Efficient Degradation of Bezafibrate Using the Fe(II)/Sulfite Process: Kinetics, Mechanism and Influence on DBP Formation

IF 2.6 4区 环境科学与生态学 Q3 ENVIRONMENTAL SCIENCES
Yu-qiong Gao, Jia-xin Ma, Yan-yan Rao, Ju-xiang Chen, Nai-yun Gao
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Abstract

Bezafibrate (BZF), an extensively used lipid-regulating agent, has been frequently detected in aqueous environments. In this work, we systematically investigated the Fe(II)/sulfite process for degrading BZF and its impact on disinfection byproducts (DBPs) during postchlorination. Degradation conditions were optimized by adjusting the pH, sulfite concentration, Fe(II), and BZF concentration. Under the conditions of pH = 4, [BZF]0 = 5 μM, [Fe(II)]0 = 25 μM, and [sulfite]0 = 250 μM, the BZF removal efficiency reaches 97.9% in 15 min. Sulfate radicals (SO4●–) and singlet oxygen (1O2) are recognized as the main reactive agents, with Fe(IV) also contributing to the removal of BZF. Common anions (Cl and HCO3) and humic acid generally impede the degradation process, except that trace amounts of Cl can slightly accelerate BZF degradation. A total of ten products are recognized by ultra high performance liquid chromatography and quadrupole time-of-flight mass spectrometry, and four major degradation pathways are proposed: hydroxylation, cleavage of amino bonds, removal of fibrate chains, and dechlorination. Meanwhile, the toxicity assessment shows that the majority of products exhibit lower biological toxicity and less bioaccumulation potential than BZF itself. The Fe(II)/sulfite pretreatment alters the DBP formation potential, especially when Br is present. The formation of trichloromethane (TCM) is diminished following pretreatment with the Fe(II)/sulfite process, whereas a noticeable increase in the formation of dichloroacetonitrile (DCAN) is found. Moreover, Fe(II)/sulfite pretreatment enhances the formation of brominated DBPs. Therefore, special consideration should be given to DBP formation when a Fe(II)/sulfite system is employed as a pretreatment for the removal of BZF in water.

Graphical abstract

Abstract Image

利用 Fe(II)/Sulfite 工艺高效降解贝扎贝特:动力学、机理及对 DBP 形成的影响
贝扎贝特(BZF)是一种广泛使用的脂质调节剂,经常在水环境中被检测到。在这项工作中,我们系统地研究了亚硫酸铁(II)/亚硫酸盐降解 BZF 的过程及其在后氯消毒过程中对消毒副产物(DBPs)的影响。通过调节 pH 值、亚硫酸盐浓度、Fe(II) 和 BZF 浓度,对降解条件进行了优化。在 pH = 4、[BZF]0 = 5 μM、[Fe(II)]0 = 25 μM、[亚硫酸盐]0 = 250 μM 的条件下,15 分钟内 BZF 的去除率达到 97.9%。硫酸根自由基(SO4●-)和单线态氧(1O2)被认为是主要的反应物,Fe(IV)也对 BZF 的去除有贡献。常见的阴离子(Cl- 和 HCO3-)和腐殖酸通常会阻碍降解过程,但微量的 Cl- 会稍微加速 BZF 的降解。超高效液相色谱法和四极杆飞行时间质谱法共识别出十种产物,并提出了四种主要降解途径:羟基化、氨基键裂解、纤酸链脱除和脱氯。同时,毒性评估结果表明,与 BZF 本身相比,大多数产物的生物毒性较低,生物累积潜力也较小。铁(II)/亚硫酸盐预处理会改变 DBP 的形成潜力,尤其是在存在溴的情况下。采用 Fe(II)/亚硫酸盐工艺进行预处理后,三氯甲烷(TCM)的生成量减少,而二氯乙腈(DCAN)的生成量则明显增加。此外,Fe(II)/亚硫酸盐预处理会增强溴化 DBPs 的形成。因此,在采用亚铁(II)/亚硫酸盐系统作为去除水中 BZF 的预处理时,应特别考虑 DBP 的形成。
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来源期刊
CiteScore
5.40
自引率
0.00%
发文量
104
审稿时长
1.7 months
期刊介绍: International Journal of Environmental Research is a multidisciplinary journal concerned with all aspects of environment. In pursuit of these, environmentalist disciplines are invited to contribute their knowledge and experience. International Journal of Environmental Research publishes original research papers, research notes and reviews across the broad field of environment. These include but are not limited to environmental science, environmental engineering, environmental management and planning and environmental design, urban and regional landscape design and natural disaster management. Thus high quality research papers or reviews dealing with any aspect of environment are welcomed. Papers may be theoretical, interpretative or experimental.
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