Highly-efficient removal of norfloxacin with nanoscale zero-valent copper activated persulfate at mild temperature

被引:113
作者
Deng, Jing [1 ,2 ,3 ]
Xu, Mengyuan [1 ]
Chen, Yijing [1 ]
Li, Jun [4 ]
Qiu, Chungen [1 ]
Li, Xueyan [5 ]
Zhou, Shiqing [6 ]
机构
[1] Zhejiang Univ Technol, Coll Civil Engn & Architecture, Hangzhou 310014, Zhejiang, Peoples R China
[2] Georgia Inst Technol, Brook Byers Inst Sustainable Syst, Atlanta, GA 30332 USA
[3] Georgia Inst Technol, Sch Civil & Environm Engn, Atlanta, GA 30332 USA
[4] Zhejiang Univ Technol, Coll Environm, Hangzhou 310014, Zhejiang, Peoples R China
[5] Suzhou Univ Sci & Technol, Sch Environm Sci & Engn, Suzhou 215009, Peoples R China
[6] Hunan Univ, Key Lab Bldg Safety & Energy Efficiency, Minist Educ, Dept Water Engn & Sci,Coll Civil Engn, Changsha 410082, Hunan, Peoples R China
基金
中国国家自然科学基金;
关键词
Nanoscale zero-valent copper; Persulfate; Norfloxacin; Mild temperature; Reactive oxygen species; Degradation pathway; WASTE-WATER TREATMENT; FREE-RADICAL REACTIONS; ENHANCED DEGRADATION; HYDROGEN-PEROXIDE; HYDROXYL RADICALS; POLYVINYL-ALCOHOL; TREATMENT PLANTS; AQUEOUS-SOLUTION; RATE CONSTANTS; OXIDATION;
D O I
10.1016/j.cej.2019.02.073
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 study, mild temperature was applied to enhance norfloxacin (NOR) degradation in nanoscale zero-valent copper (nZVC) activated persulfate (PS) process and the underlying activation mechanism was detailedly elaborated. Results showed that the activation performance of nZVC was far superior than that of micro zero-valent copper (mZVC), and almost complete elimination of 31.32 mu M NOR was achieved within only 5 min in the condition of 0.05 g/L nZVC and 1.0mM PS at 40 degrees C. The in-situ generated Cu+ was found to be the pivotal active copper species for PS activation and the presence of dissolved oxygen was favorable for its release. Mild temperature not only accelerated the Cu+ release from the nZVC corrision, but provided more opportunity for intermolecular collision to quickly form reactive oxygen species. SO4 (-center dot) and (OH)-O-center dot played the primary role for NOR destruction, while O-2(-center dot) and H2O2 served as the mediators for copper cycling. The higher PS concentration favored NOR removal, whereas overdosing nZVC exerted the negative impact. Further increasing reaction temperature significantly accelerated the elimination of NOR in nZVC/PS process. The satisfactory removal of NOR was achieved under the acidic and neutral conditions. The NOR oxidation in the tested process was found to follow four routes and the cleavage of piperazine ring was determined to be the primary one. These encouraging results demonstrated that mild temperature enhanced nZVC/PS process was a promising strategy for the treatment of refractory and non-biodegradable industrial wastewater.
引用
收藏
页码:491 / 503
页数:13
相关论文
共 62 条
[51]   Degradation of carbon tetrachloride in aqueous solution in the thermally activated persulfate system [J].
Xu, Minhui ;
Gu, Xiaogang ;
Lu, Shuguang ;
Qiu, Zhaofu ;
Sui, Qian ;
Miao, Zhouwei ;
Zang, Xueke ;
Wu, Xiaoliang .
JOURNAL OF HAZARDOUS MATERIALS, 2015, 286 :7-14
[52]   Copper-Catalyzed Hydroquinone Oxidation and Associated Redox Cycling of Copper under Conditions Typical of Natural Saline Waters [J].
Yuan, Xiu ;
Pham, A. Ninh ;
Miller, Christopher J. ;
Waite, T. David .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2013, 47 (15) :8355-8364
[53]   Efficient activation of ozone by zero-valent copper for the degradation of aniline in aqueous solution [J].
Zhang, Jing ;
Guo, Jing ;
Wu, Yao ;
Lan, Yeqing ;
Li, Ying .
JOURNAL OF THE TAIWAN INSTITUTE OF CHEMICAL ENGINEERS, 2017, 81 :335-342
[54]   Copper-catalyzed activation of molecular oxygen for oxidative destruction of acetaminophen: The mechanism and superoxide mediated cycling of copper species [J].
Zhang, Yunfei ;
Fan, Jinhong ;
Yang, Bo ;
Huang, Wutao ;
Ma, Luming .
CHEMOSPHERE, 2017, 166 :89-95
[55]   Simultaneous removal of bisphenol A and phosphate in zero-valent iron activated persulfate oxidation process [J].
Zhao, Li ;
Ji, Yuefei ;
Kong, Deyang ;
Lu, Junhe ;
Zhou, Quansuo ;
Yin, Xiaoming .
CHEMICAL ENGINEERING JOURNAL, 2016, 303 :458-466
[56]   Trends in the occurrence of human and veterinary antibiotics in the sediments of the Yellow River, Hai River and Liao River in northern China [J].
Zhou, Li-Jun ;
Ying, Guang-Guo ;
Zhao, Jian-Liang ;
Yang, Ji-Feng ;
Wang, Li ;
Yang, Bin ;
Liu, Shan .
ENVIRONMENTAL POLLUTION, 2011, 159 (07) :1877-1885
[57]   Degradation of 2,4-dichlorophenol by activating persulfate and peroxomonosulfate using micron or nanoscale zero-valent copper [J].
Zhou, Peng ;
Zhang, Jing ;
Zhang, Yongli ;
Zhang, Gucheng ;
Li, Wenshu ;
Wei, Chenmo ;
Liang, Juan ;
Liu, Ya ;
Shu, Shihu .
JOURNAL OF HAZARDOUS MATERIALS, 2018, 344 :1209-1219
[58]   Activation of hydrogen peroxide during the corrosion of nanoscale zero valent copper in acidic solution [J].
Zhou, Peng ;
Zhang, Jing ;
Zhang, Yongli ;
Liang, Juan ;
Liu, Ya ;
Liu, Bei ;
Zhang, Wei .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2016, 424 :115-120
[59]   Oxidation of microcystin-LR by copper (II) coupled with ascorbic acid: Kinetic modeling towards generation of H2O2 [J].
Zhou, Shiqing ;
Yu, Yanghai ;
Sun, Julong ;
Zhu, Shumin ;
Deng, Jing .
CHEMICAL ENGINEERING JOURNAL, 2018, 333 :443-450
[60]   Synergistic degradation of antibiotic norfloxacin in a novel heterogeneous sonochemical Fe0/tetraphosphate Fenton-like system [J].
Zhou, Tao ;
Zou, Xiaoli ;
Wu, Xiaohui ;
Mao, Juan ;
Wang, Jia .
ULTRASONICS SONOCHEMISTRY, 2017, 37 :320-327