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间接光降解磺胺嘧啶和磺胺吡啶:CDOM 成分和主要海水因素的影响。

Indirect photodegradation of sulfadimidine and sulfapyridine: Influence of CDOM components and main seawater factors.

机构信息

Key Laboratory of Marine Chemistry Theory and Technology, Ministry of Education, Ocean University of China, 238 Songling Road, Qingdao, 266100, PR China.

Key Laboratory of Marine Chemistry Theory and Technology, Ministry of Education, Ocean University of China, 238 Songling Road, Qingdao, 266100, PR China; National Marine Hazard Mitigation Service, Beijing, 100194, China.

出版信息

Chemosphere. 2023 Aug;333:138821. doi: 10.1016/j.chemosphere.2023.138821. Epub 2023 May 4.

Abstract

This study investigated the indirect photodegradation of sulfadimidine (SM) and sulfapyridine (SP) in the presence of chromophoric dissolved organic matter (CDOM), and studied the influences of main marine factors (salinity, pH, NO and HCO). Reactive intermediate (RI) trapping experiments demonstrated that triplet CDOM (CDOM*) played a major role in the photodegradation of SM with a 58% photolysis contribution, and the contributions to the photolysis of SP were 32%, 34% and 34% for CDOM*, hydroxyl radical (HO·) and singlet oxygen (O), respectively. Among the four CDOMs, JKHA, with the highest fluorescence efficiency, exhibited the fastest rate of SM and SP photolysis. The CDOMs were composed of one autochthonous humus (C1) and two allochthonous humus (C2 and C3). C3, with the strongest fluorescence intensity, had the strongest capacity to generate RIs and accounted for approximately 22%, 11%, 9% and 38% of the total fluorescence intensity of SRHA, SRFA, SRNOM and JKHA, respectively, indicating the predominance of CDOM fluorescent components in the indirect photodegradation of SM and SP. These results demonstrated the photolysis mechanism: The photosensitization of CDOM occurred after its fluorescence intensity decreased, and a large number of RIs (CDOM*, HO· and O, etc.) were generated by energy and electron transfer, then these RIs reacted with SM and SP to cause photolysis. The increase in salinity stimulated the photolysis of SM and SP consecutively. The photodegradation rate of SM first increased and then decreased with increasing pH, whereas the photolysis of SP was remarkably promoted by high pH but remained stable at low pH. NO and HCO had little effect on the indirect photodegradation of SM and SP. This research may contribute to a better understanding of the fate of SM and SP in the ocean and provide new insights into the transformation of other sulfonamides (SAs) in marine ecological environments.

摘要

本研究考察了有色溶解有机质(CDOM)存在下磺胺嘧啶(SM)和磺胺吡啶(SP)的间接光降解,并研究了主要海洋因素(盐度、pH 值、NO 和 HCO)的影响。反应中间体(RI)捕获实验表明,三重态 CDOM(CDOM*)在 SM 的光降解中起主要作用,其光解贡献为 58%,而对 SP 的光解贡献分别为 CDOM*、羟基自由基(HO·)和单线态氧(O)的 32%、34%和 34%。在四种 CDOM 中,荧光效率最高的 JKHA 表现出最快的 SM 和 SP 光解速率。CDOM 由一个自生源腐殖质(C1)和两个异生源腐殖质(C2 和 C3)组成。C3 具有最强的荧光强度,具有最强的生成 RI 的能力,分别占 SRHA、SRFA、SRNOM 和 JKHA 总荧光强度的 22%、11%、9%和 38%,表明 CDOM 荧光成分在 SM 和 SP 的间接光降解中占主导地位。这些结果表明了光解机制:CDOM 的光致敏化发生在其荧光强度降低之后,通过能量和电子转移产生大量 RI(CDOM*、HO·和 O 等),然后这些 RI 与 SM 和 SP 反应导致光解。盐度的增加连续刺激 SM 和 SP 的光解。SM 的光降解速率随着 pH 值的增加先增加后降低,而 SP 的光降解则显著受到高 pH 值的促进,但在低 pH 值下保持稳定。NO 和 HCO 对 SM 和 SP 的间接光降解影响不大。本研究有助于更好地理解 SM 和 SP 在海洋中的归宿,并为海洋生态环境中其他磺胺类药物(SAs)的转化提供新的见解。

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