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UV-Fenton 降解双氯芬酸、舒必利、磺胺甲恶唑和磺胺间甲氧嘧啶:降解机制、转化产物、毒性演变及实际水基质的影响。

UV-Fenton degradation of diclofenac, sulpiride, sulfamethoxazole and sulfisomidine: Degradation mechanisms, transformation products, toxicity evolution and effect of real water matrix.

机构信息

School of Environment, Guangdong Key Laboratory of Environmental Pollution and Health, Jinan University, Guangzhou, 510632, China.

School of Environment, Guangdong Key Laboratory of Environmental Pollution and Health, Jinan University, Guangzhou, 510632, China; Department of Civil & Environmental Engineering, National University of Singapore, 1 Engineering Drive 2, Singapore, 117576, Singapore.

出版信息

Chemosphere. 2020 Nov;258:127351. doi: 10.1016/j.chemosphere.2020.127351. Epub 2020 Jun 11.

Abstract

Four common refractory pharmaceuticals, diclofenac (DF), sulpiride (SP), sulfamethoxazole (SMX) and sulfisomidine (SIM) were detected in the Disc Tubular Reverse Osmosis (DTRO) concentrates with higher concentrations ranging from 0.85 to 11.57 μg/L from the local landfill. The effect of complex matrix of DTRO concentrates on the UV-Fenton degradation kinetics of DF, SP, SMX and SIM and their transformation products (TPs) were studied. All the four pharmaceuticals could be degraded more efficiently in the ultrapure water than that in the DTRO-concentrate matrix, which also had a significant negative effect on the kinetic constants of the degradation. Twenty-two out of forty-nine TPs were newly identified by HPLC-QTOF-MS and their peak-area evolution was presented. The main degradation pathways for four pharmaceuticals were identified. When assessing cytotoxicity by using HepG2 cells, there appeared to be an obvious toxicity-increase region for each of SP, SMX and SIM. Eleven TPs were identified as the potential toxicity-increase causing TPs by combination of the QSAR prediction, HepG2 cytotoxicity assessment and peak-area evolution of TPs. Therefore, UV-Fenton process was a promising method for the refractory pharmaceutical degradation even in the complex water matrix and choosing appropriate reaction parameters for the UV-Fenton could eliminate the cytotoxicity of the TPs.

摘要

四种常见的难处理药物,双氯芬酸(DF)、舒必利(SP)、磺胺甲恶唑(SMX)和磺胺间二甲氧嘧啶(SIM),在当地垃圾填埋场的碟管式反渗透(DTRO)浓缩物中被检测到,浓度从 0.85 到 11.57μg/L 不等。研究了 DTRO 浓缩物复杂基质对 DF、SP、SMX 和 SIM 及其转化产物(TPs)的 UV-Fenton 降解动力学的影响。所有四种药物在超纯水中的降解效率都高于 DTRO 浓缩基质中的降解效率,这也对降解动力学常数产生了显著的负面影响。通过 HPLC-QTOF-MS 新鉴定出 49 个 TPs 中的 22 个,并呈现了它们的峰面积演化。确定了四种药物的主要降解途径。当用 HepG2 细胞评估细胞毒性时,SP、SMX 和 SIM 都出现了明显的毒性增加区域。通过 QSAR 预测、HepG2 细胞毒性评估和 TPs 的峰面积演化,将 11 个 TPs 鉴定为潜在的毒性增加引起的 TPs。因此,即使在复杂的水基质中,UV-Fenton 工艺也是一种有前途的难处理药物降解方法,选择适当的 UV-Fenton 反应参数可以消除 TPs 的细胞毒性。

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