Fe(Ⅱ)活化亚硫酸盐降解卡马西平的动力学及机制研究
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X522;X592

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国家自然科学基金(21976133、22025601);中国博士后科学基金(2019M661618)


Kinetics and mechanism of carbamazepine degradation through activating sulfite by Fe(Ⅱ)
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    摘要:

    高级氧化技术是去除水中新型有机污染物的重要方法之一。研究Fe (Ⅱ)活化亚硫酸盐(Fe (Ⅱ)/亚硫酸盐)体系降解卡马西平(CBZ)的动力学及体系中活性氧化物种对CBZ降解的贡献。结果表明:当亚硫酸盐浓度由0.20 mmol/L增加至0.50 mmol/L时,反应20 min时Fe (Ⅱ)亚硫酸盐体系对CBZ的去除率不断增加,而进一步增加亚硫酸盐浓度时,卡马西平的去除率不再进一步增加。当反应初始pH值为3.0~7.0时,Fe (Ⅱ)/亚硫酸盐体系均可降解CBZ,在初始pH值为5.0时,此体系对CBZ的去除率最高,反应平衡时CBZ的去除率达87.3%。此外,铁盐中SO42-和Cl-对Fe (Ⅱ)/亚硫酸盐体系降解CBZ基本无影响。综合电子顺磁共振检测及淬灭剂实验的结果可知,Fe (Ⅱ)/亚硫酸盐体系中所产生的活性氧化物种包括硫酸根自由基(SO4-·)、羟基自由基(HO·)和过一硫酸根自由基(SO5-·),它们均对卡马西平的降解起贡献作用,其中SO4-·和HO·起主要贡献作用。

    Abstract:

    Advanced oxidation processes (AOPs) are one of the important methods to remove emerging organic contaminants in water. In this study, we investigated the degradation kinetics of carbamazepine (CBZ) during the activation of sulfite by Fe(Ⅱ) (Fe(Ⅱ)/sulfite system) and the contribution of reactive oxidative species to the degradation of CBZ in this process. The research results showed that the removal of CBZ at 20 min in the Fe(Ⅱ)/sulfite system increased with the concentration of sulfite increasing from 0.20 mmol/L to 0.50 mmol/L, while the removal of carbamazepine did not further increase with further increasing the sulfite concentration. CBZ could be degraded in the Fe(Ⅱ)/sulfite system over the initial pH (pHini) range of 3.0~7.0. The removal of CBZ at pHini 5.0 was the highest and was 87.3% at equilibrium. In addition, SO42- and Cl- in the Fe(Ⅱ) salt had no influence on the degradation of CBZ in the Fe(Ⅱ)/sulfite system. The results of electron paramagnetic resonance and quenching experiments showed that the reactive oxidative species in the Fe(Ⅱ)/sulfite system included sulfate radical (SO4-·), hydroxyl radical (HO·) and peroxymonosulfate radical (SO5-·), contributing to the degradation of CBZ,and the degradation of CBZ was mainly contributed by SO4-· and HO·.

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李阳,关小红,董红钰. Fe(Ⅱ)活化亚硫酸盐降解卡马西平的动力学及机制研究[J].土木与环境工程学报(中英文),2021,43(6):165-171. LI Yang, GUAN Xiaohong, DONG Hongyu. Kinetics and mechanism of carbamazepine degradation through activating sulfite by Fe(Ⅱ)[J]. JOURNAL OF CIVIL AND ENVIRONMENTAL ENGINEERING,2021,43(6):165-171.10.11835/j. issn.2096-6717.2021.070

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  • 收稿日期:2021-03-08
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  • 在线发布日期: 2021-08-19
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