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Elementary reaction-based kinetic model for the fate of N-nitrosodimethylamine under UV oxidation
Environmental Science: Water Research & Technology ( IF 3.5 ) Pub Date : 2021-08-20 , DOI: 10.1039/d1ew00262g
Benjamin Barrios 1 , Divya Kamath 1 , Erica Coscarelli 1 , Daisuke Minakata 1
Affiliation  

UV photolysis is an effective process to remove nitrosamines from contaminated water resources. Nitrosamines represent a class of compounds with high potential for carcinogenicity and, therefore, there are serious concerns regarding their threat to human health and their environmental toxicity. Although the photochemical parameters of parent nitrosamines and their initial reaction pathways are well understood, the fate of nitrogen-containing species and reactive nitrogen species generated from nitrosamine degradation has not yet been elucidated. In this study, we develop an elementary reaction-based kinetic model for the photolysis of N-nitrosodimethylamine (NDMA) and the photochemical transformation products. We use density functional theory quantum mechanical calculations to calculate the aqueous-phase free energies of activation and reaction to investigate the kinetics and thermodynamics properties of the elementary reactions. We generate ordinary differential equations for all species involved in the identified reactions and solve them to obtain the time-dependent concentration profiles of NDMA and the degradation products at pH 3 and pH 7. The profiles are compared to experimental results in the literature to validate our elementary reaction-based kinetic model. This is the first study to develop an elementary reaction-based kinetic model for the photochemical reaction of NDMA and reactive nitrogen species. The findings of this study have a significant impact on the active research area of nitrosative stress and advanced oxidation processes that utilize nitrogen-containing compounds such as UV/nitrate and UV/chloramine advanced oxidation processes.

中文翻译:

基于基本反应的 N-亚硝基二甲胺在紫外氧化下的归宿动力学模型

紫外线光解是从受污染的水资源中去除亚硝胺的有效方法。亚硝胺代表一类具有很高致癌性潜力的化合物,因此,它们对人类健康的威胁和环境毒性引起了严重的关注。尽管母体亚硝胺的光化学参数及其初始反应途径已被很好地理解,但亚硝胺降解产生的含氮物质和活性氮物质的归宿尚未阐明。在这项研究中,我们开发了一个基于基本反应的N光解动力学模型-亚硝基二甲胺 (NDMA) 和光化学转化产物。我们使用密度泛函理论量子力学计算来计算活化和反应的水相自由能,以研究基本反应的动力学和热力学性质。我们为所识别的反应中涉及的所有物种生成常微分方程并求解它们以获得 NDMA 的时间依赖性浓度曲线以及 pH 3 和 pH 7 下的降解产物。将这些曲线与文献中的实验结果进行比较以验证我们的基于基本反应的动力学模型。这是第一项为 NDMA 和活性氮物种的光化学反应开发基于基本反应的动力学模型的研究。
更新日期:2021-08-26
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