Sources and transport of contaminants of emerging concern: A two-year study of occurrence and spatiotemporal variation in a mixed land use watershed

David J. Fairbairn*, M. Ekrem Karpuzcu, William A. Arnold, Brian L. Barber, Elizabeth F. Kaufenberg, William C. Koskinen, Paige J. Novak, Pamela J. Rice, Deborah L. Swackhamer

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The occurrence and spatiotemporal variation of 26 contaminants of emerging concern (CECs) were evaluated in 68 water samples in 2011-2012 in the Zumbro River watershed, Minnesota, U.S.A. Samples were collected across a range of seasonal/hydrological conditions from four stream sites that varied in associated land use and presence of an upstream wastewater treatment plant (WWTP). Selected CECs included human/veterinary pharmaceuticals, personal care products, pesticides, phytoestrogens, and commercial/industrial compounds. Detection frequencies and concentrations varied, with atrazine, metolachlor, acetaminophen, caffeine, DEET, and trimethoprim detected in more than 70% of samples, acetochlor, mecoprop, carbamazepine, and daidzein detected in 30%-50% of samples, and 4-nonylphenol, cotinine, sulfamethoxazole, erythromycin, tylosin, and carbaryl detected in 10%-30% of samples. The remaining target CECs were not detected in water samples. Three land use-associated trends were observed for the detected CECs. Carbamazepine, 4-nonylphenol, erythromycin, sulfamethoxazole, tylosin, and carbaryl profiles were WWTP-dominated, as demonstrated by more consistent loading and significantly greater concentrations downstream of the WWTP and during low-flow seasons. In contrast, acetaminophen, trimethoprim, DEET, caffeine, cotinine, and mecoprop patterns demonstrated both seasonally-variable non-WWTP-associated and continual WWTP-associated influences. Surface water studies of CECs often target areas near WWTPs. This study suggests that several CECs often characterized as effluent-associated have additional important sources such as septic systems or land-applied biosolids. Finally, agricultural herbicide (atrazine, acetochlor, and metolachlor) profiles were strongly influenced by agricultural land use and seasonal application-runoff, evident by significantly greater concentrations and loadings at upstream sites and in early summer when application and precipitation rates are greatest. Our results indicate that CEC monitoring studies should consider a range of land uses, seasonality, and transport pathways in relation to concentrations and loadings. This knowledge can augment CEC monitoring programs to result in more accurate source, occurrence, and ecological risk characterizations, more precisely targeted mitigation initiatives, and ultimately, enhanced environmental decision-making.

Orijinal dilİngilizce
Sayfa (başlangıç-bitiş)605-613
Sayfa sayısı9
DergiScience of the Total Environment
Yayın durumuYayınlandı - 1 May 2016

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Publisher Copyright:
© 2016 Elsevier B.V.


This work was supported by the Minnesota Environment and Natural Resources Trust Fund ( 012-A2 ) as recommended by the Legislative-Citizen Commission on Minnesota Resources. We thank McGhie Betts, Inc. (Rochester, MN) for the technical support on watershed characterization; Dr. Megan Kelly (Water Resources Science, University of Minnesota) for her assistance with sampling and sample analysis; and Dr. Gary Oehlert (Department of Statistics, University of Minnesota) for his advice on statistical design and analysis.

FinansörlerFinansör numarası
Minnesota Environment and Natural Resources Trust Fund012-A2
Legislative-Citizen Commission on Minnesota Resources

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