Widespread occurrence and potential for biodegradation of bioactive contaminants in Congaree National Park, USA

Abstract

Organic contaminants with designed molecular bioactivity, such as pesticides and pharmaceuticals, originate from human and agricultural sources, occur frequently in surface waters, and threaten the structure and function of aquatic and terrestrial ecosystems. Congaree National Park in South Carolina (USA) is a vulnerable park unit due to its location downstream of multiple urban and agricultural contaminant sources and its hydrologic setting, being composed almost entirely of floodplain and aquatic environments. Seventy-two water and sediment samples were collected from 16 sites in Congaree National Park during 2013 to 2015, and analyzed for 199 and 81 targeted organic contaminants, respectively. More than half of these water and sediment analytes were not detected or potentially had natural sources. Pharmaceutical contaminants were detected (49 total) frequently in water throughout Congaree National Park, with higher detection frequencies and concentrations at Congaree and Wateree River sites, downstream from major urban areas. Forty-seven organic wastewater indicator chemicals were detected in water, and 36 were detected in sediment, of which approximately half are distinctly anthropogenic. Endogenous sterols and hormones, which may originate from humans or wildlife, were detected in water and sediment samples throughout Congaree National Park, but synthetic hormones were detected only once, suggesting a comparatively low risk of adverse impacts. Assessment of the biodegradation potentials of 8 C-radiolabeled model contaminants indicated poor potentials for some contaminants, particularly under anaerobic sediments conditions. Environ Toxicol Chem 2017;36:3045-3056. Published 2017 Wiley Periodicals Inc. on behalf of SETAC. This article is a US government work and, as such, is in the public domain in the United States of America.

Exposure and potential effects of pesticides and pharmaceuticals in protected streams of the US National park Service southeast region

“…These results are consistent with the widely documented occurrence of mixed contamination in developed watersheds across the US (Bradley et al, 2017b;Bradley et al, 2018a;Bradley et al, 2019;Nowell et al, 2018;Van Metre et al, 2017) and elsewhere (e.g. ; Brack et al, 2015;Busch et al, 2016;Le et al, 2017;Malaj et al, 2014;Peters et al, 2013;Posthuma et al, 2017;Rosi-Marshall and Royer, 2012;Schäfer et al, 2016) and, likewise, with the few previous reports of pesticide and pharmaceutical contaminants in protected stream systems in the US (Battaglin et al, 2018;Bradley et al, 2017c;Elliott and VanderMeulen, 2017;Weissinger et al, 2018) and elsewhere (Camacho-Muñoz et al, 2010; Gerber et al, 2016). However, the substantially lower Table 1.…”

“…Nicotine was detected at least once at every site in this study and the broad-spectrum herbicide, atrazine (or its degradate hydroxyatrazine, OIET), was detected at all but one site (Table S3b). Consistent with its pervasive detection in the floodplain-dominated Congaree National Park (Bradley et al, 2017c) and throughout the southeastern headwater streams study (Bradley et al, 2018a;Bradley et al, 2019), the anti-diabetic medicine, metformin (or its environmental metabolite, guanylurea), was detected at least once (up to more than 500 ng L À1 ; Table 3b) at all but three sites (not detected at WEKI) and in more than half of the samples (median exposure conditions) at 11 of 18 sites ( Table S3c). Only nicotine and caffeine-related compounds (caffeine, dimethylxanthine) were detected at concentrations greater than 1 mg L À1 in this NPS SER study ( Fig.…”

“…1-3 and S1-S2; Tables S3a-S3c). All detections were attributed to environmental contaminants, as no analytes were detected in any of the four water blanks (Table S3a) or the two sediment blanks (Bradley et al, 2017a;Bradley et al, 2017c) prepared for this study. Approximately 24% (80) of the 334 unique (accounting for method overlap) analytes assessed in water in this study were detected at least once (maximum exposure dataset) across all sites (Figs.…”

“…Four water blanks for pesticides and pharmaceuticals were prepared in the field (BISO4, CHAT1, CHAT2, LIRI3), as described above for samples, with Pesticide/Volatile Organic Chemical grade water; no analytes were detected in water field blanks (Table S3a). Two sediment blanks (coarse sand combusted at 500°C for 24 h and transferred to sample bottles under field conditions) were prepared in 2015 for application to this and the Congaree National Park study (Bradley et al, 2017a;Bradley et al, 2017c); no pesticide analytes were detected in sediment field blanks (Bradley et al, 2017a;Bradley et al, 2017c). LC-MS/MS pharmaceutical and pesticide water analyses included addition of 20 and 21 stable-isotope surrogate standards, respectively, to field-filtered samples to evaluate whole-method recovery (pharmaceuticals median: 102%, interquartile range [IQR]: 96-110%, range: 2-270%; pesticides median: 101%, IQR: 95-105%, range: 34-135%) (Table S4).…”

“…In the United States (US) and globally, protected areas are essential biodiversity preserves and environmental-change reference ecosystems (Foresta, 2013;Gaston et al, 2008;Stein et al, 2008), but these services are undermined by the impacts (e.g., water and sediment contamination, disconnection from external wildland corridors, invasive species) of increasing visitation and surrounding-land development (Gaston et al, 2008;Jenkins et al, 2015;Joppa et al, 2008;Palomo et al, 2013;Radeloff et al, 2010). In the US, the National Park Service (NPS) has identified the occurrence and potential adverse effects of anthropogenic bioactive contaminants on park ecosystems as resource management concerns (Landewe 2008) and several recent US Geological Survey (USGS)-NPS studies have demonstrated that intra-park human-waste management as well as fluvial and visitationmediated contaminant transport into parks from external sources are challenges for NPS surface-water ecosystems (Battaglin et al, 2018;Bradley et al, 2017c;Egler et al, 2013;Elliott and VanderMeulen, 2017;Landers et al, 2008;Landewe 2008;Mast et al, 2006;Usenko et al, 2007;Weissinger et al, 2018). Notably, the frequent detection and diversity of bioactive-contaminant mixtures in water and sediment at the floodplain-dominated Congaree National Park near Columbia, SC (Bradley et al, 2017a;Bradley et al, 2017c) highlighted growing concerns for adverse aquaticecosystem effects from surrounding development (Radeloff et al, 2005;Radeloff et al, 2010) within the rapidly urbanizing southeastern US (Terando et al, 2014;Van Metre et al, 2019).…”