ZSM-5-(C@Fe) activated peroxymonosulfate for effectively degrading ciprofloxacin: In-depth analysis of degradation mode and degradation path

被引:77
作者
Chi, Haiyuan [1 ,2 ]
Wan, Jinquan [1 ,2 ]
Ma, Yongwen [1 ,2 ]
Wang, Yan [1 ,2 ]
Huang, Mei [1 ]
Li, Xitong [1 ]
Pu, Mengjie [3 ]
机构
[1] South China Univ Technol, Coll Environm & Energy, Guangzhou 510006, Peoples R China
[2] Guangdong Plant Fiber High Valued Cleaning Utiliz, Guangzhou 510006, Peoples R China
[3] Dongguan Univ Technol, Dongguan 523000, Peoples R China
基金
中国国家自然科学基金;
关键词
ZSM-5-(C@Fe); Metal-organic framework; Advanced oxidation technology; Peroxymonosulfate; Ciprofloxacin; METAL-ORGANIC FRAMEWORKS; EFFICIENT DEGRADATION; POLLUTANTS DEGRADATION; SELECTIVE OXIDATION; DIBUTYL PHTHALATE; POROUS CARBON; PERFORMANCE; PERSULFATE; REMOVAL; MECHANISM;
D O I
10.1016/j.jhazmat.2020.123024
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
In this work, ZSM-5-(C@Fe), as a peroxymonosulfate (PMS) heterogeneous activator, was synthesized, characterized, and evaluated for activating PMS to degrade ciprofloxacin (CIP) in wastewater. Zeolite Socony Mobil 5 (ZSM-5) was utilized to enhance structural stability and provided a scaffold to graft Fe doping C nano composites activator. Pyrolytic metal-organic frameworks (MOFs) can use crystal structure to construct stable carbon-encapsulated Fe nanocomposites. The formation of C-O-Si, C-O-Al and C-Fe was the key to the stability of catalysts. Fe doping in ZSM-5-(C@Fe) formed non-radical degradation pathway was the key to improve the degradation efficiency. The experimental data indicated ZSM-5-(C@Fe) could completely remove 20 mg L-1 CIP within 15 min and achieve good results in the experiments of treating actual wastewater, which could reduce 40% COD of the paper mill aerobic pond effluent. The Fukui function calculation and UHPL C-H RMS/MS analysis elucidated that the O-1(2)-dominated electrophilic reaction and the ZSM-5-(C@Fe) complex PMS-dominated nucleophilic reaction were the main pathways for CIP degradation and the radical degradation pathway (center dot OH and SO4-) plays auxiliary role. In addition, two new degradation pathways of the N29 and C27 in quinolone ring and the N22 in piperazine ring were discovered. This finding had important implications for the removal of N from organic pollutants.
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页数:12
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共 53 条
[1]   Efficient degradation and mineralization of antibiotics via heterogeneous activation of peroxymonosulfate by using graphene supported single -atom Cu catalyst [J].
Chen, Feng ;
Wu, Xi-Lin ;
Yang, Liu ;
Chen, Chaofa ;
Lin, Hongjun ;
Chen, Jianrong .
CHEMICAL ENGINEERING JOURNAL, 2020, 394
[2]   Ferrous metal-organic frameworks with stronger coordinatively unsaturated metal sites for persulfate activation to effectively degrade dibutyl phthalate in wastewater [J].
Chi, Haiyuan ;
Wan, Jinquan ;
Ma, Yongwen ;
Wang, Yan ;
Ding, Su ;
Li, Xitong .
JOURNAL OF HAZARDOUS MATERIALS, 2019, 377 :163-171
[3]   Energy level mediation of (BiO)2CO3 via Br doping for efficient molecular oxygen activation and ciprofloxacin photodegradation [J].
Hu, Xin ;
Zhao, Huiping ;
Liang, Ying ;
Chen, Rong .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2019, 258
[4]   Facile construction of highly reactive and stable defective iron-based metal organic frameworks for efficient degradation of Tetrabromobisphenol A via persulfate activation [J].
Huang, Mei ;
Wang, Yan ;
Wan, Jinquan ;
Ma, Yongwen ;
Chi, Haiyuan ;
Xu, Yanyan ;
Qiu, Shuying .
ENVIRONMENTAL POLLUTION, 2020, 256
[5]   Efficient degradation of 2,4-dichlorophenoxyacetic acid by peroxymonosulfate/magnetic copper ferrite nanoparticles/ozone: A novel combination of advanced oxidation processes [J].
Jaafarzadeh, Nematollah ;
Ghanbari, Farshid ;
Ahmadi, Mehdi .
CHEMICAL ENGINEERING JOURNAL, 2017, 320 :436-447
[6]   Enhancing the performance of Co3O4/CNTs for the catalytic combustion of toluene by tuning the surface structures of CNTs [J].
Jiang, Shujuan ;
Song, Shaoqing .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2013, 140 :1-8
[7]   Shorter interval and multiple flooding-drying cycling enhanced the mineralization of 14C-DDT in a paddy soil [J].
Jin, Xin ;
Kengara, Fredrick O. ;
Yue, Xianhui ;
Wang, Fang ;
Schroll, Reiner ;
Munch, Jean C. ;
Gu, Cheng ;
Jiang, Xin .
SCIENCE OF THE TOTAL ENVIRONMENT, 2019, 676 :420-428
[8]   Fe(III)-Doped g-C3N4 Mediated Peroxymonosulfate Activation for Selective Degradation of Phenolic Compounds via High-Valent Iron-Oxo Species [J].
Li, Hongchao ;
Shan, Chao ;
Pan, Bingcai .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2018, 52 (04) :2197-2205
[9]   Degradation of refractory dibutyl phthalate by peroxymonosulfate activated with novel catalysts cobalt metal-organic frameworks: Mechanism, performance, and stability [J].
Li, Huanxuan ;
Wan, Jinquan ;
Ma, Yongwen ;
Wang, Yan ;
Chen, Xi ;
Guan, Zeyu .
JOURNAL OF HAZARDOUS MATERIALS, 2016, 318 :154-163
[10]   Reaction pathway and oxidation mechanisms of dibutyl phthalate by persulfate activated with zero-valent iron [J].
Li, Huanxuan ;
Wan, Jinquan ;
Ma, Yongwen ;
Wang, Yan .
SCIENCE OF THE TOTAL ENVIRONMENT, 2016, 562 :889-897