Pharmaceutically active compounds in the Xiangjiang River, China: Distribution pattern, source apportionment, and risk assessment
Graphical abstract
Introduction
River systems often serve as important drinking water sources; simultaneously, they are among the most vulnerable water bodies due to natural and anthropogenic activities (Zhang et al., 2010). As reported in a worldwide study, over 65% of the rivers in the world are polluted (Vorosmarty et al., 2010). Emerging contaminants, especially pharmaceutically active compounds (PhACs), which were widely used in agricultural practices, as veterinary additives, and in human health care (Barceló and Petrovic, 2007), heavily impact water quality.
Even at trace levels, PhACs exhibit undesired biologically active effects on non-target organisms (Zhou et al., 2016). For example, ciprofloxacin may interfere with the photosynthesis pathway of higher plants, leading to morphological abnormalities or growth inhibition (Aristilde et al., 2010). Diclofenac also has high antiovulatory effects on aquatic vertebrates (Yokota et al., 2015). In addition, previous studies have provided evidence that the prevalence of antibiotics in water bodies was strongly correlated with the population of antibiotic-resistant bacteria and they can also promote the generation of antibiotic resistance genes (Jiang et al., 2013; Varela et al., 2014; Zhang et al., 2014). These genes could be shared between microorganisms, animals, and even to humans, through horizontal gene transfer (Liu and Wong, 2013).
There is a knowledge gap regarding the environmental implications of chemical mixtures since most risk assessments have been based on individual compound (Ding et al., 2017). It should be noted that PhACs are unlikely to exist as independent constituents, a broad range are applied in combination at any real sites (Lopez-Serna et al., 2012; Paiga et al., 2016), engendering a serious mixture effect referred to as the “cocktail effect” (Du et al., 2017). Backhaus and Faust (2012) introduced a tiered assessment approach, which introduces first tier screening for chemical mixtures to determine whether more elaborate mixture risk assessment is needed. Since then, certain studies have paid close attention to the environmental implications of chemical mixtures (Backhaus and Karlsson, 2014; Liu et al., 2015; Yao et al., 2017).
To date, several studies have focused on the occurrence of PhACs in the estuary (Yan et al., 2015; Zhao et al., 2017), central and lower areas of the Yangtze River (Wu et al., 2014). These studies give rise to concerns over the potential effects of pharmaceuticals in drinking water sources. However, data that characterize the sources, exposure, and effects of pharmaceuticals in this area are still very limited. In addition, tributaries can be important contributions to pollution in the main stream. To our knowledge, no study has ever systematically addressed the pharmaceutical contaminants in the Xiangjiang River, which is a main tributary of the Yangtze River. The Xiangjiang River is 856 km in length with a catchment area of 94,660 km2, of which 90.2% is located in the Hunan Province. >40 million people live along the river bank. It is an important water resource for drinking, irrigation, industry, fisheries, and transportation. It is also the most important economic belt in the Hunan Province, and is responsible for 70% of the gross domestic product (GDP) of the province. However, water pollution in the Xiangjiang River is markedly exacerbated by increasing population, booming economy, and accelerated urbanization during recent years (Xie, 2016).
In this context, this study focused on the spatiotemporal distribution of multi-residue PhACs, which are frequently used for human and animal purposes in proximity to the Xiangjiang River. The linkages between PhAC concentrations and water quality parameters were explored. Potential pollution sources were also interpreted based on the concentration profile. In addition, both the single compound ecological risks and the mixture risks were evaluated for the aquatic environment. This work will serve to enrich the inventories of pharmaceutical pollution on a global scale, elucidate whether aquatic organisms are at risk, and help identify potential PhAC sources in the study region.
Section snippets
Chemicals and reagents
Thirty-six PhACs with high purity grade (>98%) and obtained from Dr. Ehrenstorfer GmbH (Augsburg, Germany), were selected as the targets in this study. Detailed information on the physico-chemical properties is provided in Table S1. Surrogate standards (purity > 99%), including sulfamethoxazole-D4, sulfamethazine-D4, ciprofloxacin-D8, ibuprofen-D3, roxithromycin-D7, and thiabendazole-D4, were purchased from Toronto Research Chemicals (Oakville, Canada), and meclocycline was obtained from
Occurrence and concentrations of PhACs
Among the 36 investigated compounds, 25 of them were detected during the two sampling campaigns, indicating their ubiquitous presence in the Xiangjiang River. The compounds which were not detected or concentrations below the MDL in all samples are not discussed in this study. These include sulfathiazole, sulfamerazine, sulfaquinoxaline, difloxacin, pefloxacin, tetracycline, chlortetracycline, doxycycline, tylosin, naproxen, and ketoprofen.
As shown in Table 1, the mean concentrations of PhACs in
Conclusion
In this study, the first investigation of the seasonal variation and spatial distribution of 36 PhACs was conducted on the Xiangjiang River. Twenty-five compounds were detected with concentrations ranging from ND to 830 ng L−1 (cefotaxime). Pharmaceutical contaminant levels were moderate compared with previously reported data on a global scale. Higher temperature and the dilution effect of stream flow in summer could be responsible for the dramatic seasonal variation of most compounds (p
Acknowledgement
This work was financially supported by the Special Fund for Agro-scientific Research in the Public Interest (No. 201503108) and Science & Technology Project of Hunan Province (No. 2017WK2091).
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