邯郸市两座污水处理厂中磺胺类和β-内酰胺类抗生素迁移转化特征

李清雪; 刘含雨; 刘娟; 贾励瑛; 汪庆

doi:10.7524/j.issn.0254-6108.2017122704

邯郸市两座污水处理厂中磺胺类和β-内酰胺类抗生素迁移转化特征

1.
河北工程大学能源与环境工程学院, 邯郸, 056038
基金项目:
国家自然科学基金（41703088），河北省自然科学基金（D2017402109）和河北省教育厅青年基金（QN2017035）资助.

Occurrence and fate of sulfonamide and β-lactam antibiotics in wastewater treatment plants in Handan

1.
School of Energy and Environmental Engineering, Hebei University of Engineering, Handan, 056038, China
Fund Project: Supported by the National Natural Science Foundation (41703088), the Natural Science Foundation of Hebei Province (D2017402109) and the Young Scientist Foundation of Hebei Education Department (QN2017035).

摘要: 采用固相萃取-高效液相色谱法检测9种磺胺类和6种β-内酰胺类抗生素，并考察了其在两家不同处理工艺的城市污水处理厂的存在水平及迁移转化特征.结果表明，两类抗生素在污水厂进出水中浓度水平均为μg·L-1，磺胺类抗生素平均去除率达60%以上，β-内酰胺类平均去除率仅为40%左右；脱水污泥中均存在目标抗生素残留，两类抗生素含量范围分别为磺胺类ND-4.67 μg·g-1和β-内酰胺类0.15-6.68 μg·g-1.对目标抗生素进行质量平衡分析发现，磺胺类抗生素主要通过污泥吸附去除，吸附率占总去除率的74%左右；β-内酰胺类主要通过生物降解去除，两厂中吸附率仅占33.3%和17.9%.
- 抗生素 /
- 城市污水厂 /
- 迁移转化 /
- 污泥吸附 /
- 磺胺类 /
- β< /
Abstract: Occurrence and fate of 15 antibiotics, including 9 sulfonamides and 6 β-lactams in two wastewater treatment plants (WWTPs) in Handan, were investigated by using solid-phase extraction (SPE) and high performance liquid chromatography (HPLC). The results indicated that all target antibiotics were detected at μg·L-1 levels in wastewater samples. Relatively high average removal efficiencies of over 100% were observed for sulfonamides and about 40% for β-lactams. In the sludge samples, all target antibiotics were detected with the concentrations ranging from ND to 4.67 μg·g-1 for sulfonamides and from 0.15 μg·g-1 to 6.68 μg·g-1 for β-lactams, respectively. Mass balance analysis indicated that sludge adsorption was the main removal mechanism for sulfonamides, which accounted for 74% of the total removal efficiency. Biodegradation was the main removal pathway for β-lactams, and the adsorption efficiency of β-lactams were only 33.3% and 17.9% in the two WWTPs, respectively.

Key words:
antibiotics /

wastewater treatment plant /

occurrence /

sludge adsorption /

sulfonamides /

β< /

i>-lactams /

Handan

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[2] ZHOU L J, YING G G, LIU S, et al. Occurrence and fate of eleven classes of antibiotics in two typical wastewater treatment plants in South China[J]. Science of the Total Environment, 2013, 452:365-376.

[3] 罗义,周启星.抗生素抗性基因(ARGs)——一种新型环境污染物[J]. 环境科学学报,2008, 28(8):1499-1505.
LUO Y, ZHOU Q X. Antibiotic resistance genes (ARGs) as emerging pollutants[J]. Acta Scientiae Circumstantiae, 2008, 28(8):1499-1505(in Chinese).

[4] 秦丽婷,童蕾,刘慧,等.环境中磺胺类抗生素的生物降解及其抗性基因污染现状[J]. 环境化学,2016,35(5):875-883.
QIN L T, TONG L, LIU H, et al. Biodegradation of sulfonamides and the pollution characteristics of sulfonamide resistance genes in the environment[J]. Environmental Chemistry, 2016, 35(5):875-883(in Chinese).

[5] GAO X L, SHAO M F, LUO Y, et al. Airborne bacterial contaminations in typical Chinese wet market with live poultry trade[J]. Science of the Total Environment 2016, 572:681-687.

[6] NOVO A, ANDRE S, VIANA P, et al. Antibiotic resistance, antimicrobial residues and bacterial community composition in urban wastewater[J]. Water Research, 2013, 47(5):1875-1887.

[7] 苏建强, 黄福义, 朱永官. 环境抗生素抗性基因研究进展[J]. 生物多样性, 2013, 21(4):481-487.
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[8] ZHANG T, LI B. Occurrence, transformation, and fate of antibiotics in municipal wastewater treatment plants[J]. Critical Reviews in Environmental Science and Technology 2011, 41, (11):951-998.

[9] KASPRZYK-HORDERN B, DINSDALE R M, GUWY A J. The removal of pharmaceuticals, personal care products, endocrine disruptors and illicit drugs during wastewater treatment and its impact on the quality of receiving waters[J]. Water Research, 2009, 43(2-3):363-380.

[10] WANG Q, MAO D Q, LUO Y, Ionic liquid facilitates the conjugative transfer of antibiotic resistance genes mediated by plasmid RP4[J]. Environmental Science Technology, 2015, 49(14):8731-8740.

[11] GAO P, DING Y, LI H, et al. Occurrence of pharmaceuticals in amunicipal wastewater treatment plant:mass balance and removalprocesses[J]. Chemosphere, 2012, 88(1):17-24.

[12] ROYA M, MASUD Y, SIMIN N, et al. Occurrence and fate of most prescribed antibiotics in different water environments of Tehran, Iran[J]. Science of the Total Environment, 2017, 619-620:446-459.

[13] XU J, XU Y, WANG H M, et al. Occurrence of antibiotics and antibiotic resistance genes in a sewage treatment plant and its effluent-receiving river[J]. Chemosphere, 2015, 119:1379-1385.

[14] LI W H, SHI Y L, GAO L H, et al. Occurrence of antibiotics in water, sediments, aquatic plants, and animals from Baiyangdian Lake in North China[J]. Chemosphere, 2012, 89(11):1307-1315.

[15] TONG C L, ZHUO X J, GUO Y. Occurrence and risk assessment of four typical fluoroquinolone antibiotics in raw and treated sewage and in receiving waters in Hangzhou, China.[J]. Journal of Agricultural and Food Chemistry, 2011, 59(13):7303-7309.

[16] LEUNG H W, MINH T B, MURPHY M B, et al. Distribution, fate and risk assessment of antibiotics in sewage treatment plants in Hong Kong, South China[J]. Environment International, 2012, 42(1):1-9.

[17] 甘秀梅,严青,高旭,等.典型抗生素在中国西南地区某污水处理厂中的行为和归趋[J]. 环境科学, 2014, 35(5):1817-1823.
GAN X M, YAN Q, GAO X, et al. Occurrence and fate of typical antibiotics in a wastewater treatment plant in southwest China[J]. Environmental Science. 2014, 35(5):1817-1823(in Chinese).

[18] 高俊红,王兆炜,张涵瑜,等.兰州市污水处理厂中典型抗生素的污染特征研究[J].环境科学学报,2016, 36(10):3765-3773.
GAO J H, WANG Z W, ZHANG H Y, et al. Occurrence and the fate of typical antibiotics in sewage treatment plants in Lanzhou. Acta Scientiae Circumstantiae, 36(10):3765-3773(in Chinese).

[19] 万位宁,陈熹,居学海,等.固相萃取-超高效液相色谱串联质谱法同时检测禽畜粪便中多种抗生素残留[J].分析化学,2013,41(7):993-999.
WAN W N, CHEN X, JU X H, et al. Simultaneous determination of residual antibiotics in livestock manure by solid phase extraction-ultra-high performance liquid chromatography tantem mass spectrometry[J]. Chinese Journal of Analytical Chemistry, 2013, 41(7):993-999(in Chinese).

[20] NAGESWARA RAO R, VENKATESWARLU N, NARSIMHA R. Determination of antibiotics in aquatic environment by solid-phase extraction followed by liquid chromatography-electrospray ionization mass spectrometry[J]. Journal of chromatography A, 2008, 1187(1):151-164.

[21] TAMTAM F, MERCIER F, EURIN J, et al. Ultra performance liquid chromatography tandem mass spectrometry performance evaluation for analysis of antibiotics in natural waters[J]. Analytical and bioanalytical chemistry, 2009, 393(6-7):1709-1718.

[22] 陈涛,李彦文,莫测辉,等.广州污水厂磺胺和喹诺酮抗生素污染特征研究[J].环境科学与技术,2010,33(6):144-147
,180. CHEN T, LI Y W, MO C H, et al. Screening of sulfonamide and fluroquinolone antibiotics in wastewater of sewage treatment plants in Guangzhou, South China[J]. Environmental Science & Technology, 2012, 33(6):144-147,180(in Chinese).

[23] GAO L, SHI Y, LI W, et al. Occurrence of antibiotics in eight sewage treatment plants in Beijing, China[J]. Chemosphere, 2012, 86(6):665-671.

[24] BROWN K D, KULIS J, THOMSON B, et al. Occurrence of antibiotics in hospital, residential and dairy effluent, municipal wastewater and the Rio Grande in New Mexico[J]. Science of the Total Environment, 2006, 366:772-783.

[25] MIAO X, KOENIG B G, METEALFE C D. Analysis of acidic drugs in the effluents of sewage treatment plants using liquid chromatography electrospray ionization tandem mass speetrometry[J]. Chromatogr A, 2002, 952:139-147.

[26] GOBEL A, THOMSEN A, MEARDELL C S, et al. Occurrence and sorption behavior of sulfonamides, macrolides, and trimethoprim in activated sludge treatment[J]. Environ Sci Techaol, 2005, 39(11):3981-3989.

[27] GOBEL A, MEARDELL C S, JOSS A, et al. Fate of sulfonamides, macrolides, and trimethoprim in different wastewater treatment technologies[J].Sci Total Environ, 2007, 372(2):361-371.

[28] DESHPANDE A D, BAHETI K G, CHATTERJEE N R. Degradation of β-lactam antibiotics[J]. Current Science, 2004, 87(12):1684-1695.

[29] 宋淑敏,张翔宇,周佳虹,等.超高效液相色谱串联质谱法同时测定城市污水处理厂污泥中12种抗生素[J].环境化学,2017,36(9):1923-1931.
SONG S M, ZHANG X Y, ZHOU J H, et al. Simultaneous determination of 12 antibiotics in sewage sludge by ultra performance liquid chromatography-electrospray ionization tandem mass spectrometry[J]. Environmental Chemistry, 2017, 36(9):1923-1931(in Chinese).

[30] LI B, ZHANG T. Biodegradation and adsorption of antibiotics in the activated sludge process[J]. Environmental Science & Technology, 2010, 44(9):3468-3473.

[31] CHRISTIAN T, SCHNEIDER R J, FARBER H A, et al. Determination of antibiotic residues in manure, soil, and surface waters[J]. Acta Hydrochimica et Hydrobiologica, 2003, 31(1):36-44.

[32] 邵一如,席北斗,曹金玲,等.抗生素在城市污水处理系统中的分布及去除[J].环境科学与技术,2013,36(7):85-92.
SHAO Y R, XI B D, CAO J L, et al. Occurrence of antibiotics and their removal mechanism in municipal sewage treatment plants[J]. Environmental Science & Technology, 2013, 36(7):85-92(in Chinese).

[33] GE L K, CHEN J W, ZHANG S Y, et al. Photodegradation of fluoroquinolone antibiotic gatifloxacin in aqueous solutions[J]. Environmental Chemistry, 2010, 55(15):1495-1500.

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收稿日期: 2017-12-27

刊出日期: 2018-08-15

邯郸市两座污水处理厂中磺胺类和β-内酰胺类抗生素迁移转化特征

Occurrence and fate of sulfonamide and β-lactam antibiotics in wastewater treatment plants in Handan

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邯郸市两座污水处理厂中磺胺类和β-内酰胺类抗生素迁移转化特征

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Occurrence and fate of sulfonamide and β-lactam antibiotics in wastewater treatment plants in Handan

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目录

[1]	BLASER M J. Antibiotic use and its consequences for the normal microbiome[J]. Science, 2016, 352(6285):544-545.
[2]	ZHOU L J, YING G G, LIU S, et al. Occurrence and fate of eleven classes of antibiotics in two typical wastewater treatment plants in South China[J]. Science of the Total Environment, 2013, 452:365-376.
[3]	罗义,周启星.抗生素抗性基因(ARGs)——一种新型环境污染物[J]. 环境科学学报,2008, 28(8):1499-1505. LUO Y, ZHOU Q X. Antibiotic resistance genes (ARGs) as emerging pollutants[J]. Acta Scientiae Circumstantiae, 2008, 28(8):1499-1505(in Chinese).
[4]	秦丽婷,童蕾,刘慧,等.环境中磺胺类抗生素的生物降解及其抗性基因污染现状[J]. 环境化学,2016,35(5):875-883. QIN L T, TONG L, LIU H, et al. Biodegradation of sulfonamides and the pollution characteristics of sulfonamide resistance genes in the environment[J]. Environmental Chemistry, 2016, 35(5):875-883(in Chinese).
[5]	GAO X L, SHAO M F, LUO Y, et al. Airborne bacterial contaminations in typical Chinese wet market with live poultry trade[J]. Science of the Total Environment 2016, 572:681-687.
[6]	NOVO A, ANDRE S, VIANA P, et al. Antibiotic resistance, antimicrobial residues and bacterial community composition in urban wastewater[J]. Water Research, 2013, 47(5):1875-1887.
[7]	苏建强, 黄福义, 朱永官. 环境抗生素抗性基因研究进展[J]. 生物多样性, 2013, 21(4):481-487. SU J Q, HUANG F Y, ZHU Y G. Antibiotic resistance genes in the environment[J]. Biodiversity Science, 2013, 21(4):481-487(in Chinese).
[8]	ZHANG T, LI B. Occurrence, transformation, and fate of antibiotics in municipal wastewater treatment plants[J]. Critical Reviews in Environmental Science and Technology 2011, 41, (11):951-998.
[9]	KASPRZYK-HORDERN B, DINSDALE R M, GUWY A J. The removal of pharmaceuticals, personal care products, endocrine disruptors and illicit drugs during wastewater treatment and its impact on the quality of receiving waters[J]. Water Research, 2009, 43(2-3):363-380.
[10]	WANG Q, MAO D Q, LUO Y, Ionic liquid facilitates the conjugative transfer of antibiotic resistance genes mediated by plasmid RP4[J]. Environmental Science Technology, 2015, 49(14):8731-8740.
[11]	GAO P, DING Y, LI H, et al. Occurrence of pharmaceuticals in amunicipal wastewater treatment plant:mass balance and removalprocesses[J]. Chemosphere, 2012, 88(1):17-24.
[12]	ROYA M, MASUD Y, SIMIN N, et al. Occurrence and fate of most prescribed antibiotics in different water environments of Tehran, Iran[J]. Science of the Total Environment, 2017, 619-620:446-459.
[13]	XU J, XU Y, WANG H M, et al. Occurrence of antibiotics and antibiotic resistance genes in a sewage treatment plant and its effluent-receiving river[J]. Chemosphere, 2015, 119:1379-1385.
[14]	LI W H, SHI Y L, GAO L H, et al. Occurrence of antibiotics in water, sediments, aquatic plants, and animals from Baiyangdian Lake in North China[J]. Chemosphere, 2012, 89(11):1307-1315.
[15]	TONG C L, ZHUO X J, GUO Y. Occurrence and risk assessment of four typical fluoroquinolone antibiotics in raw and treated sewage and in receiving waters in Hangzhou, China.[J]. Journal of Agricultural and Food Chemistry, 2011, 59(13):7303-7309.
[16]	LEUNG H W, MINH T B, MURPHY M B, et al. Distribution, fate and risk assessment of antibiotics in sewage treatment plants in Hong Kong, South China[J]. Environment International, 2012, 42(1):1-9.
[17]	甘秀梅,严青,高旭,等.典型抗生素在中国西南地区某污水处理厂中的行为和归趋[J]. 环境科学, 2014, 35(5):1817-1823. GAN X M, YAN Q, GAO X, et al. Occurrence and fate of typical antibiotics in a wastewater treatment plant in southwest China[J]. Environmental Science. 2014, 35(5):1817-1823(in Chinese).
[18]	高俊红,王兆炜,张涵瑜,等.兰州市污水处理厂中典型抗生素的污染特征研究[J].环境科学学报,2016, 36(10):3765-3773. GAO J H, WANG Z W, ZHANG H Y, et al. Occurrence and the fate of typical antibiotics in sewage treatment plants in Lanzhou. Acta Scientiae Circumstantiae, 36(10):3765-3773(in Chinese).
[19]	万位宁,陈熹,居学海,等.固相萃取-超高效液相色谱串联质谱法同时检测禽畜粪便中多种抗生素残留[J].分析化学,2013,41(7):993-999. WAN W N, CHEN X, JU X H, et al. Simultaneous determination of residual antibiotics in livestock manure by solid phase extraction-ultra-high performance liquid chromatography tantem mass spectrometry[J]. Chinese Journal of Analytical Chemistry, 2013, 41(7):993-999(in Chinese).
[20]	NAGESWARA RAO R, VENKATESWARLU N, NARSIMHA R. Determination of antibiotics in aquatic environment by solid-phase extraction followed by liquid chromatography-electrospray ionization mass spectrometry[J]. Journal of chromatography A, 2008, 1187(1):151-164.
[21]	TAMTAM F, MERCIER F, EURIN J, et al. Ultra performance liquid chromatography tandem mass spectrometry performance evaluation for analysis of antibiotics in natural waters[J]. Analytical and bioanalytical chemistry, 2009, 393(6-7):1709-1718.
[22]	陈涛,李彦文,莫测辉,等.广州污水厂磺胺和喹诺酮抗生素污染特征研究[J].环境科学与技术,2010,33(6):144-147 ,180. CHEN T, LI Y W, MO C H, et al. Screening of sulfonamide and fluroquinolone antibiotics in wastewater of sewage treatment plants in Guangzhou, South China[J]. Environmental Science & Technology, 2012, 33(6):144-147,180(in Chinese).
[23]	GAO L, SHI Y, LI W, et al. Occurrence of antibiotics in eight sewage treatment plants in Beijing, China[J]. Chemosphere, 2012, 86(6):665-671.
[24]	BROWN K D, KULIS J, THOMSON B, et al. Occurrence of antibiotics in hospital, residential and dairy effluent, municipal wastewater and the Rio Grande in New Mexico[J]. Science of the Total Environment, 2006, 366:772-783.
[25]	MIAO X, KOENIG B G, METEALFE C D. Analysis of acidic drugs in the effluents of sewage treatment plants using liquid chromatography electrospray ionization tandem mass speetrometry[J]. Chromatogr A, 2002, 952:139-147.
[26]	GOBEL A, THOMSEN A, MEARDELL C S, et al. Occurrence and sorption behavior of sulfonamides, macrolides, and trimethoprim in activated sludge treatment[J]. Environ Sci Techaol, 2005, 39(11):3981-3989.
[27]	GOBEL A, MEARDELL C S, JOSS A, et al. Fate of sulfonamides, macrolides, and trimethoprim in different wastewater treatment technologies[J].Sci Total Environ, 2007, 372(2):361-371.
[28]	DESHPANDE A D, BAHETI K G, CHATTERJEE N R. Degradation of β-lactam antibiotics[J]. Current Science, 2004, 87(12):1684-1695.
[29]	宋淑敏,张翔宇,周佳虹,等.超高效液相色谱串联质谱法同时测定城市污水处理厂污泥中12种抗生素[J].环境化学,2017,36(9):1923-1931. SONG S M, ZHANG X Y, ZHOU J H, et al. Simultaneous determination of 12 antibiotics in sewage sludge by ultra performance liquid chromatography-electrospray ionization tandem mass spectrometry[J]. Environmental Chemistry, 2017, 36(9):1923-1931(in Chinese).
[30]	LI B, ZHANG T. Biodegradation and adsorption of antibiotics in the activated sludge process[J]. Environmental Science & Technology, 2010, 44(9):3468-3473.
[31]	CHRISTIAN T, SCHNEIDER R J, FARBER H A, et al. Determination of antibiotic residues in manure, soil, and surface waters[J]. Acta Hydrochimica et Hydrobiologica, 2003, 31(1):36-44.
[32]	邵一如,席北斗,曹金玲,等.抗生素在城市污水处理系统中的分布及去除[J].环境科学与技术,2013,36(7):85-92. SHAO Y R, XI B D, CAO J L, et al. Occurrence of antibiotics and their removal mechanism in municipal sewage treatment plants[J]. Environmental Science & Technology, 2013, 36(7):85-92(in Chinese).
[33]	GE L K, CHEN J W, ZHANG S Y, et al. Photodegradation of fluoroquinolone antibiotic gatifloxacin in aqueous solutions[J]. Environmental Chemistry, 2010, 55(15):1495-1500.