首次了解 N-乙酰化磺酰胺从废水消毒到太阳照射受纳水体的环境归宿。

Shuiqin Shi, Zhantu Ye, Jiayan Jiang, Junmei Yan, Xin Yu, Mingbao Feng
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摘要

在全球范围内发现的新出现的有机微污染物转化产物因其未知的环境归宿和不良毒性而引发了越来越多的关注。这项研究首先探讨了普遍存在的 N-乙酰化磺酰胺(N4-AcSAs,典型的磺酰胺代谢物)从废水消毒到太阳照射受纳水体的反应动力学和机理。转化方案包括氯化/溴化、光降解和太阳能/氯处理。在 pH 值为 5.0-8.0 时,两种 N4-AcSA(N4-乙酰化磺胺嘧啶,N4-AcSDZ;N4-乙酰化磺胺甲噁唑,N4-AcSMX)的卤化反应与 pH 值有关,中性氧化剂与阴离子 N4-AcSA 之间的反应在整个过程中占主导地位。此外,在溶解有机碳含量较低的小水体中,太阳能光解显著消除了 N4-AcSAs,而由羟基自由基和碳酸自由基介导的间接光解则贡献最大。经太阳照射的废水中残留的氯促进了 N4-AcSAs 的衰变,其中生成的羟基自由基和臭氧发挥了主要作用。产物分析表明,在上述情况下,N4-AcSAs 的主要转化模式包括亲电攻击、键裂解、SO2 挤压、羟基化和重排。与 N4-AcSAs 相比,多种次级产物具有更高的持久性、流动性和对水生生物的毒性。总之,此类微污染物的自然和工程转化强调了将其降解产物纳入未来化学品管理和风险评估的必要性。
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First insight into the environmental fate of N-acetylated sulfonamides from wastewater disinfection to solar-irradiated receiving waters.

The worldwide detection of emerging transformation products of organic micropollutants has raised accumulating concerns owing to their unknown environmental fate and undesired toxicity. This work first explored the reaction kinetics and mechanisms of the prevalent N-acetylated sulfonamides (N4-AcSAs, the typical sulfonamide metabolites) from wastewater disinfection to solar-irradiated receiving waters. The transformation scenarios included chlorination/bromination, photodegradation, and solar/chlorine treatment. The halogenations of two N4-AcSAs (N4-acetylated sulfadiazine, N4-AcSDZ; N4-acetylated sulfamethoxazole, N4-AcSMX) were pH-dependent at pH 5.0-8.0, and the reactions between the neutral forms of oxidants and anionic N4-AcSAs dominated the process. Furthermore, solar-based photolysis significantly eliminated N4-AcSAs in small water bodies with low dissolved organic carbon levels, while the indirect photolysis mediated by hydroxyl radicals and carbonate radicals contributed the most. The presence of chlorine residues in solar-irradiated wastewater effluents promoted the decay of N4-AcSAs, in which the generated hydroxyl radicals and ozone played a major role. Product analysis suggested the main transformation patterns of N4-AcSAs during the above scenarios included electrophilic attack, bond cleavage, SO2 extrusion, hydroxylation, and rearrangement. Multiple secondary products maintained higher persistence, mobility, and toxicity to aquatic organisms than N4-AcSAs. Overall, the natural and engineered transformations of such micropollutants underlined the necessity of including their degradation products in future chemical management and risk assessment.

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