Abstract
This study investigated the occurrence, seasonal–spatial distribution characteristics, and attenuation process of 15 pharmaceuticals and personal care products (PPCPs) in riverside sections of Beiyun River of Beijing. The overall PPCP levels both in surface water and riverside groundwater were moderate on the global scale, and showed higher concentrations in the dry season mainly caused by water temperature variation. Caffeine (CF), carbamazepine (CBZ), metoprolol (MTP), N,N-diethyl-meta-toluamide (DEET), diclofenac (DF), bezafibrate (BF), and gemfibrozil (GF) were seven representative PPCPs, because the rest eight studied compounds occurred in low concentrations and less than 15% of the total concentration of PPCPs. Caffeine and bezafibrate, respectively, was the most abundant compound in surface water and riverside groundwater, with median concentrations of 3020.0 and 125.0 ng L−1. Total concentrations of PPCPs in surface water were much higher than those in the riverside groundwater spatially. Attenuation of PPCPs during riverbank filtration was largely depending on the sources, site hydrogeological conditions, and physical–chemical properties of PPCPs, also was influenced by dissolved organic matter and environmental physicochemical parameters. CF, MTP, DEET, and CBZ were potential groundwater attenuation contaminants; DF, BF, and GF were groundwater-enriched contaminants based on their removal rates. Predominant removal mechanism of PPCPs like CF was biodegradation. Attenuation simulation showed that the one-way supply between Beiyun River and riverside groundwater, and further confirmed Beiyun River, was the main source of pharmaceutical compounds in the riverside groundwater.
Similar content being viewed by others
References
Azinheira DL, Scott DT, Hession W, Hester ET (2014) Comparison of effects of inset floodplains and hyporheic exchange induced by in-stream structures on solute retention. Water Resour Res 50:6168–6190
Banzhaf S, Krein A, Scheytt T (2013) Using selected pharmaceutical compounds as indicators for surface water and groundwater interaction in the hyporheic zone of a low permeability riverbank. Hydrol Process 27:2892–2902
Bayani Cardenas M (2008) The effect of river bend morphology on flow and timescales of surface water–groundwater exchange across pointbars. J Hydrol 362:134–141
Benotti MJ, Song R, Wilson D, Snyder SA (2012) Removal of pharmaceuticals and endocrine disrupting compounds through pilot- and full-scale riverbank filtration. Water Sci Technol Water Supply 12:11
Bertelkamp C, Reungoat J, Botton S, Cornelissen E, Ghadiri E, de Jonge M, Singhal N, van der Hoek JP, Verliefde ARD (2012): Transformation of organic micropollutants during river bank filtration: laboratory versus field data. Water Pract Technol 7(4). doi:10.2166/wpt.2012.081
Bolong N, Ismail AF, Salim MR, Matsuura T (2009) A review of the effects of emerging contaminants in wastewater and options for their removal. Desalination 239:229–246
Brooks BW, Huggett DB, Boxall ABA (2009) Pharmaceuticals and personal care products: research needs for the next decade. Environ Toxicol Chem 28:2469–2472
Burke V, Treumann S, Duennbier U, Greskowiak J, Massmann G (2013) Sorption behavior of 20 wastewater originated micropollutants in groundwater—column experiments with pharmaceutical residues and industrial agents. J Contam Hydrol 154:29–41
Burke V, Greskowiak J, Asmuss T, Bremermann R, Taute T, Massmann G (2014) Temperature dependent redox zonation and attenuation of wastewater-derived organic micropollutants in the hyporheic zone. Sci Total Environ 482-483:53–61
Dai G, Wang B, Huang J, Dong R, Deng S, Yu G (2015) Occurrence and source apportionment of pharmaceuticals and personal care products in the Beiyun River of Beijing, China. Chemosphere 119:1033–1039
D’Alessio M, Yoneyama B, Ray C (2015) Fate of selected pharmaceutically active compounds during simulated riverbank filtration. Sci Total Environ 505:615–622
Del Rosario KL, Mitra S, Humphrey CP, O’Driscoll MA (2014) Detection of pharmaceuticals and other personal care products in groundwater beneath and adjacent to onsite wastewater treatment systems in a coastal plain shallow aquifer. Sci Total Environ 487:216–223
Dickenson ER, Snyder SA, Sedlak DL, Drewes JE (2011) Indicator compounds for assessment of wastewater effluent contributions to flow and water quality. Water Res 45:1199–1212
Dordio AV, Belo M, Martins Teixeira D, Palace Carvalho AJ, Dias CMB, Picó Y, Pinto AP (2011) Evaluation of carbamazepine uptake and metabolization by Typha spp., a plant with potential use in phytotreatment. Bioresour Technol 102:7827–7834
Heberer T (2002) Tracking persistent pharmaceutical residues from municipal sewage to drinking water. J Hydrol 266:175–189
Heberer T, Massmann G, Fanck B, Taute T, Dünnbier U (2008) Behaviour and redox sensitivity of antimicrobial residues during bank filtration. Chemosphere 73:451–460
Hedgespeth ML, Sapozhnikova Y, Pennington P, Clum A, Fairey A, Wirth E (2012) Pharmaceuticals and personal care products (PPCPs) in treated wastewater discharges into Charleston Harbor, South Carolina. Sci Total Environ 437:1–9
Henzler AF, Greskowiak J, Massmann G (2014) Modeling the fate of organic micropollutants during river bank filtration (Berlin, Germany). J Contam Hydrol 156:78–92
Hijosa-Valsero M, Matamoros V, Sidrach-Cardona R, Martin-Villacorta J, Becares E, Bayona JM (2010) Comprehensive assessment of the design configuration of constructed wetlands for the removal of pharmaceuticals and personal care products from urban wastewaters. Water Res 44:3669–3678
Hijosa-Valsero M, Matamoros V, Sidrach-Cardona R, Pedescoll A, Martín-Villacorta J, García J, Bayona JM, Bécares E (2011) Influence of design, physico-chemical and environmental parameters on pharmaceuticals and fragrances removal by constructed wetlands. Water Sci Technol 63:2527
Hoppe-Jones C, Oldham G, Drewes JE (2010) Attenuation of total organic carbon and unregulated trace organic chemicals in U.S. riverbank filtration systems. Water Res 44:4643–4659
Kim S-C, Carlson K (2007) Temporal and spatial trends in the occurrence of human and veterinary antibiotics in aqueous and river sediment matrices. Environ Sci Technol 41:50–57
Kolpin DW, Furlong ET, Meyer MT, Thurman EM, Zaugg SD, Barber LB, Buxton HT (2002) Pharmaceuticals, hormones, and other organic wastewater contaminants in U.S. streams, 1999−2000: a national reconnaissance. Environ Sci Technol 36:1202–1211
Kunkel U, Radke M (2008) Biodegradation of acidic pharmaceuticals in bed sediments: insight from a laboratory experiment. Environ Sci Technol 42:7273−7279. doi:10.1021/es801562j
Leenheer JA (1981) Comprehensive approach to preparative isolation and fractionation of dissolved organic carbon from natural waters and wastewaters. Environ Sci Technol 15:578–587
Li X, Zheng W, Kelly WR (2013) Occurrence and removal of pharmaceutical and hormone contaminants in rural wastewater treatment lagoons. Sci Total Environ 445-446:22–28
Li Z, Sobek A, Radke M (2016) Fate of pharmaceuticals and their transformation products in four small European rivers receiving treated wastewater. Environ Sci Technol 50:5614–5621
Lin AY, Lin CA, Tung HH, Chary NS (2010) Potential for biodegradation and sorption of acetaminophen, caffeine, propranolol and acebutolol in lab-scale aqueous environments. J Hazard Mater 183:242–250
Luo Y, Guo W, Ngo HH, Nghiem LD, Hai FI, Zhang J, Liang S, Wang XC (2014) A review on the occurrence of micropollutants in the aquatic environment and their fate and removal during wastewater treatment. Sci Total Environ 473-474:619–641
Ma R, Wang B, Yin L, Zhang Y, Deng S, Huang J, Wang Y, Yu G (2017) Characterization of pharmaceutically active compounds in Beijing, China: occurrence pattern, spatiotemporal distribution and its environmental implication. J Hazard Mater 323:147–155
MacLeod SL, Wong CS (2010) Loadings, trends, comparisons, and fate of achiral and chiral pharmaceuticals in wastewaters from urban tertiary and rural aerated lagoon treatments. Water Res 44:533–544
Madureira TV, Rocha MJ, Cruzeiro C, Galante MH, Monteiro RAF, Rocha E (2011) The toxicity potential of pharmaceuticals found in the Douro River estuary (Portugal): assessing impacts on gonadal maturation with a histopathological and stereological study of zebrafish ovary and testis after sub-acute exposures. Aquat Toxicol 105:292–299
Maoz A, Chefetz B (2010) Sorption of the pharmaceuticals carbamazepine and naproxen to dissolved organic matter: role of structural fractions. Water Res 44:981–989
Marschner B, Winkler R, JÖdemann D (2005) Factors controlling the partitioning of pyrene to dissolved organic matter extracted from different soils. Eur J Soil Sci 56:299–306
Massmann G, Greskowiak J, Dünnbier U, Zuehlke S, Knappe A, Pekdeger A (2006) The impact of variable temperatures on the redox conditions and the behaviour of pharmaceutical residues during artificial recharge. J Hydrol 328:141–156
Massmann G, Dünnbier U, Heberer T, Taute T (2008) Behaviour and redox sensitivity of pharmaceutical residues during bank filtration—investigation of residues of phenazone-type analgesics. Chemosphere 71:1476–1485
Meffe R, de Bustamante I (2014) Emerging organic contaminants in surface water and groundwater: a first overview of the situation in Italy. Sci Total Environ 481:280–295
Nham HT, Greskowiak J, Nodler K, Rahman MA, Spachos T, Rusteberg B, Massmann G, Sauter M, Licha T (2015) Modeling the transport behavior of 16 emerging organic contaminants during soil aquifer treatment. Sci Total Environ 514:450–458
Onesios KM, Yu JT, Bouwer EJ (2009) Biodegradation and removal of pharmaceuticals and personal care products in treatment systems: a review. Biodegradation 20:441–466
Pal A, Gin KY-H, Lin AY-C, Reinhard M (2010) Impacts of emerging organic contaminants on freshwater resources: review of recent occurrences, sources, fate and effects. Sci Total Environ 408:6062–6069
Patterson BM, Shackleton M, Furness AJ, Bekele E, Pearce J, Linge KL, Busetti F, Spadek T, Toze S (2011) Behaviour and fate of nine recycled water trace organics during managed aquifer recharge in an aerobic aquifer. J Contam Hydrol 122:53–62
Poiger T, Buser H-R, Müller MD (2001) Photodegradation of the pharmaceutical drug diclofenac in a lake: pathway, field measurements, and mathematical modeling. Environ Toxicol Chem 20:256–263
Rauch-Williams T, Hoppe-Jones C, Drewes JE (2010) The role of organic matter in the removal of emerging trace organic chemicals during managed aquifer recharge. Water Res 44:449–460
Ray C (2008) Worldwide potential of riverbank filtration. Clean Techn Environ Policy 10:223–225
Scheytt T, Mersmann P, Lindstädt R, Heberer T (2005) Determination of sorption coefficients of pharmaceutically active substances carbamazepine, diclofenac, and ibuprofen, in sandy sediments. Chemosphere 60:245–253
Schmidt C, Bayer-Raich M, Schirmer M (2006) Characterization of spatial heterogeneity of groundwater-stream water interactions using multiple depth streambed temperature measurements at the reach scale. Hydrol Earth Syst Sci Discuss 3:1419–1446
Schwarzenbach RP, Westall J (1981) Transport of nonpolar organic compounds from surface water to groundwater. Laboratory sorption studies. Environ Sci Technol 15:1360–1367
Schwarzenbach RP, Giger W, Hoehn E, Schneider JK (1983) Behavior of organic compounds during infiltration of river water to groundwater. Field studies. Environ Sci Technol 17:472–479
Sorensen JP, Lapworth DJ, Nkhuwa DC, Stuart ME, Gooddy DC, Bell RA, Chirwa M, Kabika J, Liemisa M, Chibesa M, Pedley S (2015) Emerging contaminants in urban groundwater sources in Africa. Water Res 72:51–63
Storck FR, Schmidt CK, Lange FT, Henson JW, Hahn K (2010) Removal and fate of EDCs and PPCPs in bank filtration systems. Project report 3136. Water Research Foundation, Denver
Sui Q, Huang J, Deng S, Yu G (2009) Rapid determination of pharmaceuticals from multiple therapeutic classes in wastewater by solid-phase extraction and ultra-performance liquid chromatography tandem mass spectrometry. Chin Sci Bull 54:4633–4643
Sui Q, Cao X, Lu S, Zhao W, Qiu Z, Yu G (2015) Occurrence, sources and fate of pharmaceuticals and personal care products in the groundwater: a review. Emerg Contam 1:14–24
Thiele-Bruhn S, Beck I-C (2005) Effects of sulfonamide and tetracycline antibiotics on soil microbial activity and microbial biomass. Chemosphere 59:457–465
Tixier C, Singer HP, Oellers S, Müller SR (2003) Occurrence and fate of carbamazepine, clofibric acid, diclofenac, ibuprofen, ketoprofen, and naproxen in surface waters. Environ Sci Technol 37:1061–1068
Veach AM, Bernot MJ (2011) Temporal variation of pharmaceuticals in an urban and agriculturally influenced stream. Sci Total Environ 409:4553–4563
Vieno NM, Tuhkanen T, Kronberg L (2005) Seasonal variation in the occurrence of pharmaceuticals in effluents from a sewage treatment plant and in the recipient water. Environ Sci Technol 39:8220–8226
Wang J, He J, Chen H (2012) Assessment of groundwater contamination risk using hazard quantification, a modified DRASTIC model and groundwater value, Beijing Plain, China. Sci Total Environ 432:216–226
Weeks JA, Guiney PD, Nikiforov AI (2012) Assessment of the environmental fate and ecotoxicity of N,N-diethyl-m-toluamide (DEET). Integr Environ Assess Manag 8:120–134
Wen F, Li J, Zuo Y, Zhou M (2010) Rapid determination of COD(Cr) in dyeing effluents. Dyeing Finishing 20:013
Yan C, Nie M, Yang Y, Zhou J, Liu M, Baalousha M, Lead JR (2015) Effect of colloids on the occurrence, distribution and photolysis of emerging organic contaminants in wastewaters. J Hazard Mater 299:241–248
Yang Y, Li G-M, Dong Y-H, Li M, Yang J-Q, Zhou D, Yang Z-S, Zheng F-D (2012) Influence of South to North Water Transfer on groundwater dynamic change in Beijing plain. Environ Earth Sci 65:1323–1331
Yu JT, Bouwer EJ, Coelhan M (2006) Occurrence and biodegradability studies of selected pharmaceuticals and personal care products in sewage effluent. Agric Water Manag 86:72–80
Zhang Y, Geißen S-U, Gal C (2008) Carbamazepine and diclofenac: removal in wastewater treatment plants and occurrence in water bodies. Chemosphere 73:1151–1161
Zheng CWPP (1999) MT3DMS: a modular three-dimensional multispecies transport model for simulation of advection, dispersion, and chemical reactions of contaminants in groundwater systems; documentation and user’s guide. Alabama Univ University, Alabama
Zhu J, Snow DD, Cassada DA, Monson SJ, Spalding RF (2001) Analysis of oxytetracycline, tetracycline, and chlortetracycline in water using solid-phase extraction and liquid chromatography–tandem mass spectrometry. J Chromatogr A 928:177–186
Acknowledgments
This research was financially supported by the Fundamental Research Funds for the Central Universities (no. 53200859462). The authors sincerely thank the staff of the Beijing Institute of Hydrogeology and Engineering Geology for their assistance with sample collections and the laboratory personnel of the South China Institute of Environmental Sciences, Ministry of Environmental Protection (MEP), for their help with the PPCP analyses.
Author information
Authors and Affiliations
Corresponding author
Additional information
Responsible editor: Ester Heath
Electronic supplementary material
ESM 1
(DOC 3577 kb)
Rights and permissions
About this article
Cite this article
Yang, L., He, JT., Su, SH. et al. Occurrence, distribution, and attenuation of pharmaceuticals and personal care products in the riverside groundwater of the Beiyun River of Beijing, China. Environ Sci Pollut Res 24, 15838–15851 (2017). https://doi.org/10.1007/s11356-017-8999-0
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11356-017-8999-0