识别涉及污染物间接光降解的光化学产生的反应中间体的传统方法的局限性。

IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Environmental Science: Processes & Impacts Pub Date : 2023-09-14 DOI:10.1039/D3EM00304C
Reid P. Milstead, Stephanie M. Berg, Bella M. Kelly, Christian D. Knellwolf, Cooper J. Larson, Kristine H. Wammer and Christina K. Remucal
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引用次数: 0

摘要

溶解有机物(DOM)介导的间接光降解在水生污染物的降解中起着重要作用。预测该过程的速率需要了解与感兴趣的化合物反应的光化学产生的反应中间体(PPRI),以及单个DOM样品产生PPRI的能力。关键的PPRI通常使用淬火研究来确定,但这种方法通常会导致难以解释的结果。在这项工作中,我们使用来自天然和工程水生系统的48种不同的水来分析阿托伐他汀、卡马西平、磺胺嘧啶和苯并三唑的间接光降解。我们使用这个大数据集来评估PPRI形成和间接光降解速率常数之间的关系,并将其与使用标准猝灭实验的结果进行直接比较。这些数据表明,三重态DOM(3DOM)和单线态氧(1O2)是阿托伐他汀、卡马西平和磺胺嘧啶的关键PPRI,而羟基自由基(*OH)有助于苯并三唑的间接光降解。我们警告不要依赖猝灭研究,因为3DOM的猝灭限制了1O2的形成,并且所有研究的猝灭剂都与*OH反应。此外,我们发现DOM组成直接影响间接光降解,并且低分子量的类微生物DOM与卡马西平、磺胺嘧啶和苯并三唑的间接光降解率呈正相关。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

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Limitations of conventional approaches to identify photochemically produced reactive intermediates involved in contaminant indirect photodegradation†

Dissolved organic matter (DOM) mediated indirect photodegradation can play an important role in the degradation of aquatic contaminants. Predicting the rate of this process requires knowledge of the photochemically produced reactive intermediates (PPRI) that react with the compound of interest, as well as the ability of individual DOM samples to produce PPRI. Key PPRI are typically identified using quencher studies, yet this approach often leads to results that are difficult to interpret. In this work, we analyze the indirect photodegradation of atorvastatin, carbamazepine, sulfadiazine, and benzotriazole using a diverse set of 48 waters from natural and engineered aquatic systems. We use this large data set to evaluate relationships between PPRI formation and indirect photodegradation rate constants, which are directly compared to results using standard quenching experiments. These data demonstrate that triplet state DOM (3DOM) and singlet oxygen (1O2) are critical PPRI for atorvastatin, carbamazepine, and sulfadiazine, while hydroxyl radical (˙OH) contributes to the indirect photodegradation of benzotriazole. We caution against relying on quenching studies because quenching of 3DOM limits the formation of 1O2 and all studied quenchers react with ˙OH. Furthermore, we show that DOM composition directly influences indirect photodegradation and that low molecular weight, microbial-like DOM is positively correlated with the indirect photodegradation rates of carbamazepine, sulfadiazine, and benzotriazole.

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来源期刊
Environmental Science: Processes & Impacts
Environmental Science: Processes & Impacts CHEMISTRY, ANALYTICAL-ENVIRONMENTAL SCIENCES
CiteScore
9.50
自引率
3.60%
发文量
202
审稿时长
1 months
期刊介绍: Environmental Science: Processes & Impacts publishes high quality papers in all areas of the environmental chemical sciences, including chemistry of the air, water, soil and sediment. We welcome studies on the environmental fate and effects of anthropogenic and naturally occurring contaminants, both chemical and microbiological, as well as related natural element cycling processes.
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