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.

The transport and fate of hydrophobic organic contaminants (HOCs) in the marine environment are closely linked to organic carbon (OC) cycling processes. We investigated the influence of marine versus terrestrial OC origin on HOC fluxes at two Baltic Sea coastal sites with different relative contributions of terrestrial and marine OC. Stronger sorption of the more than four-ring polycyclic aromatic hydrocarbons and penta-heptachlorinated polychlorinated biphenyls (PCBs) was observed at the marine OC-dominated site. The site-specific partition coefficients between sediment OC and water were 0.2−1.0 log units higher at the marine OC site, with the freely dissolved concentrations in the sediment pore-water 2−10 times lower, when compared with the terrestrial OC site. The stronger sorption at the site characterized with marine OC was most evident for the most hydrophobic PCBs, leading to reduced fluxes of these compounds from sediment to water. According to these results, future changes in OC cycling because of climate change, leading to increased input of terrestrial OC to the marine system, can have consequences for the availability and mobility of HOCs in aquatic systems and thereby also for the capacity of sediments to store HOCs.

Burial of persistent organic pollutants (POPs) such as polychlorinated biphenyls (PCBs) in deep-sea sediments contributes to 60% of their historical emissions. Yet, empirical data on their occurrence in the deep-ocean is scarce. Estimates of the deep-ocean POP sink are therefore uncertain. Hadal trenches, representing the deepest part of the ocean, are hotspots for organic carbon burial and decomposition. POPs favorably partition to organic carbon, making trenches likely significant sinks for contaminants. Here we show that PCBs occur in both hadal (7720–8085 m) and non-hadal (2560–4050 m) sediment in the Atacama Trench. PCB concentrations normalized to sediment dry weight were similar across sites while those normalized to sediment organic carbon increased exponentially as the inert organic carbon fraction of the sediment increased in degraded hadal sediments. We suggest that the unique deposition dynamics and elevated turnover of organic carbon in hadal trenches increase POP concentrations in the deepest places on Earth.

<p>The biogeochemistry of deep-sea trenches is strongly influenced by their V-shape topography and tectonic position in the ocean, leading to a focusing effect of sediment and organic matter into the trench centre. Recent findings showed elevated mineralization rates in trench sediments, suggesting both high carbon turnover and organic matter degradation rates. As persistent organic pollutants (POPs) favourably partition to organic matter, deep-sea trenches act as a sink for these substances. Composition, source and age of the organic matter have been shown to have a significant influence on contaminant dynamics in sediment from more shallow regions. Also, the trophic status of marine systems plays a significant role in transport of POPs from air to water and to sediment. However, knowledge about organic pollutants in deep-sea environments is scarce. In the present study, sediment samples from two deep-sea trenches with different trophic states and deposition regimes are analysed for POPs with a wide range of physicochemical properties. Concentrations will be compared between the semi-eutrophic Atacama and the oligotrophic Kermadec Trench. Sampling of sediment cores was performed at the slope, abyssal plain and trench at Atacama (depth between 2,500 and 8,000m) and at the abyssal plain and trench at Kermadec (depth of 6,000 and 9,600m). The total organic carbon content largely varied between 0.3 and 2.1% at different sites at the Atacama Trench, while values were more homogeneous at the Kermadec Trench (around 0.3%). Preliminary results from the Atacama samples demonstrate concentrations of PCBs at the pg g<sup>-1</sup> dw level, and indicate highest concentrations to occur at the highest depth in the trench. Low sedimentation- and high mineralization rates in the trench centre, as well as the funnel-effect from the topology may explain these differences.</p>

<p>Persistent organic pollutants (POPs) are ubiquitously present in the aquatic environment. They are hydrophobic substances that sorb to organic carbon (OC), and thus their environmental fate is closely linked to OC fluxes and pools. In this project, we test the hypothesis that future changes in the OC cycle can influence POP flux from air to sediment and reduce the POP sink in Baltic Sea sediments. The hypothesis relies on the assumption that the OC sorption capacity is affected by the relative contribution of terrestrial OC as well as the trophic status (oligotrophic versus eutrophic) of the area. Four different coastal sites were sampled, to capture different carbon regimes in terms of nutrient status and level of terrestrial OC influence. Concentrations of POPs were analysed along high-resolution sediment porewater- bottom water interface profiles, in total sediment, suspended matter collected in sediment traps and plankton, in the water column and in air. Stable carbon isotope signatures (δ<sup>13</sup>C) showed that the sites are different in terms of the influence of terrestrial organic matter, and the sites differ in nutrient conditions.</p><p>Preliminary results demonstrate that in general, sediments (three sites analysed) act as a source of PAHs to overlying water, whereas sediment and water more often are in equilibrium for PCBs, although there are variations for individual compounds. At the high nutrient-low terrestrial site, which was sampled at two different seasons, both air and water concentrations were higher for PAHs and PCBs in the autumn compared to the summer, indicating the importance of air as source of these contaminants to the water column. Accordingly, air seems an important source of PAHs to the water column in the low terrestrial-low nutrient site, as concentrations in the water column are increasing towards the water surface, whereas this was not observed for PCBs at the same site. Preliminary results from two contrasting sites in the Gulf of Finland, both with high nutrient levels but with different relative contribution of terrestrial OC, demonstrate higher total sediment concentrations of PAHs in the sediment with more marine OC, which was not observed as clearly for PCBs. Data from the water column indicate that marine OC is more efficient in sorbing POPs as air and water concentrations were similar at both sites, even though the OC vertical export at the high terrestrial site was more than double compared to the low terrestrial site. The full data set, will allow for further evaluation of hypotheses on the links between OC cycling and contaminant fate in the Baltic Sea.</p>