New insights into the degradation of chloramphenicol and fluoroquinolone antibiotics by peroxymonosulfate activated with FeS: Performance and mechanism

被引:101
作者
Xu, Hengduo [1 ]
Sheng, Yanqing [1 ]
机构
[1] Chinese Acad Sci, Res Ctr Coastal Environm Engn Technol Shandong Pr, Yantai Inst Coastal Zone Res, Yantai 264003, Peoples R China
关键词
Sulfate radicals; Peroxymonosulfate; Sulfur-containing minerals; Antibiotic; Reaction mechanism; ORGANIC CONTAMINANTS; IRON; PERSULFATE; WATER; REMOVAL; GENERATION; OXIDATION; PATHWAYS; RADICALS; OXIDANTS;
D O I
10.1016/j.cej.2021.128823
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
SO4?- and ?OH are recognized as valid reactive species in the FeS-activated persulfate system. However, whether other reactive species are generated in this process remains unclear. In this study, a FeS-based peroxymonosulfate (PMS) (FeS/PMS) system was developed for the degradation of chloramphenicol (i.e., chloramphenicol (CAP) and thiamphenicol (TAP)) and fluoroquinolone (i.e., ciprofloxacin (CIP) and norfloxacin (NOR)) antibiotics. In addition to SO4?- and ?OH, Fe(IV) was identified as another reactive species by using methyl phenyl sulfoxide (PMSO) and methyl phenyl sulfone (PMSO2) as probe compounds. Although Fe(IV) participated in antibiotic degradation, the contribution of Fe(IV) was smaller than that of SO4?- due to its low redox potential and weak competition ability. Efficient degradation of antibiotics was achieved in the FeS/PMS system within 120 min using 6 mM PMS and 0.6 g/L FeS at initial pH of 7.0, with removal percentages of 93.5%, 98.5%, 100% and 100% for CAP, TAP, CIP and NOR, respectively. The S2- acted as an electron donor to facilitate continuous Fe(III) reduction and Fe(II) regeneration. Based on the degradation intermediates of antibiotic, the reaction pathways were proposed to involve side chain cleavage, hydroxylation, denitration, deoxygenation, decarboxylation and dehalogenation. In addition to its performance in simulated waters, the FeS/PMS system also presented effective antibiotic degradation in real surface water. This study provides new insights into the mechanism of multiple reactive species generation in the FeS-activated PMS process and extends the potential engineering applications in antibiotic degradation and in situ water quality remediation.
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页数:9
相关论文
共 49 条
[1]   The degradation of chloramphenicol by O3/PMS and the impact of O3-based AOPs pre-oxidation on dichloroacetamide generation in post-chlorination [J].
Cao, Ying ;
Qiu, Wei ;
Zhao, Yumeng ;
Li, Juan ;
Jiang, Jin ;
Yang, Yi ;
Pang, Su-Yan ;
Liu, Guanqi .
CHEMICAL ENGINEERING JOURNAL, 2020, 401
[2]   Sulfur-doped copper-cobalt bimetallic oxides with abundant Cu(I): A novel peroxymonosulfate activator for chloramphenicol degradation [J].
Chen, Cheng ;
Liu, Li ;
Guo, Jing ;
Zhou, Lixiang ;
Lan, Yeqing .
CHEMICAL ENGINEERING JOURNAL, 2019, 361 :1304-1316
[3]   Degradation of 2,4-dichlorophenoxyacetic acid in water by persulfate activated with FeS (mackinawite) [J].
Chen, Hai ;
Zhang, Zhonglei ;
Feng, Mingbao ;
Liu, Wei ;
Wang, Wenjing ;
Yang, Qi ;
Hu, Yuanan .
CHEMICAL ENGINEERING JOURNAL, 2017, 313 :498-507
[4]   Oxidation of FeS by oxygen-bearing acidic solutions [J].
Chirita, Paul ;
Descostes, Michael ;
Schlegel, Michel L. .
JOURNAL OF COLLOID AND INTERFACE SCIENCE, 2008, 321 (01) :84-95
[5]   Activation of peroxymonosulfate using drinking water treatment residuals modified by hydrothermal treatment for imidacloprid degradation [J].
Cui, Xiaoling ;
Liu, Xitao ;
Lin, Chunye ;
He, Mengchang ;
Ouyang, Wei .
CHEMOSPHERE, 2020, 254
[6]   Insights into enhanced removal of TCE utilizing sulfide-modified nanoscale zero-valent iron activated persulfate [J].
Dong, Haoran ;
Hou, Kunjie ;
Qiao, Weiwei ;
Cheng, Yujun ;
Zhang, Lihua ;
Wang, Bin ;
Li, Long ;
Wang, Yaoyao ;
Ning, Qin ;
Zeng, Guangming .
CHEMICAL ENGINEERING JOURNAL, 2019, 359 :1046-1055
[7]   Both Fe(IV) and Radicals Are Active Oxidants in the Fe(II)/Peroxydisulfate Process [J].
Dong, Hongyu ;
Li, Yang ;
Wang, Shuchang ;
Liu, Weifan ;
Zhou, Gongming ;
Xie, Yifan ;
Guan, Xiaohong .
ENVIRONMENTAL SCIENCE & TECHNOLOGY LETTERS, 2020, 7 (03) :219-224
[8]   Presence and environmental risk assessment of selected antibiotics in coastal water adjacent to mariculture areas in the Bohai Sea [J].
Du, Juan ;
Zhao, Hongxia ;
Wang, Yan ;
Xie, Huaijun ;
Zhu, Minghua ;
Chen, Jingwen .
ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY, 2019, 177 :117-123
[9]   Mackinawite (FeS) activation of persulfate for the degradation of p-chloroaniline: Surface reaction mechanism and sulfur-mediated cycling of iron species [J].
Fan, Jinhong ;
Gu, Lin ;
Wu, Deli ;
Liu, Zhigang .
CHEMICAL ENGINEERING JOURNAL, 2018, 333 :657-664
[10]   Degradation of fluoroquinolone antibiotics by ferrate(VI): Effects of water constituents and oxidized products [J].
Feng, Mingbao ;
Wang, Xinghao ;
Chen, Jing ;
Qu, Ruijuan ;
Sui, Yunxia ;
Cizmas, Leslie ;
Wang, Zunyao ;
Sharma, Virender K. .
WATER RESEARCH, 2016, 103 :48-57