{"title":"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","authors":"Yu-qiong Gao, Jia-xin Ma, Yan-yan Rao, Ju-xiang Chen, Nai-yun Gao","doi":"10.1007/s41742-024-00658-7","DOIUrl":null,"url":null,"abstract":"<p>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]<sub>0</sub> = 5 μM, [Fe(II)]<sub>0</sub> = 25 μM, and [sulfite]<sub>0</sub> = 250 μM, the BZF removal efficiency reaches 97.9% in 15 min. Sulfate radicals (SO<sub>4</sub><sup>●–</sup>) and singlet oxygen (<sup>1</sup>O<sub>2</sub>) are recognized as the main reactive agents, with Fe(IV) also contributing to the removal of BZF. Common anions (Cl<sup>−</sup> and HCO<sub>3</sub><sup>−</sup>) and humic acid generally impede the degradation process, except that trace amounts of Cl<sup>−</sup> 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<sup>−</sup> 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.</p><h3 data-test=\"abstract-sub-heading\">Graphical abstract</h3>\n","PeriodicalId":14121,"journal":{"name":"International Journal of Environmental Research","volume":null,"pages":null},"PeriodicalIF":2.6000,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Efficient Degradation of Bezafibrate Using the Fe(II)/Sulfite Process: Kinetics, Mechanism and Influence on DBP Formation\",\"authors\":\"Yu-qiong Gao, Jia-xin Ma, Yan-yan Rao, Ju-xiang Chen, Nai-yun Gao\",\"doi\":\"10.1007/s41742-024-00658-7\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>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]<sub>0</sub> = 5 μM, [Fe(II)]<sub>0</sub> = 25 μM, and [sulfite]<sub>0</sub> = 250 μM, the BZF removal efficiency reaches 97.9% in 15 min. Sulfate radicals (SO<sub>4</sub><sup>●–</sup>) and singlet oxygen (<sup>1</sup>O<sub>2</sub>) are recognized as the main reactive agents, with Fe(IV) also contributing to the removal of BZF. Common anions (Cl<sup>−</sup> and HCO<sub>3</sub><sup>−</sup>) and humic acid generally impede the degradation process, except that trace amounts of Cl<sup>−</sup> 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<sup>−</sup> 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.</p><h3 data-test=\\\"abstract-sub-heading\\\">Graphical abstract</h3>\\n\",\"PeriodicalId\":14121,\"journal\":{\"name\":\"International Journal of Environmental Research\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":2.6000,\"publicationDate\":\"2024-09-16\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"International Journal of Environmental Research\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://doi.org/10.1007/s41742-024-00658-7\",\"RegionNum\":4,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"ENVIRONMENTAL SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"International Journal of Environmental Research","FirstCategoryId":"93","ListUrlMain":"https://doi.org/10.1007/s41742-024-00658-7","RegionNum":4,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"ENVIRONMENTAL SCIENCES","Score":null,"Total":0}
Efficient Degradation of Bezafibrate Using the Fe(II)/Sulfite Process: Kinetics, Mechanism and Influence on DBP Formation
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.
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.