Abstract
Emerging organic contaminants (EOCs) have been widely studied in landfill leachates but not in the surrounding environment of landfills. In this study, two sampling campaigns were conducted to determine 45 EOCs in landfill leachates and environmental samples near a landfill in East China. Our study focused on the seasonal occurrence and spatial distribution of the target EOCs, as well as their ecological risks. The results showed 13 out of 45 EOCs were detectable and achieved individual concentrations that ranged from 2.0 to 5080 ng/L in the landfill leachates. Most of the detected EOCs exhibited higher concentrations in the leachates collected in summer than in winter. Effective removal of the EOCs by a two-stage disc tube reverse osmosis (DTRO) system led to a significant reduction in their concentration levels (< LOQ ~ 49 ng/L) in treated leachates. Eight EOCs (< LOQ ~ 62.7 ng/L) were detected in the groundwater adjacent to the landfill and had a similar composition pattern to raw leachates. The contamination levels of the target EOCs in groundwater decreased with the distance of sampling sites from the landfill. In soil samples, the occurrence of target EOCs was not consistent with raw or treated landfill leachates. Spatially, no apparent difference in the EOC concentrations was observed in the soil nearby the landfill. Crop plants sorbed the EOCs contained in soil (< LOQ ~ 30.4 ng/L), but they were not able to bioconcentrate the contaminants in either roots or edible parts. Risk assessment suggested that the individual EOC likely posed medium to high risks to aquatic organisms in groundwater while negligible impacts to human health through consumption of vegetables. To the best of our knowledge, this is the first report on the contribution of landfill leachates to EOC contamination in both aquatic and soil environments in East China. Our findings emphasized the importance of investigating EOCs in landfill leachates and accumulative environmental risks of EOCs in the neighboring environment of landfills in China.
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References
Aydin S, Aydin ME, Ulvi A, Kilic H (2019) Antibiotics in hospital effluents: occurrence, contribution to urban wastewater, removal in a wastewater treatment plant, and environmental risk assessment. Environ Sci Pollut Res 26(1):544–558
Barnes KK, Christenson SC, Kolpin DW, Focazio MJ, Furlong ET, Zaugg SD, Meyer MT, Barber LB (2004) Pharmaceuticals and other organic waste water contaminants within a leachate plume downgradient of a municipal landfill. Groundwater Monit Remediat 24(2):119–126. https://doi.org/10.1111/j.1745-6592.2004.tb00720.x
Barron J,Boone P,Cantor-McKinney S,Chase T,Cotter P,Dixon T,Engler B,Fox R,Fox C, Graves B (1995) QA/QC guidance for sampling and analysis of sediments, water, and tissues for dredged material evaluations: chemical evaluations: Environmental Protection Agency Washington DC Office of Water
Burch KD, Han B, Pichtel J, Zubkov T (2019) Removal efficiency of commonly prescribed antibiotics via tertiary wastewater treatment. Environ Sci Pollut Res 26(7):6301–6310
Camobreco V, Ham R, Barlaz M, Repa E, Felker M, Rousseau C, Rathle J (1999) Life-cycle inventory of a modern municipal solid waste landfill. Waste Manag Res 17(6):394–408
Chen W, Xu J, Lu S, Jiao W, Wu L, Chang AC (2013) Fates and transport of PPCPs in soil receiving reclaimed water irrigation. Chemosphere 93(10):2621–2630. https://doi.org/10.1016/j.chemosphere.2013.09.088
China, N. B. o. S. o (2017) China statistical yearbook: 2017. China Statistical Press, Beijing
Christou A, Agüera A, Bayona JM, Cytryn E, Fotopoulos V, Lambropoulou D, Manaia CM, Michael C, Revitt M, Schröder P, Fatta-Kassinos D (2017) The potential implications of reclaimed wastewater reuse for irrigation on the agricultural environment: the knowns and unknowns of the fate of antibiotics and antibiotic resistant bacteria and resistance genes – a review. Water Res 123:448–467. https://doi.org/10.1016/j.watres.2017.07.004
Christou A, Papadavid G, Dalias P, Fotopoulos V, Michael C, Bayona JM, Piña B, Fatta-Kassinos D (2019) Ranking of crop plants according to their potential to uptake and accumulate contaminants of emerging concern. Environ Res 170:422–432. https://doi.org/10.1016/j.envres.2018.12.048
Clarke BO, Smith SR (2011) Review of ‘emerging’ organic contaminants in biosolids and assessment of international research priorities for the agricultural use of biosolids. Environ Int 37(1):226–247. https://doi.org/10.1016/j.envint.2010.06.004
Clarke BO, Anumol T, Barlaz M, Snyder SA (2015) Investigating landfill leachate as a source of trace organic pollutants. Chemosphere 127:269–275. https://doi.org/10.1016/j.chemosphere.2015.02.030
Couto CF, Lange LC, Amaral MCS (2019) Occurrence, fate and removal of pharmaceutically active compounds (PhACs) in water and wastewater treatment plants—a review. J Water Process Eng 32:100927. https://doi.org/10.1016/j.jwpe.2019.100927
Dodgen LK, Li J, Parker D, Gan JJ (2013) Uptake and accumulation of four PPCP/EDCs in two leafy vegetables. Environ Pollut 182:150–156. https://doi.org/10.1016/j.envpol.2013.06.038
Du J, Zhao H, Wang Y, Xie H, Zhu M, Chen J (2019) Presence and environmental risk assessment of selected antibiotics in coastal water adjacent to mariculture areas in the Bohai Sea. Ecotoxicol Environ Saf 177:117–123. https://doi.org/10.1016/j.ecoenv.2019.03.075
Eggen T, Moeder M, Arukwe A (2010) Municipal landfill leachates: a significant source for new and emerging pollutants. Sci Total Environ 408(21):5147–5157. https://doi.org/10.1016/j.scitotenv.2010.07.049
EPA, U. (1997). Exposure factors handbook. Office of research and Development, Washington, DC, 20460, 2–6
Ferrer I, Zweigenbaum JA, Thurman EM (2010) Analysis of 70 Environmental Protection Agency priority pharmaceuticals in water by EPA method 1694. J Chromatogr A 1217(36):5674–5686. https://doi.org/10.1016/j.chroma.2010.07.002
Guerra P, Kim M, Shah A, Alaee M, Smyth SA (2014) Occurrence and fate of antibiotic, analgesic/anti-inflammatory, and antifungal compounds in five wastewater treatment processes. Sci Total Environ 473-474:235–243. https://doi.org/10.1016/j.scitotenv.2013.12.008
Hamza RA, Iorhemen OT, Tay JH (2016) Occurrence, impacts and removal of emerging substances of concern from wastewater. Environ Technol Innov 5:161–175. https://doi.org/10.1016/j.eti.2016.02.003
Hernando MD, Mezcua M, Fernández-Alba AR, Barceló D (2006) Environmental risk assessment of pharmaceutical residues in wastewater effluents, surface waters and sediments. Talanta 69(2):334–342. https://doi.org/10.1016/j.talanta.2005.09.037
Huerta-Fontela M, Galceran MT, Ventura F (2011) Occurrence and removal of pharmaceuticals and hormones through drinking water treatment. Water Res 45(3):1432–1442. https://doi.org/10.1016/j.watres.2010.10.036
Kapelewska J, Kotowska U, Karpińska J, Kowalczuk D, Arciszewska A, Świrydo A (2018) Occurrence, removal, mass loading and environmental risk assessment of emerging organic contaminants in leachates, groundwaters and wastewaters. Microchem J 137:292–301. https://doi.org/10.1016/j.microc.2017.11.008
Lapworth DJ, Baran N, Stuart ME, Ward RS (2012) Emerging organic contaminants in groundwater: a review of sources, fate and occurrence. Environ Pollut 163:287–303. https://doi.org/10.1016/j.envpol.2011.12.034
Lee CO, Howe KJ, Thomson BM (2012) Ozone and biofiltration as an alternative to reverse osmosis for removing PPCPs and micropollutants from treated wastewater. Water Res 46(4):1005–1014. https://doi.org/10.1016/j.watres.2011.11.069
Li B, Zhang T, Xu Z, Fang HHP (2009) Rapid analysis of 21 antibiotics of multiple classes in municipal wastewater using ultra performance liquid chromatography-tandem mass spectrometry. Anal Chim Acta 645(1):64–72. https://doi.org/10.1016/j.aca.2009.04.042
Liu J-L, Wong M-H (2013) Pharmaceuticals and personal care products (PPCPs): a review on environmental contamination in China. Environ Int 59:208–224. https://doi.org/10.1016/j.envint.2013.06.012
Liu Y, Zhang S, Song N, Guo R, Chen M, Mai D, Yan Z, Han Z, Chen J (2017) Occurrence, distribution and sources of bisphenol analogues in a shallow Chinese freshwater lake (Taihu Lake): implications for ecological and human health risk. Sci Total Environ 599-600:1090–1098. https://doi.org/10.1016/j.scitotenv.2017.05.069
Liu X, Liang C, Liu X, Zhao F, Han C (2020) Occurrence and human health risk assessment of pharmaceuticals and personal care products in real agricultural systems with long-term reclaimed wastewater irrigation in Beijing, China. Ecotoxicol Environ Saf 190:110022. https://doi.org/10.1016/j.ecoenv.2019.110022
López-Serna R, Jurado A, Vázquez-Suñé E, Carrera J, Petrović M, Barceló D (2013) Occurrence of 95 pharmaceuticals and transformation products in urban groundwaters underlying the metropolis of Barcelona, Spain. Environ Pollut 174:305–315. https://doi.org/10.1016/j.envpol.2012.11.022
Lu M-C, Chen YY, Chiou M-R, Chen MY, Fan H-J (2016) Occurrence and treatment efficiency of pharmaceuticals in landfill leachates. Waste Manag 55:257–264. https://doi.org/10.1016/j.wasman.2016.03.029
Masoner JR, Kolpin DW, Furlong ET, Cozzarelli IM, Gray JL, Schwab EA (2014) Contaminants of emerging concern in fresh leachate from landfills in the conterminous United States. Environ Sci: Processes Impacts 16(10):2335–2354
Musson SE, Townsend TG (2009) Pharmaceutical compound content of municipal solid waste. J Hazard Mater 162(2):730–735. https://doi.org/10.1016/j.jhazmat.2008.05.089
Ojemaye CY, Petrik L (2019) Occurrences, levels and risk assessment studies of emerging pollutants (pharmaceuticals, perfluoroalkyl and endocrine disrupting compounds) in fish samples from Kalk Bay harbour, South Africa. Environ Pollut 252:562–572. https://doi.org/10.1016/j.envpol.2019.05.091
Padhye LP, Yao H, Kung’u FT, Huang C-H (2014) Year-long evaluation on the occurrence and fate of pharmaceuticals, personal care products, and endocrine disrupting chemicals in an urban drinking water treatment plant. Water Res 51:266–276. https://doi.org/10.1016/j.watres.2013.10.070
Pan M, Wong CK, Chu L (2014) Distribution of antibiotics in wastewater-irrigated soils and their accumulation in vegetable crops in the Pearl River Delta, southern China. J Agric Food Chem 62(46):11062–11069
Peng X, Ou W, Wang C, Wang Z, Huang Q, Jin J, Tan J (2014a) Occurrence and ecological potential of pharmaceuticals and personal care products in groundwater and reservoirs in the vicinity of municipal landfills in China. Sci Total Environ 490:889–898. https://doi.org/10.1016/j.scitotenv.2014.05.068
Peng X, Wang C, Zhang K, Wang Z, Huang Q, Yu Y, Ou W (2014b) Profile and behavior of antiviral drugs in aquatic environments of the Pearl River Delta, China. Sci Total Environ 466-467:755–761. https://doi.org/10.1016/j.scitotenv.2013.07.062
Prosser RS, Sibley PK (2015) Human health risk assessment of pharmaceuticals and personal care products in plant tissue due to biosolids and manure amendments, and wastewater irrigation. Environ Int 75:223–233. https://doi.org/10.1016/j.envint.2014.11.020
Qi C, Huang J, Wang B, Deng S, Wang Y, Yu G (2018) Contaminants of emerging concern in landfill leachate in China: a review. Emerg Contam 4(1):1–10. https://doi.org/10.1016/j.emcon.2018.06.001
Renou S, Givaudan JG, Poulain S, Dirassouyan F, Moulin P (2008) Landfill leachate treatment: review and opportunity. J Hazard Mater 150(3):468–493. https://doi.org/10.1016/j.jhazmat.2007.09.077
Sanderson H, Brain RA, Johnson DJ, Wilson CJ, Solomon KR (2004) Toxicity classification and evaluation of four pharmaceuticals classes: antibiotics, antineoplastics, cardiovascular, and sex hormones. Toxicology 203(1):27–40. https://doi.org/10.1016/j.tox.2004.05.015
Sarmah AK, Meyer MT, Boxall ABA (2006) A global perspective on the use, sales, exposure pathways, occurrence, fate and effects of veterinary antibiotics (VAs) in the environment. Chemosphere 65(5):725–759. https://doi.org/10.1016/j.chemosphere.2006.03.026
Sidhu H, O’Connor G, Kruse J (2019) Plant toxicity and accumulation of biosolids-borne ciprofloxacin and azithromycin. Sci Total Environ 648:1219–1226. https://doi.org/10.1016/j.scitotenv.2018.08.218
Song L, Li L, Yang S, Lan J, He H, McElmurry SP, Zhao Y (2016) Sulfamethoxazole, tetracycline and oxytetracycline and related antibiotic resistance genes in a large-scale landfill, China. Sci Total Environ 551-552:9–15. https://doi.org/10.1016/j.scitotenv.2016.02.007
Sui Q, Huang J, Deng S, Chen W, Yu G (2011) Seasonal variation in the occurrence and removal of pharmaceuticals and personal care products in different biological wastewater treatment processes. Environ Sci Technol 45(8):3341–3348. https://doi.org/10.1021/es200248d
Sui Q, Zhao W, Cao X, Lu S, Qiu Z, Gu X, Yu G (2017) Pharmaceuticals and personal care products in the leachates from a typical landfill reservoir of municipal solid waste in Shanghai, China: occurrence and removal by a full-scale membrane bioreactor. J Hazard Mater 323:99–108. https://doi.org/10.1016/j.jhazmat.2016.03.047
Sun Q, Li M, Ma C, Chen X, Xie X, Yu C-P (2016) Seasonal and spatial variations of PPCP occurrence, removal and mass loading in three wastewater treatment plants located in different urbanization areas in Xiamen, China. Environ Pollut 208:371–381. https://doi.org/10.1016/j.envpol.2015.10.003
Tsarpali V, Kamilari M, Dailianis S (2012) Seasonal alterations of landfill leachate composition and toxic potency in semi-arid regions. J Hazard Mater 233-234:163–171. https://doi.org/10.1016/j.jhazmat.2012.07.007
Wang J, Wang S (2016) Removal of pharmaceuticals and personal care products (PPCPs) from wastewater: a review. J Environ Manag 182:620–640. https://doi.org/10.1016/j.jenvman.2016.07.049
Wang W, Zhou L, Gu X, Chen H, Zeng Q, Mao Z (2018) Occurrence and distribution of antibiotics in surface water impacted by crab culturing: a case study of Lake Guchenghu, China. Environ Sci Pollut Res 25(23):22619–22628
Wu D, Huang Z, Yang K, Graham D, Xie B (2015) Relationships between antibiotics and antibiotic resistance gene levels in municipal solid waste leachates in Shanghai, China. Environ Sci Technol 49(7):4122–4128. https://doi.org/10.1021/es506081z
Yang Y, Ok YS, Kim K-H, Kwon EE, Tsang YF (2017) Occurrences and removal of pharmaceuticals and personal care products (PPCPs) in drinking water and water/sewage treatment plants: a review. Sci Total Environ 596-597:303–320. https://doi.org/10.1016/j.scitotenv.2017.04.102
Yi X, Tran NH, Yin T, He Y, Gin KY-H (2017) Removal of selected PPCPs, EDCs, and antibiotic resistance genes in landfill leachate by a full-scale constructed wetlands system. Water Res 121:46–60. https://doi.org/10.1016/j.watres.2017.05.008
You X, Wu D, Wei H, Xie B, Lu J (2018) Fluoroquinolones and β-lactam antibiotics and antibiotic resistance genes in autumn leachates of seven major municipal solid waste landfills in China. Environ Int 113:162–169. https://doi.org/10.1016/j.envint.2018.02.002
Yu D, Zheng L, Yu S (2015) Influence analysis of waste landfill in southern Jinan to groundwater quality. Shandong Land Resour 31(08):5
Yu X, Sui Q, Lyu S, Zhao W, Cao X, Wang J, Yu G (2020) Do high levels of PPCPs in landfill leachates influence the water environment in the vicinity of landfills? A case study of the largest landfill in China. Environ Int 135:105404. https://doi.org/10.1016/j.envint.2019.105404
Zhang Q-Q, Ying G-G, Pan C-G, Liu Y-S, Zhao J-L (2015) Comprehensive evaluation of antibiotics emission and fate in the river basins of China: source analysis, multimedia modeling, and linkage to bacterial resistance. Environ Sci Technol 49(11):6772–6782
Zhao R, Feng J, Yin X, Liu J, Fu W, Berendonk TU, Zhang T, Li X, Li B (2018) Antibiotic resistome in landfill leachate from different cities of China deciphered by metagenomic analysis. Water Res 134:126–139. https://doi.org/10.1016/j.watres.2018.01.063
Zhao F, Yang L, Chen L, Li S, Sun L (2019) Bioaccumulation of antibiotics in crops under long-term manure application: occurrence, biomass response and human exposure. Chemosphere 219:882–895. https://doi.org/10.1016/j.chemosphere.2018.12.076
Acknowledgments
The authors are grateful to the staff in the studied landfill for providing sampling and information survey reports.
Funding
The Special Funds for Environment Protection from Jinan Ecological Environment Bureau (20180112) financially supported the research.
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Wang, K., Reguyal, F. & Zhuang, T. Risk assessment and investigation of landfill leachate as a source of emerging organic contaminants to the surrounding environment: a case study of the largest landfill in Jinan City, China. Environ Sci Pollut Res 28, 18368–18381 (2021). https://doi.org/10.1007/s11356-020-10093-8
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DOI: https://doi.org/10.1007/s11356-020-10093-8