Skip to main content
SpringerLink
Log in

Source-specific sewage pollution detection in urban river waters using pharmaceuticals and personal care products as molecular indicators

  • Research Article
  • Published:
Environmental Science and Pollution Research Aims and scope Submit manuscript

Abstract

Source-specific elucidation of domestic sewage pollution caused by various effluent sources in an urban river water, as conducted for this study, demands knowledge of the relation between concentrations of pharmaceuticals and personal care products (PPCPs) as molecular indicators (caffeine, carbamazepine, triclosan) and water quality concentrations of total nitrogen (T-N) and total phosphorous (T-P). River water and wastewater samples from the Asahikawa River Basin in northern Japan were analyzed using derivatization-gas chromatography/mass spectrometry. Caffeine, used as an indicator of domestic sewage in the Asahikawa River Basin, was more ubiquitous than either carbamazepine or triclosan (92–100 %). Its concentration was higher than any target compound used to assess the basin: <4.4–370 ng/L for caffeine, <0.6–3.9 ng/L for carbamazepine, and <1.1–13 ng/L for triclosan. Higher caffeine concentrations detected in wastewater effluents and the strongly positive mutual linear correlation between caffeine and T-N or T-P (R 2 > 0.759) reflect the contribution of septic tank system effluents to the lower Asahikawa River Basin. Results of relative molecular indicators in combination with different molecular indicators (caffeine/carbamazepine and triclosan/carbamazepine) and cluster analysis better reflect the contribution of sewage than results obtained using concentrations of respective molecular indicators and cluster analysis. Relative molecular indicators used with water quality parameters (e.g., caffeine/T-N ratio) in this study provide results more clearly, relatively, and quantitatively than results obtained using molecular indicators alone. Moreover, the caffeine/T-N ratio reflects variations of caffeine flux from effluent sources. These results suggest strongly relative molecular indicators are also useful indicators, reflecting differences in spatial contributions of domestic sources for PPCPs in urban areas.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7

Similar content being viewed by others

References

  • Akita City (2011.3.) The Sixth Akita City Comprehensive Master Plan, Department of Land Development, Akita City Planning Division. http://www.city.akita.akita.jp/city/ur/im/keikaku/6thmasterplan/default.htm. Accessed 20 August 2015 (in Japanese)

  • Alonso SG, Catalá M, Maroto RR, Gil JLR, Miguel ÁGD, Valcárcel Y (2010) Pollution by psychoactive pharmaceuticals in the rivers of Madrid metropolitan area (Spain). Environ Int 36:195–201

    Article  Google Scholar 

  • Bendz D, Paxéus NA, Ginn TR, Loge FJ (2005) Occurrence and fate of pharmaceutically active compounds in the environment, a case study: Höje River in Sweden. J Hazard Mater 122:195–204

    Article  CAS  Google Scholar 

  • Bernot MJ, Smith L, Frey J (2013) Human and veterinary pharmaceutical abundance and transport in a rural central Indiana stream influenced by confined animal feeding operations (CAFOs). Sci Total Environ 445–446:219–230

    Article  Google Scholar 

  • Boyd GR, Palmeri JM, Zhan S, Grimm DA (2004) Pharmaceuticals and personal care products (PPCPs) and endocrine disrupting chemicals (EDCs) in stormwater canals and Bayou St John in New Orleans, Louisiana, USA. Sci Total Environ 333:137–148

    Article  CAS  Google Scholar 

  • Buerge IJ, Poiger T, Müller MD, Buser HR (2003) Caffeine, an anthropogenic marker for wastewater contamination of surface waters. Environ Sci Technol 37(4):691–700

    Article  CAS  Google Scholar 

  • Carrara C, Ptacek CJ, Robertson W, Blowes DW, Moncur MC, Sverko E, Backus S (2008) Fate of pharmaceutical and trace organic compounds in three septic system plumes, Ontario, Canada. Environ Sci Technol 42(8):2805–2811

    Article  CAS  Google Scholar 

  • Choi K, Kim Y, Park J, Park CK, Kim MY, Kim HS, Kim P (2008) Seasonal variations of several pharmaceutical residues in surface water and sewage treatment plants of Han River, Korea. Sci Total Environ 405:120–128

    Article  CAS  Google Scholar 

  • Cody K (2010) Pharmaceuticals & personal care products and on-site systems Ontario Rural Wastewater Centre, Newsletters & Factsheets. http://www.uoguelph.ca/orwc/Resources/newsletters.html. Accessed 20 August 2015

  • Ellis JB (2006) Pharmaceutical and personal care products (PPCPs) in urban receiving waters. Environ Pollut 144:184–189

    Article  CAS  Google Scholar 

  • Gardinali PR, Zhao X (2002) Trace determination of caffeine in surface water samples by liquid chromatography—atmospheric pressure chemical ionization—mass spectrometry (LC–APCI–MS). Environ Int 28:521–528

    Article  CAS  Google Scholar 

  • Glassmeyer ST, Furlong ET, Kolpin DW, Cahill JD, Zaugg SD, Werner SL, Meyer MT, Kryak DD (2005) Transport of chemical and microbial compounds from known wastewater discharges: potential for use as indicators of human fecal contamination. Environ Sci Technol 39(14):5157–5169

    Article  CAS  Google Scholar 

  • Hernando MD, Mezcua M, Fernandez-Alba AR, Barcelo D (2006) Environmental risk assessment of pharmaceutical residues in wastewater effluents, surface waters and sediments. Talanta 69(2):334–342

    Article  CAS  Google Scholar 

  • Hua W, Bennett ER, Letcher RJ (2005) Triclosan in waste and surface waters from the upper Detroit River by liquid chromatography-electrospray-tandem quadrupole mass spectrometry. Environ Int 31:621–630

    Article  CAS  Google Scholar 

  • Jjemba PK (2006) Excretion and ecotoxicity of pharmaceutical and personal care products in the environment. Ecotoxicol Environ Saf 63:113–130

    Article  CAS  Google Scholar 

  • Kim J-W, Jang H-S, Kim J-G, Ishibashi H, Hirano M, Nasu K, Ichikawa N, Takao Y, Shinohara R, Arizono K (2009) Occurrence of pharmaceutical and personal care products (PPCPs) in surface water from Mankyung River, South Korea. J Health Sci 55(2):249–258

    Article  CAS  Google Scholar 

  • Kim SD, Cho J, Kim IS, Vanderford BJ, Snyder SH (2007) Occurrence and removal of pharmaceuticals and endocrine disruptors in South Korean surface, drinking, and waste waters. Water Res 41:1013–1021

    Article  CAS  Google Scholar 

  • Kobayashi Y, Okuda T, Yamashita N, Tanaka H, Tanaka S, Fujii S, Konishi C, Houwa I (2006) The occurrence of pharmaceuticals during advanced wastewater treatment. Environ Eng Res 43:65–72 in Japanese

    Google Scholar 

  • Kolpin DW, Furlong ET, Meyer MT, Thurman ET, Zaugg SD, Barber LB, Buxton HT (2002) Pharmaceuticals, hormones, and other organic wastewater contaminants in the US. Streams, 1999–2000: a National Reconnaissance. Environ Sci Technol 36(6):1202–1211

  • Komori K, Suzuki Y (2009) Occurrence of pharmaceuticals and their Enviromental risk assessment of urban streams whose basins have different wastewater treatment conditions. J Jpn Soc Water Environ 32(3):133–138 in Japanese

    Article  CAS  Google Scholar 

  • Kuster M, López de Alda MJ, Hernando MD, Petrovic M, Martín-Alonso J, Barceló D (2008) Analysis and occurrence of pharmaceuticals, estrogens, progestogens and polar pesticides in sewage treatment plant effluents, river water and drinking water in the Llobregat River Basin (Barcelona, Spain). J Hydrol 358(1–2):112–123

    Article  CAS  Google Scholar 

  • Lishman L, Smyth SA, Sarafin K, Sonya Kleywegt S, Toito J, Peart T, Lee B, Servos M, Beland M, Seto P (2006) Occurrence and reductions of pharmaceuticals and personal care products and estrogens by municipal wastewater treatment plants in Ontario, Canada. Sci Total Environ 367:544–558

    Article  CAS  Google Scholar 

  • López-Serna R, Petrović M, Barceló D (2012) Occurrence and distribution of multi-class pharmaceuticals and their active metabolites and transformation products in the Ebro River basin (NE Spain). Sci Total Environ 440:280–289

    Article  Google Scholar 

  • Miao X-S, Metcalfe CD (2003) Determination of carbamazepine and its metabolites in aqueous samples using liquid chromatography–electrospray tandem mass spectrometry. Anal Chem 75(15):3731–3738

    Article  CAS  Google Scholar 

  • Ministry of Environment, Government of Japan (2009.3.) Preliminary assessment (seventh survey) of environmental risks of chemical substances. http://www.env.go.jp/chemi/report/h21-01/index.html. Accessed 20 August 2015 (in Japanese)

  • Ministry of Land, Infrastructure, Transport and Tourism, Government of Japan (2007) Summary of nationwide survey of pharmaceuticals in major Japanese rivers. Accessed 10 August 2010. site now discontinued. (in Japanese)

  • Moldovan Z (2006) Occurrences of pharmaceutical and personal care products as micropollutants in rivers from Romania. Chemosphere 64(11):1808–1817

    Article  CAS  Google Scholar 

  • Murata A, Takada H, Mutoh K, Hosoda H, Harada A, Nakada N (2011) Nationwide monitoring of selected antibiotics: distribution and sources of sulfonamides, trimethoprim, and macrolides in Japanese rivers. Sci Total Environ 409:5305–5312

    Article  CAS  Google Scholar 

  • Nakada N, Kiri K, Shinohara H, Harada A, Kuroda K, Takizawa S, Takada H (2008) Evaluation of pharmaceuticals and personal care products as water-soluble molecular markers of sewage. Environ Sci Technol 42(17):6347–6353

    Article  CAS  Google Scholar 

  • Nakada N, Komori K, Suzuki Y, Konishi C, Houwa I, Tanaka H (2007) Occurrence of 70 pharmaceutical and personal care products in Tone River basin in Japan. Water Sci Technol 56(12):133–140

    Article  CAS  Google Scholar 

  • Nakada N, Tanishima T, Shinohara H, Kiri K, Takada H (2006) Pharmaceutical chemicals and endocrine disrupters in municipal wastewater in Tokyo and their removal during activated sludge treatment. Water Res 40(17):3297–3303

    Article  CAS  Google Scholar 

  • Nishi I, Kawakami T, Onodera S (2008) Monitoring of triclosan in the surface water of the Tone Canal, Japan. Bull Environ Contam Toxicol 80:163–166

    Article  CAS  Google Scholar 

  • Public Works Research Institute, Ministry of Land, Infrastructure and Transport (2012) FY2011 annual report of wastewater management and water quality control. 95–100 (in Japanese)

  • Rabiet M, Togola A, Brissaud F, Seidel JL, Budzinski H, Elbaz-Poulichet F (2006) Consequences of treated water recycling as regards pharmaceuticals and drugs in surface and ground waters of a medium-sized Mediterranean catchment. Environ Sci Technol 40(17):5282–5288

    Article  CAS  Google Scholar 

  • Ramaswamy BR, Shanmugam G, Velu G, Rengarajan B, Larsson DG (2011) GC–MS analysis and ecotoxicological risk assessment of triclosan, carbamazepine and parabens in Indian rivers. J Hazard Mater 186(2–3):1586–1593

    Article  CAS  Google Scholar 

  • Richardson BJ, Lam PKS, Martin M (2005) Emerging chemicals of concern: pharmaceuticals and personal care products (PPCPs) in Asia, with particular reference to southern China. Mar Pollut Bull 50:913–920

    Article  CAS  Google Scholar 

  • Sabaliunasa D, Webb SF, Hauk A, Jacob M, Eckhoff WS (2003) Environmental fate of triclosan in the River Aire Basin, UK. Water Res 37:3145–3154

    Article  Google Scholar 

  • Seiler RL, Zaugg SD, Thomas JM, Howcroft DL (1999) Caffeine and pharmaceuticals as indicators of waste water contamination in wells. Ground Water 37:405–410

    Article  CAS  Google Scholar 

  • Shala L, Foster GD (2010) Surface water concentrations and loading budgets of pharmaceuticals and other domestic-use chemicals in an urban watershed (Washington, DC, USA). Arch Environ Contam Toxicol 58(3):551–561

    Article  CAS  Google Scholar 

  • Shimizu A, Takada H, Koike T, Takeshita A, Saha M, Rinawati NN, Murata A, Suzuki T, Suzuki S, Chiem NH, Tuyen BC, Viet PH, Siringan MA, Kwan C, Zakaria MP, Reungsang A (2013) Ubiquitous occurrence of sulfonamides in tropical Asian waters. Sci Total Environ 452–453:108–115

    Article  Google Scholar 

  • Sim WJ, Lee JW, Oh JE (2010) Occurrence and fate of pharmaceuticals in wastewater treatment plants and rivers in Korea. Environ Pollut 158(5):1938–1947

    Article  CAS  Google Scholar 

  • Singh PS, Azua A, Chaudhary A, Khan S, Willett KL, Gardinali PR (2010) Occurrence and distribution of steroids, hormones and selected pharmaceuticals in South Florida coastal environments. Ecotoxicology 19:338–350

    Article  CAS  Google Scholar 

  • Sosiak A, Hebben T (2005) A preliminary survey of pharmaceuticals and endocrine disrupting compounds in treated municipal wastewaters and receiving rivers of Alberta. Alberta Environ. http://environment.gov.ab.ca/info/listing.asp. Accessed 20 August 2015

  • Tixier C, Singer HP, Canonica S, Müller SR (2002) Phototransformation of triclosan in surface waters: a relevant elimination process for this widely used biocide laboratory studies, field measurements, and modeling. Environ Sci Technol 36(16):3482–3489

    Article  CAS  Google Scholar 

  • UNEP (2013) UNEP rear book emerging issues in our global environment. http://www.unep.org/yearbook/2013/. Accessed 20 August 2015

  • U. S. Environmental Protection Agency (2000) Decentralized systems technology fact sheet aerobic treatment. Municipal Technology Branch, U.S. EPA. http://water.epa.gov/infrastructure/septic/factsheets.cfm. Accessed 20 August 2015

  • Veach AM, Bernot MJ (2011) Temporal variation of pharmaceuticals in an urban and agriculturally influenced stream. Sci Total Environ 409(21):4553–4563

    Article  CAS  Google Scholar 

  • Weigel S, Kallenborn R, Hühnerfuss H (2004) Simultaneous solid-phase extraction of acidic, neutral and basic pharmaceuticals from aqueous samples at ambient (neutral) pH and their determination by gas chromatography—mass spectrometry. J Chromatogr A 1023:183–195

    Article  CAS  Google Scholar 

  • Wu C, Huang X, Witter JD, Spongberg AL, Wang K, Wang D, Liu J (2014) Occurrence of pharmaceuticals and personal care products and associated environmental risks in the central and lower Yangtze River, China. Ecotoxicol Environ Saf 106:19–26

    Article  CAS  Google Scholar 

  • Yang X, Chen F, Meng F, Xie Y, Chen H, Young K, Luo W, Ye T, Fu W (2013) Occurrence and fate of PPCPs and correlations with water quality parameters in urban riverine waters of the Pearl River Delta, South China. Environ Sci Pollut Res Int 20(8):5864–5875

    Article  CAS  Google Scholar 

  • Ying GG, Kookana RS (2007) Triclosan in wastewaters and biosolids from Australian wastewater treatment plants. Environ Int 33(2):199–205

    Article  CAS  Google Scholar 

  • Zhao JL, Ying GG, Liu YS, Chen F, Yang JF, Wang L (2010) Occurrence and risks of triclosan and triclocarban in the Pearl River system, South China: from source to the receiving environment. J Hazard Mater 179(1–3):215–222

    Article  CAS  Google Scholar 

Download references

Author information

Authors and Affiliations

  1. Faculty of Bioresource Sciences, Akita Prefectural Univ., 241-438 Kaidobata-nishi, Shimoshinjo-nakano, Akita, 010-0195, Japan

    Osamu Kiguchi

  2. Graduate School of BioResource Science, Akita Pref. Univ., 241-438 Kaidobata-nishi, Shimoshinjo-nakano, Akita, 010-0195, Japan

    Go Sato

  3. Akita Research Center for Public Health and Environment, 6-6 Senshu-kubotacho, Akita, 010-0874, Japan

    Takashi Kobayashi

Authors
  1. Osamu Kiguchi
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Go Sato
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Takashi Kobayashi
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Osamu Kiguchi.

Additional information

Responsible Editor: Kenneth Mei Yee Leung

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Kiguchi, O., Sato, G. & Kobayashi, T. Source-specific sewage pollution detection in urban river waters using pharmaceuticals and personal care products as molecular indicators. Environ Sci Pollut Res 23, 22513–22529 (2016). https://doi.org/10.1007/s11356-016-7437-z

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-016-7437-z

Keywords

Search

Navigation