Efficient degradation of haloacetic acids by vacuum ultraviolet-activated peroxymonosulfate: Kinetics, mechanisms and theoretical calculations.

Journal of hazardous materials Pub Date : 2024-10-05 Epub Date: 2024-08-24 DOI:10.1016/j.jhazmat.2024.135539
Feifei Wang, Jie Liu, Liang Zhang, Hongjie Wang, Zilong Zhao, Yihua Chen, Ji Li, Xiaolei Zhang, Wenyi Dong
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Abstract

Efficient degradation of haloacetic acids (HAAs) is crucial due to their potential risks. This study firstly proposed vacuum ultraviolet - activated peroxymonosulfate (VUV/PMS) to remove HAAs (i.e., monochloroacetic acid (MCAA), monobromoacetic acid (MBAA), dichloroacetic acid (DCAA), etc). VUV/PMS achieved 99.51 % MCAA and 63.29 % TOC removal within 10 min. Electron paramagnetic resonance (EPR), quenching and probe experiments demonstrated that •OH was responsible for MCAA degradation. MCAA degradation followed pathways of dehalogenation (major) and decarboxylation (minor). VUV/PMS showed application potential under various reaction parameters. Broad spectrum of VUV/PMS on various HAAs was further explored. Chlorinated HAAs (Cl-HAAs) were primarily degraded by oxidation reactions, while brominated HAAs (Br-HAAs) by direct VUV photolysis. The density functional theory-based calculations (DFT) revealed that reaction rates of HAAs correlated with the highest occupied molecular orbital (HOMO) and energy gap (ΔE), indicating that HAAs degradation depends on their chemical structures. The Fukui function (f0 values) and bond length showed vulnerability of the halogen atom in Cl-HAAs and C-Br bond in Br-HAAs. Overall, this study provides an in-depth perspective on the oxidation performance and mechanism of HAAs using VUV/PMS. It not only demonstrates a green and efficient method but also inspires new strategies for HAAs remediation.

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真空紫外线活化过氧单硫酸盐对卤乙酸的高效降解:动力学、机理和理论计算。
由于卤乙酸(HAAs)具有潜在风险,因此有效降解卤乙酸至关重要。本研究首次提出用真空紫外线-活化过硫酸盐(VUV/PMS)去除卤乙酸(即一氯乙酸(MCAA)、一溴乙酸(MBAA)、二氯乙酸(DCAA)等)。在 10 分钟内,VUV/PMS 对 MCAA 和 TOC 的去除率分别达到 99.51% 和 63.29%。电子顺磁共振(EPR)、淬火和探针实验表明,-OH 是 MCAA 降解的原因。MCAA 的降解途径是脱卤(主要)和脱羧(次要)。在不同的反应参数下,VUV/PMS 显示出应用潜力。进一步探讨了 VUV/PMS 对各种 HAAs 的广谱性。氯化 HAAs(Cl-HAAs)主要通过氧化反应降解,而溴化 HAAs(Br-HAAs)则通过直接紫外光解降解。基于密度泛函理论的计算(DFT)显示,HAAs 的反应速率与最高占据分子轨道(HOMO)和能隙(ΔE)相关,这表明 HAAs 的降解取决于其化学结构。福井函数(f0 值)和键长显示了 Cl-HAAs 中卤素原子和 Br-HAAs 中 C-Br 键的脆弱性。总之,本研究从一个深入的角度探讨了利用 VUV/PMS 氧化 HAAs 的性能和机理。它不仅展示了一种绿色、高效的方法,还为 HAAs 的修复提供了新策略。
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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