Occurrence and distribution of pharmaceutical and personal care products, artificial sweeteners, and pesticides in groundwater from an agricultural area in Korea
Graphical abstract
Introduction
Pollutants entering groundwater through anthropogenic activities, such as sewage leakages, livestock breeding, and leaching from agricultural activities, are a growing concern (Sui et al., 2015). However, groundwater pollution is relatively poorly understood compared to other freshwater bodies, although the long-term potential risk to groundwater resources is increasingly recognized (Lapworth et al., 2012; Stuart et al., 2012). Among such pollutants, the occurrence and potential risk of pharmaceutical and personal care products (PPCPs), which are regarded as emerging groundwater contaminants, have been recently reported by many researchers (Kolar and Finizio, 2017; Peng et al., 2014; Yao et al., 2017). Most studies of groundwater contamination have focused on locations near septic systems (James et al., 2016; Kolpin et al., 2002; Kuroda et al., 2012; Müller et al., 2012; Robertson et al., 2016, Robertson et al., 2013; Wolf et al., 2012; Yang et al., 2017) or close to the effluent discharge points of wastewater treatment plants (WWTPs) (Buerge et al., 2009; Clara et al., 2004; Kahle et al., 2009; Nakada et al., 2008). Various pharmaceuticals, life-style compounds, hormones, and food additives are frequently detected in groundwater. Some PPCPs, such as caffeine (Buerge et al., 2006; Nakada et al., 2006), crotamiton (Kahle et al., 2009; Kuroda et al., 2012), carbamazepine (Clara et al., 2004), and artificial sweeteners (ASs) (e.g., acesulfame and sucralose) (Buerge et al., 2009; Oppenheimer et al., 2011; Robertson et al., 2013; Soh et al., 2011) have been proposed as indicators of groundwater contamination from sewage leakage.
However, studies of groundwater contamination from agriculture (Hu et al., 2010; Spielmeyer et al., 2017; Watanabe et al., 2010, Watanabe et al., 2008), livestock waste (Bartelt-Hunt et al., 2011), or confined animal feeding operations (CAFOs) (Batt et al., 2006) are relatively limited, although there is the potential for groundwater contamination in agricultural areas due to fertilization with manure and sewage leaks (Bartelt-Hunt et al., 2011; Hu et al., 2010; Spielmeyer et al., 2017; Watanabe et al., 2010, Watanabe et al., 2008). In addition, pesticides and veterinary drugs are used widely for agricultural purposes, resulting in groundwater contamination (Capece et al., 2009; Sarmah et al., 2006; Sukul and Spiteller, 2006). The irrigation with contaminated agricultural groundwater can contaminate crops and might contribute to human exposure through the ingestion of contaminated crops or groundwater.
In Korea, studies of emerging pollutants in groundwater are rare, with most research focusing on WWTPs and rivers (Kim et al., 2009, Kim et al., 2007; Yoon et al., 2010). However, in 2003, the use of veterinary pharmaceuticals in meat production (0.72 kg/t meat production) in Korea was higher than in the United States (0.24 kg/t), Japan (0.36 kg/t), Denmark (0.04 kg/t), and Sweden (0.03 kg/t) (MAFRA, 2010). About 76% of all veterinary pharmaceuticals used in Korea in 2016 were consumed in animal husbandry (MAFRA, 2017). In addition, in 2009, pesticide usage per unit agricultural area (10.3 kg/ha) in Korea was higher than for other OECD countries, except Japan (13.2 kg/ha) and Israel (12.7 kg/ha) (OECD, 2013). Therefore, agricultural groundwater contamination by PPCPs, including veterinary pharmaceuticals and pesticides, in Korean groundwater is a growing concern.
In this study, 33 PPCPs including antibiotics and anthelmintics were selected based on their concentration and detection frequencies in previous Korean studies on PPCPs in WWTPs and water environment (Kim et al., 2017; Sim et al., 2013, Sim et al., 2011). Additionally, five artificial sweeteners as known markers of sewage leakage and six pesticides widely used in Korea (KCPA, 2012; Kim et al., 2016) were selected to determine the contamination status of groundwater in Korea. In addition, the characteristic patterns of occurrence of these chemicals in groundwater due to agricultural activities were investigated by comparing groundwater samples from the rural agricultural and rural non-agricultural areas. This enabled an assessment of the effect of the proximity to sources on the levels of these compounds in groundwater. This is the first study to determine the residual levels of PPCPs in Korean groundwater.
Section snippets
Chemicals and materials
In this study, the levels of 33 PPCPs, five ASs, and six pesticides were measured in groundwater. Table 1 presents specific information on the target compounds according to the groups and these compounds selected by the usage, the species that have maximum residue limits (MRLs) in food (Livestock) and potential effects of groundwater contamination based on the previous studies (Kim et al., 2016, Kim et al., 2017; Sim et al., 2013; Subedi et al., 2014). Acetaminophen-d3, atenolol-d7, BPA-d16,
Occurrence of target chemicals in groundwater
As shown in Table 1, the 44 compounds analyzed in this study were categorized into six groups: antibiotics, anthelmintics, β-blockers, other PPCPs, pesticides, and ASs. A total of 31 compounds (15 antibiotics, four anthelmintics, two β-blockers, five other PPCPs, one pesticide, and four ASs) were detected in groundwater samples, while 13 compounds (three antibiotics, three anthelmintics, one β-blocker, five pesticides, and one AS) were not detected. The concentrations of PPCPs, ASs, and
Conclusion
This study determined the occurrence and distribution of PPCPs, ASs, and pesticides in groundwater in South Korea for the first time. The groundwater concentration distributions of target compounds differed between rural agricultural and rural non-agricultural areas, which was attributed to the presence of different contamination sources. Carbofuran, sulfathiazole, sulfamethoxazole, and oxfendazole were frequently observed in agricultural groundwater samples, but not in non-agricultural
Acknowledgment
This work was supported by a grant from the National Institute of Environment Research (NIER), funded by the Ministry of Environment (MOE) of the Republic of Korea (NIER-SP2016-333) and Korea Environment Industry & Technology Institute (KEITI) through “The Chemical Accident Prevention Technology Development Project” funded by Korea Ministry of Environment (MOE) (A1180019708020000000000000).
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