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基于响应面优化的 Fe-亚硫酸盐配合增强过硫酸盐类 Fenton 体系降解抗生素。

Fe-sulfite complexation enhanced persulfate Fenton-like process for antibiotic degradation based on response surface optimization.

机构信息

Hebei Key Laboratory of Heavy Metal Deep-Remediation in Water and Resource Reuse, Hebei Key Laboratory of Applied Chemistry, School of Environmental and Chemical Engineering, Yanshan University, Qinhuangdao 066004, PR China.

Hebei Key Laboratory of Heavy Metal Deep-Remediation in Water and Resource Reuse, Hebei Key Laboratory of Applied Chemistry, School of Environmental and Chemical Engineering, Yanshan University, Qinhuangdao 066004, PR China.

出版信息

Sci Total Environ. 2020 Jul 20;727:138773. doi: 10.1016/j.scitotenv.2020.138773. Epub 2020 Apr 18.

Abstract

To improve the cycle between Fe and Fe in persulfate (PS) Fenton-like system, sulfite (NaSO) was used as the iron complexing agent to enhance the degradation of sulfamethoxazole (SMX) antibiotic in water. Response surface methodology (RSM) was applied to regulate the operation parameters for the Fe/NaSO/PS synergistic system. Based on the RSM, the SMX could be completely degraded when the concentration of Fe, NaSO, and PS were 0.4, 0.5, and 2.5 mM, respectively. The result showed that the synergistic process represented a high Fe utilization rate and SMX degradation efficiency. After 1 h reaction, 100.00% of SMX and 27.80% of total organic carbon were removed under the ambient conditions containing the initial SMX concentration of 10 μM and initial pH of 5.96. Free radical masking and electron spin-resonance tests proved that hydroxyl radical (HO) and oxysulfur radicals (SO, x = 3, 4, 5) were all played the significant role in the antibiotic removal, and the primary active radical was HO. The SMX decomposition pathways based on the formed intermediates was proposed through the high-performance liquid chromatography and mass spectrum analyses. The toxicity assessment prediction indicated that the toxicities of decomposed SMX byproducts were reduced after the coupling treatment.

摘要

为了提高过硫酸盐芬顿类体系中 Fe 和 Fe 的循环利用率,采用亚硫酸盐(NaSO)作为铁络合剂来增强水中磺胺甲恶唑(SMX)抗生素的降解。响应面法(RSM)被应用于调控 Fe/NaSO/PS 协同体系的操作参数。基于 RSM,当 Fe、NaSO 和 PS 的浓度分别为 0.4、0.5 和 2.5 mM 时,SMX 可以完全降解。结果表明,协同过程具有高的铁利用率和 SMX 降解效率。在 1 h 的反应时间内,在初始 SMX 浓度为 10 μM 和初始 pH 值为 5.96 的环境条件下,100.00%的 SMX 和 27.80%的总有机碳被去除。自由基掩蔽和电子顺磁共振测试证明,羟基自由基(HO)和氧硫自由基(SO,x=3、4、5)都在抗生素去除中发挥了重要作用,主要的活性自由基是 HO。通过高效液相色谱和质谱分析提出了基于形成的中间产物的 SMX 分解途径。毒性评估预测表明,经过偶联处理后,分解的 SMX 副产物的毒性降低。

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