Geospatial Variability of Fluorescent Dissolved Organic Matter in Urban Watersheds: Relationships with Land Cover and Wastewater Infrastructure.

We investigated the fluorescent dissolved organic matter (FDOM) composition in two watersheds with variable land cover and wastewater infrastructure, including sanitary sewers and septic systems. A four-component parallel factor analysis model was constructed from 295 excitation-emission matrices recorded for stream samples to examine relationships between FDOM and geospatial parameters. The contributions of humic acid- and fulvic acid-like fluorescence components (e.g., C1, C2, C3) were fairly consistent across a 12 month period for the 27 sampling sites. In contrast, the protein-like fluorescence component (C4) and a related ratiometric wastewater indicator (C4/C3) exhibited high variability in urban tributaries, suggesting that some sites were impacted by leaking sewer infrastructure. Principal component analysis indicated that urban areas clustered with impervious surfaces and sanitary sewer density, and cross-covariance analysis identified strong positive correlations between C4, impervious surfaces, and sanitary sewer density at short lag distances. The presence of wastewater was confirmed by detection of sucralose (up to 1,660 ng L-1) and caffeine (up to 1,740 ng L-1). Our findings not only highlight the potential for C4 to serve as an indicator of nearby, compromised sanitary sewer infrastructure, but also suggest that geospatial data can be used to predict areas vulnerable to wastewater contamination.

Geospatial and co-occurrence analysis of antibiotics, hormones, and UV filters in the Chesapeake Bay (USA) to confirm inputs from wastewater treatment plants, septic systems, and animal feeding operations.

Previous studies have reported select contaminants of emerging concern (CECs) in limited areas of the Chesapeake Bay (USA), but no comprehensive efforts have been conducted. In this work, 43 antibiotics, 9 hormones, 11 UV filters, and sucralose, were measured in matched water, sediment, and oyster samples from 58 sites. The highest sucralose concentration was 3051 ng L-1 in a subwatershed with 4.43 million liters of wastewater effluent per day (MLD) and 4385 septic systems. Although antibiotic occurrence was generally low in subwatersheds located in less populated areas, 102 ng L-1 ciprofloxacin was detected downstream of 0.58 MLD wastewater effluent and 10 animal feeding operations. Hormones were not regularly detected in water (2%) or oysters (37%), but the high detection frequencies in sediment (74%) were associated with septic systems. UV filters were ubiquitously detected in oysters, and octisalate exhibited the highest concentration (423 ng g-1). Oyster-phase oxybenzone and aqueous-phase sucralose concentrations were significantly correlated to wastewater effluent and septic systems, respectively. Toxicity outcomes were predicted for homosalate and octisalate throughout the Bay, and antimicrobial resistance concerns were noted for the Chester River. The geospatial and co-occurrence relationships constitute crucial advances to understanding CEC occurrence in the Chesapeake Bay and elsewhere.