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Comparison of emerging contaminants in receiving waters downstream of a conventional wastewater treatment plant and a forest-water reuse system

Abstract

Forest-water reuse (FWR) systems treat municipal, industrial, and agricultural wastewaters via land application to forest soils. Previous studies have shown that both large-scale conventional wastewater treatment plants (WWTPs) and FWR systems do not completely remove many contaminants of emerging concern (CECs) before release of treated wastewater. To better characterize CECs and potential for increased implementation of FWR systems, FWR systems need to be directly compared to conventional WWTPs. In this study, both a quantitative, targeted analysis and a nontargeted analysis were utilized to better understand how CECs release to waterways from an FWR system compared to a conventional treatment system. Quantitatively, greater concentrations and total mass load of CECs was exhibited downstream of the conventional WWTP compared to the FWR. Average summed concentrations of 33 targeted CECs downstream of the conventional system were ~ 1000 ng/L and downstream of the FWR were ~ 30 ng/L. From a nontargeted chemical standpoint, more tentatively identified chemicals were present, and at a greater relative abundance, downstream of the conventional system as well. Frequently occurring contaminants included phthalates, pharmaceuticals, and industrial chemicals. These data indicate that FWR systems represent a sustainable wastewater treatment alternative and that emerging contaminant release to waterways was lower at a FWR system than a conventional WWTP.

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References

  • Aalizadeh R, Thomaidis NS, Bletsou AA, Gago-Ferrero P (2016) Quantitative structure–retention relationship models to support nontarget high-resolution mass spectrometric screening of emerging contaminants in environmental samples. J Chem Inf Model 56:1384–1398. https://doi.org/10.1021/acs.jcim.5b00752

    CAS  Article  Google Scholar 

  • Agüera A, Martínez Bueno MJ, Fernández-Alba AR (2013) New trends in the analytical determination of emerging contaminants and their transformation products in environmental waters. Environ Sci Pollut Res 20:3496–3515. https://doi.org/10.1007/s11356-013-1586-0

    Article  Google Scholar 

  • Bade R, Bijlsma L, Miller TH, Barron LP, Sancho JV, Hernández F (2015) Suspect screening of large numbers of emerging contaminants in environmental waters using artificial neural networks for chromatographic retention time prediction and high resolution mass spectrometry data analysis. Sci Total Environ 538:934–941

    CAS  Article  Google Scholar 

  • Bartelt-Hunt SL, Snow DD, Damon T, Shockley J, Hoagland K (2009) The occurrence of illicit and therapeutic pharmaceuticals in wastewater effluent and surface waters in Nebraska. Environ Pollut 157:786–791. https://doi.org/10.1016/j.envpol.2008.11.025

    CAS  Article  Google Scholar 

  • Birch AL, Nichols EG, James AL, Emanuel RE (2016) Hydrologic impacts of municipal wastewater irrigation to a temperate forest watershed. J Environ Qual. https://doi.org/10.2134/jeq2015.11.0577

  • Blaženović I et al (2017) Comprehensive comparison of in silico MS/MS fragmentation tools of the CASMI contest: database boosting is needed to achieve 93% accuracy. J Cheminform 9:32

    Article  Google Scholar 

  • Bourgin M et al (2018) Evaluation of a full-scale wastewater treatment plant upgraded with ozonation and biological post-treatments: abatement of micropollutants, formation of transformation products and oxidation by-products. Water Res 129:486–498. https://doi.org/10.1016/j.watres.2017.10.036

    CAS  Article  Google Scholar 

  • Braatz S, Kandiah A (1996) The use of municipal waste water for forest and tree irrigation. Food and Agriculture Organization of the United Nations. http://www.fao.org/docrep/w0312e/w0312e09.htm. Accessed 02/11/2016

  • Bradley PM et al (2017) Expanded target-chemical analysis reveals extensive mixed-organic-contaminant exposure in U.S. streams. Environ Sci Technol 51:4792–4802. https://doi.org/10.1021/acs.est.7b00012

    CAS  Article  Google Scholar 

  • Bringolf RB, Heltsley RM, Newton TJ, Eads CB, Fraley SJ, Shea D, Cope WG (2010) Environmental occurrence and reproductive effects of the pharmaceutical fluoxetine in native freshwater mussels. Environ Toxicol Chem 29:1311–1318

    CAS  Google Scholar 

  • Brooks BW et al (2003) Waterborne and sediment toxicity of fluoxetine to select organisms. Chemosphere 52:135–142. https://doi.org/10.1016/S0045-6535(03)00103-6

    CAS  Article  Google Scholar 

  • Crites RW (1984) Land use of wastewater and sludge. Environ Sci Technol 18:140A–147A. https://doi.org/10.1021/es00123a712

    CAS  Article  Google Scholar 

  • Crites RW, Middlebrooks EJ, Bastian RK (2014) Natural wastewater treatment systems. CRC Press, Boca Raton

    Book  Google Scholar 

  • Ebele AJ, Abou-Elwafa Abdallah M, Harrad S (2017) Pharmaceuticals and personal care products (PPCPs) in the freshwater aquatic environment. Emerg Contam 3:1–16. https://doi.org/10.1016/j.emcon.2016.12.004

    Article  Google Scholar 

  • Fairbairn DJ et al (2016) Contaminants of emerging concern: Mass balance and comparison of wastewater effluent and upstream sources in a mixed-use watershed. Environ Sci Technol 50:36–45. https://doi.org/10.1021/acs.est.5b03109

    CAS  Article  Google Scholar 

  • Fent K, Weston AA, Caminada D (2006) Ecotoxicology of human pharmaceuticals. Aquat Toxicol 76:122–159. https://doi.org/10.1016/j.aquatox.2005.09.009

    CAS  Article  Google Scholar 

  • Fick J, Söderström H, Lindberg RH, Phan C, Tysklind M, Larsson DGJ (2009) Contamination of surface, ground, and drinking water from pharmaceutical production. Environ Toxicol Chem 28:2522–2527. https://doi.org/10.1897/09-073.1

    CAS  Article  Google Scholar 

  • Gao P, Munir M, Xagoraraki I (2012) Correlation of tetracycline and sulfonamide antibiotics with corresponding resistance genes and resistant bacteria in a conventional municipal wastewater treatment plant. Sci Total Environ 421–422:173–183. https://doi.org/10.1016/j.scitotenv.2012.01.061

    Article  Google Scholar 

  • Gatica J, Cytryn E (2013) Impact of treated wastewater irrigation on antibiotic resistance in the soil microbiome. Environ Sci Pollut Res 20:3529–3538. https://doi.org/10.1007/s11356-013-1505-4

    CAS  Article  Google Scholar 

  • Hirsch R, Ternes T, Haberer K, Kratz K-L (1999) Occurrence of antibiotics in the aquatic environment. Sci Total Environ 225:109–118. https://doi.org/10.1016/S0048-9697(98)00337-4

    CAS  Article  Google Scholar 

  • Hug C, Ulrich N, Schulze T, Brack W, Krauss M (2014) Identification of novel micropollutants in wastewater by a combination of suspect and nontarget screening. Environ Pollut 184:25–32. https://doi.org/10.1016/j.envpol.2013.07.048

    CAS  Article  Google Scholar 

  • Hughes SR, Kay P, Brown LE (2012) Global synthesis and critical evaluation of pharmaceutical data sets collected from river systems. Environ Sci Technol 47:661–677

    Article  Google Scholar 

  • Hutchins SR, Tomson MB, Bedient PB, Ward CH, Wilson JT (1985) Fate of trace organics during land application of municipal wastewater. Crit Rev Environ Sci Technol 15:355–416

    CAS  Google Scholar 

  • Ingram KT, Dow K, Carter L, Anderson J (2013) Climate of the Southeast United States: variability, change, impacts, and vulnerability. Springer, Berlin

    Book  Google Scholar 

  • Isosaari P, Hermanowicz SW, Rubin Y (2010) Sustainable natural systems for treatment and disposal of food processing wastewater. Crit Rev Environ Sci Technol 40:662–697

    Article  Google Scholar 

  • 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 42:3498–3518

    CAS  Article  Google Scholar 

  • 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 43:363–380. https://doi.org/10.1016/j.watres.2008.10.047

    CAS  Article  Google Scholar 

  • 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

    CAS  Article  Google Scholar 

  • Krauss M, Singer H, Hollender J (2010) LC–high resolution MS in environmental analysis: from target screening to the identification of unknowns. Anal Bioanal Chem 397:943–951. https://doi.org/10.1007/s00216-010-3608-9

    CAS  Article  Google Scholar 

  • Little J, Williams A, Pshenichnov A, Tkachenko V (2012) Identification of known unknowns utilizing accurate mass data and ChemSpider. J Am Soc Mass Spectrom 23. https://doi.org/10.1007/s13361-011-0265-y

  • Loos R et al (2013) EU-wide monitoring survey on emerging polar organic contaminants in wastewater treatment plant effluents. Water Res 47:6475–6487. https://doi.org/10.1016/j.watres.2013.08.024

    CAS  Article  Google Scholar 

  • Loraine GA, Pettigrove ME (2006) Seasonal variations in concentrations of pharmaceuticals and personal care products in drinking water and reclaimed wastewater in Southern California. Environ Sci Technol 40:687–695. https://doi.org/10.1021/es051380x

    CAS  Article  Google Scholar 

  • Luna TO, Plautz SC, Salice CJ (2013) Effects of 17α-ethynylestradiol, fluoxetine, and the mixture on life history traits and population growth rates in a freshwater gastropod. Environ Toxicol Chem

  • Luo Y et al (2014) A review on the occurrence of micropollutants in the aquatic environment and their fate and removal during wastewater treatment. Sci Total Environ 473:619–641. https://doi.org/10.1016/j.scitotenv.2013.12.065

    Article  Google Scholar 

  • Martínez Bueno MJ, Agüera A, Gómez MJ, Hernando MD, García-Reyes JF, Fernández-Alba AR (2007) Application of liquid chromatography/quadrupole-linear ion trap mass spectrometry and time-of-flight mass spectrometry to the determination of pharmaceuticals and related contaminants in wastewater. Anal Chem 79:9372–9384

    Article  Google Scholar 

  • McEachran AD, Shea D, Bodnar W, Nichols EG (2016) Pharmaceutical occurrence in groundwater and surface waters in forests land-applied with municipal wastewater. Environ Toxicol Chem 35:898–905. https://doi.org/10.1002/etc.3216

    CAS  Article  Google Scholar 

  • McEachran AD, Shea D, Nichols EG (2017a) Pharmaceuticals in a temperate forest-water reuse system. Sci Total Environ 581–582:705–714. https://doi.org/10.1016/j.scitotenv.2016.12.185

    Article  Google Scholar 

  • McEachran AD, Sobus JR, Williams AJ (2017b) Identifying known unknowns using the US EPA’s CompTox Chemistry Dashboard. Anal Bioanal Chem 409:1729–1735. https://doi.org/10.1007/s00216-016-0139-z

    CAS  Article  Google Scholar 

  • McEachran AD, Mansouri K, Newton SR, Beverly BEJ, Sobus JR, Williams AJ (2018) A comparison of three liquid chromatography (LC) retention time prediction models. Talanta. https://doi.org/10.1016/j.talanta.2018.01.022

  • Merel S, Nikiforov A, Snyder S (2014) Monitoring DEET in Water: Fundamental Study to Evaluate the Plausibility of Mimics. Environmental Analysis Techniques Workshop, pp 18-19

  • Metcalfe CD, Chu S, Judt C, Li H, Oakes KD, Servos MR, Andrews DM (2010) Antidepressants and their metabolites in municipal wastewater, and downstream exposure in an urban watershed. Environ Toxicol Chem 29:79–89. https://doi.org/10.1002/etc.27

    CAS  Article  Google Scholar 

  • Newton SR, McMahen RL, Sobus JR, Mansouri K, Williams AJ, McEachran AD, Strynar MJ (2018) Suspect screening and non-targeted analysis of drinking water using point-of-use filters. Environ Pollut 234:297–306. https://doi.org/10.1016/j.envpol.2017.11.033

    CAS  Article  Google Scholar 

  • Nichols EG (2016) Current and future opportunities for forest land application systems of wastewater. In: Ansari AA, Gill SS, Gill R, Lanza GR, Newman L (ed) Phytoremediation Management of Environmental Contaminants, Vol III

  • Péry ARR et al (2008) Fluoxetine effects assessment on the life cycle of aquatic invertebrates. Chemosphere 73:300–304. https://doi.org/10.1016/j.chemosphere.2008.06.029

    Article  Google Scholar 

  • Petrie B, Barden R, Kasprzyk-Hordern B (2015) A review on emerging contaminants in wastewaters and the environment: Current knowledge, understudied areas and recommendations for future monitoring. Water Res 72:3–27. https://doi.org/10.1016/j.watres.2014.08.053

    CAS  Article  Google Scholar 

  • Pound CE, Crites RW (1973) Wastewater treatment and reuse by land application, vol 1. Office of Research and Development, US Environmental Protection Agency, Washington, DC

    Google Scholar 

  • Quesnel D, Nakhla G (2005) Characterization and treatability of aerobic bacterial thermophilically treated wastewater by a conventional activated sludge and granular activated carbon. Water Res 39:677–687. https://doi.org/10.1016/j.watres.2004.11.010

    CAS  Article  Google Scholar 

  • Quinn B, Gagné F, Blaise C (2008) An investigation into the acute and chronic toxicity of eleven pharmaceuticals (and their solvents) found in wastewater effluent on the cnidarian, Hydra attenuata. Sci Total Environ 389:306–314. https://doi.org/10.1016/j.scitotenv.2007.08.038

    CAS  Article  Google Scholar 

  • Rager JE et al (2016) Linking high resolution mass spectrometry data with exposure and toxicity forecasts to advance high-throughput environmental monitoring. Environ Int 88. https://doi.org/10.1016/j.envint.2015.12.008

  • Richard AM, Williams CR (2002) Distributed structure-searchable toxicity (DSSTox) public database network: a proposal. Mutat Res Fundam Mol Mech Mutagen 499(1):27–52

    CAS  Article  Google Scholar 

  • Roberts PH, Thomas KV (2006) The occurrence of selected pharmaceuticals in wastewater effluent and surface waters of the lower Tyne catchment. Sci Total Environ 356:143–153

    CAS  Article  Google Scholar 

  • Ruttkies C, Schymanski EL, Wolf S, Hollender J, Neumann S (2016) MetFrag relaunched: incorporating strategies beyond in silico fragmentation. J Cheminform 8:1–16. https://doi.org/10.1186/s13321-016-0115-9

    Article  Google Scholar 

  • Schymanski EL, Jeon J, Gulde R, Fenner K, Ruff M, Singer HP, Hollender J (2014a) Identifying small molecules via high resolution mass spectrometry: communicating confidence. Environ Sci Technol 48:2097–2098

    CAS  Article  Google Scholar 

  • Schymanski EL et al (2014b) Strategies to characterize polar organic contamination in wastewater: exploring the capability of high resolution mass spectrometry. Environ Sci Technol 48:1811–1818. https://doi.org/10.1021/es4044374

    CAS  Article  Google Scholar 

  • Shifflett SD, Hazel DW, Frederick DJ, Nichols EG (2014) Species trials of short rotation woody crops on two wastewater application sites in North Carolina, USA. BioEnergy Res 7:157–173

    Article  Google Scholar 

  • Singer HP, Wössner AE, McArdell CS, Fenner K (2016) Rapid screening for exposure to “non-target” pharmaceuticals from wastewater effluents by combining HRMS-based suspect screening and exposure modeling. Environ Sci Technol. https://doi.org/10.1021/acs.est.5b03332

  • Sobus JR et al (2017) Integrating tools for non-targeted analysis research and chemical safety evaluations at the US EPA. J Expo Sci Environ Epidemiol. https://doi.org/10.1038/s41370-017-0012-y

  • Stanley JK, Ramirez AJ, Chambliss CK, Brooks BW (2007) Enantiospecific sublethal effects of the antidepressant fluoxetine to a model aquatic vertebrate and invertebrate. Chemosphere 69:9–16. https://doi.org/10.1016/j.chemosphere.2007.04.080

    CAS  Article  Google Scholar 

  • 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 44:417–426. https://doi.org/10.1016/j.watres.2009.07.010

    CAS  Article  Google Scholar 

  • Trenberth KE (1999) Conceptual framework for changes of extremes of the hydrological cycle with climate change. In: Weather and Climate Extremes. Springer, Berlin, pp 327–339

    Chapter  Google Scholar 

  • Trier X, Granby K, Christensen JH (2011) Tools to discover anionic and nonionic polyfluorinated alkyl surfactants by liquid chromatography electrospray ionisation mass spectrometry. J Chromatogr A 1218:7094–7104. https://doi.org/10.1016/j.chroma.2011.07.057

    CAS  Article  Google Scholar 

  • United States Environmental Protection Agency (2006) Process design manual: Land treatment of municipal wastewater effluents. Cincinnati

  • United States Environmental Protection Agency (2007) Method 1694: pharmaceuticals and personal care products in water, soil, sediment, and biosolids by HPLC/MS/MS. Washington, DC

  • Veach AM, Bernot MJ (2011) Temporal variation of pharmaceuticals in an urban and agriculturally influenced stream. Sci Total Environ 409:4553–4563. https://doi.org/10.1016/j.scitotenv.2011.07.022

    CAS  Article  Google Scholar 

  • Webb SF (2001) A data based perspective on the environmental risk assessment of human pharmaceuticals II—aquatic risk characterisation. In: Kümmerer K (ed) Pharmaceuticals in the environment: sources, fate, effects and risks. Springer Berlin Heidelberg, Heidelberg, pp 203–219. https://doi.org/10.1007/978-3-662-04634-0_16

    Chapter  Google Scholar 

  • Wickham H (2009) ggplot2: elegant graphics for data analysis. Springer-Verlag, New York

    Book  Google Scholar 

  • Williams AJ et al (2017) The CompTox Chemistry Dashboard: a community data resource for environmental chemistry. J Cheminform 9:61. https://doi.org/10.1186/s13321-017-0247-6

    Article  Google Scholar 

  • Winter MJ et al (2008) Defining the chronic impacts of atenolol on embryo-larval development and reproduction in the fathead minnow (Pimephales promelas). Aquat Toxicol 86:361–369. https://doi.org/10.1016/j.aquatox.2007.11.017

    CAS  Article  Google Scholar 

  • Zhang K, Niu ZG, Lv Z, Zhang Y (2017) Occurrence and distribution of antibiotic resistance genes in water supply reservoirs in Jingjinji area, China. Ecotoxicology. https://doi.org/10.1007/s10646-017-1853-9

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Acknowledgements

The authors would like to thank Wanda Bodnar and Leonard Collins of the UNC Biomarker Mass Spectrometry Center for instrument use and technical assistance. We additionally would like to thank Andrew Birch and Hallie Hartley for field and technical assistance and Jon Sobus, Sarah Laughlin-Toth, and Jarod Grossman for data processing assistance. This study was supported with funding from the North Carolina State University Department of Forestry and Environmental Resources, the North Carolina Department of Agriculture and Consumer Services Bioenergy Research Initiative (G40100278314RSD), the National Institute of Environmental Health Sciences (NIEHS) Superfund Basic Research Program (Grant 5 P42ES005948), and the UNC Center for Environmental Health and Susceptibility (P30ES010126). This work was supported in part by an appointment to the ORISE Research Participation Program at the Office of Research and Development, US EPA, through an interagency agreement between the US EPA and DOE. This work has been internally reviewed at the US EPA and has been approved for publication. The views expressed in this paper are those of the authors and do not necessarily represent the views or policies of the US Environmental Protection Agency.

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McEachran, A.D., Hedgespeth, M.L., Newton, S.R. et al. Comparison of emerging contaminants in receiving waters downstream of a conventional wastewater treatment plant and a forest-water reuse system. Environ Sci Pollut Res 25, 12451–12463 (2018). https://doi.org/10.1007/s11356-018-1505-5

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Keywords

  • Wastewater
  • Contaminants of emerging concern (CECs)
  • Forest-water reuse
  • Nontargeted analysis
  • Surface water
  • Water reuse