Removal of Sulfonamide Antibiotics in Peracetic Acid-Mediated Natural Polyphenol Systems via an Overlooked Polymerization Pathway: Role of ortho-Quinones

IF 11.3 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL 环境科学与技术 Pub Date : 2025-04-14 DOI:10.1021/acs.est.4c13612
Sheng Li, Jing Zou, Jianying Wu, Linfeng He, Chenyu Tang, Fei Li, Bo Sun, Min Zhao, Qingsong Li, Panpan Wang, Lengshen Huang, Qingfeng Cheng, Haoqiang Tan, Jun Ma
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Abstract

Natural polyphenols can be oxidized into reactive quinones, which might play a key role in the removal of specific contaminants in natural polyphenol-related advanced oxidation processes (AOPs). In this study, peracetic acid (PAA) was employed in combination with natural protocatechuic acid (PCA) to remove sulfonamide antibiotics (SAs) from water. More than 95% removal of sulfamethoxazole (SMX) and other SAs was observed in the PCA/PAA system, and neutral pH conditions (5.0–8.0) were more conducive to the removal of SMX. The PCA/PAA system exhibited a great anti-interference ability against complex water matrices. ortho-Quinone, generated from the oxidation of PCA by PAA, played a dominant role in the SMX removal. Electrons tended to transfer from SMX to the generated ortho-quinones and form covalent bonds, resulting in the production of less toxic oligomers via the overlooked polymerization pathway. A reduction in the toxicity of the SMX solution was found following treatment with the PCA/PAA system. More interestingly, several polyphenols structurally related to PCA could also facilitate SMX removal using PAA as the oxidant. Overall, this study proposes a novel strategy for developing reactive quinones dominated AOPs with robust anti-interference performance, as well as enhances the understanding of contaminant removal via an overlooked polymerization pathway in natural polyphenol-related AOPs.

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通过被忽视的聚合途径去除过乙酸介导的天然多酚体系中的磺酰胺类抗生素:原醌的作用
天然多酚可以被氧化成活性醌类化合物,在与天然多酚相关的高级氧化过程(AOPs)中,活性醌类化合物可能在去除特定污染物方面发挥关键作用。本研究采用过乙酸(PAA)与天然原儿茶酸(PCA)相结合的方法去除水中的磺胺类抗生素(SAs)。在 PCA/PAA 系统中,磺胺甲噁唑(SMX)和其他 SAs 的去除率超过 95%,中性 pH 条件(5.0-8.0)更有利于 SMX 的去除。PCA/PAA 系统对复杂的水基质具有很强的抗干扰能力。PAA 氧化 PCA 生成的邻醌在去除 SMX 的过程中发挥了主导作用。电子倾向于从 SMX 转移到生成的邻醌并形成共价键,从而通过忽略聚合途径产生毒性较低的低聚物。经 PCA/PAA 系统处理后,SMX 溶液的毒性有所降低。更有趣的是,使用 PAA 作为氧化剂,与 PCA 结构相关的几种多酚也能促进 SMX 的去除。总之,本研究提出了一种新的策略,用于开发具有强大抗干扰性能的以活性醌为主的 AOP,并加深了人们对天然多酚相关 AOP 中被忽视的聚合途径去除污染物的理解。
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来源期刊
环境科学与技术
环境科学与技术 环境科学-工程:环境
CiteScore
17.50
自引率
9.60%
发文量
12359
审稿时长
2.8 months
期刊介绍: Environmental Science & Technology (ES&T) is a co-sponsored academic and technical magazine by the Hubei Provincial Environmental Protection Bureau and the Hubei Provincial Academy of Environmental Sciences. Environmental Science & Technology (ES&T) holds the status of Chinese core journals, scientific papers source journals of China, Chinese Science Citation Database source journals, and Chinese Academic Journal Comprehensive Evaluation Database source journals. This publication focuses on the academic field of environmental protection, featuring articles related to environmental protection and technical advancements.
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