Expanded Target-Chemical Analysis Reveals Extensive Mixed-Organic-Contaminant Exposure in USA Streams

摘要

Surface water from 38 streams nationwide was assessed using 14 target-organic methods (719 compounds). Designed-bioactive anthropogenic contaminants (biocides, pharmaceuticals) comprised 57% of 406 organics detected at least once. The 10 most-frequently detected anthropogenic-organics included 8 pesticides (desulfinylfipronil, AMPA, chlorpyrifos, dieldrin, metolachlor, atrazine, CIAT, glyphosate) and 2 pharmaceuticals (caffeine, metformin) with detection frequencies ranging 66–84% of all sites. Detected contaminant concentrations varied from less than 1 ng L⁻¹ to greater than 10 μg L⁻¹, with 77 and 278 having median detected concentrations greater than 100 ng L⁻¹ and 10 ng L⁻¹, respectively. Cumulative detections and concentrations ranged 4-161 compounds (median 70) and 8.5–102,847 ng L⁻¹, respectively, and correlated significantly with wastewater discharge, watershed development, and Toxic Release Inventory metrics. Log10 concentrations of widely monitored HHCB, triclosan, and carbamazepine explained 71%–82% of the variability in the total number of compounds detected (linear regression; p-values: <0.001–0.012), providing a statistical inference tool for unmonitored contaminants. Due to multiple modes of action, high bioactivity, biorecalcitrance, and direct environment application (pesticides), designed-bioactive organics (median 41 per site at μg L⁻¹ cumulative concentrations) in developed watersheds present aquatic health concerns, given their acknowledged potential for sub-lethal effects to sensitive species and lifecycle stages at low ng L⁻¹.