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在水溶液中六嗪酮的光降解和吸附:去除效率、动力学和机制。

Photodegradation and adsorption of hexazinone in aqueous solutions: removal efficiencies, kinetics, and mechanisms.

机构信息

Department of Civil and Environmental Engineering, The University of Auckland, Auckland, New Zealand.

出版信息

Environ Sci Pollut Res Int. 2022 Jul;29(32):48330-48339. doi: 10.1007/s11356-022-19205-y. Epub 2022 Feb 21.

DOI:10.1007/s11356-022-19205-y
PMID:35190983
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9252970/
Abstract

Hexazinone, a globally applied broad-spectrum triazine herbicide, has not been mechanistically investigated previously under advanced oxidation processes (AOPs) and adsorption on activated carbon. In this study, its fate during UV-based oxidation with/without hydrogen peroxide (HO) and adsorption on coconut shell-based granular activated carbon (CSGAC) in water matrices was investigated. A comparison between various irradiation sources (visible, UVA, UVB, and UVC) revealed the highest degradation rate under UVC. More than 98% degradation of hexazinone was observed under 3 J cm UVC fluence in the presence of 0.5 mM HO at pH 7. Moreover, the degradation rate enhanced significantly with an increase in the initial dosage of HO, UV fluence, and contact time in the UV/HO process. The rate of degradation was lower using secondary effluent than that of Milli-Q water due to the presence of dissolved organics in wastewater. However, the reactions in both matrices obeyed pseudo-first-order kinetics. The effect of different scavengers, including methanol, potassium iodide (KI), and tert-butyl alcohol (TBA), showed that hydroxyl radicals (OH) played a dominant role in hexazinone degradation in the UV/HO process. Hexazinone was effectively adsorbed by CSGAC through π-π electron donor-acceptor interactions between hexazinone's triazine ring and CSGAC's surface functional groups. The isotherm and kinetic studies showed that the adsorption followed the Freundlich model and pseudo-second-order reaction, respectively, suggesting chemisorption. This study provided mechanistic insights on the removal of hexazinone at the tertiary stage of wastewater treatment or the advanced treatment of wastewater reuse.

摘要

六嗪酮是一种全球应用的广谱三嗪除草剂,以前在高级氧化工艺 (AOPs) 和活性炭吸附中没有进行过机理研究。在这项研究中,研究了它在水基质中通过基于 UV 的氧化(有/没有过氧化氢 (HO))和在椰子壳基颗粒活性炭 (CSGAC) 上吸附的过程中的命运。各种辐照源(可见光、UVA、UVB 和 UVC)之间的比较表明,在 UVC 下降解速率最高。在 pH 7 下,在 0.5 mM HO 和 3 J/cm 的 UVC 辐照下,观察到超过 98%的六嗪酮降解。此外,在 UV/HO 过程中,随着初始 HO 剂量、UV 辐照和接触时间的增加,降解速率显著提高。由于废水中存在溶解有机物,二级出水的降解速率低于 Milli-Q 水。然而,两种基质中的反应都遵循准一级动力学。不同猝灭剂(包括甲醇、碘化钾 (KI) 和叔丁醇 (TBA))的影响表明,在 UV/HO 过程中,羟基自由基 (OH) 在六嗪酮降解中起主导作用。六嗪酮通过六嗪环和 CSGAC 表面官能团之间的π-π电子供体-受体相互作用,被 CSGAC 有效吸附。等温线和动力学研究表明,吸附遵循 Freundlich 模型和准二级反应,表明化学吸附。这项研究提供了关于在废水处理的三级阶段或废水再利用的高级处理中去除六嗪酮的机制见解。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7a98/9252970/b26fc937da55/11356_2022_19205_Fig8_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7a98/9252970/77217a6a0428/11356_2022_19205_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7a98/9252970/d82e931d709d/11356_2022_19205_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7a98/9252970/5944d97583bc/11356_2022_19205_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7a98/9252970/6ab6439f24c4/11356_2022_19205_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7a98/9252970/e49068ff1962/11356_2022_19205_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7a98/9252970/2c7e49f39c8f/11356_2022_19205_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7a98/9252970/c6896d4fca83/11356_2022_19205_Fig7_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7a98/9252970/b26fc937da55/11356_2022_19205_Fig8_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7a98/9252970/77217a6a0428/11356_2022_19205_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7a98/9252970/d82e931d709d/11356_2022_19205_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7a98/9252970/5944d97583bc/11356_2022_19205_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7a98/9252970/6ab6439f24c4/11356_2022_19205_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7a98/9252970/e49068ff1962/11356_2022_19205_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7a98/9252970/2c7e49f39c8f/11356_2022_19205_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7a98/9252970/c6896d4fca83/11356_2022_19205_Fig7_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7a98/9252970/b26fc937da55/11356_2022_19205_Fig8_HTML.jpg

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