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Does Long-Term Irrigation with Untreated Wastewater Accelerate the Dissipation of Pharmaceuticals in Soil?

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† Institute of Crop Science and Resource Conservation − Soil Science and Soil Ecology, University of Bonn, Bonn, Germany
‡ Instituto de Geología, Universidad Nacional Autónoma de México, México D.F., México
§ Research Unit for Environmental Genomics, Helmholtz Zentrum München, Oberschleissheim, Germany
*Phone +228 73 2965, fax: +228 73 2782; e-mail: [email protected]
Cite this: Environ. Sci. Technol. 2014, 48, 9, 4963–4970
Publication Date (Web):April 4, 2014
https://doi.org/10.1021/es501180x
Copyright © 2014 American Chemical Society
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Abstract

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Long-term irrigation with untreated wastewater may increase soil microbial adaptation to pollution load and lead to enhanced natural attenuation. We hypothesized that long-term wastewater irrigation accelerates the dissipation of pharmaceuticals. To test our hypothesis we performed an incubation experiment with soils from the Mezquital Valley, Mexico that were irrigated for 0, 14, or 100 years. The results showed that the dissipation half-lives (DT50) of diclofenac (<0.1–1.4 days), bezafibrate (<0.1–4.8 days), sulfamethoxazole (2–33 days), naproxen (6–19 days), carbamazepine (355–1,624 days), and ciprofloxacin were not affected by wastewater irrigation. Trimethoprim dissipation was even slower in soils irrigated for 100 years (DT50: 45–72 days) than in nonirrigated soils (DT50: 12–16 days), was negatively correlated with soil organic matter content and soil-water distribution coefficients, and was inhibited in sterilized soils. Applying a kinetic fate model indicated that long-term irrigation enhanced sequestration of cationic or uncharged trimethoprim and uncharged carbamazepine, but did not affect sequestration of fast-dissipating zwitterions or negatively charged pharmaceuticals. We conclude that microbial adaptation processes play a minor role for pharmaceutical dissipation in wastewater-irrigated soils, while organic matter accumulation in these soils can retard trimethoprim and carbamazepine dissipation.

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The Supporting Information includes details on laboratory and analytical methods. Furthermore, it presents concentrations of pharmaceuticals in wastewater and unspiked soil, estimated rate constants (kEAS, kRES, and qEAS), as well as initial values (C0(EAS) and C0(RES)) obtained by fitting the model to the respective data set. Concentrations of carbamazepine extracted via the first and second CaCl2 extraction (easily extractable fraction), as well as concentrations extracted via ASE (residual fraction) are shown in an additional figure. This material is available free of charge via the Internet at http://pubs.acs.org.

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