Yiwen Luo, Qing Zheng, Zhiyong Luo, Shuqing Xiang, Mei Dai
{"title":"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","authors":"Yiwen Luo, Qing Zheng, Zhiyong Luo, Shuqing Xiang, Mei Dai","doi":"10.1039/d4ew00274a","DOIUrl":null,"url":null,"abstract":"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.","PeriodicalId":75,"journal":{"name":"Environmental Science: Water Research & Technology","volume":null,"pages":null},"PeriodicalIF":3.5000,"publicationDate":"2024-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Removal of 3,4-dichlorophenol from water utilizing ferrate(VI): Kinetic and mechanistic investigations, and effect of coexisting anions\",\"authors\":\"Yiwen Luo, Qing Zheng, Zhiyong Luo, Shuqing Xiang, Mei Dai\",\"doi\":\"10.1039/d4ew00274a\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"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.\",\"PeriodicalId\":75,\"journal\":{\"name\":\"Environmental Science: Water Research & Technology\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":3.5000,\"publicationDate\":\"2024-05-28\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Environmental Science: Water Research & Technology\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://doi.org/10.1039/d4ew00274a\",\"RegionNum\":4,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"ENGINEERING, ENVIRONMENTAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Environmental Science: Water Research & Technology","FirstCategoryId":"93","ListUrlMain":"https://doi.org/10.1039/d4ew00274a","RegionNum":4,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
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.
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.