Degradation of ciprofloxacin using α-MnO2 activated peroxymonosulfate process: Effect of water constituents, degradation intermediates and toxicity evaluation

被引:298
作者
Deng, Jing [1 ,2 ]
Ge, Yongjian [1 ]
Tan, Chaoqun [3 ]
Wang, Hongyu [1 ]
Li, Qingsong [4 ]
Zhou, Shiqing [5 ]
Zhang, Kejia [2 ]
机构
[1] Zhejiang Univ Technol, Coll Civil Engn & Architecture, Hangzhou 310014, Zhejiang, Peoples R China
[2] Zhejiang Univ, Coll Civil Engn & Architecture, Hangzhou 310058, Zhejiang, Peoples R China
[3] Southeast Univ, Sch Civil Engn, Nanjing 210096, Jiangsu, Peoples R China
[4] Xiamen Univ Technol, Coll Environm Sci & Engn, Xiamen 361024, Peoples R China
[5] Hunan Univ, Coll Civil Engn, Changsha 410082, Hunan, Peoples R China
基金
中国国家自然科学基金; 中国博士后科学基金;
关键词
alpha-MnO2; Peroxymonosulfate (PMS); Ciprofloxacin (CIP); Degradation; Intermediates; Acute toxicity; ANTIEPILEPTIC DRUG CARBAMAZEPINE; ADVANCED OXIDATION PROCESSES; ACID ORANGE 7; PHOTOCATALYTIC DEGRADATION; PHOTOCHEMICAL DEGRADATION; HETEROGENEOUS CATALYST; EFFICIENT DEGRADATION; PHENOL DEGRADATION; HYDROGEN-PEROXIDE; SULFATE RADICALS;
D O I
10.1016/j.cej.2017.07.137
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Nanoscale alpha-MnO2 with different morphologies (nanoparticles, nanoflowers and nanorods) were synthesized via a facile hydrothermal method and tested in peroxymonosulfate (PMS) activation for ciprofloxacin (CIP) degradation. The catalytic activity of alpha-MnO2 mainly relied on the specific surface area and crystallinity, and followed the order of alpha-MnO2 nanoflowers > alpha-MnO2 nanorods > alpha-MnO2 nanoparticles > commercial MnO2. Acidic condition was more beneficial to CIP removal than neutral condition, and the degradation would be greatly accelerated in alkaline circumstance. The introduction of chloride and bicarbonate displayed concentration-dependent dual effect. The presence of natural organic matter (NOM) exerted the detrimental effect on CIP degradation. Eleven oxidation products were identified by UPLC-MS/MS and the changes of their concentrations were monitored, five products showed monotonous uptrend while four intermediates present monotonous downtrend once they were generated. Piperazine ring cleavage, hydroxylation and F/OH substitution were found to be the important oxidation pathways. The acute toxicity of resulted solution gradually decreased with the lapse of time, and higher PMS concentration favored the detoxification. The CIP removal in alpha-MnO2/PMS process was also efficient under the actual water background, which was testified by the results of fluorescence excitation-emission matrix (EEM).
引用
收藏
页码:1390 / 1400
页数:11
相关论文
共 57 条
[1]   Kinetics and mechanism of advanced oxidation processes (AOPs) in degradation of ciprofloxacin in water [J].
An, Taicheng ;
Yang, Hai ;
Li, Guiying ;
Song, Weihua ;
Cooper, William J. ;
Nie, Xiangping .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2010, 94 (3-4) :288-294
[2]   Chemical and microbial decontamination of pool water using activated potassium peroxymonosulfate [J].
Anipsitakis, George P. ;
Tufano, Thomas P. ;
Dionysiou, Dionysios D. .
WATER RESEARCH, 2008, 42 (12) :2899-2910
[3]   Radical generation by the interaction of transition metals with common oxidants [J].
Anipsitakis, GP ;
Dionysiou, DD .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2004, 38 (13) :3705-3712
[4]   A review of the occurrence of pharmaceuticals and personal cue products in Indian water bodies [J].
Balakrishna, Keshava ;
Rath, Amlan ;
Praveenkumarreddy, Yerabham ;
Guruge, Keerthi Ski ;
Subedi, Bikram .
ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY, 2017, 137 :113-120
[5]   An overview of the application of Fenton oxidation to industrial wastewaters treatment [J].
Bautista, P. ;
Mohedano, A. F. ;
Casas, J. A. ;
Zazo, J. A. ;
Rodriguez, J. J. .
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY, 2008, 83 (10) :1323-1338
[6]   Oxidative degradation kinetics and products of chlortetracycline by manganese dioxide [J].
Chen, Gao ;
Zhao, Ling ;
Dong, Yuan-hua .
JOURNAL OF HAZARDOUS MATERIALS, 2011, 193 :128-138
[7]   Fluorescence excitation - Emission matrix regional integration to quantify spectra for dissolved organic matter [J].
Chen, W ;
Westerhoff, P ;
Leenheer, JA ;
Booksh, K .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2003, 37 (24) :5701-5710
[8]   Heterogeneous activation of peroxymonosulfate using ordered mesoporous Co3O4 for the degradation of chloramphenicol at neutral pH [J].
Deng, Jing ;
Feng, ShanFang ;
Zhang, Kejia ;
Li, Jun ;
Wang, Hongyu ;
Zhang, Tuqiao ;
Ma, Xiaoyan .
CHEMICAL ENGINEERING JOURNAL, 2017, 308 :505-515
[9]   Heterogeneous degradation of Orange II with peroxymonosulfate activated by ordered mesoporous MnFe2O4 [J].
Deng, Jing ;
Feng, ShanFang ;
Ma, Xiaoyan ;
Tan, Chaoqun ;
Wang, Hongyu ;
Zhou, Shiqing ;
Zhang, Tuqiao ;
Li, Jun .
SEPARATION AND PURIFICATION TECHNOLOGY, 2016, 167 :181-189
[10]   CoFe2O4 magnetic nanoparticles as a highly active heterogeneous catalyst of oxone for the degradation of diclofenac in water [J].
Deng, Jing ;
Shao, Yisheng ;
Gao, Naiyun ;
Tan, Chaoqun ;
Zhou, Shiqing ;
Hu, Xuhao .
JOURNAL OF HAZARDOUS MATERIALS, 2013, 262 :836-844