Citation: | WANG Jialin, PAN Jinwei, LIU Fei. Study on the characteristics and mechanism of antibiotic pollution in different aquifers[J]. Hydrogeology & Engineering Geology, 2024, 51(2): 13-22. doi: 10.16030/j.cnki.issn.1000-3665.202311008 |
The risk posed by antibiotics in various aquifers has attracted wide attention. This study investigated the pollution characteristics and controlling factors of antibiotics in different types of aquifers, and identified the indicator factors of antibiotic pollution in aquifers based on a total of 309 sets of samples from Songnen Plain, North China Plain, and Southwest Karst area. The concentrations of 35 antibiotics were analyzed using ultra-high-performance liquid chromatography-tandem mass spectrometry (UPLC-MS/MS). The results show that: (1) all 35 antibiotics were detected, with karst aquifers (34 types) and North China porous aquifers (32 types) mainly containing quinolones and macrolide antibiotics, while only 6 types of antibiotics, mainly erythromycin, were detected in Northeast porous aquifers. In porous aquifers, the overall pollution in Northeast China is characterized by low concentrations (median = 2.07 ng/L, detection rate = 100%), while the pollution in North China is relatively heavy (11.76 ng/L), accounting for 49% of the spatial distribution. In the karst aquifers, the antibiotic pollution is characterized by high concentrations (37.5 ng/L) and a large spatial extent (87%). (2) The characteristic differences in antibiotic pollution between karst and porous aquifers are attributed to the hydrogeological conditions (openness and permeability), while the emission intensity of antibiotics is the primary reason for the differences between porous aquifers in different regions. (3) Cluster analysis based on correlation coefficients identified the indicator factors of antibiotics in different types of aquifers. Total organic carbon (TOC) can effectively indicate the antibiotic pollution in porous aquifers, while ${\mathrm{NH}}_4^+ $ and ${\mathrm{SO}}_4^{2-} $ reveal a positive correlation between human activities and antibiotics. Groundwater property parameters are reliable indicators of antibiotic pollution in karst aquifers, with lower antibiotic concentrations observed in alkaline and oxidizing karst water. The research results can provide scientific basis for regional prevention and control of emerging organic contaminants in groundwater.
[1] | WANG Kelin,ZHANG Chunhua,CHEN Hongsong,et al. Karst landscapes of China:Patterns,ecosystem processes and services[J]. Landscape Ecology,2019,34(12):2743 − 2763. doi: 10.1007/s10980-019-00912-w |
[2] | LI Sinan,ZHAO Xiaoqing,PU Junwei,et al. Optimize and control territorial spatial functional areas to improve the ecological stability and total environment in Karst areas of Southwest China[J]. Land Use Policy,2021,100:104940. doi: 10.1016/j.landusepol.2020.104940 |
[3] | HE Keqiang,JIA Yuyue,WANG Fei,et al. Overview of karst geo-environments and karst water resources in north and south China[J]. Environmental Earth Sciences,2011,64(7):1865 − 1873. doi: 10.1007/s12665-011-0998-8 |
[4] | KALHOR K,GHASEMIZADEH R,RAJIC L,et al. Assessment of groundwater quality and remediation in Karst aquifers:A review[J]. Groundwater for Sustainable Development,2019,8:104 − 121. doi: 10.1016/j.gsd.2018.10.004 |
[5] | XIANG Shizheng,WANG Xusheng,MA Wen,et al. Response of microbial communities of Karst river water to antibiotics and microbial source tracking for antibiotics[J]. Science of the Total Environment,2020,706:135730. doi: 10.1016/j.scitotenv.2019.135730 |
[6] | FORD D,WILLIAMS P. Introduction to Karst[M]. New Zealand:Karst Hydrogeology and Geomorphology,2007:1 − 8. |
[7] | WEARY D,DOCTOR D,WEARY D J,et al. Karst in the United States:A digital map compilation and database[J]. Center for Integrated Data Analytics Wisconsin Science Center,2014. |
[8] | WHITE W B,CULVER D C,HERMAN J S,et al. Karst lands[J]. American Scientist,1995,83(5):450 − 459. |
[9] | HUANG Fuyang,ZOU Shengzhang,DENG Dongdong,et al. Antibiotics in a typical Karst river system in China:Spatiotemporal variation and environmental risks[J]. Science of the Total Environment,2019,650:1348 − 1355. doi: 10.1016/j.scitotenv.2018.09.131 |
[10] | ZOU Shengzhang,HUANG Fuyang,CHEN Liang,et al. The occurrence and distribution of antibiotics in the Karst river system in Kaiyang,Southwest China[J]. Water Science & Technology(Water Supply),2018,18(5/6):2044 − 2052. |
[11] | LAPWORTH D J,BARAN N,STUART M E,et al. Emerging organic contaminants in groundwater:A review of sources,fate and occurrence[J]. Environmental Pollution,2012,163:287 − 303. doi: 10.1016/j.envpol.2011.12.034 |
[12] | LUKAČ REBERSKI J,TERZIĆ J,MAURICE L D,et al. Emerging organic contaminants in Karst groundwater:A global level assessment[J]. Journal of Hydrology,2022,604:127242. doi: 10.1016/j.jhydrol.2021.127242 |
[13] | BEN Weiwei,PAN Xun,QIANG Zhimin. Occurrence and partition of antibiotics in the liquid and solid phases of swine wastewater from concentrated animal feeding operations in Shandong Province,China[J]. Environmental Science-Processes & Impacts,2013,15(4):870 − 875. |
[14] | CHEN Yongshan,ZHANG Haibo,LUO Yongming,et al. Occurrence and dissipation of veterinary antibiotics in two typical swine wastewater treatment systems in east China[J]. Environmental Monitoring and Assessment,2012,184(4):2205 − 2217. doi: 10.1007/s10661-011-2110-y |
[15] | JIANG Hongyou,ZHANG Dandan,XIAO Shichang,et al. Occurrence and sources of antibiotics and their metabolites in river water,WWTPs,and swine wastewater in Jiulongjiang River basin,south China[J]. Environmental Science and Pollution Research,2013,20(12):9075 − 9083. doi: 10.1007/s11356-013-1924-2 |
[16] | LI Cheng,CHEN Jiayi,WANG Jihua,et al. Occurrence of antibiotics in soils and manures from greenhouse vegetable production bases of Beijing,China and an associated risk assessment[J]. Science of the Total Environment,2015,521:101 − 107. |
[17] | WANG Yuwen,LI Yan,HU Anyi,et al. Monitoring,mass balance and fate of pharmaceuticals and personal care products in seven wastewater treatment plants in Xiamen City,China[J]. Journal of Hazardous Materials,2018,354:81 − 90. doi: 10.1016/j.jhazmat.2018.04.064 |
[18] | WEI Ruicheng,GE Feng,HUANG Siyu,et al. Occurrence of veterinary antibiotics in animal wastewater and surface water around farms in Jiangsu Province,China[J]. Chemosphere,2011,82(10):1408 − 1414. doi: 10.1016/j.chemosphere.2010.11.067 |
[19] | ZHANG Qianqian,YING Guangguo,PAN Changgui,et al. Comprehensive evaluation of antibiotics emission and fate in the river basins of China:Source analysis,multimedia modeling,and linkage to bacterial resistance[J]. Environmental Science & Technology,2015,49(11):6772 − 6782. |
[20] | WATKINSON A J,MURBY E J,COSTANZO S D. Removal of antibiotics in conventional and advanced wastewater treatment:Implications for environmental discharge and wastewater recycling[J]. Water Research,2007,41(18):4164 − 4176. doi: 10.1016/j.watres.2007.04.005 |
[21] | BALZER F,ZÜHLKE S,HANNAPPEL S. Antibiotics in groundwater under locations with high livestock density in Germany[J]. Water Science and Technology-Water Supply,2016,16(5):1361 − 1369. doi: 10.2166/ws.2016.050 |
[22] | BURKE V,RICHTER D,GRESKOWIAK J,et al. Occurrence of antibiotics in surface and groundwater of a drinking water catchment area in Germany[J]. Water Environment Research,2016,88(7):652 − 659. doi: 10.2175/106143016X14609975746604 |
[23] | SZEKERES E,CHIRIAC C M,BARICZ A,et al. Investigating antibiotics,antibiotic resistance genes,and microbial contaminants in groundwater in relation to the proximity of urban areas[J]. Environmental Pollution,2018,236:734 − 744. doi: 10.1016/j.envpol.2018.01.107 |
[24] | ZAINAB S M,JUNAID M,XU N,et al. Antibiotics and antibiotic resistant genes (ARGs) in groundwater:A global review on dissemination,sources,interactions,environmental and human health risks[J]. Water Research,2020,187:116455. doi: 10.1016/j.watres.2020.116455 |
[25] |
彭聪,巴俊杰,胡芬,等. 广西会仙岩溶湿地典型抗生素污染特征及生态风险评估[J]. 环境科学学报,2019,39(7):2207 − 2217. [PENG Cong,BA Junjie,HU Fen,et al. Typical antibiotic pollution characteristics and ecological risk assessment of Huixian Karst wetland in Guangxi,China[J]. Acta Scientiae Circumstantiae,2019,39(7):2207 − 2217. (in Chinese with English abstract)]
|
[26] | QIN Litang,PANG Xinrui,ZENG Honghu,et al. Ecological and human health risk of sulfonamides in surface water and groundwater of Huixian Karst wetland in Guilin,China[J]. Science of the Total Environment,2020,708:134552. doi: 10.1016/j.scitotenv.2019.134552 |
[27] | WANG Jialin,ZHANG Chong,XIONG Ling,et al. Changes of antibiotic occurrence and hydrochemistry in groundwater under the influence of the South-to-North Water Diversion (the Hutuo River,China)[J]. Science of the Total Environment,2022,832:154779. doi: 10.1016/j.scitotenv.2022.154779 |
[28] |
黄福杨,单婷倩,林静,等. 典型西南岩溶地下水抗生素污染指示因子识别[J/OL]. 地质科技通报,(2023-02-24)[2023-11-03] [HUANG Fuyang,SHAN Tingqian,LIN Jing,et al. Identification of indicators for antibiotic pollution in typical karst groundwater, Southwest China[J]. Bulletin of Geological Science and Technology,(2023-02-24)[2023-11-03]. https://doi.org/10.19509/j.cnki.dzkq.tb20220466. (in Chinese with English abstract)]
|
[29] |
赵兰坡,冯君,王宇,等. 松嫩平原盐碱地种稻开发的理论与技术问题[J]. 吉林农业大学学报,2012,34(3):237 − 241. [ZHAO Lanpo,FENG Jun,WANG Yu,et al. Theoretical and technological problems in the development of planting paddy in saline-alkali land of Songnen Plain[J]. Journal of Jilin Agricultural University,2012,34(3):237 − 241. (in Chinese with English abstract)]
|
[30] | HUANG Fuyang,LI Zeyan,ZHANG Chong,et al. Pesticides in the typical agricultural groundwater in Songnen Plain,northeast China:Occurrence,spatial distribution and health risks[J]. Environmental Geochemistry and Health,2019,41(6):2681 − 2695. doi: 10.1007/s10653-019-00331-5 |
[31] | FOSTER S,GARDUNO H,EVANS R,et al. Quaternary aquifer of the north China Plain:Assessing and achieving groundwater resource sustainability[J]. Hydrogeology Journal,2004,12(1):81 − 93. doi: 10.1007/s10040-003-0300-6 |
[32] | LIU Changming,YU Jingjie,KENDY E. Groundwater exploitation and its impact on the environment in the North China Plain[J]. Water International,2001,26(2):265 − 272. doi: 10.1080/02508060108686913 |
[33] | LU Yintao,TANG Changyuan,CHEN Jianyao,et al. Spatial characteristics of water quality,stable isotopes and tritium associated with groundwater flow in the Hutuo River alluvial fan plain of the North China Plain[J]. Hydrogeology Journal,2008,16(5):1003 − 1015. doi: 10.1007/s10040-008-0292-3 |
[34] | LI Zhenwei,XU Xianli,LIU Meixian,et al. State-space prediction of spring discharge in a Karst catchment in southwest China[J]. Journal of Hydrology,2017,549:264 − 276. doi: 10.1016/j.jhydrol.2017.04.001 |
[35] | XUE Qiang,QI Yinjie,LIU Fei. Ultra-high performance liquid chromatography-electrospray tandem mass spectrometry for the analysis of antibiotic residues in environmental waters[J]. Environmental Science and Pollution Research,2015,22(21):16857 − 16867. doi: 10.1007/s11356-015-4900-1 |
[36] | LINDSEY M E,MEYER T M,THURMAN E M. Analysis of trace levels of sulfonamide and tetracycline antimicrobials in groundwater and surface water using solid-phase extraction and liquid chromatography/mass spectrometry[J]. Analytical Chemistry,2001,73(19):4640 − 4646. doi: 10.1021/ac010514w |
[37] | SABRI N A,VAN HOLST S,SCHMITT H,et al. Fate of antibiotics and antibiotic resistance genes during conventional and additional treatment technologies in wastewater treatment plants[J]. Science of the Total Environment,2020,741:140199. doi: 10.1016/j.scitotenv.2020.140199 |
[38] | ZOU Hua,HE Jiangtao,HE Baonan,et al. Sensitivity assessment of denitrifying bacteria against typical antibiotics in groundwater[J]. Environmental Science-Processes & Impacts,2019,21(9):1570 − 1579. |
[39] |
张玉叶,何江涛,邓璐,等. 洛美沙星和诺氟沙星对水中生物反硝化过程的影响模拟试验[J]. 地学前缘,2022,29(5):497 − 507. [ZHANG Yuye,HE Jiangtao,DENG Lu,et al. Effects of lomefloxacin and norfloxacin on the biological water denitrification process:An experimental study[J]. Earth Science Frontiers,2022,29(5):497 − 507. (in Chinese with English abstract)]
|
[40] |
邓璐,何江涛,邹华,等. 洛美沙星对水中反硝化过程的影响模拟试验[J]. 中国环境科学,2020,40(7):2934 − 2942. [DENG Lu,HE Jiangtao,ZOU Hua,et al. Simulation experiments on effects of lomefloxacin on denitrification process in water[J]. China Environmental Science,2020,40(7):2934 − 2942. ( in Chinese with English abstract)]
|
[41] | FORD D,WILLIAMS P. Karst hydrogeology [M]. New Zealand:Karst Hydrogeology and Geomorphology,2007:103 − 144. |
[42] | GOLDSCHEIDER N,DREW D. Methods in Karst hydrogeology [M]. London:Taylor & Francis,2007:264. |
[43] | WORTHINGTON S R H,FORD D C. Self-organized permeability in carbonate aquifers[J]. Ground Water,2009,47(3):326 − 336. doi: 10.1111/j.1745-6584.2009.00551.x |
[44] | LOOS R,GAWLIK B M,LOCORO G,et al. EU-wide survey of polar organic persistent pollutants in European River waters[J]. Environmental Pollution,2009,157(2): |
[45] | ZHOU Tian,HUANG Fuyang,ZHANG Chong,et al. Effects of hydrogeochemical conditions on the distribution of pesticides in the Karst River system[J]. Environmental Science and Pollution Research,2020,27(24):30468 − 30478. doi: 10.1007/s11356-020-09262-6 |
[46] | BOY-ROURA M,MAS-PLA J,PETROVIC M,et al. Towards the understanding of antibiotic occurrence and transport in groundwater:Findings from the Baix Fluvià alluvial aquifer (NE Catalonia,Spain)[J]. Science of the Total Environment,2018,612:1387 − 1406. doi: 10.1016/j.scitotenv.2017.09.012 |
[47] | MENCIÓ A,MAS-PLA J. Assessing the influence of environmental factors on groundwater antibiotic occurrence by means of variation partitioning[J]. Water,2019,11(7). |
[48] | DZHAMALOV R G,ZLOBINA V L. Precipitation pollution effect on groundwater hydrochemical regime[J]. Environmental Geology,1995,25(1):65 − 68. doi: 10.1007/BF01061831 |
[49] | YANG Qingchun,WANG Luchen,MA Hongyun,et al. Hydrochemical characterization and pollution sources identification of groundwater in Salawusu aquifer system of Ordos Basin,China[J]. Environmental Pollution,2016,216:340 − 349. doi: 10.1016/j.envpol.2016.05.076 |
[50] | CARPENTER C M G,HELBLING D E. Widespread micropollutant monitoring in the Hudson River Estuary reveals spatiotemporal micropollutant clusters and their sources[J]. Environmental Science & Technology,2018,52(11):6187 − 6196. |
[51] | GROS M,CATALÁN N,MAS-PLA J,et al. Groundwater antibiotic pollution and its relationship with dissolved organic matter:Identification and environmental implications[J]. Environmental Pollution,2021,289:117927. doi: 10.1016/j.envpol.2021.117927 |
[52] |
王巧莲,蒋勇军,陈宇. 岩溶流域地下水 TOC 输出及影响因素分析:以重庆丰都雪玉洞地下河流域为例[J]. 环境科学,2016,37(5):1788 − 1797. [WANG Qiaolian,JIANG Yongjun,CHEN Yu. Export of total organic carbon (TOC) from Karst watershed and its influencing factors:An example from Xueyudong underground river system,Chongqing[J]. Environmental Science,2016,37(5):1788 − 1797. (in Chinese with English abstract)]
|
[53] | ZHI Dan,YANG Danxing,ZHENG Yongxin,et al. Current progress in the adsorption,transport and biodegradation of antibiotics in soil[J]. Journal of Environmental Management,2019,251:109598. doi: 10.1016/j.jenvman.2019.109598 |
[54] | INGERSLEV F,TORÄNG L,LOKE M L,et al. Primary biodegradation of veterinary antibiotics in aerobic and anaerobic surface water simulation systems[J]. Chemosphere,2001,44(4):865 − 872. doi: 10.1016/S0045-6535(00)00479-3 |
Sampling points distribution in the study area
Concentration and detection frequencies of antibiotics in differen aquifers
Cumulative concentration of antibiotics in the sampling points in different aquifers
The relationship between hydrogeological conditions and antibiotic pollution
Relationship between antibiotics and hydrochemical indices in different aquifers