Green synthesis of sulfur-doped g-C3N4 nanosheets for enhanced removal of oxytetracycline under visible-light irradiation and reduction of its N-nitrosodimethylamine formation potential

被引:13
作者
Dou, Yicheng [1 ,2 ]
Shen, Xingyu [3 ]
Zou, Jinte [4 ]
Shi, Runzhe [1 ]
Yan, Tingting [1 ]
Sun, Qiya [1 ]
Wang, Lin [1 ,2 ]
机构
[1] Tongji Univ Shanghai China, Coll Environm Sci & Engn, State Key Lab Pollut Control & Resource Reuse, Key Lab Yangtze River Water Environm, Shanghai 200092, Peoples R China
[2] Shanghai Inst Pollut Control & Ecol Secur, Shanghai, Peoples R China
[3] Shanghai Weiyu High Sch, Shanghai, Peoples R China
[4] Zhejiang Univ Technol, Key Lab Microbial Technol Ind Pollut Control Zhej, Coll Environm, Hangzhou, Peoples R China
关键词
veterinary antibiotics; visible‐ light photocatalysis; photocatalytic degradation; nitrosamine disinfection byproducts; removal mechanism;
D O I
10.1002/jctb.6674
中图分类号
Q81 [生物工程学(生物技术)]; Q93 [微生物学];
学科分类号
071005 ; 0836 ; 090102 ; 100705 ;
摘要
BACKGROUND In this study, sulfur-doped g-C3N4 (SCN) nanosheets were synthesized using thiourea as a precursor, and then used to catalyze the degradation of oxytetracycline (OTC) under visible-light irradiation. OTC was chosen as target contaminant because of it being an important precursor of N-nitrosodimethylamine (NDMA). RESULTS The removal of OTC was influenced by its initial concentration, initial pH, SCN dosage and water matrices. OTC (<= 10 mg L-1) was almost completely removed in 40 min under the conditions of an initial pH of 7.0 and a SCN dose of 1.0 g L-1, and its degradation was well described by the pseudo-first-order kinetics model. Water matrices would also influence the degradation of OTC in the system. Electron paramagnetic resonance analysis and trapping experiments confirmed that the function of the radicals for OTC removal followed the order of O-center dot(2)- > (OH)-O-center dot > h(+). Eight transformation products were determined during the degradation of OTC, it being removed through four pathways: methyl oxidization, demethylation, decarbonylation and secondary alcohol oxidation. SCN was stable in the system, as the removal efficiency of OTC was not significantly reduced even after three recycles. In addition, 55.5% of NDMA formation potential of OTC was reduced after SCN catalytic oxidation. CONCLUSIONS The results imply that the visible-light-driven SCN catalytic oxidation is an effective technology not only for the removal of OTC but also for the reduction of NDMA formation potential. (c) 2021 Society of Chemical Industry
引用
收藏
页码:1580 / 1592
页数:13
相关论文
共 43 条
[1]   Sulfur-doped g-C3N4 nanosheets with carbon vacancies: General synthesis and improved activity for simulated solar-light photocatalytic nitrogen fixation [J].
Cao, Shihai ;
Fan, Bin ;
Feng, Yanchao ;
Chen, Huan ;
Jiang, Fang ;
Wang, Xin .
CHEMICAL ENGINEERING JOURNAL, 2018, 353 :147-156
[2]   Nitrogen photofixation by ultrathin amine-functionalized graphitic carbon nitride nanosheets as a gaseous product from thermal polymerization of urea [J].
Cao, Shihai ;
Chen, Huan ;
Jiang, Fang ;
Wang, Xin .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2018, 224 :222-229
[3]   Photoproducts of tetracycline and oxytetracycline involving self-sensitized oxidation in aqueous solutions: Effects of Ca2+ and Mg2+ [J].
Chen, Yong ;
Li, Hua ;
Wang, Zongping ;
Tao, Tao ;
Hu, Chun .
JOURNAL OF ENVIRONMENTAL SCIENCES, 2011, 23 (10) :1634-1639
[4]   HOMOGENEOUS PYROLYSIS OF ACETYLACETONE AT HIGH-TEMPERATURES IN SHOCK-WAVES [J].
CHOUDHURY, TK ;
LIN, MC .
INTERNATIONAL JOURNAL OF CHEMICAL KINETICS, 1990, 22 (05) :491-504
[5]   Contribution of the Antibiotic Chloramphenicol and Its Analogues as Precursors of Dichloroacetamide and Other Disinfection Byproducts in Drinking Water [J].
Chu, Wenhai ;
Krasner, Stuart W. ;
Gao, Naiyun ;
Templeton, Michael R. ;
Yin, Daqiang .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2016, 50 (01) :388-396
[6]   Performance of a novel microwave-based treatment technology for atrazine removal and destruction: Sorbent reusability and chemical stability, and effect of water matrices [J].
Hu, Erdan ;
Hu, Yuanan ;
Cheng, Hefa .
JOURNAL OF HAZARDOUS MATERIALS, 2015, 299 :444-452
[7]   Facile synthesis of Z-scheme composite of TiO2 nanorodig-C3N4 nanosheet efficient for photocatalytic degradation of ciprofloxacin [J].
Hu, Kang ;
Li, Ruiqi ;
Ye, Chenlu ;
Wang, Anqi ;
Wei, Weiqi ;
Hu, Di ;
Qiu, Rongliang ;
Yan, Kai .
JOURNAL OF CLEANER PRODUCTION, 2020, 253
[8]  
Jiang LB, 2018, ENVIRON SCI-NANO, V5, P2604, DOI [10.1039/c8en00807h, 10.1039/C8EN00807H]
[9]   Doping of graphitic carbon nitride for photocatalysis: A reveiw [J].
Jiang, Longbo ;
Yuan, Xingzhong ;
Pan, Yang ;
Liang, Jie ;
Zeng, Guangming ;
Wu, Zhibin ;
Wang, Hou .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2017, 217 :388-406
[10]   Aqueous oxytetracycline degradation and the toxicity change of degradation compounds in photoirradiation process [J].
Jiao Shaojun ;
Meng Shourong ;
Yin Daqiang ;
Wang Lianhong ;
Chen Liangyan .
JOURNAL OF ENVIRONMENTAL SCIENCES, 2008, 20 (07) :806-813