{"title":"铈调节 Mg3FeO4@biochar 活化过硫酸盐,提高四环素水溶液的降解:铈的主导作用","authors":"Jiahui Liu, Junfeng Zhu, Xue Ma, Xiangchu Zeng, Guanghua Zhang, Yonghui Sun, Guodong Fan","doi":"10.1016/j.apsusc.2024.161416","DOIUrl":null,"url":null,"abstract":"The role of cerium (Ce) in Ce-regulated Mg<sub>3</sub>FeO<sub>4</sub>@biochar (CMF@BC) and the mechanism by which CMF@BC activates persulfate (PS) remain unclear. In this work, a novel CMF@BC was synthesized through the simple impregnation–pyrolysis process and utilized as a PS activator for the removal of aqueous tetracycline (TC). Under the optimal degradation conditions, the removal efficiency and mineralization rate of TC reached 92.7 % and 84.2 % within 60 min, respectively, the corresponding rate constant was 0.0487 min<sup>−1</sup>. The CMF@BC catalyst exhibited extremely high stability and excellent reusability after five cycles. The characterization results identified Fe<sup>2+</sup> and oxygen vacancies as major catalytic sites. The Ce dopant inhibited the aggregation of metal ions of Mg<sub>3</sub>FeO<sub>4</sub> during the high-temperature pyrolysis process and the Ce<sup>3+</sup>/Ce<sup>4+</sup> redox cycle promoted Fe<sup>2+</sup> regeneration, thus improving the catalyst performance. The degradation process was dominated by non-free radical (<sup>1</sup>O<sub>2</sub>) pathways. The possible TC-removal pathway was inferred from liquid chromatography–mass spectrometry results and density functional theory calculations. The toxicity of the degradation products was also evaluated. The CMF@BC catalyst displayed excellent catalytic performance and recyclability, wide pH adaptability, and a low ion-leaching rate, confirming its broad application prospects as a PS activator in antibiotic wastewater treatment.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":null,"pages":null},"PeriodicalIF":6.3000,"publicationDate":"2024-10-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Cerium-regulated Mg3FeO4@biochar activated persulfate to enhance degradation of aqueous tetracycline: The dominant role of cerium\",\"authors\":\"Jiahui Liu, Junfeng Zhu, Xue Ma, Xiangchu Zeng, Guanghua Zhang, Yonghui Sun, Guodong Fan\",\"doi\":\"10.1016/j.apsusc.2024.161416\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The role of cerium (Ce) in Ce-regulated Mg<sub>3</sub>FeO<sub>4</sub>@biochar (CMF@BC) and the mechanism by which CMF@BC activates persulfate (PS) remain unclear. In this work, a novel CMF@BC was synthesized through the simple impregnation–pyrolysis process and utilized as a PS activator for the removal of aqueous tetracycline (TC). Under the optimal degradation conditions, the removal efficiency and mineralization rate of TC reached 92.7 % and 84.2 % within 60 min, respectively, the corresponding rate constant was 0.0487 min<sup>−1</sup>. The CMF@BC catalyst exhibited extremely high stability and excellent reusability after five cycles. The characterization results identified Fe<sup>2+</sup> and oxygen vacancies as major catalytic sites. The Ce dopant inhibited the aggregation of metal ions of Mg<sub>3</sub>FeO<sub>4</sub> during the high-temperature pyrolysis process and the Ce<sup>3+</sup>/Ce<sup>4+</sup> redox cycle promoted Fe<sup>2+</sup> regeneration, thus improving the catalyst performance. The degradation process was dominated by non-free radical (<sup>1</sup>O<sub>2</sub>) pathways. The possible TC-removal pathway was inferred from liquid chromatography–mass spectrometry results and density functional theory calculations. The toxicity of the degradation products was also evaluated. The CMF@BC catalyst displayed excellent catalytic performance and recyclability, wide pH adaptability, and a low ion-leaching rate, confirming its broad application prospects as a PS activator in antibiotic wastewater treatment.\",\"PeriodicalId\":247,\"journal\":{\"name\":\"Applied Surface Science\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":6.3000,\"publicationDate\":\"2024-10-05\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Surface Science\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1016/j.apsusc.2024.161416\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Surface Science","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1016/j.apsusc.2024.161416","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Cerium-regulated Mg3FeO4@biochar activated persulfate to enhance degradation of aqueous tetracycline: The dominant role of cerium
The role of cerium (Ce) in Ce-regulated Mg3FeO4@biochar (CMF@BC) and the mechanism by which CMF@BC activates persulfate (PS) remain unclear. In this work, a novel CMF@BC was synthesized through the simple impregnation–pyrolysis process and utilized as a PS activator for the removal of aqueous tetracycline (TC). Under the optimal degradation conditions, the removal efficiency and mineralization rate of TC reached 92.7 % and 84.2 % within 60 min, respectively, the corresponding rate constant was 0.0487 min−1. The CMF@BC catalyst exhibited extremely high stability and excellent reusability after five cycles. The characterization results identified Fe2+ and oxygen vacancies as major catalytic sites. The Ce dopant inhibited the aggregation of metal ions of Mg3FeO4 during the high-temperature pyrolysis process and the Ce3+/Ce4+ redox cycle promoted Fe2+ regeneration, thus improving the catalyst performance. The degradation process was dominated by non-free radical (1O2) pathways. The possible TC-removal pathway was inferred from liquid chromatography–mass spectrometry results and density functional theory calculations. The toxicity of the degradation products was also evaluated. The CMF@BC catalyst displayed excellent catalytic performance and recyclability, wide pH adaptability, and a low ion-leaching rate, confirming its broad application prospects as a PS activator in antibiotic wastewater treatment.
期刊介绍:
Applied Surface Science covers topics contributing to a better understanding of surfaces, interfaces, nanostructures and their applications. The journal is concerned with scientific research on the atomic and molecular level of material properties determined with specific surface analytical techniques and/or computational methods, as well as the processing of such structures.