RESUMEN
Though bioaccumulation of pharmaceuticals by aquatic organisms continues to receive scientific attention, the internal disposition of these contaminants among different tissue compartments of fish species has been infrequently investigated, particularly among fish at different trophic positions. We tested a human to fish biological read-across hypothesis for contaminant disposition by examining tissue-specific accumulation in three understudied species, longnose gar (Lepisosteus osseus; piscivore), gizzard shad (Dorosoma cepedianum; planktivore/detritivore), and smallmouth buffalo (Ictiobus bubalus; benthivore), from a river influenced by municipal effluent discharge. In addition to surface water, fish plasma, and brain, gill, gonad, liver, and lateral muscle fillet tissues were analyzed via isotope dilution liquid chromatography tandem mass spectrometry. Caffeine and sucralose, two common effluent tracers, were quantitated at low micrograms per liter levels in surface water, while an anticonvulsant, carbamazepine, was observed at levels up to 37 ng/L. The selective serotonin reuptake inhibitors (SSRIs) fluoxetine and sertraline and primary metabolites were detected in at least one tissue of all three species at low micrograms per kilogram concentrations. Within each species, brain and liver of select fish contained the highest levels of SSRIs compared to plasma and other tissues, which is generally consistent with human tissue disposition patterns. However, we observed differential accumulation among specific tissue types and species. For example, mean levels of sertraline in brain and liver tissues were 13.4 µg/kg and 1.5 µg/kg in gizzard shad and 1.3 µg/kg and 7.3 µg/kg in longnose gar, respectively. In contrast, smallmouth buffalo did not consistently accumulate SSRIs to detectable levels. Tissue-specific eco-exposome efforts are necessary to understand mechanisms associated with such marked bioaccumulation and internal dispositional differences among freshwater fish species occupying different trophic positions. Environ Toxicol Chem 2024;00:1-9. © 2024 The Author(s). Environmental Toxicology and Chemistry published by Wiley Periodicals LLC on behalf of SETAC.
RESUMEN
Sewage effluents are the main source of entry of Human Pharmaceutical Active Ingredients (HPAIs) to surface water bodies. Carbamazepine (CBZ), psychiatric drug, enalapril (ENA) antihypertensive, and sildenafil (SIL), to treat erectile dysfunction, have been frequently detected in receiving wastewater and in wild fish species from Argentina. This study aimed to assess the bioconcentration of selected HPAIs in native fish species of the Del Plata Basin. In a first trial, the bioconcentration factors of CBZ, ENA, and SIL were obtained by exposing Cnesterodon decemmaculatus, respectively, to 135, 309, and 70 µg/L during 96 h. Then the bioconcentration kinetic of SIL was comparatively assessed in C. decemmaculatus and Piaractus mesopotamicus exposed, respectively, to 44.1 and 16.2 µg/L during a one-week, followed by a four-day depuration phase. HPAIs concentrations in water and tissue were measured by HPLC-MS after 0.22 µm filtration and direct injection or solid-liquid extraction, respectively. Bioconcentration factors obtained empirically (BCFe) for C. decemmaculatus were CBZ = 1.5, SIL = 1.4, and ENA = 0.007. Parameters estimated by the SIL bioconcentration kinetic model for C. decemmaculatus were: uptake rate constant (k1) = 5.5 L/kg d, elimination rate constant during uptake phase (k2u) = 0.00175 d-1, maximum predicted tissue concentration (Ct(max)) = 138588 µg/kg, estimated bioconcentration factor (BCFm) = 3143, lag time between the exposure and the first detection in tissue (tlag) = 0 d, elimination rate constant in the depuration phase (k2d) = 0.49 d-1 and half-life in the tissue (t1/2) = 1.4 d. The model parameters for P. mesopotamicus were k1: 7.3 L/kg d, k2u: 0.0836 d-1, Ct(max): 1423 µg/kg, BCFm: 88, tlag: 3.8 d in the uptake phase and k2d: 0.31 d-1 and t1/2: 2.3 d in the depuration phase. The reached conclusions were: 1) the bioconcentration capacity of CBZ and SIL are similar but around 200 times higher than ENA, 2) the time to reach the bioconcentration equilibrium for SIL is longer than 1 week, then estimated BCFm are between 1 and 3 orders of magnitude higher than BCFe obtained after 96 h exposure, but actual values need to be verified, 3) substantial differences (≈30 fold) were observed in the estimated BCF of SIL among species, indicating the need for further studies toward understanding such diversity to improve HPAIs ecological risk assessment worldwide.
RESUMEN
Environmental exposure to active pharmaceutical ingredients (APIs) can have negative effects on the health of ecosystems and humans. While numerous studies have monitored APIs in rivers, these employ different analytical methods, measure different APIs, and have ignored many of the countries of the world. This makes it difficult to quantify the scale of the problem from a global perspective. Furthermore, comparison of the existing data, generated for different studies/regions/continents, is challenging due to the vast differences between the analytical methodologies employed. Here, we present a global-scale study of API pollution in 258 of the world's rivers, representing the environmental influence of 471.4 million people across 137 geographic regions. Samples were obtained from 1,052 locations in 104 countries (representing all continents and 36 countries not previously studied for API contamination) and analyzed for 61 APIs. Highest cumulative API concentrations were observed in sub-Saharan Africa, south Asia, and South America. The most contaminated sites were in low- to middle-income countries and were associated with areas with poor wastewater and waste management infrastructure and pharmaceutical manufacturing. The most frequently detected APIs were carbamazepine, metformin, and caffeine (a compound also arising from lifestyle use), which were detected at over half of the sites monitored. Concentrations of at least one API at 25.7% of the sampling sites were greater than concentrations considered safe for aquatic organisms, or which are of concern in terms of selection for antimicrobial resistance. Therefore, pharmaceutical pollution poses a global threat to environmental and human health, as well as to delivery of the United Nations Sustainable Development Goals.
