电子束辐照降解水体中的金霉素

Abstract
Figure/Table
References (45)
Related Citation (15)

Download: PDF (514 KB) HTML (1 KB)
Export: BibTeX | EndNote (RIS)

Abstract

The process of removing chlorotetracycline (CTC) 30mg/L in aqueous solution was preliminarily explored by electron beam irradiation (EBI). Several factors such as dose, the existence of tert-butyl alcohol under different atmosphere conditions, initial pH and inorganic salts affecting on the removal efficiency were examined. Degradation mechanism and the toxicity of degradation products were proposed through experimental data. The experiment results show that:EB irradiation can effectively remove CTC from water, and the reduction radicals play the key role; It was more effective when pH is alkaline; the presence of 0.005mol/LCO₃^2-、SO₄^2-、NO₃^- or Cl^- promotes the degradation. Ten kinds of possible degradation products and corresponding degradation pathways were deduced from the analysis of the degradation products by ultra-high performance liquid chromatography-mass spectrometry (UHPLC-MS) with the assistance of theoretical calculation results. Finally, the toxicity test of Vibrio fernuli shows that the toxicity of the irradiated intermediates increases firstly and then decrease slowly, however, it is still toxic at the absorption dose of 5.0kGy.

Key words： chlorotetracycline electron beam irradiation transformation products degradation pathways toxicity

Received: 21 July 2018

PACS:

X703

	Service

	E-mail this article
	Add to my bookshelf
	Add to citation manager
	E-mail Alert
	RSS
	Articles by authors
	XIAO Yang
	LUO Min
	MA Ling-ling
	ZHANG Yang
	XU Dian-dou
	WU Ming-hong
	XU Gang

Cite this article:

XIAO Yang,LUO Min,MA Ling-ling等. Degradation of chlorotetracycline by electron beam irradiation in aqueous solution[J]. CHINA ENVIRONMENTAL SCIENCECE, 2019, 39(2): 625-633.

URL:

http://www.zghjkx.com.cn/EN/ OR http://www.zghjkx.com.cn/EN/Y2019/V39/I2/625

[1]	Sarmah A K, Meyer M T, Boxall A B A. A global perspective on the use, sales, exposure pathways, occurrence, fate and effects of veterinary antibiotics (VAs) in the environment[J]. Chemosphere, 2006,65(5):725-759.
[2]	Collignon P, Voss A. China, what antibiotics and what volumes are used in food production animals?[J]. Antimicrob Resist Infect Control, 2015,4(1):1-4.
[3]	Liousia M, Gousia P, Conomou V, et al. Screening for antibiotic residues in swine and poultry tissues using the STAR test[J]. International Journal of Food Safety Nutrition & Public Health, 2015,Vol.5(No.2):173-183.
[4]	Sanz D, Razquin P, Condón S, et al. Incidence of antimicrobial residues in meat using a broad spectrum screening strategy[J]. European Journal of Nutrition and Food Safety, 2015,Vol.5(3):156-165.
[5]	Kumar K,Gupta S C,Chander Y,et al.Antibiotic use in agriculture and its impact on the terrestrial environment[J]. Advances in Agronomy, 2005,87(5):1-54.
[6]	Jian Z.Dynamics and mechanism of degradation of three tetracycline antibiotics from chicken feces in brown soil[J]. Acta Scientiae Circumstantiae, 2011,31(5):1039-1044.
[7]	Li X, Liu C, Chen Y, et al. Antibiotic residues in liquid manure from swine feedlot and their effects on nearby groundwater in regions of North China.[J]. Environmental Science and Pollution Research, 2018,(4):1-11.
[8]	Wang H, Wang N, Wang B, et al. Antibiotics detected in urines and adipogenesis in school children[J]. Environment International, 2016,89-90:204-211.
[9]	Liu X, Steele J C, Meng X Z. Usage, residue, and human health risk of antibiotics in Chinese aquaculture:A review[J]. Environmental Pollution, 2017,223:161-169.
[10]	Chen W R, Huang C H. Transformation kinetics and pathways of tetracycline antibiotics with manganese oxide[J]. Environmental Pollution, 2011,159(5):1092-1100.
[11]	Wang H, Yao H, Pei J, et al. Photodegradation of tetracycline antibiotics in aqueous solution by UV/ZnO[J]. Desalination and Water Treatment, 2015:1-7.
[12]	童蕾,曾梦玲,李民敬,等.铁锰氧化物对地下水环境中金霉素的降解[J]. 环境化学, 2016,35(5):917-924. Tong L, Zeng M L, Li M J, et al. Degradation of chlorotetracycline by iron and manganese oxides under simulated groundwater environment[J]. Environmental Chemistry, 2016,35(5):917-924.
[13]	Gómez-Pacheco C V, Sánchez-Polo M, Rivera-Utrilla J, et al. Tetracycline degradation in aqueous phase by ultraviolet radiation[J]. Chemical Engineering Journal, 2012,187(2):89-95.
[14]	Ji Y, Shi Y, Dong W, et al. Thermo-activated persulfate oxidation system for tetracycline antibiotics degradation in aqueous solution[J]. Chemical Engineering Journal, 2016,298(225):225-233.
[15]	林于廉,田伟,杨志敏,等.微波-Fenton对沼液中抗生素和激素的高级氧化[J]. 环境工程学报, 2013,7(1):164-168. Lin Y L, Tian W, Yang Z M, et al. Advanced oxidation of olaquindox and tetracycline antibiotics in biogas slurry by microwave-Fenton[J]. Chinese Journal of Environmental Engineering, 2013,7(1):164-168.
[16]	Lee H, Lee E, Lee C H, et al. Degradation of chlorotetracycline and bacterial disinfection in livestock wastewater by ozone-based advanced oxidation[J]. Journal of Industrial & Engineering Chemistry, 2011,17(3):468-473.
[17]	Li Z Q, Qi M Y, Tu C Y, et al. Highly efficient removal of chlorotetracycline from aqueous solution using graphene oxide/TiO2 composite:Properties and mechanism[J]. Applied Surface Science, 2017,425:765-775.
[18]	Chen W R, Huang C H. Adsorption and transformation of tetracycline antibiotics with aluminum oxide.[J]. Chemosphere, 2010,79(8):779-785.
[19]	关连珠,赵亚平,张广才,等.玉米秸秆生物质炭对外源金霉素的吸持与解吸[J]. 中国农业科学, 2012,45(24):5057-5064. Guan L Z, Zhao Y P, Zhang G C, et al. Retention and desorption of exogenous chlortetracycline (CTC) on corn-straw derived biochar[J]. Scientia Agricultura Sinica, 2012,45(24):5057-5064.
[20]	Zhang D, Niu H, Zhang X, et al. Strong adsorption of chlorotetracycline on magnetite nanoparticles[J]. Journal of Hazardous Materials, 2011, 192(3):1088.
[21]	Zhang Z, Lan H, Liu H, et al. Removal of tetracycline antibiotics from aqueous solution by amino-Fe(Ⅲ) functionalized SBA15[J]. Colloids and Surfaces A Physicochemical and Engineering Aspects, 2015, 471:133-138.
[22]	吴明红,徐刚,刘宁,等.电子束辐照处理难降解有机污染物[J]. 上海大学学报(自然科学版), 2011,17(4):549-554. Wu M H, Xu G, Liu N, et al. Radiolytic degradation of persistent organic pollutants by electron beam irradiation[J]. Journal of Shanghai University (Natural Science), 2011,17(4):549-554.
[23]	张洋,付兴明,罗敏,等.电子束辐照降解水体中磺胺间甲氧嘧啶[J]. 中国环境科学, 2018,38(7),2520-2526. Zhang Y, Fu X M, Luo M, et al. Studies on the degradation of sulfamonomethoxine by electron beam irradiation in aqueous solution[J]. China Environmental Science, 2018,38(7):2520-2526.
[24]	付兴明,罗敏,马玲玲,等.电子束辐照降解水中氧氟沙星的研究[J]. 中国环境科学, 2016,36(10):3033-3039. Fu X M, Luo M, Ma L L, et al. Studies on the degradation of ofloxacin by Electron Beam irradiation in aqueous solution[J]. China Environmental Science, 2016,36(10):3033-3039.
[25]	Buxton G V, Greenstock C L, Helman W P, et al. Critical review of rate constants for reactions of hydrated electrons, hydrogen atoms and hydroxyl radicals (·OH/·O-) in aqueous solution[J]. Journal of Physical and Chemical Reference Data, 2009,17(2):513-886.
[26]	吴彦霖,诸秀芬,赵建夫,等.羟基自由基和水合电子降解对叔丁基酚的研究[J]. 中国环境科学, 2016,36(8):2323-2328. Wu Y L, Zhu X F, Zhao J F, et al. The study on the degradation of 4-tert-butylphenol by hydroxyl radical and hydrated electron attacking[J]. China Environmental Science, 2016,36(8):2323-2328.
[27]	Cho J Y, Chung B Y, Hwang S A. Detoxification of the veterinary antibiotic chloramphenicol using electron beam irradiation[J]. Environmental Science and Pollution Research, 2015,22(13):9637-9645.
[28]	Xu G, Bu T, Wu M H, et al. Electron beam induced degradation of clopyralid in aqueous solutions[J]. Journal of Radioanalytical and Nuclear Chemistry, 2011,288(3):759-764.
[29]	Sági G, Csay T, Pátzay G, et al. Oxidative and reductive degradation of sulfamethoxazole in aqueous solutions:decomposition efficiency and toxicity assessment[J]. Journal of Radioanalytical and Nuclear Chemistry, 2014,301(2):475-482.
[30]	李硕,高乃云,邢美燕,等.紫外激活过硫酸盐技术去除水中金霉素[J]. 哈尔滨工业大学学报, 2016,48(8):96-101. Li S, Gao N Y, Xing M Y, et al. Study on the removal of chlortetracycline in water through UV-activated persulfate process[J]. Journal of Harbin Institute of Technology, 2016,48(8):96-101.
[31]	郑丽英.金霉素的水解动力学研究[J]. 广州化工, 2010,38(12):182-183. Zheng L Y. Hydrolysis kinetics of the chlortetracycline[J]. Guangzhou Chemical Industry, 2010,38(12):182-183.
[32]	Salazar-Rábago J J, Sánchez-Polo M, Rivera-Utrilla J, et al. Role of 1[O2]* in chlortetracycline degradation by solar radiation assisted by ruthenium metal complexes[J]. Chemical Engineering Journal, 2016,284:896-904.
[33]	Umschlag T, Herrmann H. The carbonate radical (HCO3·/CO3-·)as a reactive intermediate in water chemistry:kinetics and modelling[J]. CLEAN -Soil, Air, Water, 2010,27(4):214-222.
[34]	Atinault E, De Waele V, Schmidhammer U, et al. Scavenging of es-and OH rad, radicals in concentrated HCl and NaCl aqueous solutions[J]. Chemical Physics Letters, 2008,460(4):461-465.
[35]	Truong G L, Laat J D, Legube B. Effects of chloride and sulfate on the rate of oxidation of ferrous ion by H2O2[J]. Water Research, 2004, 38(9):2384-2394.
[36]	Poskrebyshev G A, Neta P, Huie R E. Equilibrium constant of the reaction·OH+HNO3·H2O+NO3. in aqueous solution[J]. Journal of Geophysical Research Atmospheres, 2001,106(D5):4995-5004.
[37]	Jeong J, Song W H, Cooper W J, et al. Degradation of tetracycline antibiotics:Mechanisms and kinetic studies for advanced oxidation/reduction processes[J]. Chemosphere, 2010,78(5):533-540.
[38]	Chen W R, Huang C H. Transformation kinetics and pathways of tetracycline antibiotics with manganese oxide.[J]. Environmental Pollution, 2011,159(5):1092-1100.
[39]	Khan M H, Jung J Y. Ozonation of chlortetracycline in the aqueous phase:Degradation intermediates and pathway confirmed by NMR[J]. Chemosphere, 2016,152:31-38.
[40]	Pulicharla R, Brar S K, Rouissi T, et al. Degradation of chlortetracycline in wastewater sludge by ultrasonication, Fenton oxidation, and ferro-sonication.[J]. Ultrasonics Sonochemistry, 2017, 34:332-342.
[41]	Halling-sørensen B, Lykkeberg A, Ingerslev F, et al. Characterisation of the abiotic degradation pathways of oxytetracyclines in soil interstitial water using LC-MS-MS.[J]. Chemosphere, 2003,50(10):1331-1342.
[42]	Chen G, Zhao L, Dong Y H. Oxidative degradation kinetics and products of chlortetracycline by manganese dioxide.[J]. Journal of Hazardous Materials, 2011,193(20):128-138.
[43]	Halling-Sørensen B, Sengeløv G, Tjørnelund J. Toxicity of Tetracyclines and Tetracycline Degradation Products to Environmentally Relevant Bacteria, Including Selected Tetracycline-Resistant Bacteria[J]. Archives of Environmental Contamination and Toxicology, 2002,42(3):263-271.
[44]	孙成华,刘保献,衡丽娜,等.发光细菌急性毒性-费氏弧菌冻干法方法建立及质控[J]. 现代科学仪器, 2014,6:155-159. Sun C H, Liu B X, Heng L N, et al. Construction of standard test program and quality control of inhibitory effect of samples on light emission of freezed-dried vibrio fischeri[J]. Modern Scientific Instruments, 2014,6:155-159.
[45]	张耀亭,白世基,张维.改进的水中痕量过氧化氢的分光光度测定法[J]. 环境与健康杂志, 2006,23(3):258-261. Zhang Y T, Bai S J, Zhang W. An improved method for determination of trace hydrogen peroxide in water[J]. Journal of Environ. Health, 2006, 23(3):258-261.