Elsevier

Ecological Engineering

Volume 162, 1 April 2021, 106175
Ecological Engineering

Sulfonamide antibiotics in groundwater and their migration in the vadose zone: A case in a drinking water resource

https://doi.org/10.1016/j.ecoleng.2021.106175Get rights and content

Highlights

  • Sulfonamides contamination in a drinking water resource observed.

  • Adsorption batch tests and a column experiment conducted.

  • Factors influencing on sulfonamides transport analyzed.

  • Sulfonamides showed migration ability to groundwater with the order: SMX > SM2 > SMP.

Abstract

Vadose zone is an important channel for sulfonamide contamination into groundwater, and the processes of adsorption and migration in the vadose zone are complicated. In this study, we focused on three sulfonamide antibiotics (sulfamethoxazole, sulfamethazine and sulfamethoxypyridazine) in the groundwater of Limin drinking water resource in northeastern China and assessed their migration potential in aquifers. Analysis was based on adsorption batch tests, a column experiment. Some key influencing factors including pH, iron, manganese and ammonia were considered. The results showed that the concentration of sulfamethoxypyridazine in groundwater is higher, ranging between 7 and 30 ng/L, the concentrations of sulfamethoxazole and sulfamethazine are relatively lower and no more than 1 ng/L. The adsorption capacity of the three antibiotics on vadose zone materials shows the following order: sulfamethoxypyridazine > sulfamethazine > sulfamethoxazole. Furthermore, for the three sulfonamides, the adsorption is higher in the medium of 0–20 cm (finer particle size, higher clay content and lower sand content) than that in 80–100 cm. Coexisting ions (iron, manganese and ammonia) promote the adsorption of sulfonamides, and the adsorption of sulfonamides decreases as the water pH increases. The column experiment also shows that the three sulfonamides have strong migration abilities and pose a considerable risk to groundwater.

Introduction

As one of the most important groups of pharmaceutically active compounds, antibiotics have been widely used in both human and veterinary medicine (Tuc Dinh et al., 2011; Goldman, 2004). The worldwide antibiotic consumption is estimated between 100,000 and 200,000 tons per year (Wise, 2002). China is the largest producer of antibiotics in the world, and its total usage of 36 frequently detected antibiotics reached approximately 92,700 tons in 2013, with respective human and veterinary antibiotic proportions of 48% and 52% (Zhang et al., 2015).

Sulfonamide antibiotics are a class of antibiotics widely used in treating human and animal diseases and also in animal feed additives (Avisar et al., 2009; Garoma et al., 2010; Jiang et al., 2011; Kools et al., 2008; Zhang et al., 2015). Since they are only partially metabolized, their metabolites and parent compounds are released into the environment via urine and feces discharge (Bound and Voulvoulis, 2004; Gao et al., 2012), pharmaceutical production plants and hospital effluent discharge (Azanu et al., 2018; Chang et al., 2010; Hirsch et al., 1999), as well as human wastewater discharge (Jiang et al., 2011; Liu et al., 2018; Wei et al., 2011). In the Limin area, wastewater from pharmacy factories can be discharged to the municipal sewage network, then entered into the sewage treatment plant for treatment and finally discharged into the Hulan River.

The sulfonamides metabolite remained in manure still maintain significant residual activity for a long time (Hirsch et al., 1999). In Ghana, hospital sulfonamide wastewater and other effluents are directly discharged into nearby streams and eventually used to irrigate vegetables (Azanu et al., 2018). Antibiotics have been reported in surface water, groundwater and plants (Dolliver et al., 2007; He et al., 2016; Tuc Dinh et al., 2011; Zhao et al., 2016). There is a growing concern about the risk of the development and spread of antibiotic resistant genes and pathogens in the environment (Heuer and Smalla, 2007; Xu et al., 2018).

Contaminants are stored by soils and to be taken up by plants and leached into water bodies or transported to other places (Hou et al., 2017; Song et al., 2018; Wang et al., 2019; Wu et al., 2016). Leaching through the vadose zone and entering into groundwater is an important migration pathway for the contamination of sulfonamide antibiotics (Burkhardt and Stamm, 2007; Kreuzig et al., 2005). To understand the leaching potential of sulfonamide antibiotics, the evaluation of their adsorption and migration behavior in vadose zone is crucial (Unold et al., 2009). Various techniques such as laboratory modeling (Ahmed et al., 2017; Chen et al., 2017; Wang et al., 2016; Zhang et al., 2014), geochemical analysis (Spielmeyer et al., 2017) and numerical modeling (Engelhardt et al., 2015; Unold et al., 2009; Zhou et al., 2016) can be applied to evaluate the adsorption and migration of sulfonamides. The sulfonamides have a high polarity and water solubility, easier to enter into the groundwater and move with the groundwater flow, which result in a high migration capacity (Thiele-Bruhn et al., 2004).

It has been determined that the adsorption and migration of sulfonamides in the unsaturated zone is strongly related to soil particle composition and mineral composition (Crini and Badot, 2008; Fan et al., 2011; Kahle and Stamm, 2007), organic matter (Chu et al., 2013), pH (Park and Huwe, 2016), coexisting ion, and cation exchange capacity (Carballa et al., 2008), which have different impacts on their fate in the vadose zone and aquifers (Zhang et al., 2014). The finer of the medium particles are, the more adsorption sites can provided, with the increasing of adsorption capacity (Crini and Badot, 2008). Kahle and Stamm (2007) investigated the adsorption behavior of sulfathiazole to clay minerals and ferrihydrite for varying pH and contact times, results revealed that sulfathiazole cation were significantly adsorbed by clay minerals, and ferrihydrite was showing significant sorption only between pH 5.5–7. Sulfonamide adsorption enhances with greater organic matter content due to increased hydrophobic interactions (Chu et al., 2013). Decreasing pH values leads to increasing adsorption potential of antibiotics on soil material in pH range of 4–8 (Park and Huwe, 2016). The adsorption of sulfonamides tends to be higher with increasing cation exchange capacity of soils (Carballa et al., 2008). The real scenario of groundwater contamination by antibiotics is very much dependent on their leaching behavior in the vadose zone.

The objectives of this study are to investigate the contamination of three common sulfonamide antibiotics (sulfamethoxazole, sulfamethazine and sulfamethoxypyridazine) in the Limin groundwater resource, and further illustrate the underlying mechanisms of their movement in the vadose zone. As emerging pollutants of groundwater in the Limin drinking water resource, the three sulfonamide antibiotics adsorption and migration behaviors are crucial for study, which can provide a scientific guidance for controlling the antibiotics contamination in the vadose zone and groundwater.

Section snippets

The study area

The Limin area is located in the northern part of Harbin City, Heilongjiang Province, northeastern China, as shown in Fig. 1. The study area has a middle temperate continental monsoon climate with an average rainfall of 547.5 mm/yr, average potential evapotranspiration of 1314.3 mm/yr and an average annual temperature is 3.6 °C. The river system mainly includes the Songhua River and its tributary, the Hulan River. The Songhua River flows from the west to the east from the southern edge of the

Concentration of tested antibiotics

The concentrations of antibiotics in the Limin area are shown in Fig. 3, Table S2. In addition to three sulfonamides, macrolides (Lincomycin hydrochloride, LIN for short; Cefaclor, CCR for short), chloramphenicol (Florfenicol, FLO for short), β-lactams (Ampicillin sodium, AMP for short Antibiotics) were also detected. The order of magnitude of the sum of the antibiotics was in a narrow range: 10–30 ng/L in the groundwater, which is the same in the surface water. SMP was dominating in all GW

Conclusions

In this paper, the adsorption and migration behavior of three typical sulfonamide antibiotics (sulfamethoxazole, sulfamethazine and sulfamethoxypyridazine) were studied in samples from the vadose zone in the Limin area. Batch adsorption tests and a sediment column experiment were carried out for three target antibiotics.

The results showed presence of these three sulfonamides in the aquifer at concentrations ranging between 7 and 30 ng/L. The adsorption of the three sulfonamide antibiotics in

Declaration of Competing Interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgements

We thank the National Natural Science Foundation of China (Nos. 41672228, 41877181 and 41831283), and the National Water Pollution Control and Treatment Science and Technology Major Project (No. 2018ZX07109-003) and 111 Project (No. B18006) to support this work.

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