Abstract:Antibiotic contamination in groundwater has been concerned in recent years. Due to the trace-level concentration of antibiotics, the processes for sampling, extraction and detection are highly required. The diffusive gradients in thin films (DGT) is used to establish the in situ enrichment sampling method of antibiotics in groundwater, and antibiotics such as sulfonamides, quinolones, tetracyclines and macrolides are successfully enriched. Besides, the ultra-high performance liquid chromatogrphy tandem mass spectrometry (UPLC-MS/MS) is applied for the detection method of 26 typical antibiotics in groundwater, with optimized extraction conditions. The results show that the sampling and testing methods have good enrichment effect and detection sensitivity for analysis of antibiotics in groundwater. The appropriate in-situ enrichment sampling time of groundwater is 20-30 d, with instrument detection limit of 0.002-0.074 ng/L, average recovery of 47.7%-94.6% and precision of 4.45%-10.84%. The in situ enrichment sampling method of antibiotics in groundwater through DGT is simple and can be used for trace analysis of antibiotics in groundwater combined with UPLC-MS/MS.
张泽宇, 王鑫, 李丽君, 马健生. 薄膜梯度扩散(DGT)-UPLC-MS/MS法测量地下水中26种抗生素[J]. 地质与资源, 2022, 31(2): 235-242.
ZHANG Ze-yu, WANG Xin, LI Li-jun, MA Jian-sheng. DETERMINATION OF 26 ANTIBIOTICS IN GROUNDWATER BY DIFFUSIVE GRADIENTS IN THIN FILMS TECHNIQUE COMBINED WITH UPLC-MS/MS. GEOLOGY AND RESOURCES, 2022, 31(2): 235-242.
Tong L, Yao L L, Liu H, et al. Review on the environmental behavior and ecological effect of antibiotics in groundwater system[J]. Asian Journal of Ecotoxicology, 2016, 11(2):27-36.童蕾,姚林林,刘慧,等.抗生素在地下水系统中的环境行为及生态效应研究进展[J].生态毒理学报, 2016, 11(2):27-36.
[2]
Gao L H, Shi Y L, Li W H, et al. Environmental behavior and impacts of antibiotics[J]. Environmental Chemistry, 2013, 32(9):1619-1633.高立红,史亚利,厉文辉,等.抗生素环境行为及其环境效应研究进展[J].环境化学, 2013, 32(9):1619-1633.
[3]
Yang C Q, Wang L X, Hou X H, et al. Analysis of pollution levels of 16 antibiotics in the river water of Daliao River water system[J]. Chinese Journal of Chromatography, 2012, 30(8):756-762.杨常青,王龙星,侯晓虹,等.大辽河水系河水中16种抗生素的污染水平分析[J].色谱, 2012, 30(8):756-762.
[4]
Chen W P, Peng C W, Yang Y, et al. Distribution characteristics and risk analysis of antibiotic in the groundwater in Beijing[J]. Environmental Science, 2017, 38(12):5074-5080.陈卫平,彭程伟,杨阳,等.北京市地下水中典型抗生素分布特征与潜在风险[J].环境科学, 2017, 38(12):5074-5080.
[5]
Zhang Q, Xin Q, Zhu J M, et al. The antibiotic contaminations in the main water bodies in China and the associated environmental and human health impacts[J]. Environmental Chemistry, 2014, 33(7):1075-1083.章强,辛琦,朱静敏,等.中国主要水域抗生素污染现状及其生态环境效应研究进展[J].环境化学, 2014, 33(7):1075-1083.
[6]
Guo X Y, Wang N, Hao L J, et al. Simultaneous detection of 25 kinds of veterinary antibiotics in soil, manure and water samples using liquid chromatography-tandem mass spectrometry[J]. Chinese Journal of Analytical Chemistry, 2015, 43(1):13-20.郭欣妍,王娜,郝利君,等.超高效液相色谱/串联质谱法同时测定水、土壤及粪便中25种抗生素[J].分析化学, 2015, 43(1):13-20.
[7]
Pan M, Chu L M. Transfer of antibiotics from wastewater or animal manure to soil and edible crops[J]. Environmental Pollution, 2017, 231:829-836.
[8]
Chen G L, Su F, Wu G Y. Review on the pollution and risk assessment of antibiotics in the groundwater system in China[J]. Guangdong Chemical Industry, 2018, 45(3):111-113.陈桂淋,苏帆,武广元.我国地下水抗生素污染及风险评估研究进展[J].广东化工, 2018, 45(3):111-113.
[9]
Wang X G, Guo C L, He H Y, et al. Study on the classification of groundwater depression cone[J]. Geology and Resources, 2019, 28(5):487-492.王晓光,郭常来,何海洋,等.地下水降落漏斗分类研究[J].地质与资源, 2019, 28(5):487-492.
[10]
Qi Y J, Liu F. Analysis of antibiotics in groundwater:a review[J]. Rock and Mineral Analysis, 2014, 33(1):1-11.祁彦洁,刘菲.地下水中抗生素污染检测分析研究进展[J].岩矿测试, 2014, 33(1):1-11.
[11]
Zhang J, Luo Y, Pan M M, et al. Analysis of sulfonamide, tetracycline and quinolones antibiotics in surface water[J]. Environmental Monitoring in China, 2013, 29(4):111-115.张俊,罗阳,潘曼曼,等.水体中磺胺、四环素、喹诺酮类抗生素检测方法[J].中国环境监测, 2013, 29(4):111-115.
[12]
Zhang J, Zong D L, Chang A M, et al. Determination of common antibiotics in aquatic environment by solid-phase extraction and ultra pressure liquid chromatography-tandem mass spectrometry (UPLC-MS/MS)[J]. Environmental Chemistry, 2015, 34(8):1446-1452.张金,宗栋良,常爱敏,等.水环境中典型抗生素SPE-UPLC-MS/MS检测方法的建立[J].环境化学, 2015, 34(8):1446-1452.
[13]
Kim C, Ryu H D, Chung E G, et al. A review of analytical procedures for the simultaneous determination of medically important veterinary antibiotics in environmental water:Sample preparation, liquid chromatography, and mass spectrometry[J]. Journal of Environmental Management, 2018, 217:629-645.
[14]
Sun Q, Xu L, Ding S M, et al. Environmental influences on the measurement of dissolved arsenic using Zr-oxide DGT[J]. China Environmental Science, 2016, 36(5):1482-1490.孙琴,徐律,丁士明,等.薄膜扩散梯度技术测量砷的影响因素及其应用[J].中国环境科学, 2016, 36(5):1482-1490.
[15]
Wang Y P, Guan Q W, Li C, et al. A study of in situ synchronous measurement of available phosphorus and sulfur in the sediments of lake Chaohu by diffusive gradients in thin films (DGT)[J]. Acta Scientiae Circumstantiae, 2015, 35(8):2512-2518.王艳平,关庆伟,李超,等.巢湖沉积物有效态磷与硫的DGT原位同步分析研究[J].环境科学学报, 2015, 35(8):2512-2518.
[16]
Chen C E, Zhang H, Jones K C. A novel passive water sampler for in situ sampling of antibiotics[J]. Journal of Environmental Monitoring, 2012, 14(6):1523-1530.
[17]
Song Z T, Zhao Y J, Zhou Q W, et al. Effects of soil porosity on available Cd content extracted by DGT[J]. Chinese Agricultural Science Bulletin, 2016, 32(12):139-144.宋志廷,赵玉杰,周其文,等.不同土壤孔隙度对DGT提取Cd有效态含量的影响研究[J].中国农学通报, 2016, 32(12):139-144.
[18]
Rong N, Zhu J L, Zhou D K, et al. A study of synchronous measurement of phosphorous, iron and sulfur in the sediment of malodorous black rivers by diffusive gradients in thin films (DGT)[J]. Acta Scientiae Circumstantiae, 2018, 38(7):2599-2606.荣楠,朱家亮,周道坤,等.黑臭河流沉积物磷、铁、硫的DGT同步分析研究[J].环境科学学报, 2018, 38(7):2599-2606.
[19]
Chen C E, Zhang H, Ying G G, et al. Evidence and recommendations to support the use of a novel passive water sampler to quantify antibiotics in wastewaters[J]. Environmental Science& Technology, 2013, 47(23):13587-13593.
[20]
Chen W, Li Y Y, Chen C E, et al. DGT passive sampling for quantitative in situ measurements of compounds from household and personal care products in waters[J]. Environmental Science& Technology, 2017, 51(22):13274-13281.