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高铁酸盐(VI)-臭氧联合工艺降解四溴双酚A:优势、优化及机理分析

Degradation of tetrabromobisphenol A by a ferrate(vi)-ozone combination process: advantages, optimization, and mechanistic analysis.

作者信息

Han Qi, Dong Wenyi, Wang Hongjie, Ma Hang, Gu Yurong, Tian Yu

机构信息

School of Civil and Environmental Engineering, Harbin Institute of Technology (Shenzhen) Shenzhen 518055 China

Shenzhen Key Laboratory of Water Resource Utilization and Environmental Pollution Control Shenzhen 518055 China.

出版信息

RSC Adv. 2019 Dec 17;9(71):41783-41793. doi: 10.1039/c9ra07774j. eCollection 2019 Dec 13.

DOI:10.1039/c9ra07774j
PMID:35541608
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9076470/
Abstract

This study systematically investigated the ferrate(vi)-ozone combination process for TBBPA degradation. Firstly, the advantages of a ferrate(vi)-ozone combination process were assessed as compared with a sole ozone and ferrate(vi) oxidation process. Then, the performance of the ferrate(vi)-ozone combination process was investigated under different experimental conditions, including the dosing orders of oxidants, dosing concentrations of oxidants, and the initial solution pH. At the same time, toxicity control (including the acute and chronic toxicity) and mineralization were analyzed after optimization. Finally, a mechanism was proposed about the synergetic effects of the ferrate(vi)-ozone combination process for decontamination. The ferrate(vi)-ozone combination process proved to be an efficient and promising technology for removing TBBPA from water. After being pre-oxidized by ferrate(vi) for 3 min and then co-oxidized by the two oxidants, TBBPA of 1.84 μmol L could be completely degraded by dosing only 0.51 μmol L of ferrate(vi) and 10.42 μmol L of ozone within 10 min in wide ranges of pH (5.0-11.0). Up to 91.3% of debromination rate and 80.5% of mineralization rate were obtained, respectively. In addition, no bromate was detected and the acute and chronic toxicity were effectively controlled. The analysis of the proposed mechanism showed that there might exist a superposition effect of the oxidation pathways. In addition, the interactions between the two oxidants were beneficial for the oxidation efficiency of ferrate(vi) and ozone, including the catalytic effect of ferrate(vi) intermediates on ozone and the oxidation of low-valent iron compounds by ozone and the generated ·OH radical.

摘要

本研究系统地考察了高铁酸盐(VI)-臭氧联合工艺对双酚A(TBBPA)的降解效果。首先,将高铁酸盐(VI)-臭氧联合工艺与单独的臭氧氧化工艺和高铁酸盐(VI)氧化工艺进行比较,评估其优势。然后,研究了在不同实验条件下高铁酸盐(VI)-臭氧联合工艺的性能,包括氧化剂的投加顺序、氧化剂的投加浓度以及初始溶液的pH值。同时,在优化后分析了毒性控制(包括急性和慢性毒性)和矿化情况。最后,提出了高铁酸盐(VI)-臭氧联合工艺去污协同效应的机制。结果表明,高铁酸盐(VI)-臭氧联合工艺是一种从水中去除TBBPA的高效且有前景的技术。在pH值范围较宽(5.0 - 11.0)的情况下,先经高铁酸盐(VI)预氧化3分钟,然后两种氧化剂共同氧化,仅投加0.51 μmol/L的高铁酸盐(VI)和10.42 μmol/L的臭氧,1.84 μmol/L的TBBPA在10分钟内可完全降解。分别获得了高达91.3%的脱溴率和80.5%的矿化率。此外,未检测到溴酸盐,急性和慢性毒性得到有效控制。对所提出机制的分析表明,氧化途径可能存在叠加效应。此外,两种氧化剂之间的相互作用有利于高铁酸盐(VI)和臭氧的氧化效率,包括高铁酸盐(VI)中间体对臭氧的催化作用以及臭氧和生成的·OH自由基对低价铁化合物的氧化作用。

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