煤焦油沥青衍生多孔碳活化过硫酸盐非自由基左氧氟沙星降解

IF 4.5 3区 工程技术 Q2 ENGINEERING, CHEMICAL
Lili Zhang, Shuguang Shen, Chongyan Chen, Jie Wang, Yongmei Liu, Jing Li, Ruxue Sun
{"title":"煤焦油沥青衍生多孔碳活化过硫酸盐非自由基左氧氟沙星降解","authors":"Lili Zhang,&nbsp;Shuguang Shen,&nbsp;Chongyan Chen,&nbsp;Jie Wang,&nbsp;Yongmei Liu,&nbsp;Jing Li,&nbsp;Ruxue Sun","doi":"10.1007/s11705-025-2591-9","DOIUrl":null,"url":null,"abstract":"<div><p>The persistent presence of levofloxacin (LEV) residues in aquatic environments considerably threatens ecological safety and human health, owing to the potential spread of microbial resistance genes, creating an urgent need for effective removal technologies. In this study, porous carbon materials with high specific surface areas were synthesized using a one-step KOH activation method, with medium-low-temperature coal tar pitch serving as a carbon precursor. In addition, the performance and mechanism of LEV degradation via peroxydisulfate (PDS) activation were systematically explored. Characterization techniques such as X-ray diffraction, Raman spectroscopy, N<sub>2</sub> adsorption-desorption analysis, and field-emission scanning electron microscopy revealed that K11 possessed abundant pores, a specific surface area of up to 1220 m<sup>2</sup>·g<sup>−1</sup>, and numerous defects, which collectively provided a structural basis for its catalytic activity. Degradation experiments demonstrated that the LEV removal rate exceeded 91% under conditions of a 0.2 g·L<sup>−1</sup> PDS dosage, a 0.1 g·L<sup>−1</sup> K11 dosage, pH levels ranging from 3 to 9, and a temperature of 30 °C, with robust resistance to interference from co-existing ions and humic acid. Even in real water bodies, a removal rate of over 77.84% was maintained. Free-radical quenching experiments and electron spin resonance assays confirmed that the reaction proceeded predominantly via non-radical pathways, primarily involving the generation of singlet oxygen by PDS, along with a minor contribution from direct electron transfer pathways. High-performance liquid chromatography-mass spectrometry identified LEV degradation intermediates, suggesting that the degradation pathways include piperazine ring cleavage, defluorination, and oxidation of the quinolone backbone. This study offers theoretical insights and technical guidance for the resource utilization of coal tar pitch and the control of antibiotic pollution.\n</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":571,"journal":{"name":"Frontiers of Chemical Science and Engineering","volume":"19 9","pages":""},"PeriodicalIF":4.5000,"publicationDate":"2025-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Coal tar pitch-derived porous carbon activates persulfate for non-radical levofloxacin degradation\",\"authors\":\"Lili Zhang,&nbsp;Shuguang Shen,&nbsp;Chongyan Chen,&nbsp;Jie Wang,&nbsp;Yongmei Liu,&nbsp;Jing Li,&nbsp;Ruxue Sun\",\"doi\":\"10.1007/s11705-025-2591-9\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The persistent presence of levofloxacin (LEV) residues in aquatic environments considerably threatens ecological safety and human health, owing to the potential spread of microbial resistance genes, creating an urgent need for effective removal technologies. In this study, porous carbon materials with high specific surface areas were synthesized using a one-step KOH activation method, with medium-low-temperature coal tar pitch serving as a carbon precursor. In addition, the performance and mechanism of LEV degradation via peroxydisulfate (PDS) activation were systematically explored. Characterization techniques such as X-ray diffraction, Raman spectroscopy, N<sub>2</sub> adsorption-desorption analysis, and field-emission scanning electron microscopy revealed that K11 possessed abundant pores, a specific surface area of up to 1220 m<sup>2</sup>·g<sup>−1</sup>, and numerous defects, which collectively provided a structural basis for its catalytic activity. Degradation experiments demonstrated that the LEV removal rate exceeded 91% under conditions of a 0.2 g·L<sup>−1</sup> PDS dosage, a 0.1 g·L<sup>−1</sup> K11 dosage, pH levels ranging from 3 to 9, and a temperature of 30 °C, with robust resistance to interference from co-existing ions and humic acid. Even in real water bodies, a removal rate of over 77.84% was maintained. Free-radical quenching experiments and electron spin resonance assays confirmed that the reaction proceeded predominantly via non-radical pathways, primarily involving the generation of singlet oxygen by PDS, along with a minor contribution from direct electron transfer pathways. High-performance liquid chromatography-mass spectrometry identified LEV degradation intermediates, suggesting that the degradation pathways include piperazine ring cleavage, defluorination, and oxidation of the quinolone backbone. This study offers theoretical insights and technical guidance for the resource utilization of coal tar pitch and the control of antibiotic pollution.\\n</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>\",\"PeriodicalId\":571,\"journal\":{\"name\":\"Frontiers of Chemical Science and Engineering\",\"volume\":\"19 9\",\"pages\":\"\"},\"PeriodicalIF\":4.5000,\"publicationDate\":\"2025-07-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Frontiers of Chemical Science and Engineering\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s11705-025-2591-9\",\"RegionNum\":3,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Frontiers of Chemical Science and Engineering","FirstCategoryId":"5","ListUrlMain":"https://link.springer.com/article/10.1007/s11705-025-2591-9","RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0

摘要

由于微生物耐药基因的潜在传播,左氧氟沙星(LEV)残留在水生环境中的持续存在严重威胁着生态安全和人类健康,因此迫切需要有效的去除技术。本研究以中低温煤焦油沥青为碳前驱体,采用一步KOH活化法合成了具有高比表面积的多孔碳材料。此外,系统探讨了过硫酸氢盐(PDS)活化降解LEV的性能和机理。x射线衍射、拉曼光谱、N2吸附-解吸分析、场发射扫描电镜等表征技术表明,K11具有丰富的孔隙、高达1220 m2·g−1的比表面积和众多的缺陷,为其催化活性提供了结构基础。降解实验表明,在PDS用量为0.2 g·L−1、K11用量为0.1 g·L−1、pH值为3 ~ 9、温度为30℃的条件下,LEV去除率超过91%,具有较强的抗共存离子和腐植酸干扰能力。即使在真实水体中,去除率也保持在77.84%以上。自由基猝灭实验和电子自旋共振分析证实,该反应主要通过非自由基途径进行,主要涉及PDS产生单线态氧,以及直接电子转移途径的少量贡献。高效液相色谱-质谱分析鉴定了LEV降解中间体,表明其降解途径包括哌嗪环裂解、去氟化和喹诺酮骨架氧化。本研究为煤沥青资源化利用和抗生素污染治理提供了理论见解和技术指导。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Coal tar pitch-derived porous carbon activates persulfate for non-radical levofloxacin degradation

The persistent presence of levofloxacin (LEV) residues in aquatic environments considerably threatens ecological safety and human health, owing to the potential spread of microbial resistance genes, creating an urgent need for effective removal technologies. In this study, porous carbon materials with high specific surface areas were synthesized using a one-step KOH activation method, with medium-low-temperature coal tar pitch serving as a carbon precursor. In addition, the performance and mechanism of LEV degradation via peroxydisulfate (PDS) activation were systematically explored. Characterization techniques such as X-ray diffraction, Raman spectroscopy, N2 adsorption-desorption analysis, and field-emission scanning electron microscopy revealed that K11 possessed abundant pores, a specific surface area of up to 1220 m2·g−1, and numerous defects, which collectively provided a structural basis for its catalytic activity. Degradation experiments demonstrated that the LEV removal rate exceeded 91% under conditions of a 0.2 g·L−1 PDS dosage, a 0.1 g·L−1 K11 dosage, pH levels ranging from 3 to 9, and a temperature of 30 °C, with robust resistance to interference from co-existing ions and humic acid. Even in real water bodies, a removal rate of over 77.84% was maintained. Free-radical quenching experiments and electron spin resonance assays confirmed that the reaction proceeded predominantly via non-radical pathways, primarily involving the generation of singlet oxygen by PDS, along with a minor contribution from direct electron transfer pathways. High-performance liquid chromatography-mass spectrometry identified LEV degradation intermediates, suggesting that the degradation pathways include piperazine ring cleavage, defluorination, and oxidation of the quinolone backbone. This study offers theoretical insights and technical guidance for the resource utilization of coal tar pitch and the control of antibiotic pollution.

求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
CiteScore
7.60
自引率
6.70%
发文量
868
审稿时长
1 months
期刊介绍: Frontiers of Chemical Science and Engineering presents the latest developments in chemical science and engineering, emphasizing emerging and multidisciplinary fields and international trends in research and development. The journal promotes communication and exchange between scientists all over the world. The contents include original reviews, research papers and short communications. Coverage includes catalysis and reaction engineering, clean energy, functional material, nanotechnology and nanoscience, biomaterials and biotechnology, particle technology and multiphase processing, separation science and technology, sustainable technologies and green processing.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术官方微信