Haotian Mu, Chuanping Feng, Nan Chen, Weiwu Hu, Boaiqi Zhang, Ning An
{"title":"基于电场下直接电子转移的双金属铁钴对氟苯尼考的脱卤性能研究","authors":"Haotian Mu, Chuanping Feng, Nan Chen, Weiwu Hu, Boaiqi Zhang, Ning An","doi":"10.1016/j.seppur.2025.133451","DOIUrl":null,"url":null,"abstract":"<div><div>Dehalogenation of halogenated antibiotics is an effective pretreatment method aimed to eliminate the toxicity. In this study, a novel electrode was developed utilizing single-step electrodeposition for the in-situ generation of bimetallic iron-cobalt nanoparticles on copper foam (CF). The synthesized cathode material (Fe@Co/CF) was utilized for the electrochemical reductive dehalogenation of florfenicol (C<sub>12</sub>H<sub>14</sub>Cl<sub>2</sub>FNO<sub>4</sub>S, FLO), a representative halogenated antibiotic. The presence of a positive charge on the surface of the bimetallic iron-cobalt was proved by density functional theory (DFT) calculations, enhancing the adsorption of the C-Cl bond and reducing the activation energy. The removal of FLO was >99 % under the optimal conditions of 10 mA and pH 6.0 by Fe@Co/CF and the dechlorinating efficiency of FLO was approximately 83 %, which was significantly superior to other cathode materials. Great treatment performance on Fe@Co/CF for other chlorinated antibiotics was demonstrated. The primary mechanism for FLO dehalogenation by Fe@Co/CF was direct electron transfer (DET), which was augmented by the synergistic effect of the bimetallic iron-cobalt. During the electrochemical reductive dehalogenation, FLO was sequentially decomposed to C<sub>12</sub>H<sub>14</sub>ClFNO<sub>4</sub>S and then to C<sub>12</sub>H<sub>14</sub>FNO<sub>4</sub>S, significantly reducing biotoxicity. After practical water treatment and cycles, high treatment efficiency of Fe@Co/CF was maintained. The developed electrode for the dehalogenation of halogenated antibiotics in this study has demonstrated great potential for dechlorinating halogenated pollutants in wastewater.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"372 ","pages":"Article 133451"},"PeriodicalIF":8.1000,"publicationDate":"2025-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Dehalogenation performance of florfenicol by bimetallic iron-cobalt based on direct electron transfer under electric field\",\"authors\":\"Haotian Mu, Chuanping Feng, Nan Chen, Weiwu Hu, Boaiqi Zhang, Ning An\",\"doi\":\"10.1016/j.seppur.2025.133451\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Dehalogenation of halogenated antibiotics is an effective pretreatment method aimed to eliminate the toxicity. In this study, a novel electrode was developed utilizing single-step electrodeposition for the in-situ generation of bimetallic iron-cobalt nanoparticles on copper foam (CF). The synthesized cathode material (Fe@Co/CF) was utilized for the electrochemical reductive dehalogenation of florfenicol (C<sub>12</sub>H<sub>14</sub>Cl<sub>2</sub>FNO<sub>4</sub>S, FLO), a representative halogenated antibiotic. The presence of a positive charge on the surface of the bimetallic iron-cobalt was proved by density functional theory (DFT) calculations, enhancing the adsorption of the C-Cl bond and reducing the activation energy. The removal of FLO was >99 % under the optimal conditions of 10 mA and pH 6.0 by Fe@Co/CF and the dechlorinating efficiency of FLO was approximately 83 %, which was significantly superior to other cathode materials. Great treatment performance on Fe@Co/CF for other chlorinated antibiotics was demonstrated. The primary mechanism for FLO dehalogenation by Fe@Co/CF was direct electron transfer (DET), which was augmented by the synergistic effect of the bimetallic iron-cobalt. During the electrochemical reductive dehalogenation, FLO was sequentially decomposed to C<sub>12</sub>H<sub>14</sub>ClFNO<sub>4</sub>S and then to C<sub>12</sub>H<sub>14</sub>FNO<sub>4</sub>S, significantly reducing biotoxicity. After practical water treatment and cycles, high treatment efficiency of Fe@Co/CF was maintained. The developed electrode for the dehalogenation of halogenated antibiotics in this study has demonstrated great potential for dechlorinating halogenated pollutants in wastewater.</div></div>\",\"PeriodicalId\":427,\"journal\":{\"name\":\"Separation and Purification Technology\",\"volume\":\"372 \",\"pages\":\"Article 133451\"},\"PeriodicalIF\":8.1000,\"publicationDate\":\"2025-05-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Separation and Purification Technology\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1383586625020489\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Separation and Purification Technology","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1383586625020489","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Dehalogenation performance of florfenicol by bimetallic iron-cobalt based on direct electron transfer under electric field
Dehalogenation of halogenated antibiotics is an effective pretreatment method aimed to eliminate the toxicity. In this study, a novel electrode was developed utilizing single-step electrodeposition for the in-situ generation of bimetallic iron-cobalt nanoparticles on copper foam (CF). The synthesized cathode material (Fe@Co/CF) was utilized for the electrochemical reductive dehalogenation of florfenicol (C12H14Cl2FNO4S, FLO), a representative halogenated antibiotic. The presence of a positive charge on the surface of the bimetallic iron-cobalt was proved by density functional theory (DFT) calculations, enhancing the adsorption of the C-Cl bond and reducing the activation energy. The removal of FLO was >99 % under the optimal conditions of 10 mA and pH 6.0 by Fe@Co/CF and the dechlorinating efficiency of FLO was approximately 83 %, which was significantly superior to other cathode materials. Great treatment performance on Fe@Co/CF for other chlorinated antibiotics was demonstrated. The primary mechanism for FLO dehalogenation by Fe@Co/CF was direct electron transfer (DET), which was augmented by the synergistic effect of the bimetallic iron-cobalt. During the electrochemical reductive dehalogenation, FLO was sequentially decomposed to C12H14ClFNO4S and then to C12H14FNO4S, significantly reducing biotoxicity. After practical water treatment and cycles, high treatment efficiency of Fe@Co/CF was maintained. The developed electrode for the dehalogenation of halogenated antibiotics in this study has demonstrated great potential for dechlorinating halogenated pollutants in wastewater.
期刊介绍:
Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.