive to SMX degradation. HCO3- and humic acid showed significant inhibition on the degradation of SMX, whereas Cl- showed weak inhibition. In addition, through a free radical quenching experiment and electron paramagnetic resonance (EPR) detection, acetoxy radical (CH3CO2CO3·) were the main active species for the degradation of organic pollutants in the system. Transformation products (TPs) of SMX were analyzed by U-HPLC-Q-Exactive Orbitrap HRMS, and a possible degradation path of SMX was proposed. At the same time, the catalyst recycling experiment showed that the nano core-shell Co@NC catalyst had good stability and reusability. |
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