利用六价铬铁去除水中的 3,4-二氯苯酚:动力学和机理研究以及共存阴离子的影响

IF 3.5 4区 环境科学与生态学 Q3 ENGINEERING, ENVIRONMENTAL Environmental Science: Water Research & Technology Pub Date : 2024-05-28 DOI:10.1039/d4ew00274a
Yiwen Luo, Qing Zheng, Zhiyong Luo, Shuqing Xiang, Mei Dai
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引用次数: 0

摘要

在工业和生活污水中检测到的 3,4-二氯苯酚(3,4-DCP)对人类健康造成了不利影响。反应动力学对 pH 值的依赖性很强,随着 pH 值从 6.5 升至 10.5,二阶反应速率常数 k 从 (342.82 ± 21.81) M-1s-1 非线性变化至 (8.21 ± 0.27) M-1s-1,而对温度的依赖性很弱。利用最小二乘回归法获得了该反应的各物种特定二阶速率常数。质子化的 Fe(VI)比非质子化的 Fe(VI)具有更高的反应活性,而 3,4-DCP 则恰恰相反,因此在四个平行反应中,HFeO4- 与 3,4-DCP- 的反应速度最快。值得注意的是,3,4-二氯丙醇的去除动力学受到共存阴离子的抑制。同时,还测定了在不同的六价铬浓度、溶液 pH 值和共存阴离子条件下,六价铬去除 3,4-DCP 的效率。此外,还确定了 3,4-二氯丙醇氧化的八个中间产物,并提出了铁(VI)/3,4-二氯丙醇反应的羟基化、取代、脱氯和开环等步骤的详细机理。在真实水体中,3,4-二氯丙醇的去除率有所提高,这表明铁(六价铬)可被视为去除水中 3,4-二氯丙醇的有效技术。
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Removal of 3,4-dichlorophenol from water utilizing ferrate(VI): Kinetic and mechanistic investigations, and effect of coexisting anions
3,4-dichlorophenol (3,4-DCP) has been detected in industrial and domestic effluents, posing adverse effects on human health. Herein, ferrate (Fe(VI)) oxidation of 3,4-DCP was systemically and comprehensively investigated by determining its kinetics, mechanisms, and effect of anions. pH dependence of reaction kinetics was strong and the second-order reaction rate constant k varied nonlinearly from (342.82 ± 21.81) M-1s-1 to (8.21 ± 0.27) M-1s-1 with an increase in pH from 6.5 to 10.5, whereas its temperature dependence was quite weak. The individual species-specific second-order rate constants for the reaction were obtained using least-squares regression approach. Protonated Fe(VI) has higher reactivity than its unprotonated specie while 3,4-DCP is just the opposite, leading to the reaction of HFeO4- with 3,4-DCP- occurring fastest among four parallel reactions. Significantly, 3,4-DCP removal kinetics was inhibited by coexisting anions. Meanwhile, efficiency of 3,4-DCP removal by Fe(VI) at different Fe(VI) concentrations, solution pH, and coexisting anions was determined. Furthermore, eight intermediates of 3,4-DCP oxidation were identified, and a detailed mechanism involving hydroxylation, substitution, dechlorination, and ring-opening steps of Fe(VI)/3,4-DCP reaction was proposed. Removal of 3,4-DCP was enhanced in authentic waters, demonstrating that Fe(VI) could be regarded as an efficient technology for removing 3,4-DCP from water.
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来源期刊
Environmental Science: Water Research & Technology
Environmental Science: Water Research & Technology ENGINEERING, ENVIRONMENTALENVIRONMENTAL SC-ENVIRONMENTAL SCIENCES
CiteScore
8.60
自引率
4.00%
发文量
206
期刊介绍: Environmental Science: Water Research & Technology seeks to showcase high quality research about fundamental science, innovative technologies, and management practices that promote sustainable water.
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