Environmental Science and Pollution Research

, Volume 20, Issue 8, pp 5864–5875 | Cite as

Occurrence and fate of PPCPs and correlations with water quality parameters in urban riverine waters of the Pearl River Delta, South China

  • Xin Yang
  • Feng Chen
  • Fangang Meng
  • Yuanyu Xie
  • Hui Chen
  • Kyana Young
  • Wangxing Luo
  • Tingjin Ye
  • Wenjie Fu
Research Article

Abstract

The occurrence and fate of eight PPCPs was studied in river waters from upstream to downstream of the three rivers in the Pearl River Delta, China. The correlations of PPCP levels and water quality parameters were also investigated. The analytes of the highest concentrations were caffeine, acetaminophen, and ciprofloxacin. Carbamazepine and erythromycin-H2O were detected at the lowest concentrations. The highest concentrations of PPCPs were found in the Shijing River, with 865 ng/L caffeine, 339 ng/L acetaminophen, and 304 ng/L ciprofloxacin. In general, the levels of PPCPs in the Zhujiang River were higher at sites where the metropolitan city Guangzhou is located and decreased from the epicenter along the river. Low levels of PPCPs were generally found in the Beijiang River. Positive correlations were found between PPCP levels, total nitrogen, ammonium nitrogen, and cumulative fluorescence excitation-emission matrix (EEM) volume. Among the four PPCPs evaluated (caffeine, acetaminophen, ciprofloxacin, and sulfamethoxazole), caffeine had the best correlations with the correlation coefficients ranging from 0.62 to 0.98. The prediction of PPCP concentrations at specified locations can be substantially simplified.

Keywords

Pharmaceuticals Caffeine Pearl River Delta Total nitrogen Fluorescence 

Notes

Acknowledgments

We thank China's Fundamental Research Funds for the Central Universities (Project No. 11lgpy95) to financially support this study.

Supplementary material

11356_2013_1641_MOESM1_ESM.doc (1.8 mb)
ESM 1 (DOC 1820 kb)

References

  1. Andreozzi R, Raffaele M, Nicklas P (2003) Pharmaceuticals in STP effluents and their solar photodegradation in aquatic environment. Chemosphere 50(10):1319–1330CrossRefGoogle Scholar
  2. Baker A (2001) Fluorescence excitation-emission matrix characterization of some sewage-impacted rivers. Environ Sci Technol 35(5):948–953CrossRefGoogle Scholar
  3. Baker A, Spencer RGM (2004) Characterization of dissolved organic matter from source to sea using fluorescence and absorbance spectroscopy. Sci Total Environ 333(1–3):217–232CrossRefGoogle Scholar
  4. Baker DR, Kasprzyk-Hordern B (2011) Multi-residue analysis of drugs of abuse in wastewater and surface water by solid-phase extraction and liquid chromatography-positive electrospray ionisation tandem mass spectrometry. J Chromatography A 1218(12):1620–1631CrossRefGoogle Scholar
  5. Benotti MJ, Trenholm RA, Vanderford BJ, Holady JC, Stanford BD, Snyder SA (2009) Pharmaceuticals and endocrine disrupting compounds in U.S. drinking water. Environ Sci Technol 43(3):597–603CrossRefGoogle Scholar
  6. Buerge IJ, Poiger T, Muller MD, Buser HR (2003) Caffeine, an anthropogenic marker for wastewater contamination of surface waters. Environ Sci Technol 37(4):691–700CrossRefGoogle Scholar
  7. Cardoza LA, Knapp CW, Larive CK, Belden JB, Lydy M, Graham DW (2005) Factors affecting the fate of ciprofloxacin in aquatic field systems. Water Air Soil Poll 161(1–4):383–398CrossRefGoogle Scholar
  8. Castiglioni S, Pomati F, Miller K, Burns BP, Zuccato E, Calamari D, Neilan BA (2008) Novel homologs of the multiple resistance regulator marA in antibiotic-contaminated environments. Water Res 42(16):4271–4280CrossRefGoogle Scholar
  9. Chen W, Westerhoff P, Leenheer JA, Booksh K (2003) Fluorescence excitation-emission matrix regional integration to quantify spectra for dissolved organic matter. Environ Sci Technol 37(24):5701–5710CrossRefGoogle Scholar
  10. Chinese-NEPA (1997) Water and wastewater monitoring methods. Environmental Science Publishing House, Beijing (In Chinese)Google Scholar
  11. Costanzo SD, Watkinson AJ, Murby EJ, Kolpin DW, Sandstrom MW (2007) Is there a risk associated with the insect repellent DEET (N, N-diethyl-m-toluamide) commonly found in aquatic environments? Sci Total Environ 384(1–3):214–220CrossRefGoogle Scholar
  12. Diaz-Cruz MS, Garcia-Galan MJ, Barcelo D (2008) Highly sensitive simultaneous determination of sulfonamide antibiotics and one metabolite in environmental waters by liquid chromatography-quadrupole linear ion trap-mass spectrometry. J Chromatogr A 1193(1–2):50–59Google Scholar
  13. Ehlers LJ, Luthy RG (2003) Are veterinary medicines causing environmental risks? Environ Sci Technol 37:286A–294ACrossRefGoogle Scholar
  14. EPA C (2002) Environmental quality standards for surface water (Chinese). GB 3838–2002. Beijing (In Chinese)Google Scholar
  15. Fenech C, Rock L, Nolan K, Tobin J, Morrissey A (2012) The potential for a suite of isotope and chemical markers to differentiate sources of nitrate contamination: a review. Water Res 46(7):2023–2041CrossRefGoogle Scholar
  16. Focazio MJ, Kolpin DW, Barnes KK, Furlong ET, Meyer MT, Zaugg SD, Barber LB, Thurman ME (2008) A national reconnaissance for pharmaceuticals and other organic wastewater contaminants in the United States—II) untreated drinking water sources. Sci Total Environ 402(2–3):201–216CrossRefGoogle Scholar
  17. Fono LJ, Kolodziej EP, Sedlak DL (2006) Attenuation of wastewater-derived contaminants in an effluent-dominated river. Environ Sci Technol 40(23):7257Google Scholar
  18. Galapate RP, Baes AU, Ito K, Mukai T, Shoto E, Okada M (1998) Detection of domestic wastes in Kurose river using synchronous fluorescence spectroscopy. Water Res 32(7):2232–2239CrossRefGoogle Scholar
  19. Gobel A, McArdell CS, Joss A, Siegrist H, Giger W (2007) Fate of sulfonamides, macrolides, and trimethoprim in different wastewater treatment technologies. Sci Total Environ 372(2–3):361–371CrossRefGoogle Scholar
  20. Golet EM, Xifra I, Siegrist H, Alder AC, Giger W (2003) Environmental exposure assessment of fluoroquinolone antibacterial agents from sewage to soil. Environ Sci Technol 37(15):3243–3249CrossRefGoogle Scholar
  21. Henderson RK, Baker A, Murphy KR, Hambly A, Stuetz RM, Khan SJ (2009) Fluorescence as a potential monitoring tool for recycled water systems: a review. Water Res 43(4):863–881CrossRefGoogle Scholar
  22. Hendriks AJ, Maas-Diepeveen JL, Noordsij A, Van der Gaag MA (1994) Monitoring response of XAD-concentrated water in the rhine delta: a major part of the toxic compounds remains unidentified. Water Res 28(3):581–598CrossRefGoogle Scholar
  23. Hirsch R, Ternes TA, Haberer K, Mehlich A, Ballwanz F, Kratz K-L (1998) Determination of antibiotics in different water compartments via liquid chromatography-electrospray tandem mass spectrometry. J Chromatogr A 815(2):213–223CrossRefGoogle Scholar
  24. Hudson N, Baker A, Ward D, Reynolds DM, Brunsdon C, Carliell-Marquet C, Browning S (2008) Can fluorescence spectrometry be used as a surrogate for the Biochemical Oxygen Demand (BOD) test in water quality assessment? An example from South West England. Sci Total Environ 391(1):149–158CrossRefGoogle Scholar
  25. Johnson AC, Jurgens MD, Williams RJ, Kummerer K, Kortenkamp A, Sumpter JP (2008) Do cytotoxic chemotherapy drugs discharged into rivers pose a risk to the environment and human health? An overview and UK case study. J Hydrol 348(1–2):167–175CrossRefGoogle Scholar
  26. Joss A, Keller E, Alder AC, Gobel A, McArdell CS, Ternes T, Siegrist H (2005) Removal of pharmaceuticals and fragrances in biological wastewater treatment. Water Res 39(14):3139–3152CrossRefGoogle Scholar
  27. Karthikeyan KG, Meyer MT (2006) Occurrence of antibiotics in wastewater treatment facilities in Wisconsin, USA. Sci Total Environ 361(1–3):196–207CrossRefGoogle Scholar
  28. Kasprzyk-Hordern B, Dinsdale RM, Guwy AJ (2008) The occurrence of pharmaceuticals, personal care products, endocrine disruptors and illicit drugs in surface water in South Wales, UK. Water Res 42(13):3498–3518CrossRefGoogle Scholar
  29. Kasprzyk-Hordern B, Dinsdale RM, Guwy AJ (2009) The removal of pharmaceuticals, personal care products, endocrine disruptors and illicit drugs during wastewater treatment and its impact on the quality of receiving waters. Water Res 43(2):363–380CrossRefGoogle Scholar
  30. Kim SD, Cho J, Kim IS, Vanderford BJ, Snyder SA (2007) Occurrence and removal of pharmaceuticals and endocrine disruptors in South Korean surface, drinking, and waste waters. Water Res 41(5):1013–1021CrossRefGoogle Scholar
  31. Kleywegt S, Pileggi V, Yang P, Hao C, Zhao X, Rocks C, Thach S, Cheung P, Whitehead B (2011) Pharmaceuticals, hormones and bisphenol A in untreated source and finished drinking water in Ontario, Canada—occurrence and treatment efficiency. Sci Total Environ 409(8):1481–1488CrossRefGoogle Scholar
  32. 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(6):1202–1211CrossRefGoogle Scholar
  33. Kummerer K (2003) Significance of antibiotics in the environment. J Antimicrob Chemother 52(1):5–7CrossRefGoogle Scholar
  34. Kunkel U, Radke M (2012) Fate of pharmaceuticals in rivers: Deriving a benchmark dataset at favorable attenuation conditions. Water Res 46(17):5551–5565Google Scholar
  35. Lange R, Hutchinson TH, Croudace CP, Siegmund F, Schweinfurth H, Hampe P, Panter GH, Sumpter JP (2001) Effects of the synthetic estrogen 17R-ethinylestradiol over the life-cycle of the fat head minnow (Pimephales promelas). Environ Toxicol Chem 20:1216–1227Google Scholar
  36. Lin AY-C, Lin C-A, Tung H-H, Chary NS (2010) Potential for biodegradation and sorption of acetaminophen, caffeine, propranolol and acebutolol in lab-scale aqueous environments. J Hazard Mater 183(1–3):242–250CrossRefGoogle Scholar
  37. Luo JH (2002) On water pollution of Shijing River in Guangzhou and its influence on the drinking water source (in Chinese). Chongqing Environ Sci 24(5):70–72 (In Chinese)Google Scholar
  38. Nageswara Rao R, Venkateswarlu N, Narsimha R (2008) Determination of antibiotics in aquatic environment by solid-phase extraction followed by liquid chromatography-electrospray ionization mass spectrometry. J Chromatogr A 1187(1–2):151–164Google Scholar
  39. Oaks JL, Gilbert M, Virani MZ, Watson RT, Meteyer CU, Rideout BA, Shivaprasad HL, Ahmed S, Iqbal Chaudhry MJ, Arshad M, Mahmood S, Ali A, Ahmed Khan A (2004) Diclofenac residues as the cause of vulture population decline in Pakistan. Nature 427(6975):630–633CrossRefGoogle Scholar
  40. Oppenheimer J, Stephenson R, Burbano A, Liu L (2007) Characterizing the passage of personal care products through wastewater treatment processes. Water Environ Res 79:2564–2577CrossRefGoogle Scholar
  41. Peeler KA, Opsahl SP, Chanton JP (2006) Tracking anthropogenic inputs using caffeine, indicator bacteria, and nutrients in rural freshwater and urban marine systems. Environ Sci Technol 40(24):7616–7622CrossRefGoogle Scholar
  42. Peng X, Yu Y, Tang C, Tan J, Huang Q, Wang Z (2008) Occurrence of steroid estrogens, endocrine-disrupting phenols, and acid pharmaceutical residues in urban riverine water of the Pearl River Delta, South China. Sci Total Environ 397(1–3):158–166CrossRefGoogle Scholar
  43. Sedlak DL, Huang CH, Pinkston K (2004) Strategies for selecting pharmaceuticals to assess attenuation during indirect potable water reuse. In: Kummerer K (ed) Pharmaceuticals in the Environment: Sources, Fate, Effects and Risks. Berlin, Heidelberg, New York: Springer, pp 107–120Google Scholar
  44. Simonich SL, Federle TW, Eckhoff WS, Rottiers A, Webb S, Sabaliunas D, Wolf WD (2002) Removal of fragrance materials during U.S. and European wastewater treatment. Environ Sci Technol 36:2839–2847CrossRefGoogle Scholar
  45. Stackelberg PE, Gibs J, Furlong ET, Meyer MT, Zaugg SD, Lippincott RL (2007) Efficiency of conventional drinking-water-treatment processes in removal of pharmaceuticals and other organic compounds. Sci Total Environ 377(2–3):255–272CrossRefGoogle Scholar
  46. Stedmon CA, Seredyriska-Sobecka B, Boe-Hansen R, Le Tallec N, Waul CK, Arvin E (2011) A potential approach for monitoring drinking water quality from groundwater systems using organic matter fluorescence as an early warning for contamination events. Water Res 45(18):6030–6038CrossRefGoogle Scholar
  47. Suarez S, Carballa M, Omil F, Lema JM (2008) How are pharmaceutical and personal care products (PPCPs) removed from urban wastewaters? Rev Environ Sci Biotechnol 7:125–138CrossRefGoogle Scholar
  48. Sui Q, Huang J, Deng S, Yu G, Fan Q (2010) Occurrence and removal of pharmaceuticals, caffeine and DEET in wastewater treatment plants of Beijing, China. Water Res 44(2):417–426CrossRefGoogle Scholar
  49. Ternes TA (1998) Occurrence of drugs in German sewage treatment plants and rivers. Water Res 32(11):3245–3260CrossRefGoogle Scholar
  50. Ternes TA, Joss A, Siegrist H (2004) Scrutinizing pharmaceuticals and personal care products in wastewater treatment. Environ Sci Technol 38:392A–399ACrossRefGoogle Scholar
  51. Thomas PM, Foster GD (2005) Tracking acidic pharmaceuticals, caffeine, and triclosan through the wastewater treatment process. Environ Toxicol Chem 24:25–30Google Scholar
  52. Vanderford BJ, Pearson RA, Rexing DJ, Snyder SA (2003) Analysis of endocrine disruptors, pharmaceuticals, and personal care products in water using liquid chromatography/tandem mass spectrometry. Anal Chem 75(22):6265–6274CrossRefGoogle Scholar
  53. Vieno NM, Harkki H, Tuhkanen T, Kronberg L (2007) Occurrence of pharmaceuticals in river water and their elimination in a pilot-scale drinking water treatment plant. Environ Sci Technol 41(14):5077–5084CrossRefGoogle Scholar
  54. Voogt P, Janex-Habibi ML, Sacher F, Puijker L, Mons M (2008) Development of a Common Priority List of Pharmaceuticals Relevant for the Water Cycle. Paper presented at the IWA World Water Congress and Exhibition, Vienna, Austria, September 7–12Google Scholar
  55. Wang C, Shi H, Adams CD, Gamagedara S, Stayton I, Timmons T, Ma Y (2011) Investigation of pharmaceuticals in Missouri natural and drinking water using high performance liquid chromatography-tandem mass spectrometry. Water Res 45(4):1818–1828CrossRefGoogle Scholar
  56. Watkinson AJ, Murby EJ, Kolpin DW, Costanzo SD (2009) The occurrence of antibiotics in an urban watershed: from wastewater to drinking water. Sci Total Environ 407(8):2711–2723CrossRefGoogle Scholar
  57. Weigela S, Bergerb U, Jensenc E, Kallenbornb R, Thoresenc H, Hühnerfuss H (2004) Determination of selected pharmaceuticals and caffeine in sewage and seawater from Tromsø/Norway with emphasis on ibuprofen and its metabolites. Chemosphere 56(6):583–592CrossRefGoogle Scholar
  58. Wiegel S, Aulinger A, Brockmeyer R, Harms H, Loffler J, Reincke H, Schmidt R, Stachel B, von Tumpling W, Wanke A (2004) Pharmaceuticals in the river Elbe and its tributaries. Chemosphere 57(2):107–126CrossRefGoogle Scholar
  59. Withka J, Moncuse P, Baziotis A, Maskiewicz R (1987) Use of high-performance size-exclusion, ion-exchange, and hydrophobic interaction chromatography for the measurement of protein conformational change and stability. J Chromatogr A 398:175–202CrossRefGoogle Scholar
  60. Xu B, Mao D, Luo Y, Xu L (2011) Sulfamethoxazole biodegradation and biotransformation in the water-sediment system of a natural river. Bioresour Technol 102(14):7069–7076CrossRefGoogle Scholar
  61. Xu W, Zhang G, Li X, Zou S, Li P, Hu Z, Li J (2007) Occurrence and elimination of antibiotics at four sewage treatment plants in the Pearl River Delta (PRD), South China. Water Res 41(19):4526–4534CrossRefGoogle Scholar
  62. Yang X, Flowers RC, Weinberg HS, Singer PC (2011) Occurrence and removal of pharmaceuticals and personal care products (PPCPs) in an advanced wastewater reclamation plant. Water Res 45(16):5218–5228CrossRefGoogle Scholar
  63. Ye Z, Weinberg HS, Meyer MT (2007) Trace analysis of trimethoprim and sulfonamide, macrolide, quinolone, and tetracycline antibiotics in chlorinated drinking water using liquid chromatography electrospray tandem mass spectrometry. Anal Chem 79(3):1135–1144CrossRefGoogle Scholar
  64. Young TA, Heidler J, Matos-Perez CR, Sapkota A, Toler T, Gibson KE, Schwab KJ, Halden RU (2008) Ab initio and in situ comparison of caffeine, triclosan, and triclocarban as indicators of sewage-derived microbes in surface waters. Environ Sci Technol 42(9):3335–3340CrossRefGoogle Scholar

Copyright information

© Springer-Verlag Berlin Heidelberg 2013

Authors and Affiliations

  • Xin Yang
    • 1
    • 2
  • Feng Chen
    • 3
  • Fangang Meng
    • 1
    • 2
  • Yuanyu Xie
    • 1
    • 2
  • Hui Chen
    • 1
    • 2
  • Kyana Young
    • 4
  • Wangxing Luo
    • 3
  • Tingjin Ye
    • 3
  • Wenjie Fu
    • 1
    • 2
  1. 1.Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation TechnologyGuangzhouChina
  2. 2.SYSU-HKUST Research Center for Innovative Environmental Technology (SHRCIET), School of Environmental Science and EngineeringSun Yat-sen UniversityGuangzhouChina
  3. 3.Foshan Water GroupFoshanChina
  4. 4.Department of Environmental EngineeringUniversity of WisconsinMadisonUSA

Personalised recommendations